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
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TLDR
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).Abstract:
Carbon dioxide (CO 2 ) electroreduction could provide a useful source of ethylene, but low conversion efficiency, low production rates, and low catalyst stability limit current systems. Here we report that a copper electrocatalyst at an abrupt reaction interface in an alkaline electrolyte reduces CO 2 to ethylene with 70% faradaic efficiency at a potential of −0.55 volts versus a reversible hydrogen electrode (RHE). Hydroxide ions on or near the copper surface lower the CO 2 reduction and carbon monoxide (CO)–CO coupling activation energy barriers; as a result, onset of ethylene evolution at −0.165 volts versus an RHE in 10 molar potassium hydroxide occurs almost simultaneously with CO production. Operational stability was enhanced via the introduction of a polymer-based gas diffusion layer that sandwiches the reaction interface between separate hydrophobic and conductive supports, providing constant ethylene selectivity for an initial 150 operating hours.read more
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Ethylene Selectivity in Electrocatalytic CO2 Reduction on Cu Nanomaterials: A Crystal Phase-Dependent Study.
Ye Chen,Zhanxi Fan,Jiong Wang,Chongyi Ling,Chongyi Ling,Wenxin Niu,Wenxin Niu,Zhiqi Huang,Guigao Liu,Bo Chen,Zhuangchai Lai,Xiaozhi Liu,Bing Li,Yun Zong,Lin Gu,Jinlan Wang,Xin Wang,Hua Zhang +17 more
TL;DR: Density functional theory cal-culations suggest that the 4H phase and 4H/fcc interface of Cu favor the C2H4 formation pathway compared to the fcc Cu, leading to the crystal phase-dependent C 2H4 selectivity.
Journal ArticleDOI
Composition Tailoring via N and S Co-doping and Structure Tuning by Constructing Hierarchical Pores: Metal-Free Catalysts for High-Performance Electrochemical Reduction of CO 2
Hengpan Yang,Yu Wu,Qing Lin,Liangdong Fan,Xiaoyan Chai,Qianling Zhang,Jianhong Liu,Chuanxin He,Zhiqun Lin +8 more
TL;DR: A facile route to scalable production of N and S co-doped, hierarchically porous carbon nanofiber (NSHCF) membranes (ca. 400 cm2 membrane in a single process) is reported, with outstanding CO Faradaic efficiency and ultra-high current density.
Journal ArticleDOI
Recent Advances in Design of Electrocatalysts for High‐Current‐Density Water Splitting
Manish Chhowalla,Bilu Liu +1 more
TL;DR: In this article , a multiscale design strategy that considers these aspects comprehensively for developing high-current-density electrocatalysts is highlighted, and perspectives on the future directions in this emerging field are also put forward.
Journal ArticleDOI
Role of the Carbon-Based Gas Diffusion Layer on Flooding in a Gas Diffusion Electrode Cell for Electrochemical CO 2 Reduction
TL;DR: In this paper, the role of carbon gas diffusion layers (GDLs) in the advent of flooding during CO2 reduction was investigated, finding that applied potential plays a central role in the observed instabilities.
Journal ArticleDOI
Formation of carbon-nitrogen bonds in carbon monoxide electrolysis.
Matthew Jouny,Jing-Jing Lv,Jing-Jing Lv,Tao Cheng,Tao Cheng,Byung Hee Ko,Jun-Jie Zhu,William A. Goddard,Feng Jiao +8 more
TL;DR: It is demonstrated that C–N bonds can be formed through co-electrolysis of CO and NH3 with acetamide selectivity of nearly 40% at industrially relevant reaction rates.
References
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Generalized Gradient Approximation Made Simple
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Journal ArticleDOI
Improved tangent estimate in the nudged elastic band method for finding minimum energy paths and saddle points
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A grid-based Bader analysis algorithm without lattice bias
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