Single-Atom Pt Catalyst for Effective C-F Bond Activation via Hydrodefluorination

被引:79
作者
Huang, Dahong [1 ,2 ]
de Vera, Glen Andrew [2 ,3 ]
Chu, Chiheng [2 ]
Zhu, Qianhong [2 ]
Stavitski, Eli [4 ]
Mao, Jing [5 ]
Xin, Huolin [5 ]
Spies, Jacob A. [6 ,7 ]
Schmuttenmaer, Charles A. [6 ,7 ]
Niu, Junfeng [8 ]
Haller, Gary L. [2 ]
Kim, Jae-Hong [2 ]
机构
[1] Beijing Normal Univ, Sch Environm, State Key Lab Water Environm Simulat, Beijing 100875, Peoples R China
[2] Yale Univ, Dept Chem & Environm Engn, New Haven, CT 06520 USA
[3] Southern Nevada Water Author, Appl Res & Dev Ctr, Las Vegas, NV 89193 USA
[4] Brookhaven Natl Lab, Natl Synchrotron Light Source 2, Upton, NY 11973 USA
[5] Brookhaven Natl Lab, Ctr Funct Nanomat, Upton, NY 11973 USA
[6] Yale Univ, Yale Energy Sci Inst, New Haven, CT 06520 USA
[7] Yale Univ, Dept Chem, 225 Prospect St, New Haven, CT 06520 USA
[8] Dongguan Univ Technol, Sch Environm & Civil Engn, Dongguan 523808, Guangdong, Peoples R China
基金
美国国家科学基金会; 瑞士国家科学基金会;
关键词
C-F bond activation; single-atom catalysis; hydrodefluorination; high platinum loading; silicon carbide; hydrogen spillover; PERFLUOROOCTANE SULFONATE PFOS; HYDROGEN-EVOLUTION; EFFICIENT; ACID; MECHANISMS; PLATINUM; CARBON; DEFLUORINATION; SURFACTANTS; ELECTRODE;
D O I
10.1021/acscatal.8b02660
中图分类号
O64 [物理化学(理论化学)、化学物理学];
学科分类号
070304 ; 081704 ;
摘要
This study presents a single-atom Pt catalyst that achieves efficient C-F bond activation, which is a challenging reaction in both chemical synthesis and environmental remediation of recalcitrant fluorinated hydrocarbons. Up to 1.6 wt % Pt was loaded as a single-atom on SiC substrate (Pt-1/SiC) using a facile, scalable wet-chemical method developed based on anchor-site and photoreduction techniques. The high catalytic activity of Pt-1/SiC for hydrodefluorination of perfluorooctanoic acid, which is a select perfluorinated pollutant of significant environmental concern, is attributed to the effective hydrogen spillover from isolated Pt onto the SiC surface where the resulting Si-H bond further redistributes with the C-F bond to accomplish hydrodefluorination.
引用
收藏
页码:9353 / 9358
页数:11
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