Unraveling Precise Locations of Indium Atoms in g‐C3N4 for Ameliorating Hydrogen Peroxide Piezo‐Photogeneration

Solar RRL - Tập 8 Số 8 - 2024
Nguyen Hoai Anh1,2, Duc‐Viet Nguyen3, Tuyen Anh Luu4, Pham Duc Minh Phan1,2, Huynh Phuoc Toan1,2, Pho Phuong Ly1,2, Hung Minh Nguyen5, Ngoc Linh Nguyen6,7, Seung Hyun Hur3, Phạm Thị Huế4, Nguyen Thi Ngoc Hue4, Minh‐Thuan Pham8, Thuy Dieu Thi Ung9, Danh Bich10, Vinh Ai Dao11, Huan V. Doan12, Mark A. Isaacs13,14,15, Minh Chien Nguyen16, Woo Jong Yu16, Yen‐Yi Lee8, Guo‐Ping Chang‐Chien8, Hoai‐Thanh Vuong17
1Faculty of Chemical Engineering, Ho Chi Minh City University of Technology (HCMUT), 268 Ly Thuong Kiet, District 10, Ho Chi Minh City, 700000 Vietnam
2Vietnam National University Ho Chi Minh City (VNU-HCM) Linh Trung Ward Thu Duc City Ho Chi Minh City 700000 Vietnam
3School of Chemical Engineering, University of Ulsan, Ulsan, 44610 South Korea
4Center for Nuclear Technologies, Vietnam Atomic Energy Institute, Ho Chi Minh City 700000, Vietnam
5Insitute of Fundamental and Applied Sciences Duy Tan University Ho Chi Minh City 700000 Vietnam
6Faculty of Materials Science and Engineering Phenikaa University Ha Noi 12116 Vietnam
7Phenikaa Research and Technology Institute (PRATI) A&A Green Phoenix Group JSC 167 Hoang Ngan Trung Hoa Cau Giay Ha Noi 11313 Vietnam
8Center for Environmental Toxin and Emerging-contaminant Research, Cheng Shiu University, Kaohsiung 83347, Taiwan
9Institute of Materials Science, Vietnam Academy of Science and Technology, Hanoi, 100000 Vietnam
10Department of Physics Hanoi National University of Education 136 Xuan Thuy Ha Noi 100000 Vietnam
11Department of Physics Faculty of Applied Sciences Ho Chi Minh City University of Technology and Education Ho Chi Minh City 700000 Vietnam
12Research School of Chemistry, Australian National University, Canberra, 2601, Australia
13Department of Chemistry University College London Euston London WC1H 0AJ UK
14Diamond Light Source, Harwell Science and Innovation Campus, Didcot OX11 0DE, UK
15HarwellXPS Research Complex at Harwell Rutherford Appleton Laboratories Didcot OX11 0FA UK
16Department of Electrical and Computer Engineering, Sungkyunkwan University, Suwon, 16419, Republic of Korea
17Department of Chemistry and Biochemistry University of California Santa Barbara (UCSB) Santa Barbara California 93106 USA

Tóm tắt

Increasing active sites in catalysts is of utmost importance for catalytic processes. In this regime, single‐atom dispersing on graphitic carbon nitrides (g‐C3N4) to produce fine chemicals, such as hydrogen peroxide (H2O2), is of current interest due to not only enhancing catalytic performance but also reducing the loading of necessary metals. Herein, g‐C3N4 is engineered by atomically dispersing aluminum (Al) or indium (In) sites to provide catalytic active centers via one‐step thermal shock polymerization. The addition of Al and In sites can accelerate the catalytic efficacy owing to the Lewis acid–base interactions between these metals and oxygen (O2). Under catalytic conditions, the formation of oxygenic radicals will strongly be associated with the enhanced formation of H2O2, confirmed by in situ electron paramagnetic resonance spectroscopy. Furthermore, the empirical analyses from positron annihilation spectroscopy show that In atoms will occupy the near positions of carbon vacancies (VC) to form NVC@InO bonds. This replacement will produce the highest formation energy based on the density functional theory calculations, improving the stability of atom‐dispersive materials. Therefore, via the combination of experimental and theoretical proofs, this study suggests the exact location of In atoms in g‐C3N4 structures, which can help boost the catalytic production of H2O2.

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