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Engineering Oxidation States of a Platinum Cocatalyst over Chemically Oxidized Graphitic Carbon Nitride Photocatalysts for Photocatalytic Hydrogen Evolution

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Abstract
In this study, we prepared platinum (Pt)-containing graphitic carbon nitride (g-C3N4) catalysts using Pt photodeposition onto g-C3N4 modified by chemical oxidation, and the chemically oxidized Pt/g-C3N4 catalysts were applied to photocatalytic hydrogen evolution tests. The hydrogen production rates of the chemically oxidized Pt/g-C3N4 photocatalysts (2471.7 and 3640.8 μmol g?1 h?1) were found to be at least 5 times higher than those of bulk Pt/g-C3N4 (429.3 and 728.8 μmol g?1 h?1). Compared with bulk g-C3N4, the chemically oxidized g-C3N4 was composed of more positively charged locales induced nearby the oxygen-containing edges, which was proven by DFT calculations. As a result, the chemically oxidized Pt/g-C3N4 catalysts maintained the high ratio of Pt2+/Pt0 among the Pt nanoparticles during the Pt photodeposition. The higher proportion of Pt2+ sites on the chemically oxidized g-C3N4 enhanced the hydrogen evolution rate by their favorable water adsorption and hydrogen intermediates (Hads) desorption, thus suppressing the reversible reaction route of H2 to 2H+. Additionally, the chemically oxidized g-C3N4 with oxygen-containing functional groups improved the separation efficiency of photoexcited charges over Pt/gC3N4.
Author(s)
강성구다오 득 쾅신은우웬 티 킴 안
Issued Date
2021
Type
Article
Keyword
Pt/g-C3N4Chemical oxidationPt oxidation stateCharge separationHydrogen evolution
DOI
10.1021/acssuschemeng.1c05297
URI
https://oak.ulsan.ac.kr/handle/2021.oak/9246
https://ulsan-primo.hosted.exlibrisgroup.com/primo-explore/fulldisplay?docid=TN_cdi_crossref_primary_10_1021_acssuschemeng_1c05297&context=PC&vid=ULSAN&lang=ko_KR&search_scope=default_scope&adaptor=primo_central_multiple_fe&tab=default_tab&query=any,contains,Engineering%20Oxidation%20States%20of%20a%20Platinum%20Cocatalyst%20over%20Chemically%20Oxidized%20Graphitic%20Carbon%20Nitride%20Photocatalysts%20for%20Photocatalytic%20Hydrogen%20Evolution&offset=0&pcAvailability=true
Publisher
ACS SUSTAINABLE CHEMISTRY & ENGINEERING
Location
미국
Language
영어
ISSN
2168-0485
Citation Volume
9
Citation Number
1
Citation Start Page
14537
Citation End Page
14549
Appears in Collections:
Engineering > Chemical Engineering
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