scholarly journals Optimizing C–C Coupling on Oxide-Derived Copper Catalysts for Electrochemical CO2 Reduction

2017 ◽  
Vol 121 (26) ◽  
pp. 14191-14203 ◽  
Author(s):  
Yanwei Lum ◽  
Binbin Yue ◽  
Peter Lobaccaro ◽  
Alexis T. Bell ◽  
Joel W. Ager
Keyword(s):  
Co2 Reduction ◽  
Copper Catalysts ◽  
Electrochemical Co2 Reduction

scholarly journals Operando surface chemistry of micro- and nanocubic copper catalysts for electrochemical CO2 reduction

2021 ◽  
Author(s):  
Karla Banjac ◽  
Thanh Hai Phan ◽  
Fernando P. Cometto ◽  
Patrick Alexa ◽  
Yunchang Liang ◽  
...  
Keyword(s):  
Co2 Reduction ◽  
Copper Catalysts ◽  
Product Formation ◽  
Atomic Processes ◽  
Renewable Chemicals ◽  
Electrochemical Co2 Reduction ◽  
Tunnelling Microscopy ◽  
Reduction Of Co2 ◽  
Cu Nanostructures

The electrochemical reduction of CO2 (CO2RR) into multicarbon compounds is a promising pathway towards renewable chemicals. Structure-product selectivity studies highlight that copper (100) facets favour C2+ product formation. However, the atomic processes leading to the formation of (100)-rich Cu cubes remains elusive. Herein, we use Cu and graphene-protected Cu surfaces to reveal the differences in structure and composition of common Cu-based electrocatalysts, from nano to micrometer scales. We show that stripping/electrodeposition cycles lead to thermodynamically controlled growth of Cu2O micro/nanocubes, while multi-layered Cu nanocuboids form universally during CO2RR upon polarization-driven re-organization of Cu0 atoms. A synergy of electrochemical characterization by scanning tunnelling microscopy (EC-STM), operando EC-Raman and quasi-operando X-Ray Photoemission spectroscopy (XPS) allows us to shed light on the role of oxygen on the dynamic interfacial processes of Cu, and to demonstrate that chloride is not needed for the stabilization of cubic Cu nanostructures.

scholarly journals In situ study of surface species and structure over Oxide-Derived Copper Catalysts for Electrochemical CO2 Reduction

2021 ◽  
Author(s):  
Chunjun Chen ◽  
Xupeng Yan ◽  
Yahui Wu ◽  
Shoujie Liu ◽  
Xiaofu Sun ◽  
...  
Keyword(s):  
Co2 Reduction ◽  
Copper Catalysts ◽  
Reaction Process ◽  
Real Structure ◽  
Surface Species ◽  
The Real ◽  
Effective Catalyst ◽  
In Situ Study ◽  
Electrochemical Co2 Reduction

The oxide-derived copper (OD-Cu) has been discovered as effective catalyst for electroreduction of CO2 to C2+ products. The real structure of the OD-Cu and surface species in the reaction process...

Covalent Triazine Framework Confined Copper Catalysts for Selective Electrochemical CO2 Reduction: Operando Diagnosis of Active Sites

ACS Catalysis ◽  
2020 ◽  
Vol 10 (8) ◽  
pp. 4534-4542 ◽  
Author(s):  
Lushan Ma ◽  
Weibo Hu ◽  
Bingbao Mei ◽  
Hong Liu ◽  
Biao Yuan ◽  
...  
Keyword(s):  
Active Sites ◽  
Co2 Reduction ◽  
Copper Catalysts ◽  
Electrochemical Co2 Reduction ◽  
Covalent Triazine Framework

Molecular Inhibition for Selective CO2 Conversion

2022 ◽  
Author(s):  
Charles Creissen ◽  
José Guillermo Rivera de la Cruz ◽  
Dilan Karapinar ◽  
Dario Taverna ◽  
Moritz Schreiber ◽  
...  
Keyword(s):  
Heterogeneous Catalysts ◽  
Co2 Reduction ◽  
Copper Catalysts ◽  
Reaction Rates ◽  
Product Distribution ◽  
Flow Cell ◽  
Novel Approach ◽  
Electrochemical Co2 Reduction ◽  
Conventional Material ◽  
Formate Production

Electrochemical CO2 reduction presents a sustainable route to the production of chemicals and fuels. Achieving a narrow product distribution with copper catalysts is challenging and conventional material modifications offer limited control over selectivity. Here, we show that the mild cathodic potentials required to reach high currents in an alkaline gas-fed flow cell permits retention of a surface-bound thiol (4-mercaptopyridine), enabling molecule-directed selective formate generation at high reaction rates. Combined experimental and computational results showed that formate production is favoured due to the inhibition of a CO producing pathway caused by destabilising interactions with the anchored molecule. The immobilisation of molecules to inhibit specific carbon-based products therefore offers a novel approach to rationally tune the selectivity of heterogeneous catalysts.

An NADH-Inspired Redox Mediator Strategy to Promote Second-Sphere Electron and Proton Transfer for Cooperative Electrochemical CO2 Reduction Catalyzed by Iron Porphyrin

2020 ◽  
Author(s):  
Peter T. Smith ◽  
Sophia Weng ◽  
Christopher Chang
Keyword(s):  
Proton Transfer ◽  
Co2 Reduction ◽  
Iron Porphyrin ◽  
Redox Mediators ◽  
Reservoir Properties ◽  
Proton Reduction ◽  
Electrochemical Co2 Reduction ◽  
Starting Point ◽  
Rate Improvement ◽  
Molecular Catalysts

We present a bioinspired strategy for enhancing electrochemical carbon dioxide reduction catalysis by cooperative use of base-metal molecular catalysts with intermolecular second-sphere redox mediators that facilitate both electron and proton transfer. Functional synthetic mimics of the biological redox cofactor NADH, which are electrochemically stable and are capable of mediating both electron and proton transfer, can enhance the activity of an iron porphyrin catalyst for electrochemical reduction of CO<sub>2</sub> to CO, achieving a 13-fold rate improvement without altering the intrinsic high selectivity of this catalyst platform for CO<sub>2</sub> versus proton reduction. Evaluation of a systematic series of NADH analogs and redox-inactive control additives with varying proton and electron reservoir properties reveals that both electron and proton transfer contribute to the observed catalytic enhancements. This work establishes that second-sphere dual control of electron and proton inventories is a viable design strategy for developing more effective electrocatalysts for CO<sub>2</sub> reduction, providing a starting point for broader applications of this approach to other multi-electron, multi-proton transformations.

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