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.
Bibliographical noteKAUST 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
- Physical and Theoretical Chemistry