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BY 4.0 license Open Access Published by De Gruyter May 21, 2022

Recent advancements in metal–organic frameworks integrating quantum dots (QDs@MOF) and their potential applications

Lopamudra Giri, Smruti Rekha Rout, Rajender S. Varma, Michal Otyepka, Kolleboyina Jayaramulu and Rambabu Dandela
From the journal Nanotechnology Reviews


Design and development of new materials and their hybrids are key to addressing current energy issues. Thanks to their tunable textural and physiochemical properties, metal–organic frameworks (MOFs) show great potential toward gas sorption, catalysis, sensing, and electrochemical energy applications. Nevertheless, practical applications of MOFs have been hampered because of their limited electrical conductivity, micropore size, and poor stability. However, smart integration of zero-dimensional quantum dots (QDs) into an MOF template, where the host structure offers suitable interactions for enhancing the stability and synergic properties, may be a solution. The objective of this review is to summarize recent advances in the field of QD@MOFs, highlighting fresh approaches to synthesis strategies and progress made in their application to optoelectronic devices, sensing, biomedical, catalysis, and energy storage. The current challenges and future directions of QDs@MOFs hybrids toward advancing energy and environmental applications are also addressed. We anticipate that this review will inspire researchers to develop novel MOF hybrids for energy, optoelectronics, and biomedical applications.

1 Introduction

Metal–organic frameworks (MOFs) have garnered tremendous attention from the research community, following the pioneering effort of Yaghi et al. that opened the floodgates to extending this field of research [1,2,3,4,5,6,7,8]. So far, the resounding success of these high surface area materials with tunable active sites has triggered infinite motivation for seeking newly fashioned materials with more unique properties that would meet current challenges [9,10,11,12,13,14,15,16,17,18]. Comprehensive research into MOFs regarding their distinctive behavior and their physical characteristics is frequently published [19,20,21,22,23,24,25]. The development and fabrication of MOFs into application-specific forms, such as nanostructures [26,27,28,29,30,31,32,33,34], reinforced membranes [35,36,37,38,39,40,41,42,43,44], and capsules [45,46,47,48,49,50,51,52,53] have become a subject of interest for researchers. MOF-based hybrid composites are also widely studied through mixing MOFs with several other materials, such as ceramics, natural polymers, nanomaterials, and proteins, which result in the evolution of novel well-designed products with improved functionalities [54,55,56,57,58,59,60].

Formally, zero-dimensional (0D) semiconductor nanocrystal materials comprising groups II–VI, III–V, or IV elements with a diameter of 2–10 nm are denoted as quantum dots (QDs) and have acquired considerable interest due to their excellent size-dependent tunable electronic properties and budding applications in the areas of sensing, catalysis, nano-medicine, and bio-imaging [61,62,63,64,65,66,67]. In most cases, this 0D material consists of core (e.g., InP, TiO2, GaAs, CdS)–shell (e.g., CdS ZnS, PbS, ZnO) structures encompassing a combination of a large number of atoms comprising mainly groups 12–16 (like ZnSe, ZnO, CdSe, etc.) or 13–15 (InP, InAs, etc.) [68,69,70,71,72,73]. Despite its several benefits, this form of QDs has a cytotoxic effect on live cells and tissues. To solve the shortcomings of traditional QDs, a new generation of QDs was designed, such as Si QDs, Ag2Se QDs, carbon dots (CDs), graphene QDs (GQDs), and perovskite. Recently, perovskite QDs have gained popularity in the field of electric and optoelectronics due to their adjustable bandgap, high light-absorption efficiency, high photoluminescence (PL) quantum yield, etc. [74,75,76,77]. Furthermore, these 0D materials can be simply modified by the surface modification method. Importantly, most of QDs are sustainable in aqueous systems and have coatings that comprise various functional groups, such as alcohols, amines, thiols, and carboxylic acids. Interestingly, a wide range of covalently conjugated molecules has been developed utilizing these functional groups. Moreover, because of the enormous surface area and quantum detention upshot, these materials have some advantages juxtaposed with traditional chromophores, such as extensive absorption bands, low photobleaching, thin and even emission bands, extended lifetimes, and high quantum yields [78,79,80,81,82]. Although QDs have excellent properties, the easy agglomeration of QDs leads directly to fluorescence quenching, which restricts their utilization in various fields [83,84,85,86]. Considerable effort has been invested in overcoming this hurdle, for example, passivation with an additional semiconductor film with a suitable bandgap, embedment of QDs with a variety of material (e.g., polymers or micelles), casing QDs with silica shell to harvest QDs@SiO2 composites, etc. [87,88,89,90,91,92,93,94,95]. However, all these methods are time-consuming and could lead to the formation of unwanted products or undesired behavior in the system. To provide QDs with multifunctional functionality, attempts to encapsulate these semiconductor nanoparticles and adjustable composite architectures must be investigated. Surprisingly, MOFs with high porosity and specific surface area provide an exciting platform, creating an ideal environment for loading QDs and preventing them from aggregation. At the same time, QDs enhance the physicochemical properties of MOFs. As a result, the amalgamation of QDs and MOFs results in good dispersion and great stability. In this context, MOF-derived QDs (QDs@MOF) have piqued curiosity and opened up a new avenue for a variety of applications [75,77,96,97,98,99,100]. These hybrid materials have captivating properties, such as outstanding PL, excellent biocompatibility, good mechanical/thermal stability, and relative simplicity of functionalization [101,102,103,104,105,106]. As displayed in Figure 1a, the number of papers on QDs@MOF has increased dramatically in recent years, particularly since 2016. A large variety of QDs@MOF materials have evolved, and their characteristics and intriguing applications have been studied ever since (Figure 1b). Although the research on QDs@MOFs is increasing (Table 1), there have been only a few review articles in this research field so far. In view of this flourishing research area, we have summarized the QDs@MOF fabrication strategy, its unique properties, and the wide-ranging applications, and we believe that this review will unfold the path toward newer innovative research and diverse applications.

Figure 1 
               (a) The number of journal articles published on QDs@MOF (source: ISI Web of Knowledge, 2010s to 2021); (b) the outline depicts recent advances in the creation of several QDs@MOFs.

Figure 1

(a) The number of journal articles published on QDs@MOF (source: ISI Web of Knowledge, 2010s to 2021); (b) the outline depicts recent advances in the creation of several QDs@MOFs.

Table 1

List of documented QDs@MOF, including the type of QDs and MOF, utilized their preparative methods and their potential applications in various fields

Sr. no. MOF QDs Method Application Ref.
1 Eu-MOFs CDs Bottle–ship Cr(vi) detection Sensing [124]
2 MIL-125(Ti) Ag2S/CdS/CuS QDs Photochemical deposition Cr(vi) reduction [114]
3 MIL-53(Fe) CDs Ship–bottle Cr(vi) reduction [133]
4 ZIF-8 CDs/AuNCs Ship–bottle Hg(ii) detection [134]
5 Eu-MOFs CDs Bottle–ship Hg(ii) detection [135]
6 Eu-MOFs N-doped CDs Bottle–ship Ag+ detection [136]
7 ZIF-8 CDs Bottle–ship Cu2+ detection [137]
8 UiO-66-NH2 CDs Bottle–ship Cu2+ detection [138]
9 ZIF-67 Polyethylene glycol (PEG)-capped ZnS QDs Bottle–ship Cu2+ detection [139]
10 ZIF-8 CDs Ship–bottle Fe3+ detection [140]
11 ZIF-8 Nitrogen-doped graphene QDs (N-GQDs) Ship–bottle Fe3+ detection [141]
12 Zn-MOFs CDs Ship–bottle Cu2+ and Fe3+ detection [142]
13 UIO-66-NH2 CDs Ship–bottle Cu2+ and quinalphos detection [138]
14 MOF‑5 CH3NH3PbBr3 QDs Ship–bottle Heavy metal ion detection [143]
15 In-MOFs CDs Bottle–ship Moisture and water detection in organics [144]
16 ZIF-365 CdTe QDs Ship–bottle l-Histidine and Cu2+ detection [125]
17 ZIF-8 CDs Bottle–ship Dopamine detection [126]
18 ZIF-8 Mn:ZnS Sol–gel Chlorpyrifos detection [145]
19 UiO-66 Amine-functionalized carbon QDs Ship–bottle 4-Nitrophenol detection [128]
20 HKUST-1 CDs Bottle–ship Catechol detection [127]
21 IRMOF-3 Nitrogen-doped CDs Ship–bottle Trinitrotoluene detection [146]
22 MOF-76 CDs Ship–bottle 2,6-Pyridinedicarboxylic acid detection [147]
23 MIL-101(Cr) GQDs Ship–bottle Benzene and toluene detection [148]
24 Cu-MOFs Carbon nitride QDs Ship–bottle Isoniazid detection [149]
25 IRMOF-3 N-GQDs Bottle–ship Procalcitonin detection [150]
26 ZIF-8 B-CDs/P-CDs Ship–bottle Triticonazole detection [151]
27 MOF-5 CdS QDs Bottle–ship Cardiac troponin I detection [152]
28 Fe(iii)-MIL-88B-NH2 ZnSe QDs Bottle–ship Antigen detection [112]
29 MIL-100(Fe) BNQDs Ship–bottle Antibiotics removal [153]
30 MIL-101(Fe) CDs Ship–bottle 6-Mercaptopurine detection [154]
31 ZIF-8 CdTe QDs Bottle–ship Oxidase activities detection [155]
32 UiO-66-NH2 BPQDs Template-assisted method Uranium extraction [106]
33 Zn-MOFs Graphitic carbon nitrides QDs Ship–bottle Riboflavin detection [156]
34 Zr-MOF CdTe QDs Ship–bottle Ascorbic acid detection [157]
35 ZIF-8 CDs Ship–bottle Ascorbic acid and ascorbate oxidase detection [158]
36 Zr-MOFs GQDs Bottle–ship Aflatoxins detection [159]
37 MIL-101(Cr) CdSe QDs Ship–bottle Alpha-fetoprotein detection [160]
38 ZIF-8 CDs Ship–bottle Quercetin detection [161]
39 Fe-BDC N, S-GQDs Drop casting Histamine detection [162]
40 Tb-MOF(MOF-76) Boric acid-modified CDs Ship–bottle 2,6-Pyridinedicarboxylic acid detection [147]
41 MIL-53 CDs Ship–bottle Diaminotoluene detection [163]
42 MIL-101-SO3H Amino-CQDs Ship–bottle 2,4-Dinitrophenol detection [164]
43 ZIF-8 CdTe QDs Bottle–ship NO detection [165]
44 UiO-66-(COOH)2 CDs Ship–bottle Temperature sensing [166]
45 Eu-MOFs N,S-CDs Bottle–ship Detection of water in organic solvents [167]
46 UiO-66-NH2 CDs Ship–bottle Water treatment membranes [168]
47 ZIF-8 GQDs Ship–bottle Removal of malachite green [55]
48 Ru-MOFs CdS QDs Drop casting Electrochemiluminescence sensor [120]
49 MIL-100(Fe) CdS QDs In situ consecutive chemical bath deposition Degradation of bisphenol [169]
50 MIL-53 Carboxymethylcellulose/graphene QDs matrix Bottle–ship Anticancer drug carrier Bio-medical [170]
51 MIL-68(In) Zn-Ag-In-S QDs Bottle–ship Screening of anticancer drug activity [171]
52 MIL-101-NH2 BPQDs Ship–bottle Photothermal therapy [131]
53 ZIF-8 GQDs Bottle–ship Chemo- and photothermal therapy [132]
54 ZIF-8 CDs Bottle–ship Drug delivery [129]
55 ZIF-8 DOX-MIPs Bottle–ship Drug delivery [130]
56 IRMOF-3 CDs Bottle–ship Drug delivery [172]
57 UiO-66-NH2 CDs Ship–bottle Bio-imaging [173]
58 ZIF-8 CdS QDs Bottle–ship Bio-imaging [174]
59 ZIF-8 CDs Ship–bottle Drug delivery [175]
60 UiO-66-NH2 CDs Bottle–ship Drug delivery [176]
61 ZIF-8 CDs Bottle–ship Photodynamic therapy [177]
62 ZIF-8 CDs Bottle–ship Monitoring of cell apoptosis [178]
63 [Zn(HCOO)3][C2H8N], Nitrogen-doped CDs (N-CQDs) Physical fusion Antimicrobial activity [179]
64 Cu-ZIF-8 CDs Bottle–ship Peroxidase mimics for assaying GSH [99]
65 PCN-224(Ni) CdS QDs Ship–bottle Hydrogen evolution Catalysis [180]
66 UiO-66 (UiOS-Cu) CdS/ZnS QDs Ship–bottle Hydrogen evolution [181]
67 PCN-222 and PCN-221 Pt/C QDs Ship–bottle Hydrogen evolution [182]
68 UiO-66-(SH)2 CdS QDs Ship–bottle Hydrogen evolution [183]
69 MIL-101 CdS, CDs Ship–bottle Hydrogen evolution [110]
70 NU-1000 CdS QDs Photo deposition Hydrogen evolution [86]
71 UIO-66-NH2 MoS2 QDs Direct deposition Hydrogen evolution [184]
72 La-MOFs CdSe QDs Direct surface functionalization Hydrogen evolution [185]
73 MIL-100(Fe) GQDs Ship–bottle CO2 reduction [186]
74 Zn-Bim-His GQDs Ship–bottle CO2 reduction [187]
75 MIL-125(Ti) g-C3N4/CuO Ship–bottle CO2 reduction [188]
76 ZIF-8/ZIF-67 CsPbBr3 QDs Bottle–ship CO2 reduction [189]
77 UIO-66(NH2) CsPbBr3 QDs Ship–bottle CO2 reduction [74]
78 PCN-221(Fe) MAPbI3 QDs Ship–bottle CO2 reduction [190]
79 Ni-MOFs Ti3C2 QDs Bottle–ship Nitrogen reduction [191]
80 Zn/Co bimetallic ZIF Co QDs Pyrolysis Oxygen reduction reaction [192]
81 CoNi-bimetallic MOF Ag QDs Ship–bottle Oxygen reduction reaction [97]
82 Ni-MOFs CDs Bottle–ship Oxygen evolution reaction [193]
83 Fe-MOFs Pt (1 1 1) Bottle–ship Electrocatalyst for water splitting [59]
84 UiO-66-NH2 GQDs Spray coating Photocatalyst [194]
85 UiO-66-NH2 GQDs Ship–bottle Photocatalyst [105]
86 ZIF-8 CDs Simple dispersion Photocatalyst [195]
87 ZIF-8 CdS QDs Ship–bottle Photocatalyst [196]
88 MIL-125-NH2 CdS QDs Ship–bottle Photocatalyst [107]
89 In-MIL-68 BiO QDs Ship–bottle Photocatalyst [197]
90 PCN-333(Fe) CsPbBr3 QDs Ship–bottle Photocatalyst [75]
91 NH2-UiO-66 Cs3Bi2I9 QDs Ship–bottle Photocatalyst [77]
92 UiO-66 S,N GQDs Ship–bottle Photocatalyst [198]
93 NH2-MIL-125(Ti) CDs Ship–bottle Photocatalyst [199]
94 MIL-101(Cr) SnO2 Ship–bottle Photocatalyst [200]
95 ZIF-8@MIL-68(In) ZnO QDs Calcination Photocatalyst [201]
96 Eu-MOFs CdTe QDs Direct surface functionalization Dye disintegration (Rh 6G) [202]
97 NTU-9 CdTe QDs Bottle–ship Dye disintegration (Rh 6G) [203]
98 UIO-66 CdSe QDs Ship–bottle Dye disintegration (RhB) [204]
99 MIL-125 CdSe QDs Physical fusion Dye disintegration (RhB) [119]
100 MIL-125- NH2 CDs Ship–bottle Dye disintegration (RhB) [205]
101 MIL-100(Fe) N-TiO2 QDs Physical fusion Dye disintegration (MB/RhB) [206]
102 Fe-MOFs CdSe QDs Bottle–ship Degradation of RhB [207]
103 ZIF-8 NDCQDs Ship–bottle Degradation of methylene blue [208]
104 Eu-MOFs CdTe QDs Bottle–ship Solar cell Energy storage [111]
105 Ni-MOFs Co9S8 QDs Intercalation Supercapacitor [118]
106 ZIF-8 ZnO QDs Co-electrospinning followed by carbonization Supercapacitor [209]
107 ZIF-8 Nb2O5 QDs Carbonization followed by hydrothermal treatment Supercapacitor [210]
108 ZIF-8 GQDs Bottle–ship Lithium-ion battery [211]
109 ZIF-8 ZnO QDs Physical fusion Lithium-ion battery [212]
110 UiO-66 SnO x QDs Ship–bottle Lithium-ion battery [213]
112 MOF-5 Ag2S QDs Physical fusion Lithium-ion battery [214]
113 Mo-MOFs MoSe2-MoO3 QDs Thermal induction Sodium-ion battery [215]
114 ZIF-8 VN QDs Ship–bottle Li–S batteries [104]
115 ZIF-8 CDs Bottle–ship Light-emitting diodes Opto-electronics [216]
116 Zr-MOFs CDs Physical fusion with a binding agent Light-emitting diodes [123]
117 Cd-MOFs CdTe QDs Direct surface functionalization Light-emitting diodes [117]
118 ZIF-8 CdSe x S1−x /ZnS QDs Ship–bottle Light-emitting diodes [217]
119 ZIF-8 CsPbX3 QDs Ship–bottle Light-emitting diodes [101]
120 EuW-MOFs CDs Bottle–ship Multiluminescent materials [218]
121 IRMOF-3 CdSe/CdS/ZnS QDs Physical fusion Photoluminescence [219]
122 Cu-MOFs Cu2SnS3 QDs Bi-sacrificial templates Nonlinear optics [220]

2 Fabrication strategy for QDs@MOF

Various fabrication strategies have been adopted for the synthesis of QDs@MOF over the last decade. Normally, the strategies comprise two customized methods, “ship-in-a-bottle” (ship–bottle) and “bottle-around-the-ship” (bottle–ship), and the additional two approaches are “photo deposition” and “direct surface functionalization” (Figure 2), which are deliberated in the following section.

Figure 2 
               Schematic representation of various approaches deployed for the preparation of QDs@MOF.

Figure 2

Schematic representation of various approaches deployed for the preparation of QDs@MOF.

2.1 Ship–bottle

The ship–bottle approach (Figure 2) involves the immobilization of small molecules or QDs precursors in the pore windows of MOFs followed by further treatment to attain the desired structure. Various methodologies, such as vapor deposition, solution infiltration, and solid-state grinding, have been employed to introduce QD precursors into MOFs, although precisely controlling the location, content, structure, and morphology of the incorporated guests is sometimes quite challenging. Based on the synthesis condition, the ship–bottle technique is further categorized into three types including “solution infiltration,” “chemical vapor infiltration,” and “double solution method.” In this context, Gao et al. [107] employed the abovementioned strategies and developed CdS QDs encapsulated in NH2-MIL-125 through two steps, including the addition of NH2-MIL-125 to TiO2 solution to acquire NH2-MIL-125@TiO2 and further inclusion of CdS QDs solution to as-synthesized solubilized NH2-MIL-125@TiO2 to form CdS/NH2-MIL-125@TiO2 (Figure 3a). Similarly, Gao et al. [108] prepared a SnO2@ZIF-8 composite by the immersion of ZIF-8 into the SnO2 QD precursors followed by the addition of hydrogen peroxide. Furthermore, Zhang et al. [109] used a thermal injection to combine UiO-67 and CsPbX3 QDs precursors to generate CsPbX3@UiO-67 at high temperatures (Figure 3b). A double-solvent technique has been successfully devised to avoid QDs’ aggregation on the exterior surface of MOFs. By using this technique, QDs precursors, which have smaller sizes than MOF pores, passed into the hydrophilic cavities of MOFs via capillary action and hydrophilic contact, thus reducing the amount of QDs deposited on the exterior part of MOF. In this context, Meng and colleagues [110] used a twofold solution approach whereby a small amount of glucose (G) and CdS QD precursor solution were co-infiltrated into the cavity of MIL-101, which resulted in the formation of G/CdS@MIL-101, further subjected to calcination at 200°C to obtain the ultimate product carbon nanodots (CDs)/CdS@MIL-101.

Figure 3 
                  (a) Graphical representation of the construction of CdS/NH2-MIL-125@TiO2 and corresponding SEM and TEM images [107]. (b) Designed fabrication strategy for CsPbBr3@Uio-67 composite formulation and accompanying structural diagrams [109]. (c) Synthesis scheme for CdS/NH2-MIL-125@TiO2 and antibody detection [112]. (d) Diagrammatic representation of the mechanism for photodeposition of Me
                      on MIL-125(Ti) [114]. (e) Illustrative representation of porphyrin-established MOFs with CdSe/ZnS core/shell QDs [116].

Figure 3

(a) Graphical representation of the construction of CdS/NH2-MIL-125@TiO2 and corresponding SEM and TEM images [107]. (b) Designed fabrication strategy for CsPbBr3@Uio-67 composite formulation and accompanying structural diagrams [109]. (c) Synthesis scheme for CdS/NH2-MIL-125@TiO2 and antibody detection [112]. (d) Diagrammatic representation of the mechanism for photodeposition of Me x S y on MIL-125(Ti) [114]. (e) Illustrative representation of porphyrin-established MOFs with CdSe/ZnS core/shell QDs [116].

It is worth noting that ship–bottle preparation procedures frequently rely on very extreme reaction conditions, such as elevated temperature and redox state, which might result in local network deterioration. This could also reduce the surface area of the MOF matrix, thus having a significant influence on applications that need porosity. However, the most significant advantage of this technology is to enable the creation of conformal MOF layers around QDs, which is a unique and demanding operation.

2.2 Bottle–ship

The bottle–ship strategy (Figure 2) is commonly known as the model synthesis methodology for QDs@MOF preparation. Following this method, QDs are initially produced and spread in a solvent-based stabilizer, such as a surfactant, to avoid agglomeration. Following that, MOF precursors are added to the solvent, which initiates MOF development around the QDs. During this process, organic linkages form divalent connections with capping moieties on the surface of the QDs. In this context, to develop a CdTe/Eu-MOF composite, Kaur et al. [111] employed CdTe QDs capped with cysteamine that were introduced to the Eu-MOF precursor solution, resulting in an ordered distribution of CdTe QDs in the Eu-MOF environment due to the interaction between the –COOH moieties of Eu-MOF and the –NH2 groups on the exterior section of the CdTe QDs. Similarly, Mo et al. [112] followed the same methodology and prepared Fe(iii)-MIL-88B-NH2@ZnSeQDs for antigen detection where the solution of a MOF precursor and ZnSe QDs were heated at 100°C (for 20 h) in a Teflon-lined reactor. The ultimate desired compound was obtained by subsequent cooling followed by centrifugation (Figure 3c). Furthermore, Wang et al. [113] employed a capped polyvinyl pyrrolidone agent, which not only maintained the firmness and distribution of the particles but also stimulated the formation of ZIF-8 on the surface, thus establishing an intimate heterogeneous assembly between them. Importantly, this method successfully lowers the quantity of the QDs accumulated on the exterior part of the MOFs by avoiding the diffusion impedance of the nanoparticles infiltrating into the environment of the MOFs. Furthermore, because nanoparticles may be agglomerated prior to the assembly of frameworks, the shape and dimension of QDs can be tailored for specific applications.

Unlike the ship–bottle and bottle–ship techniques, in which QDs were embedded in MOFs, the “photochemical-deposition” technique (Figure 2) involves depositing QDs on the exterior part of MOFs.

2.3 Photochemical deposition

The in situ synthesis and admission of QD particles into the exterior part of a MOF is aided by light in this method; photo-reduction of metallic precursors with a sufficient redox potential induces the production of QDs on the MOF surface. Direct binding with an appropriate linking group can be used to modify the surface area of MOFs with QDs. Utilizing this approach, Wang’s group [114] used UV light to create hybrid materials of MIL-125(Ti) accumulated by CdS, CuS, and Ag2S QDs. The mechanism of the photodeposition of Me x S y on MIL-125(Ti) is shown in Figure 3d. Similarly, Lin et al. [115] prepared a three-component hybrid material denoted as UiO-66/CdS/1% reduced graphene oxide, following the above-described method, and acquired significant results toward photocatalytic applications. The key drawbacks of this technology include two critical procedures to synthesize QD-MOF composites: first, it is the in situ synthesis and distribution of QDs on the interface of MOFs and, second, the adequate photoreduction potential to convert QD precursors to QDs, which might be tough at times.

2.4 Direct surface functionalization

Direct surface functionalization (Figure 2) is another tactic to suspend QDs on the interface of MOFs. The surface ligands of QDs are sequentially replaced with an appropriate capping group, which can establish direct interaction with MOF particles either by coordinative interaction or by some nonspecific contacts. The primary distinction between this strategy and the three preceding ones is that both MOFs and QDs are pre-designed prior to being assembled. Moreover, the key benefit of this type of synthesis includes the easy regulation of the form and size of QDs, as well as the construction of MOFs. To prepare porphyrin-based MOFs, Jin et al. [116] followed the abovementioned method and developed porphyrin-based MOFs with CdSe/ZnS QDs where the amino-functionalized QDs firmly adhered to the surface of the MOFs through zinc metal (Figure 3e). Similarly, employing the same strategies, Mondal et al. [117] prepared an MOF-functionalized cysteine-capped CdTe QDs, which functioned as a proficient white light-emitting phosphor material for display applications. In contrast to the previous three approaches, in this method, MOFs and QDs are pre-formed before being assembled. This approach has the advantage of enabling to control the shape and size of QDs as well as the morphology of MOFs.

2.5 Other synthesis methodologies

In addition, some other methods, such as intercalation [118], physical fusion [74,119] drop casting [120], and electrochemical depositions [121,122], have been developed for the preparation of QDs@MOF composites. The “physical mixing” approach is more simple and may be divided into two categories. The first one involves the use of physical force binding to combine QDs with MOFs, and the second one employs ultrasonic fusion. Utilizing the above-cited methods, Wang et al. [123] fabricated white light-emitting phosphor materials using carbon dots (CDs) and a Zr(IV)-MOF by physical fusion with a binding agent. Another extensively used technique is electrochemical deposition, which involves dispersing QDs in an electrolyte and depositing them on the interface of MOFs using an electric current. Recently, Chen et al. [106] adopted a slightly different tactic for the synthesis of UiO-66-NH2/black phosphorus QDs (MOF/BPQDs). The in situ synthesis of the composite was carried out on the carboxyl cellulose nanofiber (CNF) surface, which served as nucleation centers due to the presence of abundant carboxyl groups. The CNF aerogel shows high structural adaptability and little MOF erosion in BP@CNF-MOF, which demonstrates the reciprocal physical contact and involvement of CNFs, along with excellent binding affinities among MOF crystals and the CNF aerogel. According to the aforementioned methodologies, the techniques of embedding QDs within MOF matrixes are more effective than seeding MOF crystals with QDs. Not only does the encapsulation of QDs inside MOFs prevent QDs from covering MOFs, but it also inhibits QDs from clustering. In addition, after being encapsulated by MOFs, the robustness of QDs increases.

3 Application of QDs@MOFs

As a new functional hybrid material, QDs@MOFs hold greater stability, robust adsorption capacity, and unique intriguing properties, which make them ideal candidates for numerous applications. The applicability of QDs@MOFs in different fields (Figure 4), such as sensing, bio-imaging, energy generation, and energy storage, is detailed in this section and the applications of these new fields of interest are presented in Table 1.

Figure 4 
               A schematic representation of QDs@MOF for various captivating applications.

Figure 4

A schematic representation of QDs@MOF for various captivating applications.

3.1 Sensing

Sensors can help to improve the quality of life by aiding in medical diagnosis, increasing the efficiency of renewable resources, such as fuel cells and batteries, photovoltaics, pollution management, enhanced health, welfare, and security for people. Recently, QDs@MOFs have been considered attractive materials for fabricating different fluorescence sensors due to their high quantum yields, extended lives, outstanding photo-stability, and size-dependent emission wavelengths.

3.1.1 Metal ion detection

With the industrial growth, a large number of metal ions, for example, Pb2+, Fe3+, Cr2+, Cu2+, and Hg2+, have been discharged into water, destroying the water environment and posing a threat to human safety. As a result, the advancement of an effective metal ion detection technology is a precondition for heavy metal pollution prevention and management. Because of its high level of sensitivity, low detection limit, strong selectivity, broad detection array, quick response, decent anti-jamming capability, and simplicity of maneuver, metal ion detection using fluorescence-based QD biological sensors has recently drawn a lot of attention. For instance, Chen et al. [114] employed UiO-66-NH2/black phosphorus QDs (MOF/BPQDs) adorned on the CNF aerogel for uranium extraction from seawater (Figure 5a). The creation of a heterojunction between BPQDs and UiO-66-NH2 displays outstanding photocatalytic activity (Figure 5b), which efficiently kills marine bacteria by releasing a huge amount of reactive oxygen species. Similarly, to design a ratiometric fluorescence device for the recognition of Cr, Wang et al. [124] rationally developed CDs@Eu-MOFs (Figure 5c). Surprisingly, the synthesized CDs@Eu-MOFs outperform Cr(vi) in terms of excellent selectivity (Figure 5d(i)) in the presence of a wide range of metal ions (Na+, K+, Zn2+, Pb2+, NH4 +, Mn2+, Mg2+, Fe2+, Co2+, Ca2+, Cu2+, Fe3+, Hg2+, Al3+ Cr2O7 2−) with potentiometric detection of Cr(vi) under optimal circumstances, with a linear range of 2–100 µM and a low detection limit (LOD) of 0.21 µM (Figure 5d(ii)).

Figure 5 
                     (a) Under light irradiation, uranium adsorption capacity and elution efficiency in six consecutive cycles. (b) A schematic representation of the photocatalytic reduction of U(vi) utilizing MOF/BPQDs hybrid under solar-light irradiation [106]. (c) A schematic representation of the photocatalytic reduction of U(vi) utilizing MOF/BPQDs hybrid under solar-light irradiation. (d) The CDs@Eu-MOFs fluorescence selectivity spectra in the absence and presence of different metal ions [124].

Figure 5

(a) Under light irradiation, uranium adsorption capacity and elution efficiency in six consecutive cycles. (b) A schematic representation of the photocatalytic reduction of U(vi) utilizing MOF/BPQDs hybrid under solar-light irradiation [106]. (c) A schematic representation of the photocatalytic reduction of U(vi) utilizing MOF/BPQDs hybrid under solar-light irradiation. (d) The CDs@Eu-MOFs fluorescence selectivity spectra in the absence and presence of different metal ions [124].

3.1.2 Detection of biomolecules

Direct identification of biological systems, for example, an enzyme or an antigen, by means of a QDs@MOF probe should be more inventive for biological intuiting applications. Several studies have been conducted so far using QDs@MOFs for the detection of biomolecules. For example, Wang et al. [125] developed a CdTe QDs@ZIF-365 as a bi-functional ratiometric probe for highly subtle recognition of L-histidine and Cu2+ by adopting the post-synthesis strategy (Figure 6a). The experimental findings revealed that the CdTe QDs@ZIF-365 can be employed as an outstanding photo-luminescent probe for L-histidine and Cu2+ with a steep K sv (6.0507 × 108 [M−1] and 2.7417 × 107 [M−1]) value and low detection (Figure 6a). Similarly, Xie et al. [126] recently implemented LMOFs (luminous metal–organic frameworks) -CDs@ZIF-8 by incorporating blue-emitting CDs into ZIF-8 and employed it as a fluorescent sensor for highly sensitive and discerning recognition of dopamine (DA) (Figure 6b). The sustained pores in ZIF-8 not only provide free space for analytes but they may also selectively collect and intensify DA molecules through interactions between the analyte DA and the functional site of the framework. Furthermore, CDs can be used as signal probes to convert chemical signals from CD-analyte interactions into fluorescent signals. When compared to CDs, the CDs@ZIF-8 creates a novel sensing platform. As a result, the CDs@ZIF-8-based recognition technique for DA was shown to have a large concentration dynamic (0.1–200 M) and an LOD of 16.64 nM (Figure 6b and c). According to the findings, the produced QDs@MOF might be ideal probes for detecting cell biological properties and could be utilized as cell strength monitors and bio-probes.

Figure 6 
                     (a) The illustrative representation of fabrication of a CdTe QDs@ZIF-365 ratiometric fluorescence probe and its use for very delicate recognition of L-histidine and Cu2+ [125]; (b) diagrammatic representation of detection of DA through a possible mechanism. (c) FL emission bands of CDs@ZIF-8, with different DA concentrations [126].

Figure 6

(a) The illustrative representation of fabrication of a CdTe QDs@ZIF-365 ratiometric fluorescence probe and its use for very delicate recognition of L-histidine and Cu2+ [125]; (b) diagrammatic representation of detection of DA through a possible mechanism. (c) FL emission bands of CDs@ZIF-8, with different DA concentrations [126].

3.1.3 Recognition of other entities

QDs@MOFs have been investigated for the recognition of other materials. For example, Zhou et al. [127] developed a robust ultra-sensitive electrochemiluminescence sensor (CDs@HKUST-1) for the recognition of catechol. The results revealed that the definite surface area of HKUST-1 on CDs might significantly increase the sensor’s sensitivity. The as-synthesized sensor showed a varied linear range of 5.0109–2.5105 mol L−1 under ideal circumstances, with an LOD of 3.8109 mol L−1 (S/N = 3). Employing a post-synthetic modification method, Yang et al. [128] discovered an amine-CQDs@UiO-66 fluorescence probe by using amine-functionalized carbon QDs (amine-CQDs) in combination with UiO-66. In this investigation, UiO-66 was employed as an adsorbent to selectively collect and augment the target compounds. Here, the amine-CQDs were used as a template molecule to evaluate the connection between UiO-66 and the target compounds in a specific fashion and to subsequently convert these chemical reactions into recognizable fluorescence signals. As a result, QDs@MOFs provide a novel approach to creating hybrids with synergistic characteristics, fluorescence, and excellent durability for various sensing applications.

3.2 Biomedical

The unusual features (excellent biocompatibility, bioavailability, and renewability) of QDs@MOFs have attracted a lot of interest in the biomedical profession in recent years because, among other applications, they can be used for real-time tissue imaging (bioimaging), diagnostics, single-molecule probes, and medication administration. Herein, we have concentrated on two major biomedical applications: bioimaging and photothermal therapy.

3.2.1 Bioimaging

Bioimaging is a useful research strategy in contemporary biology and medicine that may quickly and easily offer clear and understandable biological information. Several investigations have shown that QDs@MOFs have great bioimaging capabilities due to their PL characteristics. For the first time, He et al. [129] used a straightforward two-step technique to create CDs and ZIF-8-based nanocomposites. The coordination contacts between Zn2+ ions and functional groups (–COOH/–N) on the CDs were reinforced to encase the CDs on the ZIF-8. The resulting CDs@ZIF-8 showed green fluorescence as well as being an excellent pH-receptive anti-cancer drug carrier and cell imaging (Figure 7a and b). According to in vitro cell studies, it has been corroborated that the nanocomposites exhibited excellent cyto-compatibility and could be endocytosed through cells for cell imaging and drug administration (Figure 7c). Furthermore, Qin and coworkers [130] recently developed a biodegradable nano-platform of molecularly imprinted polymer (MIP)-alleviated fluorescent ZIF-8 loaded with doxorubicin (DOX), (FZIF-8/DOX-MIPs) for drug delivery and imaging in a glutathione (GSH)/pH multi-stimulation system (Figure 7d and e). It is worth mentioning that CDs generate bright red fluorescence, allowing more precise tumor cell imaging. With time, the fluorescent gesture of FZIF-8/DOX-MIPs grew in the tumor location of mice. Furthermore, in an acidic tumor environment, the biological degradation of ZIF-8 and MIPs was favorable for drug release.

Figure 7 
                     (a) The picture of differential interference contrast. (b) Adopted 5-FU-encumbered C-dots@ZIF-8 with spot-like green fluorescence. (c) Cytotoxicity toward Hela cells in vitro [129]. (d) FZIF-8/DOX-MIP production and GSH/pH route of twofold stimulation and decay. (e) Graphical representation of tailored imaging and GSH/pH-receptive drug transport of FZIF-8/DOX-MIPs [130].

Figure 7

(a) The picture of differential interference contrast. (b) Adopted 5-FU-encumbered C-dots@ZIF-8 with spot-like green fluorescence. (c) Cytotoxicity toward Hela cells in vitro [129]. (d) FZIF-8/DOX-MIP production and GSH/pH route of twofold stimulation and decay. (e) Graphical representation of tailored imaging and GSH/pH-receptive drug transport of FZIF-8/DOX-MIPs [130].

3.2.2 Photothermal therapy

Photothermal treatment (PTT) using near-infrared (NIR) light for tumor hyperthermia ablation has been intensively explored in recent years and has sparked a lot of interest. PTT has fewer adverse effects than standard tumor treatment techniques because local heat may be properly regulated in temporal and spatial lobes. MOFs and other two-dimensional (2D) materials have recently been investigated as photodynamic agents (PTAs) for PTT applications in vitro and in vivo. When three-dimensional (3D) MOFs are converted into 2D sheets, the resulting MOF sheets may absorb a huge quantity of guest molecules via a noncovalent contact. Nevertheless, the poor photothermal renovation efficacy (PTCE) of 2D materials, as well as their considerable dimensional size, limits their practical application in PTT. As a result, there is a significant need for ultra-small PTAs with immense PTCE to attain a remarkable competence in photothermal tumor therapy. QDs@MOF materials, on the other hand, provide a suitable space for loading QDs and avoiding QD aggregation due to their large specific surface area and ordered pores. Furthermore, QDs help MOFs to acquire better physicochemical properties. The close heterojunction or interfacial contact between QDs and MOFs speeds up the transfer of electrons and efficiently prevents the recombination of photo-generated charges. In addition, the developed QDs@MOFs might be suitable PTAs because of their outstanding NIR adsorption and biocompatibility characteristics. For example, Liu et al. [131] employed an MOF hybridized with black phosphorus QDs (BPQDS) as a tandem catalyst to improve the treatment of hypoxic tumor cells (Figure 8a). The integrated MOF system was able to alter H2O2 to O2 in the MOF-alleviated catalase superficial layer, and then, O2 was introduced unswervingly into the MOF-sensitized BQ central, resulting in an excellent quantum yield of singlet oxygen. Remarkably, without catalase, the MOF system’s photodynamic treatment efficacy was 8.7 times higher after internalization, indicating an improved therapeutic impact besides hypoxic tumor cells (Figure 8b).

Figure 8 
                     (a) Stepwise construction of BQ-hybridized MOF catalyst and action toward hypoxic tumor cell treatment. (b) After being inoculated with BQ-MIL@cat-fMIL, time-dependent in vivo fluorescence images of a mouse carrying a subcutaneous HeLa tumor and after injection of BQ-MIL@cat-fMIL or BQ-MIL@fMIL in vivo fluorescence imaging evaluated the treatment upshot on mice malignant cells [131]. (c) Schematic representation of the development of ZIF-8/GQDs with the recapitulation of DOX. (d) After 8 h of incubation, cell viability study of 4T1 cells with and without free DOX, ZIF-8/GQD, and DOX-ZIF-8/GQD suspensions and deprived of 3 min NIR radiation [132].

Figure 8

(a) Stepwise construction of BQ-hybridized MOF catalyst and action toward hypoxic tumor cell treatment. (b) After being inoculated with BQ-MIL@cat-fMIL, time-dependent in vivo fluorescence images of a mouse carrying a subcutaneous HeLa tumor and after injection of BQ-MIL@cat-fMIL or BQ-MIL@fMIL in vivo fluorescence imaging evaluated the treatment upshot on mice malignant cells [131]. (c) Schematic representation of the development of ZIF-8/GQDs with the recapitulation of DOX. (d) After 8 h of incubation, cell viability study of 4T1 cells with and without free DOX, ZIF-8/GQD, and DOX-ZIF-8/GQD suspensions and deprived of 3 min NIR radiation [132].

These findings imply that QDs@MOFs will usher in a new era of tumor PTT. Tian et al. [132] employed a very simple one-pot technique to formulate a versatile manifesto for a symbiotic chemo- and photothermal therapy. They utilized ZIF-8 as drug nanocarriers where the implanted GQDs functioned as indigenous photothermal kernels (Figure 8c). When DOX was exploited, a prototypical anticancer drug, the findings revealed that the monodisperse ZIF-8/GQDs (size 500–1,000 Å) were able to capture DOX throughout the manufacturing phase and activate DOX discharge under acidic circumstances. The DOX-loaded ZIF-8/GQDs were able to readily transform NIR illumination into heat and, therefore, raise the temperature. When breast cancer 4T1 cells were used as a prototype biological system, the findings confirmed that combining chemo-thermal treatment and PTT with DOX-ZIF-8/GQDs had a substantial harmonious impact, leading to greater performance in killing cancer cells than the photothermal therapy and chemotherapy alone (Figure 8d). As a result, ZIF-8/GQDs might be useful as adaptable nanosystems in cancer treatment. These investigations revealed that QDs@MOFs have an extensive range of applications in biological and medical fields that are both benign and proficient.

3.3 Catalysis

Recently, tremendous progress has been achieved in the improvement of MOF-based QD materials as high competence catalysts/co-catalysts in catalysis systems, including GQDs, CDs, Se QDs, and Mxene QDs. In this context, QDs@MOFs are considered a promising catalyst/co-catalyst due to their tenability nature and robustness.

3.3.1 Electrocatalysis

Electrocatalysis is a highly advanced oxidation process (AOP) that has been extensively investigated in energy and conservational applications, such as the hydrogen reduction reaction, nitrogen reduction reaction (NRR), hydrogen evolution reaction (HER), methanol oxidation reaction, oxygen reduction reaction (ORR), and oxygen evolution reaction (OER). Among renewable-energy technologies, electrocatalytic applications are becoming highly indispensable. As a result of their outstanding characteristics, QDs@MOFs might play a significant part in the electrocatalytic processes. Despite the fact that many investigations have focused so far on the use of QDs in electrocatalysis, exploration of QDs@MOFs in electrocatalysis has just freshly come to the forefront. Zhou et al. [180] tested a unique MOF catalyst, CdS@PCN-224(Ni), and utilized it for HER in an acidic environment. The findings revealed a prodigious electrocatalytic performance with a Tafel slope of ∼91 mV dec−1, an overpotential of 120 mV, and a current density of 10 mA cm−2, which is nearly identical to the Pt/C (∼43 mV dec−1). CdS@PCN-224(Ni) has a double-layer capacitance (Cdl) of 9.75 mF cm−2, which is significantly higher than PCN-224 (2.33 mF cm−2) (Figure 9a and b). Similarly, fuel cells have been actively investigated among various energy conversion technologies because of their lower pollution levels, superior energy transformation proficiency, and fuel diversity. The oxygen reduction process, however, is significantly limiting the overall reaction efficiency of the fuel cells due to their essentially slow kinetics. In this context, Ye et al. [192] reported a new and simple approach for manufacturing ZIF-derived Co–N–C ORR catalysts by carefully regulating the rate of crystallization of ZIFs. The experimental evidence showed that in an alkaline medium, the Co–N–C catalyst has a high ORR activity (E 1/2 of 0.9 V), which can compete with commercial Pt/C (E 1/2 of 0.83 V) (Figure 9c and d). Similarly, a bifunctional electrocatalyst was prepared by Ye et al. [59] using a simple hydrothermal technique. Such highly permeable cuboids of Pt QDs@Fe-MOF material demonstrated excellent electrocatalytic activity toward HER, OER, and overall water splitting. Interestingly, in 1 M KOH, the electrocatalyst with exceptionally low Pt QD content (1.85 µg cm−2) only required an overpotential of 191 and 33 mV, respectively, to achieve a current density of 100 and 10 mA cm−2. Furthermore, the Pt QDs@Fe-MOF/NF (Ni foam) electrodes had exceptional potency, delivering a current density of 10 mA cm−2 at 1.47 V during at least 100 h of water splitting. These findings suggest that QDs@MOFs show promising potential in the realm of electrocatalysis; however, additional studies are warranted.

Figure 9 
                     (a) Overpotential of PCN-224, PCN-224(Ni), CdS@PCN-224, CdS@PCN-224(Ni), and Pt/C electrodes at the current density of 10 mA cm−3. (b) Tafel plots of PCN-224, PCN-224(Ni), CdS@PCN-224, CdS@PCN-224(Ni) and Pt/C [180]. (c) Illustrative representation of the imitation process of UF Co–N–C. (d) ORR efficiency in O2-saturated environment 0.1 M KOH electrolyte [192].

Figure 9

(a) Overpotential of PCN-224, PCN-224(Ni), CdS@PCN-224, CdS@PCN-224(Ni), and Pt/C electrodes at the current density of 10 mA cm−3. (b) Tafel plots of PCN-224, PCN-224(Ni), CdS@PCN-224, CdS@PCN-224(Ni) and Pt/C [180]. (c) Illustrative representation of the imitation process of UF Co–N–C. (d) ORR efficiency in O2-saturated environment 0.1 M KOH electrolyte [192].

3.3.2 Photocatalysis

Another proficient AOP, photocatalysis, has been extensively investigated and seems extremely promising for dealing with global energy and environmental concerns. In this context, QDs@MOFs are viewed as potential visible-light catalysts for assorted systems, namely photocatalytic CO2 reduction, H2 production, H2 reduction, pollutant degradation, and other applications in this domain. As an example, Liu et al. [186] illustrated the integration of GQDs on MIL-101(Fe) to create GQD/MIL-101(Fe)(G/M101) by employing a one-step solvothermal technique. With the use of MIL-101(Fe) and GQD sensitization, the photocatalytic reduction efficiency of CO2 to generate CO could be considerably improved. Experimental evidence revealed that the rate of CO generation over G/M101-5% (224.71 μmol h−1 g−1) is five times greater in comparison with MIL-101(Fe) (46.2 μmol h−1 g−1) (Figure 10a and b). Furthermore, photocatalytic nitrogen fixation is regarded as a potential strategy for obtaining high NH3 production, which is critical for human growth and industrial advancement. Nevertheless, because of the inert nature of nitrogen, it is important to investigate superior competence catalysts for nitrogen reduction. In this context, Qin et al. [191] used MXene QDs (Ti3C2-QDs) and a 2D nickel metalorganic framework (Ni-MOF), following a self-assembly approach, to increase the photocatalytic proficiency of the N2 reduction process. The optimum Ti3C2-QDs/Ni-MOF heterostructure produced a significant amount of ammonia (88.79 μmol  g cat 1  h−1) (Figure 10c). These findings provide space for further applications of QDs@MOF in photocatalysis.

Figure 10 
                     (a) Schematic representation for visible light-assisted reduction of CO2 over G/M101 nanocomposite. (b) Photocatalytic CO production by GQDs/MIL-101(Fe) [186]. (c) Diagrammatic representation of energy band positions, localized charge separation, and movement through the photocatalytic N2 reduction over Ti3C2-QDs/Ni-MOF [191].

Figure 10

(a) Schematic representation for visible light-assisted reduction of CO2 over G/M101 nanocomposite. (b) Photocatalytic CO production by GQDs/MIL-101(Fe) [186]. (c) Diagrammatic representation of energy band positions, localized charge separation, and movement through the photocatalytic N2 reduction over Ti3C2-QDs/Ni-MOF [191].

3.3.3 Photoelectrocatalysis (PEC)

PEC is a potent technology that combines heterogeneous photocatalysis with electrochemical methods. Extensive research has been conducted so far on the use of QDs@MOFs in PEC for water splitting. As a result of their unique characteristics, QDs@MOFs may have great application potential in PEC. Shi et al. [221] suggested that MOF-derived TiO2 can be used to boost the productivity of a TiO2-QDs established PEC system for hydrogen evolution. When compared to conventional TiO2 films, an MOF-impregnated TiO2 film stimulated by core–shell CdSe@CdS QDs demonstrated a +42.1% increase in the PEC device stability and a +47.6% increase in the PEC performance. The inclusion of mixed rutile/anatase phases enhances the performance by creating a promising band energy arrangement for the dissociation of photogenerated charges. Even though there are only a few studies on PEC with QDs@MOF-based materials, this approach is intriguing and should be given greater attention. These findings pave the way for QDs@MOFs being used in photocatalysis in the future.

3.4 Energy storage

In this twenty-first decade, increasing energy consumption, the depletion of fossil fuels, and growing concerns about industrial pollution have stimulated the improvement of eco-friendly technologies to create new alternative and renewable energy resources. In this context, QDs@MOFs are regarded as viable catalytic systems for energy storage devices because of their unique chemical, physical, and electrical features.

3.4.1 Batteries

With the advancement of science and technology, a great deal of focus has been placed on creating next-generation electrochemical energy storage technologies (a few examples are batteries, supercapacitors, solar cells, etc.). Because of their environmental friendliness and great energy density, batteries are the most frequently investigated electrochemical energy storage devices.

QDs@MOF-based materials have shown considerable promise for battery applications in recent years due to their better theoretical Li storage capacity, advantageous electrical conductivity, truncated functional voltage range, low dispersal fences for Li mobility, and outstanding mechanical characteristics. For instance, Saroha et al. [104] recently prepared multilayer porous N-doped C nanofibers encompassing vanadium nitride QDs and MOF-based hollow N-doped C nanocages for improved lithium–sulfur batteries as functional interlayers. The experimental findings revealed that because of the high sulfur concentration (80 wt%) and loading (ca. 4 mg cm−2) in the sulfur electrodes, the Li–S cell utilizing the novel nanostructured self-supporting interlayer displayed better rate proficiency and steady cycling recital (decay rate of 0.02%/cycle at 0.5 C). Interestingly, after 100 cycles of charging and discharging at 0.05 C, the Li–S cell provided a steady areal capacity of 5.0 mA h cm−2 despite an ultra-high sulfur loading of 11.0 mg cm−2 (Figure 11a–c). Zhang et al. [222] prepared ZIF-8/graphene oxide hybrids as anode materials for sodium-ion batteries. The capacity of the synthesized material was quite stable at 539 mA h g−1 at 100 mA g−1, 512 mA h g−1 at 200 mA g−1, and 456 mA h g−1 at 500 mA g−1 after 100 cycles. After 300 cycles, upon raising the current density to 1 A g−1, the capacity still attained 362 mA  g−1 (Figure 11d). This investigation revealed that QDs@MOF-based materials have the potential for developing high-performance electrode material in batteries.

Figure 11 
                     (a) Schematic illustration for the construction mechanism of N-CNF@VN/HNC. (b) Charge–discharge voltage profiles of (N-CNF@VN/HNC) at 0.05 C. (c) Rate capability analysis of (N-CNF@VN/HNC) at different C-rates [104]. (d) Galvanostatic charge/discharge profile (current density of 100 mA g−1) [222].

Figure 11

(a) Schematic illustration for the construction mechanism of N-CNF@VN/HNC. (b) Charge–discharge voltage profiles of (N-CNF@VN/HNC) at 0.05 C. (c) Rate capability analysis of (N-CNF@VN/HNC) at different C-rates [104]. (d) Galvanostatic charge/discharge profile (current density of 100 mA g−1) [222].

3.4.2 Supercapacitors

A supercapacitor, like batteries, is an imperative energy storage equipment that has the potential to be used in electric vehicles and other portable devices because of its extraordinary power density, firm charging/discharging capabilities, and extended life cycle. Due to their structural flexibility, excellent electrical conductivity, hydrophilic surface, and high surface area, QDs@MOFs have been extensively researched. These intriguing features may result in ultra-high volumetric capacitance as they provide quick electron transfer pathways and a huge electrochemically energetic surface for a quick and reversible faradaic reaction. Yang et al. [118] reported in situ formations of Co9S8 QDs in the interlayer of MOF-derived layered double hydroxide (LDH) nanoarrays for supercharged amalgamated supercapacitors. Remarkably, the selectively produced Co9S8-QDs displayed numerous active sites that enhanced the electrochemical characteristics, such as cyclic stability, capacitive performance, and electrical conductivity. Because of the mutually beneficial partnership, the composite material distributed an extremely high electrochemical capacity of 350.6 mA h g−1 (2,504 F g−1) at 1 A g−1. Moreover, blended supercapacitors produced with CF@NiCoZn-LDH/Co9S8-QDs and carbon nanosheets, enhanced by single-walled carbon nanotubes, had a remarkable energy density of 56.4 W h kg−1 at a power density of 875 W kg−1, with a capacity retention of 95.3% after 8,000 charging and discharging cycles. (Figure 12a and b). Similarly, Liu et al. [210] prepared a hybrid material, NQD-NC, made up of Nb2O5 QDs implemented on nitrogen-doped porous carbon imitative from ZIF-8 dodecahedrons, which showed excellent electrochemical enactment including ultrahigh energy and power density (76.9 W h kg−1 and 11,250 W kg−1, respectively) and longer cyclic firmness after 4,500 cycles with the retaining capacity of ∼85% at 5 A g−1 in a voltage range of 0.5–3.0 V (Figure 12c and d). In this investigation, QDs@MOFs were shown to be potential options for developing extraordinary recital supercapacitor devices.

Figure 12 
                     (a) Galvanostatic charge–discharge curves of NixCo3–xZn-LDH and CF@NiCoZn-LDH/Co9S8-QDs (current density of 5 A g−1). (b) The specific capacity and capacity retention rate of CF@NiCoZn-LDH/Co9S8-QDs (current densities of 1–20 A g−1) [118]. (c) AC/NQDs-NC HSC charge–discharge profiles (potential range of 0.5–3.0 V) at various current densities (0.2–5 A g−1. (d) Cycle performance of NQDs-NC HSC for around 4,500 cycles (current density of 5 A g−1) [210].

Figure 12

(a) Galvanostatic charge–discharge curves of NixCo3xZn-LDH and CF@NiCoZn-LDH/Co9S8-QDs (current density of 5 A g−1). (b) The specific capacity and capacity retention rate of CF@NiCoZn-LDH/Co9S8-QDs (current densities of 1–20 A g−1) [118]. (c) AC/NQDs-NC HSC charge–discharge profiles (potential range of 0.5–3.0 V) at various current densities (0.2–5 A g−1. (d) Cycle performance of NQDs-NC HSC for around 4,500 cycles (current density of 5 A g−1) [210].

3.5 Optoelectronic devices

The core and most fundamental component of optoelectronic technology is optoelectronic devices, and as the technology advances, a wide range of optoelectronics, such as optical switches, white light-emitting diodes (W-LEDs), solar cells, and lasers, are developed. In the limited range of visible light, MOFs are recognized as excellent luminous materials, whereas QDs are considered a suitable candidate for the preparation of white light-emitting devices due to their broad absorption range, high extinction coefficient, and high quantum yield. Many MOF-imitative QDs, such as GQDs, CQDs, perovskite QDs, and Mxene QDs, have recently been demonstrated to have exceptional electron donors and acceptors in their photoexcited states, making them interesting for deployment in optoelectronics. For example, Wang et al. [123] developed, by combining CDs with Zr(IV)-MOFs, a novel rare-earth free material that emits white light when excited at 365 nm, with a PL quantum yield of 37% in the solid state (Figure 13a). A CIE chromaticity coordinate of (0.31, 0.34) (Figure 13b and c), a luminous efficiency of 1.7 lm W−1, and a high color-rendering index (CRI) of 82 were achieved by dropping the CDs/Zr-MOF on a marketable UV LED chip.

Figure 13 
                  (a) Schematic representation of the construction of CDs/Zr-MOF. (b) Down-conversion WLED emission spectrum based on CDs/Zr-MOF coated on a 365 nm InGaN LED chip. (c) CIE chromaticity coordinates of (0.20, 0.22), (0.46, 0.47), and (0.31, 0.34) for the CDs LEDs, Zr-MOFs LEDs, and CDs/Zr-MOF WLEDs, respectively [123]. (d) Synthesis scheme of CsPbX3/MOF-5 composites. (e) PL spectrum of CsPbX3/MOF-5 WLED. (f) The CIE color coordinate triangle of CsPbBr3/MOF-5 (green), CsPbBr0.6I2.4/MOF-5 (red), and InGaN (blue) correlated with the National Television System Committee standard (white line) [76].

Figure 13

(a) Schematic representation of the construction of CDs/Zr-MOF. (b) Down-conversion WLED emission spectrum based on CDs/Zr-MOF coated on a 365 nm InGaN LED chip. (c) CIE chromaticity coordinates of (0.20, 0.22), (0.46, 0.47), and (0.31, 0.34) for the CDs LEDs, Zr-MOFs LEDs, and CDs/Zr-MOF WLEDs, respectively [123]. (d) Synthesis scheme of CsPbX3/MOF-5 composites. (e) PL spectrum of CsPbX3/MOF-5 WLED. (f) The CIE color coordinate triangle of CsPbBr3/MOF-5 (green), CsPbBr0.6I2.4/MOF-5 (red), and InGaN (blue) correlated with the National Television System Committee standard (white line) [76].

Ren et al. [76] employed a novel technique for solving the stability issues of CsPbX3 perovskite QDs by implanting CsPbX3 perovskite QDs into mesoporous MOF-5 crystals (Figure 13d). It has been observed that the CsPbX3/MOF composites have enhanced stability while keeping their excellent optical characteristics intact. The experimental findings revealed that, under 200 mA, CsPbX3/MOF-5 W-LED produced hot white light and the PL maximum was in agreement with the PL bands of the corresponding CsPbX3/MOF-5 (Figure 13e). From the CRI value (83) and luminous efficiency (21.6 lm W−1), it has demonstrated the excellent efficacy of CsPbX3/MOF-5 W-LED whereas the CIE color coordinate triangle of the CsPbX3/MOF5 W-LED comprehends 124% of the National Television System Committee standard (Figure 13f).

3.6 Other applications

In addition to the aforementioned uses, QDs@MOFs have shown high potential for other promising applications thanks to their exceptional characteristics. Biodegradable drug delivery transporters with long-term drug release properties are useful in cancer therapy because they help to reduce some of the adverse effects. In this context, Pooresmaeil et al. [170] developed a simple technique for fabricating MOFs inside a carboxymethylcellulose (CMC)/GQD matrix, which is utilized for anticancer drugs. The findings revealed that the MIL-53@CMC/GQDs may be offered as a viable drug delivery vehicle. Furthermore, it was observed that MIL-53@CMC/GQDs have greater DOX-loading capacity than MIL-53, as demonstrated by the pH-dependent DOX release behavior in drug release tests, showing meticulous release actions in vitro, which is in good agreement with the first-order kinetic model and the non-Fickian mechanism. The cytocompatibility of MIL-53@CMC/GQDs against the human cancerous cell lines was confirmed using a cytotoxic test (MDA-MB 231). Furthermore, by following a step-by-step bisacrificial template scheme, Zhu et al. [220] were the first to report a bimetallic sulfide QDs, Cu2SnS3 (CTS)-involved MOF nanosheets, CuBDC (BDC = 1,4-benzenedicarboxylate). According to a Z-scan investigation conducted under the illumination of a 532 nm laser, the CTS@CuBDC film exhibited significant optical limiting (OL) performance and precise truncated OL thresholds (0.92 J cm2), along with high third-order nonlinear susceptibility (1.9 × 10−6 esu). This research shows that the new methodical approach (bisacrificial templates) to producing metal sulfide QD-distributed MOF hybrid composites is interesting and practical and might be a good option for nonlinear optical applications.

4 Conclusions and prospects

In this article, we have presented a comprehensive overview of advancements in QDs@MOF hybrids, covering synthetic techniques, structures, and applications. The produced QDs@MOF hybrid demonstrated improved stability as well as novel characteristics and application potential. Recently, QDs@MOFs have gained popularity because of their remarkable physicochemical and optical–electrical characteristics and are therefore considered a cutting-edge branch of materials. Various methodologies have been adopted by which QDs@MOFs endowed with a diversity of exclusive properties, such as exceptional PL characteristics, high selectivity to target analytes, or biocompatibility, can now be prepared. Furthermore, QDs@MOFs may be employed in a broader range of applications, including catalysis, sensing, bioimaging, optoelectronics, and batteries. Despite these amazing results, a number of obstacles illustrated in Figure 14 must be addressed to encourage further progress in this field.

  1. The most straightforward way to adjust the characteristics of QDs@MOFs to specific applications is using the appropriate synthesis process. Many investigations have revealed that QDs@MOFs can be synthesized via a variety of methods. The ship–bottle/bottle–ship techniques are the most frequent in QDs@MOF synthesis, whereas photochemical decomposition/direct surface functionalization has received less attention. As a result, it is worthwhile to put more effort into QDs@MOF synthesis.

  2. Controlling the morphology and surface properties of QDs@MOFs remains a daunting task. As a result, various experimental parameters, such as temperature, reaction duration, solvent impact, and reaction device, should be used more thoroughly to identify the growth mode. This can result in an MOF-based hybrid QD material with better morphologies and surface functionalization.

  3. This field is still in its infancy and may not be appropriate for industrial manufacturing on a large scale. As a result, novel synthetic methodologies must be developed that will be not only cost-effective in terms of laboratory research but also suitable for massive commercial applications.

  4. Many studies have shown that QDs@MOFs exhibit outstanding fluorescence behavior, photonic, photothermal transformation, and photoelectronic characteristics in tests. Even though these features of QDs@MOFs have been already demonstrated, there are still challenges to address. Right away, attention should be focused more on improving their current qualities and expanding these properties to other study domains. In this context, the combination of theoretical models and actual experiments will lead to successfully investigating novel QDs@MOFs with new and better properties.

  5. Based on the categories of QDs@MOFs, it has been observed that most works were conducted employing CdS, CdSe, CdTe, GQDs, etc., meaning that other QD materials should be paid greater attention to. MXene QDs, for example, have attractive features and have shown to be useful in energy production, catalysis, and sensing owing to extremely sensitive surface terminations. As a result, MXene QDs@MOF advancement is extremely desirable.

  6. The majority of MOF hybrid QD materials addressed thus far were made of MOFs and single-QD materials. As a result, numerous different materials or MOFs coupled with some other MOFs deserve further investigation.

  7. Although a great deal of research has been done on QDs@MOF materials due to their versatile nature, their application is still a long way off. Solar cells, for example, are an important part of the solution to the worldwide energy crisis. Up to date, many resources have been investigated in the field of solar cells; nonetheless, certain drawbacks, such as short service life, low energy efficiency, or higher cost, have severely hampered their practical applicability. In the meantime, numerous studies have shown that QD-based materials are promising prospects for solar cell applications. Therefore, it is worth putting extra effort into investigating the use of QDs@MOFs in solar cells.

  8. Furthermore, diverse hybridized QDs@MOFs enable a wide range of electrochemical applications, whereas studies related to NRR are rarely conducted.

  9. Importantly, more research into the applicability of QDs@MOF-based immunosensing is required. Since there has been some research on bio(sensing)-based QDs@MOFs, more methodologies and unique protocols for the identification of cell cultures and cancer biomarkers should be developed.

  10. The relevance of hybrid materials for applications requiring NLO characteristics, upconversion, and lasing has already been emphasized by the available results. Nevertheless, this is still a relatively new and developing field of study, and factors impacting, e.g., the higher-order nonlinear optical features of QDs@MOF materials should be analyzed in an unswerving manner.

  11. Currently, the preparation of perovskite-based MOF hybrid materials is a hot topic due to their various intriguing applications [223,224], but the eco-toxicity of heavy metal ions is a key problem for lead perovskites. As a result, additional effort must be invested in the future in investigating and developing novel nontoxic and environmentally acceptable materials for the perovskite@MOF composite.

Figure 14 
               QDs@MOF: challenges and opportunities.

Figure 14

QDs@MOF: challenges and opportunities.

In general, we have presented some of the most recent research findings of QDs@MOF. This study aims to provide in-depth knowledge about the variety of synthesis, characteristics, and uses of QDs@MOF, alongside stimulating future research into these new and fascinating domains. Despite the significant accomplishments, there are still some basic and technological gaps and obstacles in this area and, therefore, considerable effort should be put into the exploration of novel preparation techniques, physicochemical characteristics, and prospective applications. The abovementioned concerns must be addressed to stimulate continued progress in the synthesis and implementation of new QDs@MOF hybrids, which will have a substantial influence on chemistry, material science, and a broad range of applications.


The authors acknowledge ICT-IOC, Bhubaneswar, for providing necessary support. Rambabu Dandela thanks DST-SERB for the Ramanujan fellowship (SB/S2/RJN-075/2016), Core research grant (CRG/2018/000782), and ICT-IOC startup grant. MO gratefully acknowledges the support of the Ministry of Education, Youth and Sports of the Czech Republic and the Operational Programme for Research, Development and Education of the European Regional Development Fund (Project No. CZ.02.1.01/0.0/0.0/16_019/0000754) K. J. R. acknowledges support from the Indian Institute of Technology Jammu for providing a seed grant (SGT-100038) and SERB SRG/2020/000865.

  1. Funding information: DST-SERB for the Ramanujan fellowship (SB/S2/RJN-075/2016), Core research grant (CRG/2018/000782), and ICT-IOC startup grant. Ministry of Education, Youth and Sports of the Czech Republic and the Operational Programme for Research, Development and Education of the European Regional Development Fund (Project No. CZ.02.1.01/0.0/0.0/16_019/0000754) K. J. R. acknowledges support from the Indian Institute of Technology Jammu for providing a seed grant (SGT-100038) and SERB SRG/2020/000865.

  2. Author contributions: All authors have accepted responsibility for the entire content of this manuscript and approved its submission.

  3. Conflict of interest: The authors state no conflict of interest.


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Received: 2021-12-17
Revised: 2022-03-13
Accepted: 2022-04-05
Published Online: 2022-05-21

© 2022 Lopamudra Giri et al., published by De Gruyter

This work is licensed under the Creative Commons Attribution 4.0 International License.