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杨梦茹, 李华静, 罗宁丹, 李锦, 周安宁, 李远刚. 二氧化碳电催化还原产乙烯: 催化剂、反应条件和反应机理[J]. 化学进展, 2019, 31(2/3): 245-257.
Mengru Yang, Huajing Li, Ningdan Luo, Jin Li, Anning Zhou, Yuangang Li. Electro-Chemical Reduction of Carbon Dioxide into Ethylene: Catalyst, Conditions and Mechanism[J]. Progress in Chemistry, 2019, 31(2/3): 245-257.
电化学还原二氧化碳为乙烯不仅能缓解温室效应而且能得到高附加值的石油化工产品乙烯。本文综述了近年来电催化还原二氧化碳产乙烯的研究进展,着重介绍了能将二氧化碳还原为乙烯的电催化剂,其中铜基催化剂是高选择性产生乙烯的有效电极材料,对铜催化剂进行掺杂、改性和修饰能够在保持催化剂高选择性产生乙烯的同时提高催化剂的稳定性和活性。本文还涉及了电催化条件下乙烯形成的机理以及反应条件对乙烯选择性的影响,简要介绍了二氧化碳在催化剂表面的三种吸附态和Cu(100)晶面形成乙烯的机理,以及不同电位、温度、压力、电解液组成和pH值对乙烯选择性的影响。最后,总结并展望了二氧化碳电催化还原产乙烯催化剂开发亟待解决的问题和未来的发展方向,期望为新型催化剂的构筑提供有益参考。
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Half-electrochemical thermodynamic reactions | Electrode potentials (V vs. SHE) |
---|---|
CO2(g) + 4H+ + 4e-=C(s) + 2H2O(l) | 0.240 |
CO2(g) + 2H2O(l) + 4e-=C(s) + 4OH- | -0.627 |
CO2(g) + 2H+ + 2e- =HCOOH(l) | -0.250 |
CO2(g) + H2O(l) + 2e-=HCOO- (aq)+ OH- | -1.078 |
CO2(g) + 2H+ + 2e- =CO(g) + H2O(l) | -0.106 |
CO2(g) + H2O(l) + 2e-=CO(g) + 2OH- | -0.934 |
CO2(g) + 4H+ + 4e- =CH2O(l) + H2O(l) | -0.070 |
CO2(g) + 3H2O(l) + 4e-=CH2O(l) + 4OH- | -0.898 |
CO2(g) + 6H+ + 6e- =CH3OH(l) + H2O(l) | 0.016 |
CO2(g) + 5H2O(l) + 6e-=CH3OH(l) + 6OH- | -0.812 |
CO2(g) + 8H+ + 8e- =CH4(g) + 2H2O(l) | 0.169 |
CO2(g) + 6H2O(l) + 8e-=CH4(g) + 8OH- | -0.659 |
2CO2(g) + 2H+ + 2e- =H2C2O4(aq) | -0.500 |
2CO2(g) + 2e- =C2(aq) | -0.590 |
2CO2(g) + 12H+ +12e- =CH2CH2(g) + 4H2O(l) | 0.064 |
2CO2(g) + 8H2O(l) + 12e-=CH2CH2(g) + 12OH- | -0.764 |
2CO2(g) + 12H+ +12e- =CH3CH2OH(l) + 3H2O(l) | 0.084 |
2CO2(g) + 9H2O(l) + 12e-=CH3CH2OH(l) + 12OH- | -0.744 |
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