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 Kang^1,2*

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