Single-Atom Pt Catalyst for Effective C–F Bond Activation via Hydrodefluorination
Abstract
This paper 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 (Pt1/SiC) using a facile, scalable wet-chemical method developed based on anchor-site and photoreduction techniques. Finally, the high catalytic activity of Pt1/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.
- Authors:
-
[3];
[5];
[6];
[3]
- Beijing Normal Univ. (China). State Key Lab. of Water Environment Simulation. School of Environment; Yale Univ., New Haven, CT (United States). Dept. of Chemical and Environmental Engineering
- Yale Univ., New Haven, CT (United States). Dept. of Chemical and Environmental Engineering; Southern Nevada Water Authority, Las Vegas, NV (United States). Applied Research and Development Center
- Yale Univ., New Haven, CT (United States). Dept. of Chemical and Environmental Engineering
- Brookhaven National Lab. (BNL), Upton, NY (United States). National Synchrotron Light Source-II
- Brookhaven National Lab. (BNL), Upton, NY (United States). Center for Functional Nanomaterials
- Yale Univ., New Haven, CT (United States). Yale Energy Sciences Inst. Dept. of Chemistry
- Dongguan Univ. of Technology (China). School of Environment and Civil Engineering
- Publication Date:
- Research Org.:
- Brookhaven National Laboratory (BNL), Upton, NY (United States); Yale Univ., New Haven, CT (United States)
- Sponsoring Org.:
- USDOE Office of Science (SC); National Science Foundation (NSF); China Scholarship Council (CSC); Swiss National Science Foundation (SNSF)
- OSTI Identifier:
- 1476272
- Report Number(s):
- BNL-209142-2018-JAAM
Journal ID: ISSN 2155-5435
- Grant/Contract Number:
- SC0012704; EEC-1449500; P2EZP2_168796
- Resource Type:
- Accepted Manuscript
- Journal Name:
- ACS Catalysis
- Additional Journal Information:
- Journal Volume: 8; Journal Issue: 10; Journal ID: ISSN 2155-5435
- Publisher:
- American Chemical Society (ACS)
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; C–F bond activation; high platinum loading; hydrodefluorination; hydrogen spillover; silicon carbide; single-atom catalysis
Citation Formats
Huang, Dahong, de Vera, Glen Andrew, Chu, Chiheng, Zhu, Qianhong, Stavitski, Eli, Mao, Jing, Xin, Huolin, Spies, Jacob A., Schmuttenmaer, Charles A., Niu, Junfeng, Haller, Gary L., and Kim, Jae-Hong. Single-Atom Pt Catalyst for Effective C–F Bond Activation via Hydrodefluorination. United States: N. p., 2018.
Web. doi:10.1021/acscatal.8b02660.
Huang, Dahong, de Vera, Glen Andrew, Chu, Chiheng, Zhu, Qianhong, Stavitski, Eli, Mao, Jing, Xin, Huolin, Spies, Jacob A., Schmuttenmaer, Charles A., Niu, Junfeng, Haller, Gary L., & Kim, Jae-Hong. Single-Atom Pt Catalyst for Effective C–F Bond Activation via Hydrodefluorination. United States. https://doi.org/10.1021/acscatal.8b02660
Huang, Dahong, de Vera, Glen Andrew, Chu, Chiheng, Zhu, Qianhong, Stavitski, Eli, Mao, Jing, Xin, Huolin, Spies, Jacob A., Schmuttenmaer, Charles A., Niu, Junfeng, Haller, Gary L., and Kim, Jae-Hong. Mon .
"Single-Atom Pt Catalyst for Effective C–F Bond Activation via Hydrodefluorination". United States. https://doi.org/10.1021/acscatal.8b02660. https://www.osti.gov/servlets/purl/1476272.
@article{osti_1476272,
title = {Single-Atom Pt Catalyst for Effective C–F Bond Activation via Hydrodefluorination},
author = {Huang, Dahong and de Vera, Glen Andrew and Chu, Chiheng and Zhu, Qianhong and Stavitski, Eli and Mao, Jing and Xin, Huolin and Spies, Jacob A. and Schmuttenmaer, Charles A. and Niu, Junfeng and Haller, Gary L. and Kim, Jae-Hong},
abstractNote = {This paper 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 (Pt1/SiC) using a facile, scalable wet-chemical method developed based on anchor-site and photoreduction techniques. Finally, the high catalytic activity of Pt1/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.},
doi = {10.1021/acscatal.8b02660},
journal = {ACS Catalysis},
number = 10,
volume = 8,
place = {United States},
year = {Mon Sep 10 00:00:00 EDT 2018},
month = {Mon Sep 10 00:00:00 EDT 2018}
}
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