author:
Yang, Chao
(Yang, Chao.)
[1]
|
Yan, Yaqin
(Yan, Yaqin.)
[2]
|
Hu, Yuncheng
(Hu, Yuncheng.)
[3]
|
Chen, Yangshen
(Chen, Yangshen.)
[4]
|
Guan, Anxiang
(Guan, Anxiang.)
[5]
|
Hu, Cejun
(Hu, Cejun.)
[6]
|
Zhang, Lijuan
(Zhang, Lijuan.)
[7]
|
Zheng, Gengfeng
(Zheng, Gengfeng.)
[8]
Unfold
Abstract:
The electrocatalytic CO2 or CO reduction reaction is a complex proton-coupled electron transfer reaction, in which protons in the electrolyte have a critical effect on the surface adsorbed *H species and the multi-carbon oxygenate products such as ethanol. However, the coupling of *H and carbon-containing intermediates into C2+ oxygenates can be severely hampered by the inappropriate distributions of those species in the catalytic interfaces. In this work, the controlled distribution of highly dispersed CeOx nanoclusters is demonstrated on Cu nanosheets as an efficient CO electroreduction catalyst, with Faradaic efficiencies of ethanol and total oxygenates of 35% and 58%, respectively. The CeOx nanoclusters (2−5 nm) enabled efficient water dissociation and appropriate distribution of adsorbed *H species on the Cu surface with carbon-containing species, thus facilitating the generation of C2+ oxygenate products. In contrast, pristine Cu without CeOx tended to form ethylene, while the aggregated CeOx nanoparticles promoted the surface density of *H and subsequent H2 evolution. © 2024 Wiley-VCH GmbH.
Keyword:
Carbon
Copper
Dissociation
Efficiency
Electrocatalysis
Electrolytes
Electrolytic reduction
Ethanol
Ethylene
Nanoclusters
Population distribution
Classification
405.3 Surveying - 533.1 Ore Treatment - 544.1 Copper - 702 Electric Batteries and Fuel Cells - 761 Nanotechnology - 801.4.1 Electrochemistry - 802.2 Chemical Reactions - 803 Chemical Agents and Basic Industrial Chemicals - 804 Chemical Products Generally - 804.1 Organic Compounds - 902.2 Codes and Standards - 913.1 Production Engineering - 933 Solid State Physics
405.3 Surveying - 533.1 Ore Treatment - 544.1 Copper - 702 Electric Batteries and Fuel Cells - 761 Nanotechnology - 801.4.1 Electrochemistry - 802.2 Chemical Reactions - 803 Chemical Agents and Basic Industrial Chemicals - 804 Chemical Products - 804.1 Organic Compounds - 902.2 Codes and Standards - 913.1 Production Engineering - 933 Solid State Physics
Type
We thank the following funding agencies for supporting this work: the National Natural Science Foundation of China (22025502, U23A20552, 22379026), the Natural Science Foundation of Shanghai (23ZR1407000), and the Science and Technology Commission of Shanghai Municipality (21DZ1206800). The computations in this research were performed using the CFFF platform of Fudan University.
Access Number
EI:20242216188635
Corresponding s email
zhanglijuan@fudan.edu.cngfzheng@fudan.edu.cn