Electron-Deficient Engineering in Large-Conjugate-Heptazine Framework to Effectively Shuttle Hot Electrons for Efficient Photocatalytic H₂O₂ Production

Pan, Ronglan1; Lv, Wei2; Ge, Xin1; Huang, Xiong2; Hu, Qichuan3; Song, Kejian3; Liu, Qiong4; Xie, Haibo1; Wu, Bo3; Yuan, Jili1,5

2024-09-01

10.1002/adfm.202414193

ADVANCED FUNCTIONAL MATERIALS   影响因子和分区

1616-301X

1616-3028

Photocatalytic oxygen reduction to H2O2 based on g-C3N4 has presented promising potential for sustainable solar-fuel production. Yet tuning the timescale of hot electron's lifetime to effectively participate in the surface reactions remains challenging. Here, an electron-deficient engineering strategy is developed by incorporating an electron-deficient structure (EDS) with different conjugate regions into large conjugate-heptazine framework (LCHF) of g-C3N4 to steer hot electrons of the different timescales to effectively activate O2 for efficient photocatalytic H2O2 production. Femtosecond transientabsorption spectroscopy reveals that introducing EDS into LCHF can steer hot electron rapid transfer to the trapping sites of EDS and notably eliminate the deeply trapped electrons as well as enhance the shallow capture. It is demonstrated that pyromellitic dianhydride not only can tune the lifetime scale of hot electrons but also provide nonpolarized active sites to effectively activate O(2 )forming H2O2 with lower energy barrier via direct or stepwise 2e- pathways. This photocatalyst achieves an H2O2 yield rate of 25.40 mmol g(-1) h(-1), enabling an apparentquantumyield of 45.7% at 400 nm and a solar-to-chemical efficiency of 2.63%, outperforming the other reported photocatalysts. This work will shed light on the design of organic photocatalysts to tune hot electrons to effectively engage in the surface reaction.

conjugate-heptazine framework electron-deficient engineering H2O2 photosynthesis oxygen reduction reaction

SCI

英语

通讯

Guizhou Provincial Basic Research Program (Natural Science)[ZK[2023]47] ; Innovation and Entrepreneurship Project for overseas Talents in Guizhou Province[[2022]02] ; Specific Natural Science Foundation of Guizhou University[X202207] ; Science and Technology Department of Guizhou Province[[2019]5607] ; Basic and Applied Basic Research Foundation of Guangdong Province[2023B1515020024] ; Guangzhou Basic and Applied Basic Research Project[2024A04J2011] ; Natural Science Foundation of Guangdong Province[2022A1515011737] ; null[22309032]

Chemistry ; Science & Technology - Other Topics ; Materials Science ; Physics

Chemistry, Multidisciplinary ; Chemistry, Physical ; Nanoscience & Nanotechnology ; Materials Science, Multidisciplinary ; Physics, Applied ; Physics, Condensed Matter

WOS:001316693700001

WILEY-V C H VERLAG GMBH

Web of Science

1.Guizhou Univ, Coll Mat & Met, Dept Polymer Mat & Engn, Guiyang 550025, Peoples R China
2.South China Normal Univ, Inst Elect Paper Displays, South China Acad Adv Optoelect, Guangdong Prov Key Lab Opt Informat Mat & Technol, Guangzhou 510006, Peoples R China
3.Southern Univ Sci & Technol, Dept Phys, Shenzhen 518055, Peoples R China
4.Guangdong Acad Sci, Inst Anal, China Natl Analyt Ctr, Guangdong Prov Key Lab Emergency Test Dangerous Ch, Guangzhou 510070, Peoples R China
5.Guizhou Univ, State Key Lab Publ Big Data, Guiyang 550025, Peoples R China

Pan, Ronglan,Lv, Wei,Ge, Xin,et al. Electron-Deficient Engineering in Large-Conjugate-Heptazine Framework to Effectively Shuttle Hot Electrons for Efficient Photocatalytic H₂O₂ Production[J]. ADVANCED FUNCTIONAL MATERIALS,2024.

Pan, Ronglan.,Lv, Wei.,Ge, Xin.,Huang, Xiong.,Hu, Qichuan.,...&Yuan, Jili.(2024).Electron-Deficient Engineering in Large-Conjugate-Heptazine Framework to Effectively Shuttle Hot Electrons for Efficient Photocatalytic H₂O₂ Production.ADVANCED FUNCTIONAL MATERIALS.

Pan, Ronglan,et al."Electron-Deficient Engineering in Large-Conjugate-Heptazine Framework to Effectively Shuttle Hot Electrons for Efficient Photocatalytic H₂O₂ Production".ADVANCED FUNCTIONAL MATERIALS (2024).