Journal
ACS NANO
Volume 15, Issue 1, Pages 1039-1047Publisher
AMER CHEMICAL SOC
DOI: 10.1021/acsnano.0c07869
Keywords
copper; lead; core-shell; synergy; CO2 reduction reaction
Categories
Funding
- Ministry of Science and Technology [2017YFA0208200, 2016YFA0204100]
- National Natural Science Foundation of China [21571135, 21905188, 21975148]
- Natural Science Foundation of Jiangsu Higher Education Institutions [SBK20190810]
- Young Thousand Talented Program
- Jiangsu Province Natural Science Fund for Distinguished Young Scholars [BK20170003]
- Jiangsu Province High-Level Talents [JNHB-106]
- China Postdoctoral Science Foundation [2019M651937, 2019M660128]
- Guangdong Provincial Key Laboratory of Energy Materials for Electric Power [2018B030322001]
- Priority Academic Program Development of Jiangsu Higher Education Institutions (PAPD)
- Program for Jiangsu Specially-Appointed Professors
- Soochow University
- Collaborative Innovation Center of Suzhou Nano Science and Technology
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The synergistic effect between Cu core and ultrathin Pb shell in Cu/Pb core/shell nanocrystals significantly enhances the electrocatalytic reduction of CO2 toward C2+ liquid products, leading to higher Faradaic efficiency and selectivity. This study highlights the importance of synergistic effect in the design of efficient Cu-based catalysts for CO2 reduction.
The design of efficient copper-based (Cu-based) carbon dioxide reduction (CO2 RR) electrocatalysts is crucial for converting CO2 to value-added liquid products. In this work, we demonstrate that the strong synergy between Cu core and ultrathin lead (Pb) shell (0.7 nm) in the Cu/Pb core/shell nanocrystals (NCs, CuPb-0.7/C) significantly boosts the electrocatalytic reduction of CO2 toward C2+ products (products with at least two carbon atoms). Specifically, when applying in a flow cell system, the Faradaic efficiency (FE) of total C2+ products and the selectivity of C2+ liquid products are as high as 81.640 and -19.590, respectively. Moreover, the current density of C2+ liquid products reaches 196.8 mA cm(-2), outperforming most of the reported Cu-based catalysts for CO2 RR toward the production of C2+ liquid products. Density functional theory calculations indicate that the synergized Cu/Pb core/shell NCs reduce the formation energies of *COOH and *OCCOH intermediates, as the two critical intermediates for the reduction of CO2 to CO and the formation of C2+ products, respectively, and leads to the significant increase in the selectivity of C-2(+) liquid products. This study provides a efficient Cu-based catalyst for the reduction of CO2, highlighting the importance of synergistic effect for the design of electrocatalysts in catalysis.
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