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Anchoring subnanometric Cu4 clusters in graphitic-C3N5 for highly efficient CO2 photoreduction to ethanol
Energy & Environmental Science ( IF 32.4 ) Pub Date : 2024-12-05 , DOI: 10.1039/d4ee02449d Entian Cui, Yulian Lu, Xiu-Li Yang, Guojun Dong, Yajun Zhang, Yingpu Bi
Energy & Environmental Science ( IF 32.4 ) Pub Date : 2024-12-05 , DOI: 10.1039/d4ee02449d Entian Cui, Yulian Lu, Xiu-Li Yang, Guojun Dong, Yajun Zhang, Yingpu Bi
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We demonstrated a facile electrochemical treatment for in situ anchoring of subnanometric Cu4 clusters in a graphitic C3N5 framework (Cu4/C3N5), leading to remarkable improvements of photocatalytic reactivity and selectivity for CO2 reduction to ethanol. In the absence of a sacrificial reagent, a record ethanol production activity of 32.2 μmol g−1 h−1 with 98.6% selectivity has been achieved under visible light irradiation (λ ≥ 420 nm). In situ characterizations and theoretical calculations reveal that the significant improvement of reactivity and selectivity should be attributed to the coexisting Cu+ and Cu0 double active-sites in Cu4/C3N5 catalysts for a highly efficient C–C coupling process. More specifically, the electron enriched Cu0 active sites could efficiently promote adsorption/activation of CO2 molecules to form *CO intermediates, which partially transferred to adjacent Cu+ sites for preferential C–C coupling to generate *COCO intermediates. After the subsequent hydrogenation process, the photocatalytic CO2-to-ethanol conversion has been achieved.
更新日期：2024-12-05
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