Enhanced indirect attack behavior of 1O2 for photocatalytic H2O2 production: Possible synergistic regulation of spin polarization and water bridge on photocatalytic reaction

Jun Luo; Chengyang Feng; Changzheng Fan; Lin Tang; Yani Liu; Zhixuan Gong; Tangshan Wu; Xinlan Zhen; Haopeng Feng; Ming Yan; Lingling Wang; Liang Xu

doi:10.1016/j.jcat.2022.08.019

Enhanced indirect attack behavior of 1O2 for photocatalytic H2O2 production: Possible synergistic regulation of spin polarization and water bridge on photocatalytic reaction

Jun Luo, Chengyang Feng, Changzheng Fan, Lin Tang, Yani Liu, Zhixuan Gong, Tangshan Wu, Xinlan Zhen, Haopeng Feng, Ming Yan, Lingling Wang, Liang Xu

Physical Sciences and Engineering

Research output: Contribution to journal › Article › peer-review

10 Scopus citations

Abstract

The indirect attack mechanism of 1O2 on electron donors (ED) provides a new idea for improving photoproduction of H2O2 (PHO). Inspired by this, we constructed oxygen activation and •O2– oxidation sites in g-C3N4 to promote the 100% conversion of •O2– to 1O2 for PHO. Based on experimental data, we unexpectedly discovered the coordinated regulation of spin polarization and water bridge (CRSPWB) in H2O2 generation reaction by theoretical calculation. The 1O2 can react with ED to produce H2O2 in the most favourable way under the CRSPWB, which modifies the electronic structures of 1O2 and ED to maximize the interaction between them. Besides, water bridge indirectly enhances the oxidation effect of 1O2 on ED. Thus, corresponding reaction barrier for H2O2 generation is reduced to as low as −0.07 eV. This work provides in-depth insights into the attack behavior of 1O2 in H2O2 generation and brand-new guidance for improving PHO.

Original language	English (US)
Pages (from-to)	1132-1145
Number of pages	14
Journal	Journal of Catalysis
Volume	413
DOIs	https://doi.org/10.1016/j.jcat.2022.08.019
State	Published - Aug 27 2022

Bibliographical note

KAUST Repository Item: Exported on 2022-09-14
Acknowledgements: This work was financially supported by the project of National Natural Science Foundation of China (NSFC): 52070075, 51679084; The National Key Research and Development Program of China (No. 2021YFC1910400); Natural Science Foundation of Hunan Province: 2020JJ4187; the National Innovative Talent Promotion Program of China (2017RA2088); the Funds for Innovative Province Construction of Hunan Province of China (2019RS3012). The authors would like to thank Ting Yang from Shiyanjia Lab (www.shiyanjia.com) for the ICP-MS analysis.

ASJC Scopus subject areas

Catalysis
Physical and Theoretical Chemistry

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10.1016/j.jcat.2022.08.019

Cite this

Luo, J., Feng, C., Fan, C., Tang, L., Liu, Y., Gong, Z., Wu, T., Zhen, X., Feng, H., Yan, M., Wang, L., & Xu, L. (2022). Enhanced indirect attack behavior of 1O2 for photocatalytic H2O2 production: Possible synergistic regulation of spin polarization and water bridge on photocatalytic reaction. Journal of Catalysis, 413, 1132-1145. https://doi.org/10.1016/j.jcat.2022.08.019

@article{04fca8a11e8848368f47f56438cb9c87,

title = "Enhanced indirect attack behavior of 1O2 for photocatalytic H2O2 production: Possible synergistic regulation of spin polarization and water bridge on photocatalytic reaction",

abstract = "The indirect attack mechanism of 1O2 on electron donors (ED) provides a new idea for improving photoproduction of H2O2 (PHO). Inspired by this, we constructed oxygen activation and •O2– oxidation sites in g-C3N4 to promote the 100% conversion of •O2– to 1O2 for PHO. Based on experimental data, we unexpectedly discovered the coordinated regulation of spin polarization and water bridge (CRSPWB) in H2O2 generation reaction by theoretical calculation. The 1O2 can react with ED to produce H2O2 in the most favourable way under the CRSPWB, which modifies the electronic structures of 1O2 and ED to maximize the interaction between them. Besides, water bridge indirectly enhances the oxidation effect of 1O2 on ED. Thus, corresponding reaction barrier for H2O2 generation is reduced to as low as −0.07 eV. This work provides in-depth insights into the attack behavior of 1O2 in H2O2 generation and brand-new guidance for improving PHO.",

author = "Jun Luo and Chengyang Feng and Changzheng Fan and Lin Tang and Yani Liu and Zhixuan Gong and Tangshan Wu and Xinlan Zhen and Haopeng Feng and Ming Yan and Lingling Wang and Liang Xu",

note = "KAUST Repository Item: Exported on 2022-09-14 Acknowledgements: This work was financially supported by the project of National Natural Science Foundation of China (NSFC): 52070075, 51679084; The National Key Research and Development Program of China (No. 2021YFC1910400); Natural Science Foundation of Hunan Province: 2020JJ4187; the National Innovative Talent Promotion Program of China (2017RA2088); the Funds for Innovative Province Construction of Hunan Province of China (2019RS3012). The authors would like to thank Ting Yang from Shiyanjia Lab (www.shiyanjia.com) for the ICP-MS analysis.",

year = "2022",

month = aug,

day = "27",

doi = "10.1016/j.jcat.2022.08.019",

language = "English (US)",

volume = "413",

pages = "1132--1145",

journal = "Journal of Catalysis",

issn = "1090-2694",

publisher = "Elsevier",

}

Luo, J, Feng, C, Fan, C, Tang, L, Liu, Y, Gong, Z, Wu, T, Zhen, X, Feng, H, Yan, M, Wang, L & Xu, L 2022, 'Enhanced indirect attack behavior of 1O2 for photocatalytic H2O2 production: Possible synergistic regulation of spin polarization and water bridge on photocatalytic reaction', Journal of Catalysis, vol. 413, pp. 1132-1145. https://doi.org/10.1016/j.jcat.2022.08.019

TY - JOUR

T1 - Enhanced indirect attack behavior of 1O2 for photocatalytic H2O2 production: Possible synergistic regulation of spin polarization and water bridge on photocatalytic reaction

AU - Luo, Jun

AU - Feng, Chengyang

AU - Fan, Changzheng

AU - Tang, Lin

AU - Liu, Yani

AU - Gong, Zhixuan

AU - Wu, Tangshan

AU - Zhen, Xinlan

AU - Feng, Haopeng

AU - Yan, Ming

AU - Wang, Lingling

AU - Xu, Liang

N1 - KAUST Repository Item: Exported on 2022-09-14 Acknowledgements: This work was financially supported by the project of National Natural Science Foundation of China (NSFC): 52070075, 51679084; The National Key Research and Development Program of China (No. 2021YFC1910400); Natural Science Foundation of Hunan Province: 2020JJ4187; the National Innovative Talent Promotion Program of China (2017RA2088); the Funds for Innovative Province Construction of Hunan Province of China (2019RS3012). The authors would like to thank Ting Yang from Shiyanjia Lab (www.shiyanjia.com) for the ICP-MS analysis.

PY - 2022/8/27

Y1 - 2022/8/27

N2 - The indirect attack mechanism of 1O2 on electron donors (ED) provides a new idea for improving photoproduction of H2O2 (PHO). Inspired by this, we constructed oxygen activation and •O2– oxidation sites in g-C3N4 to promote the 100% conversion of •O2– to 1O2 for PHO. Based on experimental data, we unexpectedly discovered the coordinated regulation of spin polarization and water bridge (CRSPWB) in H2O2 generation reaction by theoretical calculation. The 1O2 can react with ED to produce H2O2 in the most favourable way under the CRSPWB, which modifies the electronic structures of 1O2 and ED to maximize the interaction between them. Besides, water bridge indirectly enhances the oxidation effect of 1O2 on ED. Thus, corresponding reaction barrier for H2O2 generation is reduced to as low as −0.07 eV. This work provides in-depth insights into the attack behavior of 1O2 in H2O2 generation and brand-new guidance for improving PHO.

AB - The indirect attack mechanism of 1O2 on electron donors (ED) provides a new idea for improving photoproduction of H2O2 (PHO). Inspired by this, we constructed oxygen activation and •O2– oxidation sites in g-C3N4 to promote the 100% conversion of •O2– to 1O2 for PHO. Based on experimental data, we unexpectedly discovered the coordinated regulation of spin polarization and water bridge (CRSPWB) in H2O2 generation reaction by theoretical calculation. The 1O2 can react with ED to produce H2O2 in the most favourable way under the CRSPWB, which modifies the electronic structures of 1O2 and ED to maximize the interaction between them. Besides, water bridge indirectly enhances the oxidation effect of 1O2 on ED. Thus, corresponding reaction barrier for H2O2 generation is reduced to as low as −0.07 eV. This work provides in-depth insights into the attack behavior of 1O2 in H2O2 generation and brand-new guidance for improving PHO.

UR - http://hdl.handle.net/10754/680926

UR - https://linkinghub.elsevier.com/retrieve/pii/S0021951722003530

UR - http://www.scopus.com/inward/record.url?scp=85136710183&partnerID=8YFLogxK

U2 - 10.1016/j.jcat.2022.08.019

DO - 10.1016/j.jcat.2022.08.019

M3 - Article

SN - 1090-2694

VL - 413

SP - 1132

EP - 1145

JO - Journal of Catalysis

JF - Journal of Catalysis

ER -

Enhanced indirect attack behavior of 1O2 for photocatalytic H2O2 production: Possible synergistic regulation of spin polarization and water bridge on photocatalytic reaction

Abstract

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