面向CO2电化学转化的铜基催化剂研究进展

doi:10.3866/PKU.WHXB202006034

Abstract

Abstract:

Burning of fossil fuels increases CO₂ concentration in the atmosphere, resulting in a series of climate- and environment-related concerns such as global warming, sea-level rise, and melting of glaciers. Therefore, utilization of renewable energy to reduce the CO₂ concentration, in order to realize a sustainable development, is urgent. Capturing and utilizing CO₂, a greenhouse gas, can not only address these concerns but also alleviate the current scenario of energy shortage. Thermal catalytic CO₂ hydrogenation offers various pathways with high conversion efficiencies to produce fuels and industrial chemicals including CO, HCOOH, CH₃OH, and CH₄. However, CO₂ is chemically inert due to the highly stable C＝O bond. Thus, harsh reaction conditions such as high temperature and pressure are required for CO₂ hydrogenation.

Electrocatalytic CO₂ reduction using renewable electricity and water is a promising alternative to thermocatalysis. This technology can not only store and transport the intermittent solar or wind energy but can also use water as the proton source instead of H₂, which is indispensable for thermal CO₂ hydrogenation. Electrochemical CO₂ reduction under ambient conditions is a proton-coupled electron transfer process. The key to promote the electrochemical reduction of CO₂ is to develop highly selective and active catalysts with high stability. Among various CO₂ electrocatalysts, copper-based catalysts have attracted significant attention and have been extensively investigated, since they exhibit good selectivity and efficiency for the reduction of CO₂ to hydrocarbons and alcohols. A broad range of products, up to 16 different gases and liquids, can be obtained in the CO₂ electroconversion on copper. Copper is the only metal that has a negative adsorption energy for *CO and a positive adsorption energy for *H. Thus, it has a unique property of generating > 2e⁻ transfer products. However, selectivity of the target product is still low, especially for high value-added C₂₊ species (C₂H₄, C₂H₅OH, CH₃COOH, CH₃CHO, n-C₃H₇OH, etc.).

The selectivity of various products on copper-based catalysts could be enhanced by surface engineering techniques such as tuning the morphologies, particle sizes, surface facets, strains levels, and atomic coordination. Electrolyte engineering could also aid in CO₂ electroreduction. Therefore, improving the selectivity of C₂₊ products by modifying copper-based catalysts could be a hot research topic. In addition, C-C coupling is a key step in forming C₂₊ products, though the C₂₊ product formation pathway is complex, and the mechanisms are still unclear. Considering these, this paper mainly reviews the research progress in copper-based catalysts producing C₂₊ species in the last five years. It also discusses the possible reaction mechanisms and the factors that affect the product selectivities. In the end, further research directions are proposed.

Key words: Carbon dioxide, Electrochemical reduction, Copper-based catalysts, C₂₊ products, Selectivity

Click here to download Supporting Info material in PDF type

Yichen Meng, Siyu Kuang, Hai Liu, Qun Fan, Xinbin Ma, Sheng Zhang. Recent Advances in Electrochemical CO₂ Reduction Using Copper-Based Catalysts[J]. Acta Phys. -Chim. Sin. 2021, 37(5), 2006034. doi: 10.3866/PKU.WHXB202006034

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Reaction	E⁰/V (vs RHE)	Product (name, abbreviation)
2H⁺ + 2e⁻ → H₂	0	hydrogen evolution reaction, HER
CO₂ + 2H⁺ + 2e⁻ → HCOOH_(aq)	−0.12	formic acid
CO₂ + 2H⁺ + 2e^- → CO_(g) + H₂O	−0.10	carbon monoxide
CO₂ + 6H⁺ + 6e⁻ → CH₃OH_(aq) + H₂O	0.03	methanol, MeOH
CO₂ + 4H⁺ + 4e⁻ → C_(s) + 2H₂O	0.21	graphite
CO₂ + 8H⁺ + 8e⁻ → CH_4(g) + 2H₂O	0.17	methane
2CO₂ + 2H⁺ + 2e⁻ → (COOH)_2(s)	−0.47	oxalic acid
2CO₂ + 8H⁺ + 8e⁻ → CH₃COOH_(aq) + 2H₂O	0.11	acetic acid
2CO₂ + 10H⁺ + 10e⁻ → CH₃CHO_(aq) + 3H₂O	0.06	acetaldehyde
2CO₂ + 12H⁺ + 12e⁻ → ETOH_(aq) + 3H₂O	0.09	ethanol, EtOH
2CO₂ + 12H⁺ + 12e⁻ → C₂H_4(g) + 4H₂O	0.08	ethylene
2CO₂ + 14H⁺ + 14e⁻ → C₂H_6(g) + 4H₂O	0.14	ethane
3CO₂ + 16H⁺ + 16e⁻ → C₂H₅CHO_(aq) + 5H₂O	0.09	propionaldehyde
3CO₂ + 18H⁺ + 18e⁻ → C₃H₇OH_(aq) + 5H₂O	0.10	propanol, PrOH
CO + 6H⁺ + 6e⁻ → CH_4(g) + H₂O	0.26	methane
2CO + 8H⁺ + 8e⁻ → CH₃CH₂OH_(aq) + H₂O	0.19	ethanol, EtOH
2CO + 8H⁺ + 8e⁻ → C₂H_4(g) + 2H₂O	0.17	ethylene

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