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Boosted C–C coupling with Cu–Ag alloy sub-nanoclusters for CO <sub>2</sub> -to-C <sub>2</sub> H <sub>4</sub> photosynthesis

Yangyang YuResearch Center for Carbon-Neutral Environmental &amp; Energy Technology, Institute of Fundamental and Frontier Sciences, University of Electronic Science and Technology of China, Chengdu 611731, ChinaYe HeSchool of Resources and Environment, University of Electronic Science and Technology of China, Chengdu 611731, ChinaPing YanResearch Center for Carbon-Neutral Environmental &amp; Energy Technology, Institute of Fundamental and Frontier Sciences, University of Electronic Science and Technology of China, Chengdu 611731, ChinaShengyao WangCollege of Science, Huazhong Agricultural University, Wuhan 430070, ChinaFan DongResearch Center for Carbon-Neutral Environmental &amp; Energy Technology, Institute of Fundamental and Frontier Sciences, University of Electronic Science and Technology of China, Chengdu 611731, China
2023en
ABI

Аннотация

The selective photocatalytic conversion of CO 2 and H 2 O to high value-added C 2 H 4 remains a great challenge, mainly attributed to the difficulties in C–C coupling of reaction intermediates and desorption of C 2 H 4 * intermediates from the catalyst surface. These two key issues can be simultaneously overcome by alloying Ag with Cu which gives enhanced activity to both reactions. Herein, we developed a facile stepwise photodeposition strategy to load Cu–Ag alloy sub-nanoclusters (ASNCs) on TiO 2 for CO 2 photoreduction to produce C 2 H 4 . The optimized catalyst exhibits a record-high C 2 H 4 formation rate (1110.6 ± 82.5 μmol g −1 h −1 ) with selectivity of 49.1 ± 1.9%, which is an order-of-magnitude enhancement relative to current work for C 2 H 4 photosynthesis. The in situ FT-IR spectra combined with DFT calculations reveal the synergistic effect of Cu and Ag in Cu–Ag ASNCs, which enable an excellent C–C coupling capability like Ag and promoted C 2 H 4 * desorption property like Cu, thus advancing the selective and efficient production of C 2 H 4 . The present work provides a deeper understanding on cluster chemistry and C–C coupling mechanism for CO 2 reduction on ASNCs and develops a feasible strategy for photoreduction CO 2 to C 2 fuels or industrial feedstocks.

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