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 ◽  
...  
Author(s):  
Dui Ma ◽  
Ting Jin ◽  
Keyu Xie ◽  
Haitao Huang

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...


ACS Catalysis ◽  
2018 ◽  
Vol 8 (3) ◽  
pp. 2420-2427 ◽  
Author(s):  
Hyung-Kyu Lim ◽  
Youngkook Kwon ◽  
Han Seul Kim ◽  
Jiwon Jeon ◽  
Yong-Hoon Kim ◽  
...  

Catalysts ◽  
2021 ◽  
Vol 11 (5) ◽  
pp. 535
Author(s):  
Shuaikang Zhu ◽  
Xiaona Ren ◽  
Xiaoxue Li ◽  
Xiaopo Niu ◽  
Miao Wang ◽  
...  

The copper-based catalyst is considered to be the only catalyst for electrochemical carbon dioxide reduction to produce a variety of hydrocarbons, but its low selectivity and low current density to C2 products restrict its development. Herein, a core-shell xZnO@yCu2O catalysts for electrochemical CO2 reduction was fabricated via a two-step route. The high selectivity of C2 products of 49.8% on ZnO@4Cu2O (ethylene 33.5%, ethanol 16.3%) with an excellent total current density of 140.1 mA cm−2 was achieved over this core-shell structure catalyst in a flow cell, in which the C2 selectivity was twice that of Cu2O. The high electrochemical activity for ECR to C2 products was attributed to the synergetic effects of the ZnO core and Cu2O shell, which not only enhanced the selectivity of the coordinating electron, improved the HER overpotential, and fastened the electron transfer, but also promoted the multielectron involved kinetics for ethylene and ethanol production. This work provides some new insights into the design of highly efficient Cu-based electrocatalysts for enhancing the selectivity of electrochemical CO2 reduction to produce high-value C2 products.


2020 ◽  
Vol 59 (3) ◽  
pp. 1883-1892 ◽  
Author(s):  
Changcheng Jiang ◽  
Asa W. Nichols ◽  
John F. Walzer ◽  
Charles W. Machan

2022 ◽  
Author(s):  
Charles Creissen ◽  
José Guillermo Rivera de la Cruz ◽  
Dilan Karapinar ◽  
Dario Taverna ◽  
Moritz Schreiber ◽  
...  

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.


Author(s):  
Peter T. Smith ◽  
Sophia Weng ◽  
Christopher Chang

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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