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Bridge-oxygen bonding modulates Ru single atoms for peroxymonosulfate activation: Importance of high-valent Ru species and 1O2.
He, Bo; Gu, Yanling; Yang, Zhongzhu; Ling, Zhaoxiang; Hu, Huamin; Chen, Zhaoyong.
Afiliação
  • He B; College of Materials Science and Engineering, Changsha University of Science and Technology, Changsha 410114, PR China.
  • Gu Y; College of Materials Science and Engineering, Changsha University of Science and Technology, Changsha 410114, PR China. Electronic address: gyl@csust.edu.cn.
  • Yang Z; College of Environmental Science and Engineering, Hunan University, Changsha 410082, PR China; Key Laboratory of Environmental Biology and Pollution Control (Hunan University), Ministry of Education, Changsha 410082, PR China.
  • Ling Z; College of Materials Science and Engineering, Changsha University of Science and Technology, Changsha 410114, PR China.
  • Hu H; College of Materials Science and Engineering, Changsha University of Science and Technology, Changsha 410114, PR China.
  • Chen Z; College of Materials Science and Engineering, Changsha University of Science and Technology, Changsha 410114, PR China. Electronic address: chenzhaoyongcioc@126.com.
J Colloid Interface Sci ; 676: 435-444, 2024 Dec 15.
Article em En | MEDLINE | ID: mdl-39033678
ABSTRACT
The application of single-atom catalysts (SACs) to advanced oxidation processes (AOPs) based on peroxymonosulfate (PMS) has attracted considerable attention. However, the catalytic pathways and mechanisms underlying these processes remain unclear. In this study, NiFe-LDH was synthesized and single Ru atoms were stably loaded onto it by forming Ru-O-M (M=Ni or Fe) bonds (Ru@NiFe-LDH). This was demonstrated using high-angle annular dark-field scanning TEM (HAADF-STEM) and X-ray absorption fine structure spectra (XANES). The Ru@NiFe-LDH/PMS system showed a high catalytic reactivity (100 % sulfamethoxazole degradation in only 30 min), high stability (97 % reactivity was maintained after continuous operation for 400 min), and wide pH suitability (working pH range 3-11) for AOPs. The crucial roles of the high-valent species (Ru(V) = O) and 1O2 in this reaction were verified. Density functional theory (DFT) calculations revealed that electron transfer produced a positively charged Ru. This enhances the adsorption of negatively charged PMS anions onto the Ru monoatomic sites, thereby, causing the formation of Ru-PMS* complexes. This study implies that the structure-function relationship between organic compounds and SACs plays a significant role in PMS-based AOPs, and provides a comprehensive mechanism for the role of high-valent species in heterogeneous Fenton-like systems.
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Texto completo: 1 Base de dados: MEDLINE Idioma: En Revista: J Colloid Interface Sci Ano de publicação: 2024 Tipo de documento: Article

Texto completo: 1 Base de dados: MEDLINE Idioma: En Revista: J Colloid Interface Sci Ano de publicação: 2024 Tipo de documento: Article