Paramelaconite‐Enriched Copper‐Based Material as an Efficient and Robust Catalyst for Electrochemical Carbon Dioxide Reduction
Paramelaconite‐Enriched Copper‐Based Material as an Efficient and Robust Catalyst for Electrochemical Carbon Dioxide Reduction
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DOI：
10.1002/aenm.201901228
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发表时间：
2019-06
影响因子：
27.8
通讯作者：
N. Martić;C. Reller;C. Macauley;Mario Löffler;B. Schmid;David Reinisch;E. Volkova;A. Maltenberger;A. Rucki;K. Mayrhofer;G. Schmid
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文献类型：
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作者：
N. Martić;C. Reller;C. Macauley;Mario Löffler;B. Schmid;David Reinisch;E. Volkova;A. Maltenberger;A. Rucki;K. Mayrhofer;G. Schmid
提出并研究了富含副黑铜矿（Cu 4 O3）的氧化铜基催化剂作为促进CO2电还原为乙烯和其他烃的电催化剂。Cu 4 O3是氧化铜家族的成员，具有有趣的混合价性质，在其晶体结构中包含相同数量的Cu+和Cu 2+离子。该材料使用溶剂热合成路线合成，其结构通过粉末X射线衍射、基于透射电子显微镜的选区电子衍射和X射线光电子能谱确认。利用配备有气体扩散电极的流动反应器来测试在CO2还原条件下富含Cu 4 O3相的铜基催化剂。富含Cu 4 O3的催化剂（PrC）在400 mA cm−2下显示出超过40%的乙烯法拉第效率。相对于可逆氢电极，在-0.64处，实现了4.8的最高C2+/C1产物比，C2+法拉第效率超过61%。此外，该催化剂在200 mA cm-2的恒定电流密度下表现出24 h的稳定性能。
A copper‐oxide‐based catalyst enriched with paramelaconite (Cu4O3) is presented and investigated as an electrocatalyst for facilitating electroreduction of CO2 to ethylene and other hydrocarbons. Cu4O3 is a member of the copper‐oxide family and possesses an intriguing mixed‐valance nature, incorporating an equal number of Cu+ and Cu2+ ions in its crystal structure. The material is synthesized using a solvothermal synthesis route and its structure is confirmed via powder X‐ray diffraction, transmission electron microscope based selected area electron diffraction, and X‐ray photoelectron spectroscopy. A flow reactor equipped with a gas diffusion electrode is utilized to test a copper‐based catalyst enriched with the Cu4O3 phase under CO2 reduction conditions. The Cu4O3‐rich catalyst (PrC) shows a Faradaic efficiency for ethylene over 40% at 400 mA cm−2. At −0.64 versus reversible hydrogen electrode, the highest C2+/C1 product ratio of 4.8 is achieved, with C2+ Faradaic efficiency over 61%. Additionally, the catalyst exhibits a stable performance for 24 h at a constant current density of 200 mA cm−2.