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
Reads0
Chats0
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
Intermediate Binding Control Using Metal–Organic Frameworks Enhances Electrochemical CO2 Reduction
Dae-Hyun Nam,Osama Shekhah,Geonhui Lee,Arijit Mallick,Hao Jiang,Fengwang Li,Bin Chen,Joshua Wicks,Mohamed Eddaoudi,Edward H. Sargent +9 more
TL;DR: The use of reticular chemistry to control the binding of CO2RR intermediates on metal catalysts encapsulated inside metal-organic frameworks (MOFs) is reported, thereby allowing us to improveCO2RR electrocatalysis.
Journal ArticleDOI
Selective Etching Quaternary MAX Phase toward Single Atom Copper Immobilized MXene (Ti3C2Clx) for Efficient CO2 Electroreduction to Methanol.
Qi Zhao,Chao Zhang,Riming Hu,Zhiguo Du,Jianan Gu,Yanglansen Cui,Xiao Chen,Wenjie Xu,Zongju Cheng,Songmei Li,Bin Li,Yuefeng Liu,Weihua Chen,Chuntai Liu,Jiaxiang Shang,Li Song,Shubin Yang +16 more
TL;DR: In this paper, a single-atom copper immobilized MXene for electrocatalytic CO2 reduction to methanol via selective etching of hybrid A layers (Al and Cu) in quaternary MAX phases (Ti3(Al1-xCux)C2) due to the different saturated vapor pressures of Al and Cu-containing products.
Journal ArticleDOI
Heterogeneous Catalysis for the Valorization of CO2: Role of Bifunctional Processes in the Production of Chemicals
TL;DR: In this paper, the authors present several routes that rely on the use of renewable energy for the transportation of carbon dioxide in the form of CO2 from CO2-rich carbon dioxide feedstock.
Journal ArticleDOI
Modeling the electrical double layer to understand the reaction environment in a CO2 electrocatalytic system
TL;DR: In this paper, the authors resolve the species concentrations and potential profiles in the electrical double layer (EDL) of a CO2ER system by self-consistently solving the migration, diffusion and reaction phenomena using the generalized modified Poisson-Nernst-Planck (GMPNP) equations which include the effect of volume exclusion due to the solvated size of solution species.
Journal ArticleDOI
Covalent Triazine Framework Confined Copper Catalysts for Selective Electrochemical CO2 Reduction: Operando Diagnosis of Active Sites
Lushan Ma,Wei-Bo Hu,Bingbao Mei,Hong Liu,Biao Yuan,Jian Zang,Tao Chen,Liangliang Zou,Zhiqing Zou,Bo Yang,Yi Yu,Jingyuan Ma,Zheng Jiang,Ke Wen,Ke Wen,Hui Yang +15 more
TL;DR: In this paper, the authors developed efficient catalysts for steering the electrochemical CO2 reduction reaction (CO2RR) toward high-value chemicals beyond CO and formic acid.
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