提高酸性CO2电解的选择性:阳离子效应和催化剂创新

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

催化学报 ›› 2024, Vol. 63: 61-80.DOI: 10.1016/S1872-2067(24)60073-2

提高酸性CO₂电解的选择性:阳离子效应和催化剂创新

黄子超, 杨婷惠, 张颖冰, 管超群, 桂文科, 况敏^*(), 杨建平^*()

东华大学材料科学与工程学院, 纤维材料改性国家重点实验室, 上海 201620

收稿日期:2024-04-12 接受日期:2024-06-11 出版日期:2024-08-18 发布日期:2024-08-19
通讯作者: *电子信箱: jianpingyang@dhu.edu.cn (杨建平),mkuang@dhu.edu.cn (况敏).
基金资助:
国家自然科学基金项目(52122312);国家自然科学基金项目(22209024);上海市浦江计划项目(22PJ1400200);彤程研发基金(CPCIF-RA-0102);东华大学纤维材料改性国家重点实验室

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

摘要/Abstract

摘要：

随着全球人口持续增长和工业化加速, 化石能源的过度消耗导致了CO₂过量排放, 引起全球气候变暖和一系列随之而来的生态环境问题. 可再生能源驱动的电催化CO₂还原能够在温和的条件下将CO₂转化为一系列的增值化学品, 是实现碳中和的有前景的技术之一. 为了提高产物的选择性, 电催化CO₂还原通常在中性和碱性介质中进行. 然而, 在反应过程中CO₂不可避免地会在阴极转化为碳酸盐, 降低了CO₂还原的效率. 酸性介质作为一种解决方案, 可以解决碳酸盐问题, 但引入了析氢反应的问题, 降低了酸性环境下CO₂的转化效率. 目前, 在平衡碳效率和CO₂还原性能之间存在挑战, 因此, 本文在总结近年来酸性电催化CO₂还原工作的基础上, 对催化剂的设计方法进行了综述.

本文从阳离子效应和催化剂设计两方面综述了近年来酸性介质中CO₂电解研究的主要进展, 强调了提高酸性介质中CO₂电解选择性的必要性. 首先简要回顾了酸性介质中CO₂电解的发展历程, 讨论了该领域面临的挑战, 即快速的析氢反应以及严苛的反应环境. 随后, 进一步阐明了碱金属阳离子(Li, Na, K和Cs)在酸性介质中的作用. 碱金属阳离子能够最大限度地富集CO₂, 通过稳定关键中间体和调节溶液中H⁺的扩散来改善CO₂还原的动力学. 在此基础上, 列举了通过催化剂设计直接或间接利用阳离子效应的例子, 包括催化剂形态设计、润湿性调节、功能材料改性以及串联结构的构建等. 此外, 还进一步介绍了无金属阳离子酸性介质中的电催化CO₂还原结果. 最后展望了未来的发展方向, 构建更加高效、稳定的催化系统, 深入发展原位表征技术以及模拟计算方法以加深对反应机理的理解, 以及全方面拓展CO₂还原技术将加速CO₂还原的工业化进程.

综上, 本文对提高酸性CO₂电解的选择性进行了综述, 相信能够为新型催化剂的研发提供思路. 总体而言, 电催化CO₂还原从基础研究到工业应用的旅程充满了挑战. 尽管如此, 相信正在进行的研究将很快将大规模电催化CO₂转化定位为全球碳循环可持续管理的关键战略.

关键词: 酸性二氧化碳电解, 高选择性, 阳离子效应, 催化剂设计, 竞争性析氢反应

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

黄子超, 杨婷惠, 张颖冰, 管超群, 桂文科, 况敏, 杨建平. 提高酸性CO₂电解的选择性:阳离子效应和催化剂创新[J]. 催化学报, 2024, 63: 61-80.

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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图/表 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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提高酸性CO₂电解的选择性:阳离子效应和催化剂创新

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

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