Jian-Peng Dong, Yue Xu, Ling Yao, Le Wang, Gang Li, Rui Wang, Shuang-Quan Zang
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引用次数: 0
Abstract
Copper nanoclusters (Cu NCs) have emerged as a remarkable class of CO2 reduction reaction catalysts that are distinguished by their unparalleled reactivity, but effectively modulating the transport pathway of charge carriers between Cu NCs by feasible chemical means is still challenging. Herein, a thermally induced covalent crosslinking strategy is proposed to modulate the fast electron transport pathway formed between clusters. A copper-sulfur-nitrogen cluster [Cu4(SN)4] (denoted Cu4SN) is first synthesized; subsequently, the SN ligands in Cu4SN are coupled covalently via a thermally induced covalent crosslinking strategy to yield CC-Cu4SN, which exhibits enhanced conductivity and photocarrier transport. As expected, CC-Cu4SN shows a high photocatalytic CO production rate of 29.98 µmol g-1 h-1 with ≈99.5% selectivity in CO2 reduction with H2O as sacrificial agents, which is more than 10 times superior to that observed with Cu4SN. Systematic experiments and density functional theory calculations reveal that the covalent crosslinks between clusters accelerate the dynamic transfer of photoexcited charge carriers, increase the light utilization ability, favor CO2 adsorption and *COOH generation, thereby accounting for the increased CO2 photoreduction activity. This work presents a novel thermally induced internal covalent crosslinking strategy for synthesizing novel cluster-based covalent polymers with enhanced stability and catalytic activity.
期刊介绍:
Advanced Science is a prestigious open access journal that focuses on interdisciplinary research in materials science, physics, chemistry, medical and life sciences, and engineering. The journal aims to promote cutting-edge research by employing a rigorous and impartial review process. It is committed to presenting research articles with the highest quality production standards, ensuring maximum accessibility of top scientific findings. With its vibrant and innovative publication platform, Advanced Science seeks to revolutionize the dissemination and organization of scientific knowledge.