Site-Selective Loading of Single-Atom Pt on TiO2 for Photocatalytic Oxidation and Reductive Hydrodefluorination

  • Seunghyun Weon
    Seunghyun Weon
    Department of Chemical and Environmental Engineering and Nanosystems Engineering Research Center for Nanotechnology-Enabled Water Treatment (NEWT), Yale University, New Haven, Connecticut 06511, United States
    School of Health and Environmental Science, Korea University, Seoul 02841, Republic of Korea
  • Min-Jeong Suh
    Min-Jeong Suh
    Department of Chemical and Environmental Engineering and Nanosystems Engineering Research Center for Nanotechnology-Enabled Water Treatment (NEWT), Yale University, New Haven, Connecticut 06511, United States
  • Chiheng Chu
    Chiheng Chu
    Department of Chemical and Environmental Engineering and Nanosystems Engineering Research Center for Nanotechnology-Enabled Water Treatment (NEWT), Yale University, New Haven, Connecticut 06511, United States
    Department of Environmental Science, Zhejiang University, Hangzhou 310058, China
    More by Chiheng Chu
  • Dahong Huang
    Dahong Huang
    Department of Chemical and Environmental Engineering and Nanosystems Engineering Research Center for Nanotechnology-Enabled Water Treatment (NEWT), Yale University, New Haven, Connecticut 06511, United States
    More by Dahong Huang
  • Eli Stavitski
    Eli Stavitski
    National Synchrotron Light Source-II, Brookhaven National Laboratory, Upton, New York 11973, United States
  • , and 
  • Jae-Hong Kim*
    Jae-Hong Kim
    Department of Chemical and Environmental Engineering and Nanosystems Engineering Research Center for Nanotechnology-Enabled Water Treatment (NEWT), Yale University, New Haven, Connecticut 06511, United States
    *Phone: +1 (203) 432-4386. E-mail: [email protected]
    More by Jae-Hong Kim
Cite this: ACS EST Engg. 2021, 1, 3, 512–522
Publication Date (Web):February 2, 2021
https://doi.org/10.1021/acsestengg.0c00210
Copyright © 2021 American Chemical Society
Article Views
1658
Altmetric
-
Citations
LEARN ABOUT THESE METRICS
Read OnlinePDF (6 MB)
Supporting Info (1)»

Abstract

Separating the redox sites of photocatalysts is one of most promising strategies to promote an efficient photoinduced charge transfer of semiconductor photocatalysis. Herein, we present a site-selective loading of single-atom Pt (Pt1) on facet-engineered TiO2 to achieve decomposition of recalcitrant halogenated water pollutants, including perfluorooctanoic acid (PFOA). Positively charged Pt1 are atomically dispersed catalytic sites that are selectively loaded onto the reductive sites of tailored TiO2 to attract the photoinduced electrons efficiently. This enhances the number of holes, and consequently hydroxyl radicals, remaining on the sites of facet-engineered TiO2, confirmed by the enhancement of degradation of sulfamethoxazole and 2,4-dichlorophenoxyacetic acid. While Pt nanoparticle cocatalysts consume photoinduced electrons for the reduction of oxygen molecules, site-specifically loaded Pt1 produce surface hydrogen atoms and enhance hydrogen spillover onto the TiO2 surface, to achieve efficient hydrodefluorination of PFOA via the cleavage of the C–F bond with the Ti–H bond. The site-selective loading of Pt1 on facet-engineered TiO2 serves as a versatile platform that harnesses both reductive and oxidative degradation of emerging aqueous pollutants.

Supporting Information

ARTICLE SECTIONS
Jump To

The Supporting Information is available free of charge at https://pubs.acs.org/doi/10.1021/acsestengg.0c00210.

  • Calculation of percentage of each facet on facet-engineered TiO2; XAFS data fitting; synthesis of PtNP/P25; best-fit parameters extracted from fitting of FT EXAFS spectra of Pt1/facet-engineered TiO2; dark-field and HR-TEM images; ζ potential variations during the synthesis of Pt1/facet-engineering TiO2; TEM images; energy-dispersive X-ray spectroscopy; fitting result for Pt1/facet-engineered TiO2; repeated photocatalytic cycles; X-ray photoelectron spectroscopy analysis; mass balance of fluorine during PFOA decomposition; and cyclic degradation of PFOA with Pt1/facet-engineered TiO2 (PDF)

Terms & Conditions

Most electronic Supporting Information files are available without a subscription to ACS Web Editions. Such files may be downloaded by article for research use (if there is a public use license linked to the relevant article, that license may permit other uses). Permission may be obtained from ACS for other uses through requests via the RightsLink permission system: http://pubs.acs.org/page/copyright/permissions.html.

Cited By


This article is cited by 4 publications.

  1. Baljeet Singh, Manoj B. Gawande, Arun D. Kute, Rajender S. Varma, Paolo Fornasiero, Peter McNeice, Rajenahally V. Jagadeesh, Matthias Beller, Radek Zbořil. Single-Atom (Iron-Based) Catalysts: Synthesis and Applications. Chemical Reviews 2021, 121 (21) , 13620-13697. https://doi.org/10.1021/acs.chemrev.1c00158
  2. Dahong Huang, David J. Kim, Kali Rigby, Xuechen Zhou, Xuanhao Wu, Aidan Meese, Junfeng Niu, Eli Stavitski, Jae-Hong Kim. Elucidating the Role of Single-Atom Pd for Electrocatalytic Hydrodechlorination. Environmental Science & Technology 2021, 55 (19) , 13306-13316. https://doi.org/10.1021/acs.est.1c04294
  3. Domenico Leonello, Murilo Alexandre Fendrich, Francesco Parrino, Nainesh Patel, Michele Orlandi, Antonio Miotello. Light-Induced Advanced Oxidation Processes as PFAS Remediation Methods: A Review. Applied Sciences 2021, 11 (18) , 8458. https://doi.org/10.3390/app11188458
  4. Xiao Xu, Haotian Liu, Jian Wang, Ting Chen, Xing Ding, Hao Chen. Insight into surface hydroxyl groups for environmental purification: characterizations, applications and advances. Surfaces and Interfaces 2021, 25 , 101272. https://doi.org/10.1016/j.surfin.2021.101272