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Stabilization of Cu+ by tuning a CuO–CeO2 interface for selective electrochemical CO2 reduction to ethylene
Green Chemistry ( IF 9.3 ) Pub Date : 2020-09-01 , DOI: 10.1039/d0gc02279a Senlin Chu 1, 2, 3, 4 , Xupeng Yan 5, 6, 7, 8, 9 , Changhyeok Choi 10, 11, 12, 13 , Song Hong 1, 2, 3, 4 , Alex W. Robertson 14, 15, 16, 17 , Justus Masa 18, 19, 20, 21 , Buxing Han 5, 6, 7, 8, 9 , Yousung Jung 10, 11, 12, 13 , Zhenyu Sun 1, 2, 3, 4, 22
Green Chemistry ( IF 9.3 ) Pub Date : 2020-09-01 , DOI: 10.1039/d0gc02279a Senlin Chu 1, 2, 3, 4 , Xupeng Yan 5, 6, 7, 8, 9 , Changhyeok Choi 10, 11, 12, 13 , Song Hong 1, 2, 3, 4 , Alex W. Robertson 14, 15, 16, 17 , Justus Masa 18, 19, 20, 21 , Buxing Han 5, 6, 7, 8, 9 , Yousung Jung 10, 11, 12, 13 , Zhenyu Sun 1, 2, 3, 4, 22
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Electrochemical conversion of carbon dioxide (CO2) into multi-carbon fuels and chemical feedstocks is important but remains challenging. Here, we report the stabilization of Cu+ within a CuO–CeO2 interface for efficient and selective electrocatalytic CO2 reduction to ethylene under ambient conditions. Tuning the CuO/CeO2 interfacial interaction permits dramatic suppression of proton reduction and enhancement of CO2 reduction, with an ethylene faradaic efficiency (FE) as high as 50.0% at −1.1 V (vs. the reversible hydrogen electrode) in 0.1 M KHCO3, in stark contrast to 22.6% over pure CuO immobilized on carbon black (CB). The composite catalyst presents a 2.6-fold improvement in ethylene current compared to that of CuO/CB at similar overpotentials, which also exceeds many recently reported Cu-based materials. The FE of C2H4 remained at over 48.0% even after 9 h of continuous polarization. The Cu+ species are believed to be the adsorption as well as active sites for the activation of CO2 molecules, which remain almost unchanged after 1 h of electrolysis. Further density functional theory calculations demonstrate the preferred formation of Cu+ at the CuO–CeO2 interface. This work provides a simple avenue to convert CO2 into high-value hydrocarbons by rational stabilization of Cu+ species.
中文翻译：
通过调节CuO–CeO2界面以选择性地将CO2电化学还原为乙烯来稳定Cu +
二氧化碳（CO 2）电化学转化为多碳燃料和化学原料很重要，但仍具有挑战性。在这里，我们报告了在环境条件下，CuO–CeO 2界面内Cu +的稳定作用，可有效且选择性地将电催化CO 2还原为乙烯。调整CuO / CeO 2界面相互作用可显着抑制质子还原并增强CO 2还原，在0.1M KHCO中于-1.1 V时乙烯法拉第效率（FE）高达50.0％（相对于可逆氢电极）3，与固定在炭黑（CB）上的纯CuO相比形成了22.6％的鲜明对比。在类似的超电势下，该复合催化剂的乙烯电流比CuO / CB的乙烯电流提高了2.6倍，这也超过了许多最近报道的基于Cu的材料。即使连续极化9 h，C 2 H 4的FE仍保持在48.0％以上。认为Cu +物种是CO 2分子活化的吸附和活性位点，在电解1 h后几乎保持不变。进一步的密度泛函理论计算证明了在CuO–CeO 2界面上优选形成Cu +。这项工作提供了转换CO的简单途径通过合理稳定Cu +物种将2转化为高价值的碳氢化合物。
更新日期：2020-10-05
中文翻译：
通过调节CuO–CeO2界面以选择性地将CO2电化学还原为乙烯来稳定Cu +
二氧化碳（CO 2）电化学转化为多碳燃料和化学原料很重要，但仍具有挑战性。在这里，我们报告了在环境条件下，CuO–CeO 2界面内Cu +的稳定作用，可有效且选择性地将电催化CO 2还原为乙烯。调整CuO / CeO 2界面相互作用可显着抑制质子还原并增强CO 2还原，在0.1M KHCO中于-1.1 V时乙烯法拉第效率（FE）高达50.0％（相对于可逆氢电极）3，与固定在炭黑（CB）上的纯CuO相比形成了22.6％的鲜明对比。在类似的超电势下，该复合催化剂的乙烯电流比CuO / CB的乙烯电流提高了2.6倍，这也超过了许多最近报道的基于Cu的材料。即使连续极化9 h，C 2 H 4的FE仍保持在48.0％以上。认为Cu +物种是CO 2分子活化的吸附和活性位点，在电解1 h后几乎保持不变。进一步的密度泛函理论计算证明了在CuO–CeO 2界面上优选形成Cu +。这项工作提供了转换CO的简单途径通过合理稳定Cu +物种将2转化为高价值的碳氢化合物。
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