Abstract
Membrane reactors are attracting increasing attention for ultrapure hydrogen production from fossil fuel, integrating catalytic reaction and separation processes into one single unit thus can realize the removal of hydrogen or introduction of reactant in situ, which removes the thermodynamic bottleneck and improves hydrogen yield and selectivity. In this review, the state-of-the-art concepts for hydrogen production through membrane reactors are introduced, mainly including fixed bed membrane reactors, fluidized bed membrane reactors, and micro-channel membrane reactors, referring higher hydrocarbons as feedstock, such as ethanol, propane, or heptane; novel heating methods, like solar energy realized through molten salt; new modular designs, including panel and tubular configurations; ultra-compact micro-channel designs; carbon dioxide capture with chemical looping; multifuel processors for liquid and/or solid hydrocarbons; etc. Recent developments and commercialization hurdles for each type of membrane reactor are summarized. Modeling the reactor is fundamental to explore complex hydrodynamics in reactor systems, meaningful to investigate the effects of some important operating factors on reactor performances. Researches for reactor modeling are also discussed. Reaction kinetics for hydrocarbons reforming and reactor hydrodynamics are summarized respectively. Cold model is introduced to investigate physical phenomena in reactors.
Funding statement: Funding: Specialized Research Fund for the Doctoral Program of Higher Education of China (Grant/Award Number: “20130172110011”); China Scholarship Council (Grant/Award Number: “201406150038”); Guangdong Scientific Development Program (Grant/Award Number: “2013B010405001”).
Acknowledgements
Financial supports from the Guangdong Scientific Development Program (project # 2013B010405001), Specialized Research Fund for the Doctoral Program of Higher Education of China (project # 20130172110011), and China Scholarship Council are gratefully acknowledged.
Nomenclature
Latin symbols
- Ar
Archimedes number, –
- Ai
Arrhenius pre-exponential factor, units depend on the reactions
- Cep
Membrane permeation capacity (ratio of membrane surface area to thickness), [km]
- C0
Initial concentration of CH4, [mol m–3]
- Ceq
Equilibrium concentration, [mol m–3]
- Csj
Concentration of active sites on the surface for jth reaction, [mol m−2]
- Deff
Effectivity diffusion coefficient of hydrogen, [m2 s−1]
- dp
Average particle diameter, [m]
- Eact,Pv
Activation energy for the perovskite membrane, [J mol–1]
- Eact,I
Activation energy for ith reaction, [J mol–1]
- Ep
Activation energy for permeation, [J mol–1]
- g
Gravity acceleration rate, [m s–2]
- Gp core
Solids circulation flux in the core area of reactor [kg m–2 s–1]
- k
Pre-exponential factor, [mol km–1 h–1 Pa–0.5]
- ki
Reaction rate for ith reaction, [mol s–1]
- Kia(b)
Equilibrium constants for reversible reactions, –
- L0
Reactor length, [m]
- L
Reactor bed length, [m]
- n
Pressure order for membrane permeation, –
- nmol
moles in a conventional flow reactor, –
- NRep
Particle Reynolds number, –
- O/C
Oxygen to carbon ratio, –
- P
Reactor pressure, [Pa]
- Pe
Pecklet number, –
- Pm,Pv0
Permeability of the perovskite membrane, [mol cm–1 s–1 K–1]
- PMH2
Hydrogen partial pressures in membrane permeate side, [Pa]
- PO2,f
Partial pressure of O2 in the feed side, [Pa]
- PO2,p
Partial pressure of O2 in the permeate side, [Pa]
- PRH2
Hydrogen partial pressures in reactor side, [Pa]
- QH2
Hydrogen permeation rate, [mol h–1]
- QO2
Oxygen flux through a membrane, [mol cm–2 s–1]
- r
Reaction rate in Table 2, [mol s–1]
- rr
Reaction rate in membrane reactor for IE 2, [mol g−1 s−1]
- R
Gas constant, [J mol−1 K−1]
- R1
Inner radius of the reactor, [m]
- R2
Inner radius of the membrane tube, [m]
- Re
Reynolds number, –
- Sg
Surface area of catalyst, [m2 kg−1]
- S/C
Steam to carbon ratio, –
- T
Temperature, [K]
- tm,Pv
Perovskite membrane thickness, [m]
- u
Reactant velocity, [m s−1]
- U
Superficial gas velocity, [m s−1]
- Ucore
Superficial gas velocity in core area of the reactor, [m s−1]
- Umf
Minimum fluidization velocity, [m s−1]
- x
Distance in axial direction of reactor bed, [m]
- X
Molar fraction of each component, –
Greek letters
- μ
Fluid viscosity, [Pa s]
- ρ
Fluid density, [kg m−3]
- ρf
Gas density, [kg m−3]
- ρp
Particle density, [kg m−3]
- θ
Tapered bed angle, [°]
- ΔC
Concentration difference of H2, [mol m−3]
- Δρ
Density difference between fluid and solid, [kg m−3]
- ΔHo298
Enthalpy change, [kJ mol−1]
- ΔGi
Gibbs free energy for ith reaction, [mol s–1]
Abbreviations
- ATR
Autothermal reforming
- CLC
Chemical looping combustion
- CLR
Chemical looping reforming
- CSTR
Continuously ideally stirred tank reactor
- DIA
Digital image analysis
- FBMR
Fluidized bed membrane reactor
- ICFBMR
Internally circulating fluidized bed membrane reactor
- MA-CLR
Membrane-assisted chemical looping reforming
- MFBMR
Micro-structured fluidized bed membrane reactor
- PSA
Pressure swing adsorption
- PIV
Particle image velocimetry
- SMR
Steam methane reforming
- TCD
Thermal conductivity detector
- TCTMR
Thermally coupled two-membrane reactor
- TMAFBR
Tapered membrane-assisted fluidized bed reactor
- WGS
Water gas shift
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