文献类型：期刊文献

中文题名：Installation of high-valence tungsten in MIL-125(Ti) for boosted photocatalytic hydrogen evolution

英文题名：MIL-125(Ti)中引入高价态钨元素以促进光催化产氢性能

作者：Yijun Zhang[1];Fangxin Mao[1];Yuanwei Liu[1];Xuefeng Wu[1];Chunfang Wen[1];Sheng Dai[2];Pengfei Liu[1];Huagui Yang[1]

机构：[1]Key Laboratory for Ultrafine Materials of Ministry of Education,Shanghai Engineering Research Center of Hierarchical Nanomaterials,School of Materials Science and Engineering,East China University of Science and Technology,Shanghai 200237,China;[2]Key Laboratory for Advanced Materials and Feringa Nobel Prize Scientist Joint Research Center,Institute of Fine Chemicals,School of Chemistry and Molecular Engineering,East China University of Science and Technology,Shanghai 200237,China

年份：2022

卷号：65

期号：5

起止页码：1237

中文期刊名：Science China Materials

外文期刊名：中国科学（材料科学（英文版）

收录：CSTPCD;;Scopus;CSCD:【CSCD2021_2022】；PubMed;

基金：This work was financially supported by the National Natural Science Funds for Distinguished Young Scholars (51725201), the International (Regional) Cooperation and Exchange Projects of the National Natural Science Foundation of China (51920105003), the Innovation Program of Shanghai Municipal Education Commission (E00014), China Postdoctoral Science Foundation Funded Project (2020M681201) and Shanghai Engineering Research Center of Hierarchical Nanomaterials (18DZ2252400). The authors acknowledge the Fundamental Research Funds for the Central Universities (JKD01211519). The authors also thank the Frontiers Science Center for Materiobiology and Dynamic Chemistry, and crew of the 1W1B beamline of the Beijing Synchrotron Radiation Facility for the constructive assistance in the XAFS measurements and data analysis. Dai S acknowledges the support by Shanghai Rising-star Program (20QA1402400) and the Program for Professor of Special Appointment (Eastern Scholar) at Shanghai Institutions of Higher Learning. Additional support was provided by the Feringa Nobel Prize Scientist Joint Research Center.

语种：英文

中文关键词：high-valence state;metal-organic frameworks;metal-to-cluster charge transfer;photocatalytic hydrogen production

摘要：Metal-organic frameworks(MOFs) possess the features of highly porosity-tunable and electronic-tunable structures,. Taking advantages of these merits, we successfully installed high-valence W6+ions onto the Ti-oxo clusters of MIL-125(Ti)(W-MIL-125). The installed W^(6+) ions which form a W–O–Ti structure trigger the metal-to-cluster charge transfer(MCCT), together with an enhanced light absorption.Structural and spectroscopic characterizations reveal that the MCCT process optimizes the charge transfer process and efficiently separates the photogenerated electron-hole spatially.The as-obtained sample of 3.45 W-MIL-125 with optimized electronic structure demonstrates an enhanced photocatalytic hydrogen evolution performance of 1110.7 ± 63.7 μmol g^(-1)h^(-1) under light irradiation, which is 4.0 times that of the pristine MIL-125(Ti). This work will open up a new avenue for local structural modification of MOFs to boost photocatalytic performance.
金属有机框架(Metal-organic frameworks, MOFs)材料具有高度可调控的多孔结构以及电子结构,在光催化领域非常有前景.本文利用MOFs的上述特性,将高价态的钨元素连接在MIL-125(Ti)中的Ti-oxo团簇上,得到了W-MIL-125.形成的W–O–Ti结构引发了从金属到团簇的电荷传输(Metal-to-cluster charge transfer, MCCT),且W-MIL-125具有更好的吸光性能.结构和谱学表征证明, MCCT过程能优化电荷的传输路径,有效地实现了载流子空间分离. W-MIL-125在光照条件下展现出更高的产氢性能,高达1110.7±63.7μmol g^(-1)h^(-1),是本体样品产氢速率的4.0倍.本工作为MOFs基材料的局域结构改性以提升光催化性能提供了新的思路.