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Article: In situ protonated-phosphorus interstitial doping induces long-lived shallow charge trapping in porous C3−xN4 photocatalysts for highly efficient H2 generation

TitleIn situ protonated-phosphorus interstitial doping induces long-lived shallow charge trapping in porous C3−xN4 photocatalysts for highly efficient H2 generation
Authors
Issue Date5-Dec-2022
PublisherRoyal Society of Chemistry
Citation
Energy & Environmental Science, 2023, v. 16, n. 2, p. 460-472 How to Cite?
Abstract

Efficient photocatalytic solar-to-H2 conversion is pivotal to zero-carbon energy supply. Graphitic carbon nitride (g-C3N4) is a promising visible-light photocatalyst but suffers from intrinsic electron–hole recombination and deep-charge trapping, limiting its efficiency. Here, we show a synergistic strategy of porosity, vacancy and shallow(trapping)-state engineering to enrich catalytic sites and promote the lifetime of active electrons by thermochemical treatment and phosphorus-interstitial-doping. The latter enhances the electron delocalization in the π-conjugate polymeric structure. The optimized photocatalyst shows a ∼800% increase in H2 generation (6323 μmol h−1 g−1) and an about 5-fold increase in quantum efficiency (QE420 nm = 5.08%). The superior performance is attributed to the long-lived shallow charge trapping, as a result of proton-feeding to the coordinated phosphorus site during the photocatalytic reaction, which enhances the photogenerated carrier lifetime and positively optimizes the band structure of the catalyst. Femtosecond transient absorption spectroscopy reveals a doubling lifetime of shallow-trapped charges (∼405.5 ps), favoring high mobility for electron-involved photocatalytic H2 generation. This work provides a new mechanism for improving charge carrier dynamics and photocatalytic performance.


Persistent Identifierhttp://hdl.handle.net/10722/341635
ISSN
2023 Impact Factor: 32.4
2023 SCImago Journal Rankings: 10.935
ISI Accession Number ID

 

DC FieldValueLanguage
dc.contributor.authorWang, Wenchao-
dc.contributor.authorDu, Lili-
dc.contributor.authorXia, Ruiqin-
dc.contributor.authorLiang, Runhui-
dc.contributor.authorZhou, Tao-
dc.contributor.authorLee, Hung Kay-
dc.contributor.authorYan, Zhiping-
dc.contributor.authorLuo, Hao-
dc.contributor.authorShang, Congxiao-
dc.contributor.authorPhillips, David Lee-
dc.contributor.authorGuo, Zhengxiao-
dc.date.accessioned2024-03-20T06:57:55Z-
dc.date.available2024-03-20T06:57:55Z-
dc.date.issued2022-12-05-
dc.identifier.citationEnergy & Environmental Science, 2023, v. 16, n. 2, p. 460-472-
dc.identifier.issn1754-5692-
dc.identifier.urihttp://hdl.handle.net/10722/341635-
dc.description.abstract<p>Efficient photocatalytic solar-to-H<small><sub>2</sub></small> conversion is pivotal to zero-carbon energy supply. Graphitic carbon nitride (g-C<small><sub>3</sub></small>N<small><sub>4</sub></small>) is a promising visible-light photocatalyst but suffers from intrinsic electron–hole recombination and deep-charge trapping, limiting its efficiency. Here, we show a synergistic strategy of porosity, vacancy and shallow(trapping)-state engineering to enrich catalytic sites and promote the lifetime of active electrons by thermochemical treatment and phosphorus-interstitial-doping. The latter enhances the electron delocalization in the π-conjugate polymeric structure. The optimized photocatalyst shows a ∼800% increase in H<small><sub>2</sub></small> generation (6323 μmol h<small><sup>−1</sup></small> g<small><sup>−1</sup></small>) and an about 5-fold increase in quantum efficiency (QE<small><sub>420 nm</sub></small> = 5.08%). The superior performance is attributed to the long-lived shallow charge trapping, as a result of proton-feeding to the coordinated phosphorus site during the photocatalytic reaction, which enhances the photogenerated carrier lifetime and positively optimizes the band structure of the catalyst. Femtosecond transient absorption spectroscopy reveals a doubling lifetime of shallow-trapped charges (∼405.5 ps), favoring high mobility for electron-involved photocatalytic H<small><sub>2</sub></small> generation. This work provides a new mechanism for improving charge carrier dynamics and photocatalytic performance.<br></p>-
dc.languageeng-
dc.publisherRoyal Society of Chemistry-
dc.relation.ispartofEnergy & Environmental Science-
dc.rightsThis work is licensed under a Creative Commons Attribution-NonCommercial-NoDerivatives 4.0 International License.-
dc.titleIn situ protonated-phosphorus interstitial doping induces long-lived shallow charge trapping in porous C3−xN4 photocatalysts for highly efficient H2 generation-
dc.typeArticle-
dc.identifier.doi10.1039/D2EE02680E-
dc.identifier.scopuseid_2-s2.0-85144669987-
dc.identifier.volume16-
dc.identifier.issue2-
dc.identifier.spage460-
dc.identifier.epage472-
dc.identifier.eissn1754-5706-
dc.identifier.isiWOS:000898177500001-
dc.identifier.issnl1754-5692-

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