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
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
Citations
More filters
Journal ArticleDOI
Gas diffusion electrodes and membranes for CO2 reduction electrolysers
TL;DR: In this paper, the authors present material design strategies for controlling the transport of products and reactants in electrochemical reactors that convert CO2 emissions into chemicals and fuels, and discuss how the properties of GDEs and polymer electrolyte membranes affect CO2RR electrolysis.
Journal ArticleDOI
Efficient upgrading of CO to C3 fuel using asymmetric C-C coupling active sites
Xue Wang,Ziyun Wang,Tao Tao Zhuang,Cao-Thang Dinh,Jun Li,Dae-Hyun Nam,Fengwang Li,Chun Wei Huang,Chih Shan Tan,Zitao Chen,Miaofang Chi,Christine M. Gabardo,Ali Seifitokaldani,Petar Todorović,Andrew H. Proppe,Yuanjie Pang,Ahmad R. Kirmani,Yuhang Wang,Alexander H. Ip,Lee J. Richter,Benjamin Scheffel,Aoni Xu,Shen-Chuan Lo,Shana O. Kelley,David Sinton,Edward H. Sargent +25 more
TL;DR: The concept of asymmetric active sites is used to develop a class of doped Cu catalysts for C-C coupling, delivering record selectivity to n-propanol.
Journal ArticleDOI
Electrochemical Reduction of CO2 over Heterogeneous Catalysts in Aqueous Solution: Recent Progress and Perspectives
TL;DR: In this paper, a review of the recent advances of the underlying mechanistic studies and novel heterogeneous catalyst constructions for electrochemical reduction of CO2 in aqueous media, targeting at presenting a full landscape at the current stage is presented.
Journal ArticleDOI
Atomic Layer Deposition of ZnO on CuO Enables Selective and Efficient Electroreduction of Carbon Dioxide to Liquid Fuels.
Dan Ren,Jing Gao,Linfeng Pan,Zaiwei Wang,Jingshan Luo,Jingshan Luo,Shaik M. Zakeeruddin,Anders Hagfeldt,Michael Grätzel +8 more
TL;DR: CuZn bimetallic catalysts were synthesized by in situ electrochemical reduction of ZnO-shell/CuO-core bi-metal-oxide by showing preference towards ethanol formation, with the ratio of ethanol/ethylene increasing over five times regardless of applied potential.
Journal ArticleDOI
Isolated copper single sites for high-performance electroreduction of carbon monoxide to multicarbon products.
Haihong Bao,Yuan Qiu,Xianyun Peng,Jiaao Wang,Yuying Mi,Shunzheng Zhao,Xijun Liu,Xijun Liu,Yifan Liu,Rui Cao,Longchao Zhuo,Junqiang Ren,Jiaqiang Sun,Jun Luo,Xuping Sun +14 more
TL;DR: In this article, a single atom copper catalyst supported on MXene with high CO reduction performance and stability is presented, achieving an ultra high selectivity of 98% for the formation of multicarbon products.
References
More filters
Journal ArticleDOI
Generalized Gradient Approximation Made Simple
TL;DR: A simple derivation of a simple GGA is presented, in which all parameters (other than those in LSD) are fundamental constants, and only general features of the detailed construction underlying the Perdew-Wang 1991 (PW91) GGA are invoked.
Journal ArticleDOI
Efficient iterative schemes for ab initio total-energy calculations using a plane-wave basis set.
Georg Kresse,Jürgen Furthmüller +1 more
TL;DR: An efficient scheme for calculating the Kohn-Sham ground state of metallic systems using pseudopotentials and a plane-wave basis set is presented and the application of Pulay's DIIS method to the iterative diagonalization of large matrices will be discussed.
Journal ArticleDOI
From ultrasoft pseudopotentials to the projector augmented-wave method
Georg Kresse,Daniel P. Joubert +1 more
TL;DR: In this paper, the formal relationship between US Vanderbilt-type pseudopotentials and Blochl's projector augmented wave (PAW) method is derived and the Hamilton operator, the forces, and the stress tensor are derived for this modified PAW functional.
Journal ArticleDOI
Improved tangent estimate in the nudged elastic band method for finding minimum energy paths and saddle points
Graeme Henkelman,Hannes Jónsson +1 more
TL;DR: An improved way of estimating the local tangent in the nudged elastic band method for finding minimum energy paths is presented, and examples given where a complementary method, the dimer method, is used to efficiently converge to the saddle point.
Journal ArticleDOI
A grid-based Bader analysis algorithm without lattice bias
TL;DR: This paper describes how accurate off-lattice ascent paths can be represented with respect to the grid points, and maintains the efficient linear scaling of an earlier version of the algorithm, and eliminates a tendency for the Bader surfaces to be aligned along the grid directions.
Related Papers (5)
Progress and Perspectives of Electrochemical CO2 Reduction on Copper in Aqueous Electrolyte
Stephanie A. Nitopi,Erlend Bertheussen,Søren Bertelsen Scott,Xinyan Liu,Albert K. Engstfeld,Albert K. Engstfeld,Sebastian Horch,Brian Seger,Ifan E. L. Stephens,Ifan E. L. Stephens,Karen Chan,Karen Chan,Christopher Hahn,Christopher Hahn,Jens K. Nørskov,Jens K. Nørskov,Jens K. Nørskov,Thomas F. Jaramillo,Thomas F. Jaramillo,Ib Chorkendorff +19 more