In Situ Implanting of Single Tungsten Sites into Defective UiO-66(Zr) by Solvent-Free Route for Efficient Oxidative Desulfurization at Room Temperature

被引：111

作者：

Ye, Gan ^{[1
,2
]}

Wang, Hanlu ^{[1
,3
]}

Chen, Wenxing ^{[4
]}

Chu, Hongqi ^{[5
]}

Wei, Jinshan ^{[1
,2
]}

Wang, Dagang ^{[1
]}

Wang, Jin ^{[1
]}

Li, Yadong ^{[6
]}

机构：

[1] Shenzhen Univ, Coll Mat Sci & Engn, Shenzhen 518060, Peoples R China

[2] Shenzhen Univ, Key Lab Optoelectron Devices & Syst, Minist Educ & Guangdong Prov, Coll Optoelectron Engn, Shenzhen 518060, Peoples R China

[3] Guangdong Univ Petrochem Technol, Coll Chem Engn, Maoming 525000, Peoples R China

[4] Beijing Inst Technol, Beijing Key Lab Construct Tailorable Adv Funct Ma, Sch Mat Sci & Engn, Beijing 100081, Peoples R China

[5] Harbin Inst Technol, Sch Chem & Chem Engn, Harbin 150001, Peoples R China

[6] Tsinghua Univ, Dept Chem, Beijing 100084, Peoples R China

来源：

ANGEWANDTE CHEMIE-INTERNATIONAL EDITION | 2021年 / 60卷 / 37期

基金：

中国国家自然科学基金; 中国博士后科学基金;

关键词：

oxidative desulfurization; single site; solvent-free; tungsten; UiO-66(Zr); METAL-ORGANIC-FRAMEWORK; ZR-WOX CLUSTERS; IONIC LIQUID; ACID; CATALYSTS; OXIDES; FUEL; POROSITY; MOFS;

D O I：

10.1002/anie.202107018

中图分类号：

O6 [化学];

学科分类号：

0703 ;

摘要：

Design of single-site catalysts with catalytic sites at atomic-scale and high atom utilization, provides new opportunities to gain superior catalytic performance for targeted reactions. In this contribution, we report a one-pot green approach for in situ implanting of single tungsten sites (up to 12.7 wt.%) onto the nodes of defective UiO-66(Zr) structure via forming Zr-O-W bonds under solvent-free condition. The catalysts displayed extraordinary activity for the oxidative removal of sulfur compounds (1000 ppm S) at room temperature within 30 min. The turnover frequency (TOF) value can reach 44.0 h(-1) at 30 degrees C, which is 109.0, 12.3 and 1.2 times higher than that of pristine UiO-66(Zr), WO3, and WCl6 (homogeneous catalyst). Theoretical and experimental studies show that the anchored W sites can react with oxidant readily and generate W-VI-peroxo intermediates that determine the reaction activity. Our work not only manifests the application of SSCs in the field of desulfurization of fuel oil but also opens a new solvent-free avenue for fabricating MOFs based SSCs.

引用

页码：20318 / 20324

页数：7