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Unraveling precise locations of indium atoms in g-C3N4 for ameliorating hydrogen peroxide piezo-photogeneration

DOI: 10.1002/solr.202400034 DOI Help

Authors: Nguyen Hoai Anh (Ho Chi Minh City University of Technology (HCMUT); Vietnam National University Ho Chi Minh City (VNU-HCM)) , Duc-Viet Nguyen (University of Ulsan) , Tuyen Anh Luu (Vietnam Atomic Energy Institute) , Pham Duc Minh Phan (Ho Chi Minh City University of Technology (HCMUT); Vietnam National University Ho Chi Minh City (VNU-HCM)) , Huynh Phuoc Toan (Ho Chi Minh City University of Technology (HCMUT); Vietnam National University Ho Chi Minh City (VNU-HCM)) , Pho Phuong Ly (Ho Chi Minh City University of Technology (HCMUT); Vietnam National University Ho Chi Minh City (VNU-HCM)) , Nguyen Quang Hung (Duy Tan University) , Ngoc Linh Nguyen (Phenikaa University; Phenikaa Research and Technology Institute (PRATI)) , Seung Hyun Hur (University of Ulsan) , Pham Thi Hue (Vietnam Atomic Energy Institute) , Nguyen Thi Ngoc Hue (Vietnam Atomic Energy Institute) , Minh-Thuan Pham (Cheng Shiu University) , Thuy Dieu Thi Ung (Vietnam Academy of Science and Technology) , Do Danh Bich (Hanoi National University of Education) , Vinh-Ai Dao (Ho Chi Minh City University of Technology and Education) , Huan V. Doan (Australian National University) , Mark Isaacs (University College London; HarwellXPS, Research Complex at Harwell; Diamond Light Source) , Minh Chien Nguyen (Sungkyunkwan University) , Woo Jong Yu (Sungkyunkwan University) , Yen-Yi Lee (Cheng Shiu University) , Guo-Ping Chang-Chien (Cheng Shiu University) , Hoai-Thanh Vuong (University of California Santa Barbara (UCSB))
Co-authored by industrial partner: No

Type: Journal Paper
Journal: Solar Rrl

State: Published (Approved)
Published: April 2024

Abstract: 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. Hence, we, in this research, engineered g-C3N4 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 would strongly be associated with the enhanced formation of H2O2, confirmed by in-situ electron paramagnetic resonance (EPR) spectroscopy. Furthermore, the empirical analyses from positron annihilation spectroscopy (PAS) show that In atoms would occupy the near positions of carbon vacancies (VC) to form N-VC@In-O bonds. This replacement would produce the highest formation energy based on the density functional theory (DFT) 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.

Journal Keywords: g-C3N4; atom dispersions; intercalation structures; mono and cluster vacancies; piezophotocatalysis

Subject Areas: Chemistry, Materials

Facility: HarwellXPS

Added On: 03/04/2024 08:50

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Physical Chemistry Catalysis Chemistry Materials Science Chemical Engineering Engineering & Technology

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