Journal ArticleDOI
Atypical Oxygen-Bearing Copper Boosts Ethylene Selectivity toward Electrocatalytic CO2 Reduction.
Wei Zhang,Chuqiang Huang,Qin Xiao,Luo Yu,Luo Yu,Ling Shuai,Pengfei An,Jing Zhang,Ming Qiu,Zhifeng Ren,Ying Yu +10 more
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TLDR
An atypical and stable OBC catalyst with a hierarchical pore and nanograin-boundary structure was constructed and was found to exhibit efficient CO2RR for production of ethylene, providing insight into the synthesis and structural characteristics of OBC, as well as its interplay with ethylene selectivity.Abstract:
Oxygen-bearing copper (OBC) has been widely studied for enabling the C-C coupling of the electrocatalytic CO2 reduction reaction (CO2RR) since this is a distinctive hallmark of strongly correlated OBC systems and may benefit many other Cu-based catalytic processes. Unresolved problems, however, include the instability of and limited knowledge regarding OBC under realistic operating conditions, raising doubts about its role in CO2RR. Here, an atypical and stable OBC catalyst with a hierarchical pore and nanograin-boundary structure was constructed and was found to exhibit efficient CO2RR for the production of ethylene with a Faradaic efficiency of 45% at a partial current density of 44.7 mA cm-2 in neutral media, and the ethylene partial current density is nearly 26 and 116 times that of oxygen-free copper (OFC) and commercial Cu foam, respectively. More importantly, the structure-activity relationship in CO2RR was explored through a comprehensive analysis of experimental data and computational techniques, thus increasing the fundamental understanding of CO2RR. A systematic characterization analysis suggests that atypical OBC (Cu4O) was formed and that it is stable even at -1.00 V [(vs the reversible hydrogen electrode (RHE)]. Density functional theory calculations show that the atypical OBC enables control over CO adsorption and dimerization, making it possible to implement a preference for the electrosynthesis of ethylene (C2) products. These results provide insight into the synthesis and structural characteristics of OBC as well as its interplay with ethylene selectivity.read more
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Posted Content
Rational Catalyst and Electrolyte Design for Co2 Electroreduction Towards Multicarbon Products
TL;DR: In this article, the authors discuss strategies to achieve high C2+ selectivity through rational design of the catalyst and electrolyte, focusing on findings extracted from in situ and operando characterizations.
Journal ArticleDOI
Photocatalytic C-C Coupling from Carbon Dioxide Reduction on Copper Oxide with Mixed-Valence Copper(I)/Copper(II).
Wei Wang,Chaoyuan Deng,Shijie Xie,Yangfan Li,Wanyi Zhang,Hua Sheng,Chuncheng Chen,Jincai Zhao +7 more
TL;DR: In this article, a hybrid photocatalyst (CuOX@p-ZnO) with CuOX uniformly dispersed among polycrystalline ZnO was synthesized upon illumination, the catalyst exhibited the ability to reduce CO2 to C2H4 with a 329% selectivity, and the evolution rate was 27 μmol·g-1·h-1 with water as a hole scavenger.
Journal ArticleDOI
Enhanced Cuprophilic Interactions in Crystalline Catalysts Facilitate the Highly Selective Electroreduction of CO2 to CH4.
Lei Zhang,Xiao-Xin Li,Zhongling Lang,Yang Liu,Jiang Liu,Lin Yuan,Wan-Yue Lu,Yuan-Sheng Xia,Long-Zhang Dong,Daqiang Yuan,Ya-Qian Lan,Ya-Qian Lan +11 more
TL;DR: In this paper, two stable copper(I)-based coordination polymer (NNU-32 and NNU-33(S)) catalysts are synthesized and integrated into a CO2 flow cell electrolyzer, which exhibited very high selectivity for electrocatalytic CO2-to-CH4 conversion due to clearly inherent intramolecular cuprophilic interactions.
Journal ArticleDOI
Regulating the oxidation state of nanomaterials for electrocatalytic CO2 reduction
TL;DR: In this paper, the authors discuss current understandings on how the oxidation state affects the catalytic properties of catalysts, and summarize recent progress in strategies used to regulate the oxidization state of the catalysts and their resultant performances toward CO2RR.
Journal ArticleDOI
High-Rate CO2 Electroreduction to C2+ Products over a Copper-Copper Iodide Catalyst.
Hefei Li,Hefei Li,Tianfu Liu,Pengfei Wei,Pengfei Wei,Long Lin,Long Lin,Dunfeng Gao,Guoxiong Wang,Xinhe Bao +9 more
TL;DR: In this article, the authors designed a Cu-CuI composite catalyst with abundant Cu0 /Cu+ interfaces by physically mixing Cu nanoparticles and CuI powders, which achieved a remarkable C2+ partial current density of 591 mA cm-2 at -10 V vs reversible hydrogen electrode in a flow cell.
References
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Electrochemical CO2 Reduction on Metal Electrodes
TL;DR: In this article, the authors defined the energy conversion efficiency, defined as the ratio of the free energy of the products obtained in electrochemical CO2 reduction and that consumed in the reduction, would be roughly 30 to 40%.
Journal ArticleDOI
CO2 electroreduction to ethylene via hydroxide-mediated copper catalysis at an abrupt interface
Cao-Thang Dinh,Thomas Burdyny,Golam Kibria,Ali Seifitokaldani,Christine M. Gabardo,F. Pelayo García de Arquer,Amirreza Kiani,Jonathan P. Edwards,Phil De Luna,Oleksandr S. Bushuyev,Chengqin Zou,Chengqin Zou,Rafael Quintero-Bermudez,Yuanjie Pang,David Sinton,Edward H. Sargent +15 more
TL;DR: A copper electrocatalyst at an abrupt reaction interface in an alkaline electrolyte reduces CO2 to ethylene with 70% faradaic efficiency at a potential of −0.55 volts versus a reversible hydrogen electrode (RHE).
Journal ArticleDOI
Advances and challenges in understanding the electrocatalytic conversion of carbon dioxide to fuels
Yuvraj Y. Birdja,Yuvraj Y. Birdja,Elena Pérez-Gallent,Marta C. Figueiredo,Marta C. Figueiredo,Adrien J. Göttle,Federico Calle-Vallejo,Federico Calle-Vallejo,Marc T. M. Koper +8 more
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