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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Electrokinetic and in situ spectroscopic investigations of CO electrochemical reduction on copper.
Jing Li,Xiaoxia Chang,Haochen Zhang,Arnav S. Malkani,Mu Jeng Cheng,Bingjun Xu,Bingjun Xu,Qi Lu +7 more
TL;DR: In this paper, the authors determined mass transport-free CORR kinetics by employing a gas-diffusion type electrode and identified dependence of catalyst surface speciation on the electrolyte pH using in-situ surface enhanced vibrational spectroscopies.
Journal ArticleDOI
Atomically dispersed asymmetric Cu–B pair on 2D carbon nitride synergistically boosts the conversion of CO into C2 products
TL;DR: In this paper, the authors proposed a novel CO reduction catalyst for the conversion of CO into more value-added ethylene and ethanol under visible light, consisting of active Cu-B atomic pair decorated graphitic carbon nitride (Cu-B@g-C3N4).
Journal ArticleDOI
Zn nanosheets coated with a ZnS subnanometer layer for effective and durable CO2 reduction
Chenglong Li,Gu-Rong Shen,Rui Zhang,Deyao Wu,Chengqin Zou,Tao Ling,Hui Liu,Cun-Ku Dong,Xi-Wen Du +8 more
TL;DR: In this paper, a conceptually new electrocatalyst, Zn nanosheets coated with a porous ZnS sub-nanometer layer, can achieve excellent catalytic performance which is comparable with that of noble metallic catalysts.
Journal ArticleDOI
Transforming active sites in nickel–nitrogen–carbon catalysts for efficient electrochemical CO2 reduction to CO
Rahman Daiyan,Xiaofeng Zhu,Zizheng Tong,Lele Gong,Amir Razmjou,Ru-Shi Liu,Zhenhai Xia,Xunyu Lu,Liming Dai,Rose Amal +9 more
TL;DR: In this paper, the authors investigated the role of possible Ni-Nx and Ni-C4 coordinations in CO2RR catalysis and developed an effective strategy to transform Ni−N4 to Ni−C4 active sites by removing N moieties within Ni embedded in a hollow nitrogen-doped carbon shell (Ni@NCH).
Journal ArticleDOI
Boosting CO2 Electroreduction over a Cadmium Single-Atom Catalyst by Tuning of the Axial Coordination Structure.
Yahui Wu,Chunjun Chen,Xupeng Yan,Xiaofu Sun,Qinggong Zhu,Pengsong Li,Yiming Li,Shoujie Liu,Jingyuan Ma,Yuying Huang,Buxing Han +10 more
TL;DR: Guided by first-principles calculations, it was found that Cd single-atom catalysts have excellent performance in activating CO2, and the introduction of axial coordination structure to Cd SACs cannot only further decrease the free energy barrier of CO2 reduction, but also suppress the hydrogen evolution reaction (HER) as discussed by the authors.
References
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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.
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