题目: | A metal-free cascaded process for efficient H2O2 photoproduction using conjugated carbonyl sites |
作者: | Tiwei He1, Hongchao Tang1, Jie Wu1, Jiaxuan Wang1, Mengling Zhang1, Cheng Lu1, Hui Huang1, Jun Zhong1, Tao Cheng1*, Yang Liu1* & Zhenhui Kang1,2* |
单位: | 1Institute of Functional Nano & Soft Materials (FUNSOM), Jiangsu Key Laboratory for Carbon-Based Functional Materials & Devices, Soochow University, Suzhou, Jiangsu 215123, China. 2Macao Institute of Materials Science and Engineering (MIMSE), MUST−SUDA Joint Research Center for Advanced Functional Materials, Macau University of Science and Technology, Taipa, Macau 999078, China. |
摘要: | Carbon-based metal-free catalysts are promising green catalysts for photocatalysis and electrocatalysis due to their low cost and environmental friendliness. A key challenge in utilizing these catalysts is identifying their active sites, given their poor crystallinity and complex structures. Here we demonstrate the key structure of the double-bonded conjugated carbon group as a metal-free active site, enabling efficient O2 photoreduction to H2O2 through a cascaded water oxidation−O2 reduction process. Using ethylenediaminetetraacetic acid as a precursor, we synthesized various carbon-based photocatalysts and analyzed their structural evolution. Under the polymerization conditions of 260 ℃ to 400 ℃, an N-ethyl-2-piperazinone-like structure was formed on the surface of the catalyst, resulting in high photocatalytic H2O2 photoproduction (2884.7 μmol g−1h−1) under visible light. A series of control experiments and theoretical calculations further confirm that the double-bond conjugated carbonyl structure is the key and universal feature of the active site of metal-free photocatalysts. |
影响因子: | 14.7 |
分区情况: | 一区 |
链接: | https://doi.org/10.1038/s41467-024-52162-3 |
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