Construction of efficient and stable low-temperature reverse-bias bipolar membrane electrolyser for CO2 reduction

doi:10.1016/S1872-2067(23)64636-4

Abstract

Abstract:

Electrochemical conversion of CO₂ and H₂O to value-added products is an attractive approach for sustainable chemical production. Significant progress has been made in the past few decades in improving activity and selectivity, advancing this technology to practical application. Considering the next step for the electrochemical CO₂ reduction reaction, improving carbon utilisation efficiency, stability, and energy efficiency are essential. Bipolar membrane (BPM)-based electrolysers, which allow electrodes to be operated under different pH, are advantageous to tackle the challenge mentioned above. Herein, we introduced the current status of CO₂ electrolysers, followed by configuration, challenges, progress and outlook for combining reverse-bias BPM with different types of electrolysers. Our aim is to provide insight into developing carbon-efficient and energy-efficient CO₂RR systems towards practical application.

Key words: Carbon dioxide reduction, Electrocatalysis, Bipolar membrane, Carbon utilisation, Energy efficiency

Yi Xie, Zhanyou Xu, Qian Lu, Ying Wang. Construction of efficient and stable low-temperature reverse-bias bipolar membrane electrolyser for CO₂ reduction[J]. Chinese Journal of Catalysis, 2024, 59: 82-96.

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URL: https://www.cjcatal.com/EN/10.1016/S1872-2067(23)64636-4

https://www.cjcatal.com/EN/Y2024/V59/I4/82

Figures/Tables 10

Table 1 Performance of recently reported CO2 electrolyser with current density higher than 100 mA cm-2.

Catalyst	Membrane	j_total (mA cm^-2)	Major product	FE of major product (%)	Stability (> 90% retention)	SPCE of major product (%)	EE of major product (%)	Ref.
SS-Cu	BPM	300	C₂₊	52	1000 h	N/A*	18.2	[22]
Cu-PTFE	BPM	300	C₂₊	65	14 h	69	17	[23]
Cu NPs	BPM	200	C₂H₄	42	40 h	12	12	[24]
Ag NPs	BPM	100	CO	65	24 h	N/A	24	[25]
[Ni(CycCOOH)]²⁺	BPM	100	CO	33	N/A	N/A	9.5	[26]
Sputtered Ag	BPM	200	CO	50	N/A	9	14	[27]
SSC@Cu NPs-Cu PTFE	CEM	1200	C₂₊	45	12 h	50	N/A	[28]
Cu-TE	CEM	1000	C₂₊	55-60	68 h	N/A	N/A	[29]
Cu-Pd	CEM	500	C₂₊	87	4.5 h	60	N/A	[30]
COF:PFSA/Cu-PTFE	CEM	200	C₂₊	75	10 h	75	25	[31]
CuBaO_x	AEM	400	EtOH	61	20 h	N/A	N/A	[32]
F-Cu	AEM	1600	C₂H₄	65	N/A	2.6	N/A	[4]
SSC@Cu-PTFE	AEM	1500	C₂H₄	65-75	< 1 h	2.7	N/A	[12]
Cu-Mg	AEM	1000	C₂H₄	70	48 h	1.8	N/A	[33]
N-arylpyridinium @Cu-PTFE	AEM	120	C₂H₄	64	190 h	< 1	20	[34]
Cu(100)	AEM	120	C₂H₄	55.8	4.5 h	1.7	26.4	[35]
Cu(100)	AEM	500	C₂₊	70	2.5 h	13.2	N/A	[35]

Fig. 1. (a) Performance comparison of alkaline and acidic CO2RR electrolyser. Schematic illustration of CO2 electrolyser with AEM (b), CEM (c), forward-bias BPM (d), and reverse-bias BPM (e). (f) Different anode catalysts are used under acidic, alkaline, and neutral pH. (g) Current density and reaction time by using different anode catalysts [21]. Copyright 2022, American Chemical Society.

Fig. 2. Summary diagram of advantages, challenges, and optimisation strategies of reverse-bias BPM electrolyser for CO2RR.

Fig. 3. Functionalities from CEM (left) and AEM (right) (a) and their combination in a BPM (b) [1]. Copyright 2022, Springer Nature. (c,d) Performance in forward-bias BPM electrolyser. (c) C2H4 and voltage stability at 50 mA cm-2 [40]. Copyright 2021, American Chemical Society. (d) A picture of BPM after funning for 2 h at 50 mA cm-2 [40]. Ion migration in forward-bias BPM configuration leads to water, salt, and gas accumulation at the bipolar junction and device failure. Copyright 2021, American Chemical Society.

Fig. 4. (a) Voltage distribution of an BPM electrolyser [43]. Copyright 2021 American Chemical Society. (b) Charge distribution, electric field, electrostatic potential and chemical potential of BPM at open circuit (OCV) [69]. Copyright 2020, American Chemical Society. (c) Qualitative i-V curve at forward bias and reverse bias [53]. Copyright 2020, Elsevier B.V. (d) A schematic i-V curve at reverse bias in salt electrolyte [70]. Copyright 2002, American Chemical Society. i-V curve at reverse bias for concentrations of 0.01, 0.1, 1 and 3 mol L-1 of H2SO4 and K2HPO4/K2HPO4 (e) and 0.1, 1, and 3 mol L-1 of KOH and K2HPO4/K2HPO4 (f) [71]. Copyright 2018, the Royal Society of Chemistry.

Fig. 5. Strategies for BPM optimisation. (a) Schematic representation of (1) ohmic losses, (2) water dissociation reaction, and (3) diffusion boundary layer [63]. Copyright 2019, Royal Society of Chemistry. (b) Water dissociation in BPM electrolysers with thinner CEL [95]. Copyright 2020, American Chemical Society. (c) Performance of alkaline, acidic, and BPM electrolysers [75]. Copyright 2020, AAAS. Performance of BPM electrolysers with various water dissociation catalysts at 450 mA cm-2 (d) and 150 mA cm-2 (e) [80]. Copyright 2022, Springer Nature. (f) Cross-section scanning electron microscope images of BPM with 3D junction [76]. Copyright 2018, Royal Society of Chemistry. (g) Voltage increases during testing at 500 mA cm-2 for 14 h for FBM and 3D BPM [98]. Copyright 2020, American Chemical Society. (h) Schematic of multi-step 3D “mortise-tenon joint” structure interface fabrication processes [99]. The 3D physically interlocked interface maximises the catalytic active area and physical contact area for efficient water dissociation and durable operation. Copyright 2023, Springer Nature.

Fig. 6. Illustration of CO2 electrolysers for industrially relevant performance. (a) Flow cell electrolyser. (b) Membrane-assembly-electrode (MEA) electrolyser. (c) CO2 electrolyser with solid-state electrolyte (SSE).

Fig. 7. Optimisation and performance of CO2RR in flow cell with bulk acidic media. (a) Schematic illustration and mass transport in the BPM-based flow electrolyser with aqueous catholyte for CO2RR [24]. Copyright 2022, Springer Nature. (b) The simulated pH distribution near the cathode surface with different catholyte (K2SO4) chamber thickness. The surface acidity increases as the distance between the cathode and BPM decreases [24]. Copyright 2022, Springer Nature. (c) The total CO2 single-pass utilisation with different thicknesses of catholyte and input CO2 flow rates [24]. Copyright 2022, Springer Nature. (d) Proposed reaction mechanism and enhanced C-C coupling for CO2-to-C2H4 on F-Cu catalyst. Purple: potassium; blue: fluorine; red: oxygen; grey: carbon; white: hydrogen [4]. Copyright 2022, Springer Nature. (e) Relationship between C2H4 FE and calculated Bader charge for the nitrogen atom of the N-aryl-substituted tetrahydro-bipyridines prepared from different N-arylpyridinium additives. The structure of additive 1 is shown in the bottom left [34]. Copyright 2020, Springer Nature. (f) Product distribution of CO2RR in electrolytes with pH = 2 containing different Na+:K+ ratios under 220 mA cm-2 [116]. Copyright 2022, Wiley-VCH GmbH. (g) Schematic illustration of ionic environment and transport near the cathode surface functionalised by the cation-augmenting layer (CAL) [28]. Copyright 2021, AAAS. (h) FEs towards H2 and CO2RR products and SPCE on CAL-modified Cu electrode at 1.2 A cm-2 with varying CO2 flow rates [28]. Copyright 2021, AAAS. (i) Stabilisation of CO2RR intermediates with significant dipole moments by cation-introduced local electrical field [119]. Copyright 2017, American Chemical Society.

Fig. 8. Optimisation and performance of CO2RR in BPM-base MEA (BPMEA) electrolyser. (a) Current efficiency for zero-gap CO2 electrolyser combining with CEM. Red and blue labels indicate Cu and Ag, respectively, as cathode catalysts [123]. Copyright 2019, Elsevier B.V. (b) Faradaic efficiency for CO and H2 using Ni-based molecular and Ag catalysts for zero-gap CO2 electrolyser with reverse-bias BPM configuration [26]. Copyright 2022, American Chemical Society. (c) Cross-section scanning electron microscope of the cathode with a permeable CO2 regeneration layer (PCRL) on Cu/PTFE [40]. Copyright 2021, American Chemical Society. (d) CO2 distribution in CEM-based MEA with anion-selective CO2 regeneration layer under 100 mA cm-2. The CO2 crossover indicates CO2 detected from the anode tail gas [40]. Copyright 2021, American Chemical Society. FEs of H2 and CO in reverse-bias BPMEA as a function of current density with anolyte at 0.2 mol L-1 KOH (e) and 3 mol L-1 KOH (f) [27]. Copyright 2021, American Chemical Society.

Fig. 9. Optimisation and performance of CO2 electrolyser with solid-state electrolyte (SSE). (a) Schematic illustration of CO2 electrolyser with SSE [135]. Copyright 2019, Springer Nature. (b) The CO2 recovery performance of solid electrolyte reactor. The CO2 recovered by water/gas flow through the SSE includes CO2 recovered as gas and CO2 recovered in water. Crossover CO2 and its theoretical value are obtained from GC measurement and calculated based on applied current, respectively [137]. Copyright 2022, Springer Nature. (c) Schematic illustration of promoted CO2RR by poly(aryl piperidinium) functionalised anion-conducting layer [139]. Copyright 2022, Elsevier B.V. (d) COMSOL simulation of the pH distribution in SSE electrolyser under 100 mA cm-2 with different content of dissolved CO2 (100% is the ambient CO2 solubility limit) [139]. Copyright 2022, Elsevier B.V.

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Construction of efficient and stable low-temperature reverse-bias bipolar membrane electrolyser for CO₂ reduction

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