Chinese Journal of Catalysis ›› 2025, Vol. 68: 282-299.DOI: 10.1016/S1872-2067(24)60170-1

• Articles • Previous Articles     Next Articles

The design and fabrication of TiO2/Bi4O5Br2 step-scheme heterojunctions for the photodegradation of gaseous hydrogen sulfide: DFT calculation, kinetics, pathways, and mechanisms

Baofei Haoa, Younes Ahmadia, Jan Szulejkoa, Tianhao Zhangb,c, Zhansheng Lub,c, Ki-Hyun Kima,*()   

  1. aDepartment of Civil and Environmental Engineering, Hanyang University, 222 Wangsimni-ro, Seoul 04763, Republic of Korea
    bSchool of Mathematics and Physics, Beijing University of Chemical Technology, Beijing 100029, China
    cHenan Key Laboratory of Advanced Semiconductor & Functional Device Integration, School of Physics, Henan Normal University, Xinxiang 453007, Henan, China
  • Received:2024-08-10 Accepted:2024-10-08 Online:2025-01-18 Published:2025-01-02
  • Contact: * E-mail: kkim61@hanyang.ac.kr (K.-H. Kim).
  • Supported by:
    National Natural Science Foundation of China(12274118);Henan Center for Outstanding Overseas Scientists(GZS2023007);Special Project for Fundamental Research in University of Henan Province(22ZX013)

Abstract:

It is a challenging task to efficiently convert deleterious hydrogen sulfide (H2S) into less harmful products such as SO42- species. In an effort to address such issue, a step-scheme (S-scheme) heterojunction photocatalyst has been built by concatenating TiO2 (P25) and ultrathin Bi4O5Br2 into TiO2/Bi4O5Br2 (namely, x-TB-y: x and y denote the molar ratio of TiO2:Bi4O5Br2 and pH value for solution-based synthesis, respectively) via in-situ hydrothermal method. The S-scheme charge transfer pathway in TB is confirmed by electron spin resonance and band structure analysis while experimental data and density functional theory calculations suggest the formation of an internal electric field to facilitate the separation and transfer of photoinduced charge carriers. Accordingly, the optimized heterojunction photocatalyst, i.e., 5-TB-9, showcases significantly high (> 99%) removal efficiency against 10 ppm H2S in a 17 L chamber within 12 minutes (removal kinetic rate r: 0.7 mmol·h-1·g-1, specific clean air delivery rate SCADR: 5554 L·h-1·g-1, quantum yield QY: 3.24 E-3 molecules·photon-1, and space-time yield STY: 3.24 E-3 molecules·photon-1·mg-1). Combined analysis of in-situ diffuse reflectance infrared Fourier transform adsorption spectra and gas chromatography-mass spectrometry allows to evaluate the mechanisms leading to the complete degradation of H2S (i.e., into SO42- without forming any intermediate species). This work demonstrates the promising remediation potential of an S-scheme TiO2/Bi4O5Br2 photocatalyst against hazardous H2S gas for sustainable environmental remediation.

Key words: H2S removal, Photocatalysis, S-scheme heterojunction, Recyclability