Journal
ACS CATALYSIS
Volume 9, Issue 6, Pages 4824-4833Publisher
AMER CHEMICAL SOC
DOI: 10.1021/acscatal.9b00862
Keywords
dynamic evolution; atomically dispersed; Cu species; photocatalysis; CO2 reduction
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Funding
- National Natural Science Foundation of China (NSFC) [21872029, U1463204, 21173045]
- Award Program for Minjiang Scholar Professorship
- Natural Science Foundation (NSF) of Fujian Province for Distinguished Young Investigator Rolling Grant [2017J07002]
- State Key Laboratory of Photocatalysis on Energy and Environment [2014A05]
- first Program of Fujian Province for Top Creative Young Talents
- Program for Returned High-Level Overseas Chinese Scholars of Fujian province
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Probing the dynamic evolution of catalyst structure and chemical state under operating conditions is highly important for investigating the reaction mechanism of catalysis more in depth, which in turn advances the rational design of redox catalysis in using renewable energy to produce fuels. Herein, the evolution of atomically dispersed Cu species supported by mesoporous TiO2 (mTiO(2)) during the in situ photocatalytic reduction of CO, with H2O to valuable solar fuels has been reported. The results unveil that the initial atomically dispersed Cu(II) undergoes reduction to Cu(I) and ultimately to Cu(0); the Cu(I)/Cu(0) mixture is proposed to be more effective for CH4 formation. In addition, the enhanced CO, adsorption ability benefited from the structural advantage of mTiO(2) and the elevated charge carrier transfer synergistically contributes to the CO, photoreduction. It is anticipated that this work would guide the rational design of Cu-based light-harvesting catalysts for artificial CO2 reduction to value-added feedstocks and inspire further interest in using in situ techniques to study the structure-activity interplay of photocatalysts under operating reaction conditions.
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