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
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Journal ArticleDOI
Towards membrane-electrode assembly systems for CO2 reduction: a modeling study
TL;DR: In this article, a multiphysics model was developed to investigate the fundamental limitations of two MEA designs: one with gaseous feeds at both the anode and cathode (full-MEA), and the other with an aqueous anode feed (KHCO3 or KOH exchange solution) and a Gaseous cathode feed(exchange MEA).
Journal ArticleDOI
Rational catalyst design for N2 reduction under ambient conditions: Strategies towards enhanced conversion efficiency
TL;DR: Ammonia (NH3), one of the basic chemicals in most fertilizers and a promising carbon-free energy storage carrier, is typically synthesized via the Haber-Bosch process with high energy consumption as discussed by the authors.
Journal ArticleDOI
Branched Copper Oxide Nanoparticles Induce Highly Selective Ethylene Production by Electrochemical Carbon Dioxide Reduction
TL;DR: The initial branched copper oxide structure formed highly active domains with interfaces and junctions in-between during activation, which caused large surface area with high local pH leading to high selectivity and activity for ethylene production.
Journal ArticleDOI
Photoelectrochemical Synthesis of Ammonia on the Aerophilic-Hydrophilic Heterostructure with 37.8% Efficiency
Jianyun Zheng,Jianyun Zheng,Yanhong Lyu,Yanhong Lyu,Man Qiao,Ruilun Wang,Yangyang Zhou,Hao Li,Chen Chen,Yafei Li,Huaijuan Zhou,San Ping Jiang,Shuangyin Wang +12 more
TL;DR: In this paper, a unique aerophilic-hydrophilic heterostructured Si-based photocathode was designed for nitrogen-to-ammonia fixation in an acid electrolyte under mild conditions.
Journal ArticleDOI
Opportunities and Challenges for Catalysis in Carbon Dioxide Utilization
TL;DR: The environmental and societal consequences of the increasing levels of carbon dioxide in our atmosphere are among the most significant challenges society currently faces as discussed by the authors, and carbon dioxide utilisation is one of the most important challenges.
References
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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.
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