文献类型：期刊文献

英文题名：Br?nsted Acid-Driven Dynamic LMCT Sites Transform Pt/Zeolite Into a Light-Responsive Oxidation Platform

作者：Han, Xiaowei[1];Chen, Tangxuan[1];Zhang, Qingqing[1];Cheng, Jingxian[1];Wu, Xiao[1];Zhang, Jinlong[1];Hu, Yun[2];Lei, Juying[3];Zhou, Liang[3];Ye, Ziwei[1];Wang, Lingzhi[1]

机构：[1]East China Univ Sci & Technol, Inst Fine Chem, Sch Chem & Mol Engn, State Key Lab Green Chem Engn & Ind Catalysis, Shanghai, Peoples R China;[2]South China Univ Technol, Sch Environm & Energy, Guangzhou, Peoples R China;[3]East China Univ Sci & Technol, State Environm Protect Key Lab Environm Risk Asses, Shanghai, Peoples R China

年份：2026

外文期刊名：SMALL

收录：;EI(收录号：20262821065229);Scopus(收录号：2-s2.0-105043931079);WOS:【SCI-EXPANDED(收录号:WOS:001813709600001)】；

基金：National Natural Science Foundation of China (Nos. 22472056 and 22461142136), Science and Technology Commission of Shanghai Municipality (No. 24ZR1491000), Fundamental Research Funds for the Central Universities (No. 222201717003).

语种：英文

外文关键词：br & oslash;nsted acid; LMCT; O2 activation; photothermal catalysis; Pt complex

摘要：Photocatalysis provides a low-temperature oxidation route, yet typically underperforms thermal catalysis owing to inefficient O2 activation and limited surface-bounded intermediates utilization. Here, a conventional Pt/zeolite catalyst is transformed into a photothermal-photoelectronic platform by leveraging Br & oslash;nsted acid-mediated dynamic ligand-to-metal charge transfer (LMCT) sites. Using toluene oxidation over Pt/ZSM-5 as a model, we show that benzyl alcohol formed under UV irradiation undergoes acid-assisted deprotonation and coordinates with Pt, forming Pt-O-CH2-Ar complexes. These species enable visible-light absorption and O2 activation via LMCT mechanism, thereby significantly enhancing the oxidation efficiency. This UV-enabled formation and visible-light-triggered LMCT excitation of surface intermediates merges photothermal effects and photoelectronic effects, achieving complete degradation of 1000 ppm toluene under light-only conditions at 240-480 L g-1 h-1 with only 0.5 wt.% Pt. The strategy extends to other aromatic hydrocarbons through alcohol- or phenol-type intermediates. This study establishes a general approach to boost light-driven O2 activation through dynamic intermediate coordination, opening avenues for energy-efficient oxidation.