Enhancing selectivity in acidic CO2 electrolysis: Cation effects and catalyst innovation

doi:10.1016/S1872-2067(24)60073-2

Chinese Journal of Catalysis ›› 2024, Vol. 63: 61-80.DOI: 10.1016/S1872-2067(24)60073-2

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Enhancing selectivity in acidic CO₂ electrolysis: Cation effects and catalyst innovation

Zichao Huang, Tinghui Yang, Yingbing Zhang, Chaoqun Guan, Wenke Gui, Min Kuang^*(), Jianping Yang^*()

State Key Laboratory for Modification of Chemical Fibers and Polymer Materials, College of Materials Science and Engineering, Donghua University, Shanghai 201620, China

Received:2024-04-12 Accepted:2024-06-11 Online:2024-08-18 Published:2024-08-19
Contact: *E-mail: jianpingyang@dhu.edu.cn (J. Yang), mkuang@dhu.edu.cn (M. Kuang).
About author:Min Kuang is currently a professor in the College of Materials Science and Engineering in Donghua University (China). She finished her PhD from Laboratory of Advanced Materials at Fudan University. After that, she joined the School of Materials Science and Engineering at Nanyang Technological University as a postdoctoral research associate. Her research interest is concentrating on developing advanced electrochemical C₁-to-fuel conversion systems and the exploration of efficient electrocatalysts.
Jianping Yang is appointed as a Professor and Associate Dean in the College of Materials Science and Engineering at Donghua University (China). He received his PhD in Inorganic Chemistry from Fudan University in 2013, and then worked as a postdoctoral and visiting research fellow at Tongji University, University of Wollongong and Monash University. His research interests include interfacial design of functional materials for environmental electrocatalysis, sustainable energy systems. Professor Yang has been admitted as a Fellow of the Royal Society of Chemistry (FRSC), and identified in the Highly Cited Researchers in Cross Field (2023) by Web of Science-Clarivate Analytics.
Supported by:
National Natural Science Foundation of China(52122312);National Natural Science Foundation of China(22209024);Shanghai Pujiang Program(22PJ1400200);Tongcheng R&D Foundation(CPCIF-RA-0102);State Key Laboratory for Modification of Chemical Fibers and Polymer Materials, Donghua University

Abstract

Abstract:

The electrochemical reduction of CO₂ (eCO₂R) under ambient conditions is crucial for reducing carbon emissions and achieving carbon neutrality. Despite progress with alkaline and neutral electrolytes, their efficiency is limited by (bi)carbonates formation. Acidic media have emerged as a solution, addressing the (bi)carbonates challenge but introducing the issue of the hydrogen evolution reaction (HER), which reduces CO₂ conversion efficiency in acidic environments. This review focuses on enhancing the selectivity of acidic CO₂ electrolysis. It commences with an overview of the latest advancements in acidic CO₂ electrolysis, focusing on product selectivity and electrocatalytic activity enhancements. It then delves into the critical factors shaping selectivity in acidic CO₂ electrolysis, with a special emphasis on the influence of cations and catalyst design. Finally, the research challenges and personal perspectives of acidic CO₂ electrolysis are suggested.

Key words: Acidic CO₂ electrolysis, High selectivity, Cation effects, Catalyst design, Competitive HER

Zichao Huang, Tinghui Yang, Yingbing Zhang, Chaoqun Guan, Wenke Gui, Min Kuang, Jianping Yang. Enhancing selectivity in acidic CO₂ electrolysis: Cation effects and catalyst innovation[J]. Chinese Journal of Catalysis, 2024, 63: 61-80.

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Figures/Tables 13

Table 1 Comparative analysis of eCO2R techniques across various media.

Media	Cathode electrolyte	Separator	Anode electrolyte	Anode material	Characterizations
Alkaline	KOH	AEM	KOH	nickel foam	advantages: high FE of eCO₂R, low cathode overpotential; disadvantages: low carbon efficiency, high cost for KOH regeneration
Neutral	KCl	AEM	KOH	nickel foam	advantages: high FE of eCO₂R, sustainable electrolyte; disadvantages: low carbon efficiency, high resistance
Neutral	KHCO₃	CEM/AEM	KHCO₃/KOH	Pt/nickel foam
Acidic	inorganic acids and metal salts	CEM	H₂SO₄/K₂SO₄	Ir, Ru, Pt	advantages: fewer carbon loss, fewer salt precipitation, disadvantages: severe HER, sluggish eCO₂R kinetics
Acidic	inorganic acids and metal salts	BPM	KOH	nickel foam

Fig. 1. (a) A plot of log concentration of inorganic carbon species, H+ and OH- as a function of pH for an open CO2-H2O system. Reprinted with permission from Ref. [36]. Copyright 2023, Elsevier. (b) FE toward all products on sputtered Cu catalyst in 1 mol L-1 H3PO4 with different KCl concentrations at -0.4 A cm-2. Reprinted with permission from Ref. [20]. Copyright 2021, American A

Table 2 Summary of reported eCO2R performances in acidic media.

Catalyst	Electrolyte	Major product	FE (%)	Stability (h)	SPCE (%)	Ref.
Ni₅@NCN	0.25 mol L^‒1 Na₂SO₄ + H₂SO₄	CO	84.3	20	none	[68]
Ag@C	H₂SO₄ + 0.5 mol L^‒1 K₂SO₄	CO	95	9	46.2	[69]
NiNF-1100	H₂SO₄ + 0.05 mol L^‒1 K₂SO₄	CO	90	30	78	[97]
PTFE-Q/Ag	0.1 mol L^‒1 K₂SO₄ + 0.1 mol L^‒1 H₂SO₄	CO	95.6	6.6	none	[113]
PDDA-Ag	0.1 mol L^‒1 H₂SO₄	CO	95	36	none	[124]
PDDA-GO-Ag	0.01 mol L^‒1 H₂SO₄	CO	85	50	none	[126]
BiNS	0.05 mol L^‒1 H₂SO₄ +3 mol L^‒1 KCl	HCOOH	92.2	8	none	[84]
Bi RS	0.1 mol L^‒1 H₂SO₄ + 0.5 mol L^‒1 K₂SO₄	HCOOH	96.3	50	79	[85]
SiC-Nafion^TM /SnBi/PTFE	0.05 mol L^‒1 H₂SO₄ + 3 mol L^‒1 KCl	HCOOH	92	125	65	[40]
Cu₆Sn₅	0.05 mol L^‒1 H₂SO₄+3 mol L^‒1 KCl	HCOOH	91	3300	77.4	[116]
18-C-6/Cu	H₂SO₄ + 0.5 mol L^‒1 K₂SO₄	CH₄	51.2	4.4	43	[112]
Cu/PFSA	1 mol L^‒1 H₃PO₄ + 3 mol L^‒1 KCl	C₂₊	40	12	77	[20]
ER-CuNS	0.05 mol L^‒1 H₂SO₄ +3 mol L^‒1 KCl	C₂₊	83.7	30	54.4	[86]
Cu/PTFE/C	H₂SO₄ + 0.5 mol L^‒1 K₂SO₄	C₂₊	74	50	none	[106]
Pd-Cu	H₂SO₄ + 0.5 mol L^‒1 K₂SO₄	C₂₊	80	4.5	60	[32]
CG-Cu	0.2 mol L^‒1 H₂SO₄	C₂₊	80	155	90	[43]
Cu-GDL	1 mol L^‒1 KCl + 1 mol L^‒1 KOH + 1 mol L^‒1 HCl	C₂₊	87	30	42	[109]
CuO_x-dendrites	H₂SO₄ + 0.5 mol L^‒1 K₂SO₄	C₂₊	77	50	26.8	[81]

Fig. 2. Effect of cations on electric field distribution in electric bilayer. Schemes of double layer near cathode with cations (a) and without cations (b). Reprinted with permission from Ref. [56]. Copyright 2022, Springer Nature. (c) Schematic of alkali cation effects on the mass transport of H+ and the kinetics of CO2 reduction in acidic solution. The blue region represents the stern layer and the green region represents the diffuse and diffusion layers. (d) Plots of electric field strength in the stern layer based on the electrode potential in solutions containing 10 mmol L?1 HClO4 and 10 mmol L?1 MClO4 (M = Li, Na, K, Cs). Reprinted with permission from Ref. [57]. Copyright 2023, American Chemical Society. (e) In acidic solutions without and with alkali cations, the pH distribution near the cathode occurs when H+ reduction reaches the platform current density. Reprinted with permission from Ref. [58]. Copyright 2023, Elsevier. (f) Modeling of pH at different distances to cathode and current density in 1 mol L?1 H3PO4 and 3 mol L?1 KCl. Reprinted with permission from Ref. [20]. Copyright 2021, American Association for the Advancement of Science.

Fig. 3. (a) Schematic representation of the interaction of the cation with the negatively charged CO2- intermediate. Reprinted with permission from Ref. [45]. Copyright 2021, Springer Nature. (b) Schematic illustration of eCO2R at Au-water interfaces. eCO2R in AM+-free medium and medium with AM+ are shown on the left and right. The parallel red-dashed line represents the boundary of OS-ET and IS-ET. Reprinted with permission from Ref. [61]. Copyright 2023, Springer Nature.

Fig. 4. (a) pH Environment and ions transported around the Ni5@NCN catalyst. Reprinted with permission from Ref. [68]. Copyright 2022, American Chemical Society. (b) Schematic of the local reaction environment and ion transport on the Ag@C catalyst. Reprinted with permission from Ref. [69]. Copyright 2023, Royal Society of Chemistry. (c) The schematic illustrations of Cu HPE show the processes of CO2 electroreduction. (d) A reaction energy diagram for *CO to *OCCHO via the *CO + *CHO coupling pathway on Cu, Cu-H+, Cu-[K(H2O)6]+, and Cu-H+-[K(H2O)6]+. Reprinted with permission from Ref. [71]. Copyright 2024, Royal Society of Chemistry. (e) Surface K+ density and current density distributions on the surface of Au needles. The tip radius is 5 nm. Reprinted with permission from Ref. [79]. Copyright 2016, Springer Nature. (f) Adsorbed K+ and the electric field intensity at the tip, revealing that both adsorbed K+ and electrostatic field intensity increase as the tip radius decreases. Reprinted with permission from Ref. [80]. Copyright 2019, Wiley-VCH. (g) SEM image of CuOx-dendrites. (h) FE of various products at various biases collected in a flow cell of CuOx-dendrites. (i) In situ Raman spectra of CuOx-dendrites during the CO2R. Reprinted with permission from Ref. [81]. Copyright 2024, Royal Society of Chemistry.

Fig. 5. (a) Gibbs free energy diagrams of the eCO2R to HCOOH on the Bi (001) facet in the absence or presence of K+ cations. (b) Schematic diagram of eCO2R selectivity in acid modulated by K+ cations. Reprinted with permission from Ref. [84]. Copyright 2022, American Chemical Society. (c) ECSA-normalized K+ number on F-CuNS and ER-CuNS. (d) K+ distribution on ER-CuNS models obtained from COMSOL Multiphysics finite-element-based simulations. Reprinted with permission from Ref. [86]. Copyright 2022, Springer Nature.

Fig. 6. (a) The thickness of the diffusion layer varies with the mass ratio of PTFE to the diffusion layer. Reprinted with permission from Ref. [105]. Copyright 2022, Wiley-VCH. (b) Faradaic efficiencies of the electrodes with different contact angles. Reprinted with permission from Ref. [106]. Copyright 2023, Wiley-VCH. (c) Integral GDE with catalytic sites embedded within the intertwined carbon nanofibers of hierarchical porosity. (d) Catalytic stability of NiNF-1100 in H2SO4/K2SO4 (pH = 2, CK+ = 0.5 mol L?1). Reprinted with permission from Ref. [97]. Copyright 2023, Royal Society of Chemistry. (e) SEM image for high-density nanoneedles exhibiting a large contact angle (CA). (f) Relative Pz calculated toward 2φ and α. Pz is Laplace pressure, 2φ is apex angle and α is tilt angle of the needle. The more positive the Pz, the faster the gas diffuses. (g) jC2+ as a function of CCO2 (diluted gas is N2). Reprinted with permission from Ref. [109]. Copyright 2023, Springer Nature.

Fig. 7. (a) FE, total current density for different products of 35 min CO2 R in pH = 2 electrolyte by the Cu electrode (Cu) at -1.40 V and the Cu electrode with 10 mmol L-1 tolyl-pyr dissolved (Cu + 10 mmol L-1 tolyl-pyr) at -1.35, -1.41 and -1.45 V vs. RHE. (b) CVs of bare Cu RDE and Modified-Cu RDE in N2 saturated 0.1 mol L-1 KClO4/HClO4 (pH = 2.2) with different rotation rates. Reprinted with permission from Ref. [110]. Copyright 2023, Wiley-VCH. (c) Schematic illustration of ionic environment and transport near the catalyst surface functionalized by the PFSA ionomer. (d) FEs toward H2 and CO2R products as well as SPCE on CAL-modified Cu electrode at -1.2 A cm-2 with different CO2 flow rates. All experiments were performed using 1 mol L-1 H3PO4 + 3 mol L-1 KCl catholyte. Reprinted with permission from Ref. [20]. Copyright 2023, American Association for the Advancement of Science. (e) Simulated electric field strength over the distance from the outer Helmholtz plane (OHP). (f) Formation rate and KIE value of CH4 on Cu and Cu-3 catalysts at -1.05 V using 0.5 mol L-1 K2SO4 electrolyte with H2O or D2O as the solvent. Reprinted with permission from Ref. [112]. Copyright 2023, Wiley-VCH. (g) Application of the SiC-NafrionTM coated layer and the resulting regulated pH and ion concentrations near the catalyst surface. (h) CO2R chronopotentiometry curve with the HCOOH FE at -0.1 A cm-2 in a 0.05 mol L-1 H2SO4 and 3 mol L-1 KCl electrolyte at pH = 1. Reprinted with permission from Ref. [40]. Copyright 2023, Wiley-VCH.

Fig. 8. (a) The calculated adsorption energy of *OCHO, *COOH, and *H on Cu, Cu1?xSnx (x = 0.14, 0.44), and Sn catalysts. (b) In situ ATR-FTIR spectra were measured at different applied potentials for Cu6Sn5. (c) In situ ATR-FTIR spectra measured at different applied potentials for Sn. Reprinted with permission from Ref. [116]. Copyright 2024, Springer Nature. (d) SEM for Pd-Cu catalysts on PTFE. (e) Free energy diagram of CO2R via the CHO pathway toward C1 products (orange), where CH4 is used as the representative product, and the OCCOH pathway toward C2+ products (blue), where C2H4 is utilized as the representative product. Solid and dashed lines represent Pd-Cu and Cu, respectively. (f) FE values of all products on Pd-Cu catalysts under different applied current densities. Reprinted with permission from Ref. [32]. Copyright 2022, Springer Nature. (g) Schematic of the spatially decoupled strategy via tandem catalysis, showing the electron transfer and mass transport in acidic eCO2R. (h) Comparison of CO FE on CoPc@HC electrode and CoPc/C electrode in acidic eCO2R in an acidic buffer electrolyte of 0.5 mol L?1 H3PO4 and 0.5 mol L?1 KH2PO4 with 2.5 mol L?1 KCl in a flow cell. (i) FE values of eCO2R products on the CoPc@HC/Cu tandem electrode in an acidic buffer electrolyte of 0.5 mol L?1 H3PO4 and 0.5 mol L?1 KH2PO4 with 2.5 mol L?1 KCl in a flow cell. Reprinted with permission from Ref. [123]. Copyright 2023, Springer Nature.

Fig. 9. (a) Selectivity comparison of CG-low, CG-medium, and CG-high in 0.2 mol L-1 H2SO4 solution at a current density of -0.1 A cm-2. (b) SPCE of CO2 at various flow rates. (c) Electric field comparison of H+, K+, and immobilized CG at OHP. Reprinted with permission from Ref. [43]. Copyright 2023, Springer Nature. (d) FE of CO during electrolysis with a constant current density of -0.2 A cm-2. (e) The migration rate of H+ with the electrode potential of -1.8 V vs. SHE at 2 μm from OHP. (f) Plots of the electric field strength in the Stern layer based on the electrode potential. Reprinted with permission from Ref. [124]. Copyright 2023, Springer Nature. (g) Zeta potentials of PDDA, GO, and PDDA-GO dispersed in deionized water. (h) Schematic illustration of the interface modulation effect of the PDDA-GO modification layer. (i) CO FEs of PDDA-GO-, PDDA- or GO-modified Ag catalysts at different applied current densities together with the corresponding full-cell voltages of PDDA-GO-modified Ag. Reprinted with permission from Ref. [125]. Copyright 2024, Wiley-VCH.

Fig. 10. Guidelines for the design of acidic CO2 electrolytic catalysts.

Fig. 11. Further developments of eCO2R to industrial practical applications.

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Enhancing selectivity in acidic CO₂ electrolysis: Cation effects and catalyst innovation

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