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 overview of flow cell architectures design and optimization for electrochemical CO2 reduction

2021 ◽  
Author(s):  
Dui Ma ◽  
Ting Jin ◽  
Keyu Xie ◽  
Haitao Huang
Keyword(s):  
Carbon Dioxide ◽  
Global Warming ◽  
Electrochemical Reduction ◽  
Atmospheric Carbon Dioxide ◽  
Co2 Reduction ◽  
Value Added ◽  
Flow Cell ◽  
Design And Optimization ◽  
Electrochemical Co2 Reduction ◽  
Carbon Dioxide Levels

Converting CO2 into value-added fuels or chemical feedstocks through electrochemical reduction is one of the several promising avenues to reduce atmospheric carbon dioxide levels and alleviate global warming. This approach...

scholarly journals Turning manganese into gold: Efficient electrochemical CO2 reduction by a fac-Mn(apbpy)(CO)3Br complex in a gas–liquid interface flow cell

2021 ◽  
Vol 416 ◽  
pp. 129050
Author(s):  
Jonathan Filippi ◽  
Laura Rotundo ◽  
Roberto Gobetto ◽  
Hamish A. Miller ◽  
Carlo Nervi ◽  
...  
Keyword(s):  
Co2 Reduction ◽  
Flow Cell ◽  
Liquid Interface ◽  
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...

scholarly journals Operando Synthesis of High-Curvature Copper Thin Films for CO2 Electroreduction

Materials ◽  
2019 ◽  
Vol 12 (4) ◽  
pp. 602
Author(s):  
Xin Zhao ◽  
Minshu Du ◽  
Feng Liu
Keyword(s):  
Flow Rate ◽  
Co2 Reduction ◽  
Product Distribution ◽  
Reconstruction Process ◽  
Time Activity ◽  
Reduction Activity ◽  
Electrochemical Co2 Reduction ◽  
Co2 Electroreduction ◽  
Co2 Flow ◽  
Surface Morphology Modification

As the sole metal that could reduce CO2 to substantial amounts of hydrocarbons, Cu plays an important role in electrochemical CO2 reduction, despite its low energy efficiency. Surface morphology modification is an effective method to improve its reaction activity and selectivity. Different from the pretreated modification method, in which the catalysts self-reconstruction process was ignored, we present operando synthesis by simultaneous electro-dissolution and electro-redeposition of copper during the CO2 electroreduction process. Through controlling the cathodic potential and CO2 flow rate, various high-curvature morphologies including microclusters, microspheres, nanoneedles, and nanowhiskers have been obtained, for which the real-time activity and product distribution is analyzed. The best CO2 electro-reduction activity and favored C2H4 generation activity, with around 10% faradic efficiency, can be realized through extensively distributed copper nanowhiskers synthesized under 40 mL/min flow rate and −2.1 V potential.

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