Recent Advances in Membrane-Based Electrochemical Hydrogen Separation: A Review
Abstract
:1. Introduction
2. Hydrogen Separation/Purification Technologies
2.1. Pressure Swing Adsorption
2.2. Cryogenic Distillation
2.3. Membrane Technologies
2.3.1. Porous Membranes
2.3.2. Dense (Non-Porous) Membranes-Diffusion Mechanism
2.3.3. Ceramic Proton-Conducting Membranes
- H2 gas diffusion to reaction sites on the surface of the feed side;
- H2 adsorption, dissociation, and charge transfer at the membrane surface;
- Proton reduction and hydrogen re-association at the membrane surface
3. Electrochemical Hydrogen Separation
- Hydrogen, in the form of protons, is selectively transferred through the proton-conducting electrolyte;
- one-step operation provides pure hydrogen;
- the hydrogen separation rate can be controlled by the current (Faraday’s Law);
- a high hydrogen collection rate is achieved;
- simultaneous purification and compression of hydrogen is possible, in principle;
- high hydrogen separation is achieved at low cell voltages, with a high separation efficiency [156] and
- high selectivity and low permeability results in pure hydrogen (up to 99.99 vol.%) [159].
3.1. Working Principle
3.2. Current Status of Electrochemical Hydrogen Separation Technology
3.2.1. Low-Temperature EHS
“Passive” Gas Mixtures
- H2/CH4 Mixtures
- H2/Ar Mixtures
- H2/N2 Mixtures
- H2/CH4/Ar
- H2/CH4/Ethylene
“Active” Gas Mixtures
- CO and CO2-Containing Mixtures
3.2.2. High-Temperature EHS
“Passive” Gas Mixtures
- H2/CH4 Mixtures
“Active” Gas Mixtures
- CO and CO2-Containing mixtures
- H2/NH3 Mixtures
3.2.3. Review Articles
3.2.4. Overall Summary of the State of Electrochemical Hydrogen Separation
- High selectivity;
- sensitivity to catalyst deactivation (e.g., CO deactivation);
- higher tolerance to “active” impurities (e.g., CO and CO2) at higher temperatures;
- the hydrogen flux can be controlled by the current and
- simultaneous hydrogen separation and compression is possible.
4. Concluding Remarks
- Little information on component degradation, beside CO catalyst deactivation. However, the degradation studies performed on fuel cells can be used to fill this gap.
- Understanding the life cycle of an electrochemical hydrogen membrane and how an aged membrane’s performance compare to that of a membrane at the beginning of its life.
- Contribution/s of various impurities (considered separately) to the performance parameters. Impurities that commonly accompany hydrogen streams generated from various traditional hydrogen generation methods include CH4, O2, N2, CO, CO2, H2S, benzene, toluene, xylene and NH3. However, as is evident from Table 4, research articles are only available on EHS from mixtures containing CO, N2, CO2, CH4, Ar, ethylene and H2O. Furthermore, HT EHS research mainly included reformate gases. Hence, the contribution of respective impurities, separately, on the performance parameters is largely unknown.
- Further research into HT EHS. From Table 4, it is evident that more information is available on LT separation than HT separation. Further research is required to achieve a broader understanding of the expected extent of separation with respect to the various performance parameters—such as limiting currents, hydrogen recovery, selectivities and fluxes.
- One of the advantages that HT membranes present is the possibility of being able to use catalysts such as iron and cobalt. More information on this topic is required in efforts to determine how beneficial this would be—besides only focusing on the cost reduction.
- Fuel cell application. To date, no studies appear to have been conducted to verify the hydrogen purity of EHS product streams for fuel cell application. Such knowledge could be very beneficial, especially when simulated reformate streams are used from industrial hydrogen production systems.
- EHS from industrial hydrogen streams produced from fuel cells (e.g., product streams from steam methane reforming, partial oxidation and gasification of biomass and coal)
- Simultaneous EHS and electrochemical hydrogen compression, together with the process efficiency in terms of hydrogen purity, hydrogen compression, overall efficiency, etc. Specifically, the simultaneous EHS and compression from H2/CO2 streams, where both the hydrogen stream (permeate) and the carbon dioxide (retentate) is purified and compressed. Such study will be beneficial in terms of hydrogen production and CO2 sequestration (i.e., carbon capture and storage, and even carbon capture and utilization).
- Proton-conducting ceramics could be considered a new and upcoming technology and is also part of EHS. The authors suggest that future reviews be done, similar to the one presented, on this topic.
Author Contributions
Funding
Institutional Review Board Statement
Informed Consent Statement
Conflicts of Interest
References
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Method | Advantages | Disadvantages | TML * | PE ** (%) | Cleanness *** | Impurities | References |
---|---|---|---|---|---|---|---|
Reforming: | |||||||
SMR a | Most developed industrial process, lowest cost, existing infrastructure, high efficiency, best H2/CO ratio | Highest air emissions, system is complex, system is sensitive to natural gas quantities. Capital, operation, and maintenance cost. Fossil fuel feedstock. | 10 | 65–75 | NC/CCS | CO2, CO, CH4, N2 | [2,3,46,55,59,60,61,65,68,75,76,77,78,79] |
POX c | Well-established. Variety of fuels, reduced desulphurization requirement, no catalyst required | Complex handling process, high operating temperature, low H2/CO ratio. Fossil fuel feedstock | 7–9 | 50 | NC | CO, CO2, H2O, CH4, H2S, COS and sometimes CH4 | [46,60,61,65,66,78,80] |
ATR b | Lower temperatures than POX c, Requires less oxygen than POX c | Limited commercial application, required air or oxygen. Fossil fuel feedstock. | 6–8 | 60–75 | NC | CO, CO2, N2, CH4 and sometimes Ar | [60,81] |
Gasification: | |||||||
Coal | Abundant and affordable, Low-cost synthetic fuel in addition to H2 | Reactor costs, system efficiency, feedstock impurities, significant carbon footprint unless CCS is used. Separation and purification of gas products are difficult [82]. Fossil fuel feedstock (coal gasification). Season limitations and heterogeneity (biomass) | 10 | 74–85 | NC/CCS | N2, CO2, CO, CH4, H2S | [79,83,84,85] |
Biomass | 3 (R&D) | 35–50 | NC/CCS | COx, SOx and CH4 | [2,78,84,86,87] | ||
Electrolysis: | |||||||
Water electrolysis | Simplicity of process design, compactness, renewable feedstock, cost effective way to produce hydrogen locally. Does not involve moving parts. Silent operation. | Energy input is required and it is more costly than fossil-fuel alternatives. | 9–10 | 62–82 | C | H2O | [2,66,67] |
Constituent | Limits (μmol·mol−1 Unless Stated Otherwise) | Minimum Analytical Detection Limit |
---|---|---|
Hydrogen fuel index | >99.97% | |
Water a | 5 | 0.12 |
Total hydrocarbons b (C1 basis) | 2 | 0.1 |
Oxygen | 5 | 1 |
Helium | 300 | 100 |
Nitrogen, Argon | 100 | 5 |
Carbon dioxide | 2 | 0.1 |
Carbon monoxide | 0.2 | 0.01 |
Total sulphur c | 0.004 | 0.00002 |
Formaldehyde | 0.01 | 0.01 |
Formic acid | 0.2 | 0.02 |
Ammonia | 0.1 | 0.02 |
Total halogenates d | 0.05 | 0.01 |
Particulate concentration | 1 mg·kg−1 | 0.005 mg·kg−1 |
Properties | PSA | Membranes | Cryogenic |
---|---|---|---|
Min. feed purity (vol.%) | >40 | >25 | 15–80 |
Product purity (vol.%) | 98–99.999 | >98 | 95–99.8 |
Hydrogen recovery (%) | Up to 90 | Up to 99 | Up to 98 |
Year | Type | Membrane | Catalyst * | Impurities | Temp. (°C) | Refs. |
---|---|---|---|---|---|---|
2004 | Experimental | Nafion | Pt (B) | N2, CO2 | 30–70 | [166] |
2005 | Review | N/A | N/A | N/A | N/A | [167] |
2007 | Experimental | Nafion | Pt (A), Ru (C) | CO, CO2 | 20 | [156] |
Experimental/modelling | Nafion | Pt/Pt-Ru (B) | Ar, CH4 | 20–70 | [168] | |
Simulation | N/S ** | N/S ** | N2 | 25, 60 | [169] | |
2008 | Experimental | Nafion | Pt (B) | N2 | 25, 60 | [170] |
Experimental | PBI | Pt (B) | CO, CO2, N2 | 120–160 | [49] | |
2009 | Experimental/modelling | Nafion | Pt (B) | Ar/C2H4 | 25 | [171] |
Experimental | N/S ** | N/S ** | N2/CO2 | 60 | [172] | |
2010 | Experimental | PBI | N/S ** | N2; CO2, CO, CH4; N2,CO2, CO | 160–180 | [93] |
2011 | Experimental | Nafion | Pt/C (B) | CO2, H2O | 50–70 | [173] |
Experimental | Nafion | Pt (B) | N2 | 35, 55, 75 | [161] | |
Experimental | Nafion | Pt (B) | Ar | 20–70 | [159] | |
2012 | Experimental | Nafion | Pt/C, Pd/C (B) | CO2 reformate | 30–50 | [160] |
2013 | Experimental | PBI | Pt(B) | CO2 | 80, 160 | [174] |
2014 | Experimental | PBI | Pt (B) | Simulated reformate: N2, CO | 140–160 | [175] |
Experimental | Nafion | Ir/C (B) | Ar, CO2 | 25, 70 | [176] | |
2016 | Experimental | Nafion | N/S ** | CO2, CO, CH4 | 25–75 | [177] |
Experimental | SPPESK, Nafion | Pt (B) | CO2 | 20–60 | [178] | |
2018 | Experimental | Nafion | Pt-Ru (A), Pt (C) | CO2 | 25, 50 | [179] |
2019 | Experimental/modelling | Nafion | N/S ** | N2, CH4, He, CO2 | 28 | [180] |
Experimental | Nafion | N/S ** | N2, CO2 and air | 15–22.5 | [181] | |
Experimental case study: MEMPHYS (Membrane based purification of hydrogen system) system | N/S ** | N/S ** | N2 | 35 | [97] | |
2020 | Experimental | PBI | Pt (B) | N2, CO | 160–200 | [182] |
Experimental/modelling | Nafion | Pt/C (B), Pt-Ru/C (A) and Pt/C (C), Pt-Ni/C (A) and Pt/C (C) | CO/Ar; N2 | 35 | [183] | |
Experimental/modelling | Nafion | Pt/C (A), Pt-Ru/C (A) and Pt-Ru(C) | CO; CO2, CH4, CO, H2S | 35 | [184] | |
Case study/modelling | N/A | N/A | H2,N2 and CO2 | N/A | [185] | |
Review | N/A | N/A | N/A | N/A | [186] | |
Review | N/A | N/A | N/A | N/A | [187] | |
2021 | Experimental | TPS | Pt-Co/C (A) and Pt/C (C) | CH4, CO2, and NH3 | 120–160 | [188] |
Gas | Composition [%] | |||
---|---|---|---|---|
SPPESK-0.71 | Nafion 115 | Nafion 212 | Nafion/PTFE | |
H2 | >99.99 | >99.99 | 99.79 | 99.25 |
CO2 | <0.01 | <0.01 | 0.21 | 0.75 |
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Vermaak, L.; Neomagus, H.W.J.P.; Bessarabov, D.G. Recent Advances in Membrane-Based Electrochemical Hydrogen Separation: A Review. Membranes 2021, 11, 127. https://doi.org/10.3390/membranes11020127
Vermaak L, Neomagus HWJP, Bessarabov DG. Recent Advances in Membrane-Based Electrochemical Hydrogen Separation: A Review. Membranes. 2021; 11(2):127. https://doi.org/10.3390/membranes11020127
Chicago/Turabian StyleVermaak, Leandri, Hein W. J. P. Neomagus, and Dmitri G. Bessarabov. 2021. "Recent Advances in Membrane-Based Electrochemical Hydrogen Separation: A Review" Membranes 11, no. 2: 127. https://doi.org/10.3390/membranes11020127