Enhancing singlet oxygen production of dioxygen activation on the carbon-supported rare-earth oxide nanocluster and rare-earth single atom catalyst to remove antibiotics

Haonan Qin; Meina Guo; Chenliang Zhou; Jiarong Li; Xuequan Jing; Yinhua Wan; Weijie Song; Hongdong Yu; Guan Peng; Zhangwei Yao; Jiaming Liu; Kang Hu

doi:10.1016/j.watres.2024.121184

Enhancing singlet oxygen production of dioxygen activation on the carbon-supported rare-earth oxide nanocluster and rare-earth single atom catalyst to remove antibiotics

Water Res. 2024 Mar 15:252:121184. doi: 10.1016/j.watres.2024.121184. Epub 2024 Jan 25.

Authors

Haonan Qin¹, Meina Guo², Chenliang Zhou¹, Jiarong Li¹, Xuequan Jing¹, Yinhua Wan³, Weijie Song³, Hongdong Yu², Guan Peng², Zhangwei Yao¹, Jiaming Liu¹, Kang Hu⁴

Affiliations

¹ School of Rare Earths, University of Science and Technology of China, Hefei, Anhui 230026, China; Ganjiang Innovation Academy, Chinese Academy of Sciences, Ganzhou 341000, China; Key Laboratory of Rare Earth, Chinese Academy of Sciences, Ganzhou 341000, China.
² School of Rare Earths, University of Science and Technology of China, Hefei, Anhui 230026, China; Ganjiang Innovation Academy, Chinese Academy of Sciences, Ganzhou 341000, China; Key Laboratory of Rare Earth, Chinese Academy of Sciences, Ganzhou 341000, China; Jiangxi Province Key Laboratory of Cleaner Production of Rare Earths, Ganzhou 341000, China.
³ School of Rare Earths, University of Science and Technology of China, Hefei, Anhui 230026, China; Ganjiang Innovation Academy, Chinese Academy of Sciences, Ganzhou 341000, China; Key Laboratory of Rare Earth, Chinese Academy of Sciences, Ganzhou 341000, China; Jiangxi Province Key Laboratory of Cleaner Production of Rare Earths, Ganzhou 341000, China; Institute of Process Engineering, Chinese Academy of Sciences, Beijing 100190, China.
⁴ School of Rare Earths, University of Science and Technology of China, Hefei, Anhui 230026, China; Ganjiang Innovation Academy, Chinese Academy of Sciences, Ganzhou 341000, China; Key Laboratory of Rare Earth, Chinese Academy of Sciences, Ganzhou 341000, China; Jiangxi Province Key Laboratory of Cleaner Production of Rare Earths, Ganzhou 341000, China. Electronic address: hukang0602@126.com.

PMID: 38377699
DOI: 10.1016/j.watres.2024.121184

Abstract

Singlet oxygen (¹O₂) is extensively employed in the fields of chemical, biomedical and environmental. However, it is still a challenge to produce high- concentration ¹O₂ by dioxygen activation. Herein, a system of carbon-supported rare-earth oxide nanocluster and single atom catalysts (named as RE₂O₃/RE-C, RE=La, Ce, Pr, Nd, Sm, Eu, Gd, Tb, Dy, Ho, Er, Tm, Yb, Lu, Sc and Y) with similar morphology, structure, and physicochemical characteristic are constructed to activate dissolved oxygen (DO) to enhance ¹O₂ production. The catalytic activity trends and mechanisms are revealed experimentally and are also proven by theoretical analyses and calculations. The ¹O₂ generation activity trend is Gd₂O₃/Gd-C>Er₂O₃/Er-C>Sm₂O₃/Sm-C>pristine carbon (C). More than 95.0% of common antibiotics (ciprofloxacin, ofloxacin, norfloxacin and carbamazepine) can be removed in 60 min by Gd₂O₃/Gd-C. Density functional theory calculations indicate that Gd₂O₃ nanoclusters and Gd single atoms exhibit the moderate adsorption energy of ·O₂^- to enhance ¹O₂ production. This study offers a universal strategy to enhance ¹O₂ production in dioxygen activation for future application and reveals the natural essence of basic mechanisms of ¹O₂ production via rare-earth oxide nanoclusters and rare-earth single atoms.

Keywords: Antibiotic removal; Dioxygen activation; Rare-earth oxide nanocluster; Rare-earth single atom; Singlet oxygen.

MeSH terms

Anti-Bacterial Agents
Metals, Rare Earth* / analysis
Metals, Rare Earth* / chemistry
Oxides / chemistry
Oxygen
Singlet Oxygen*

Substances

Singlet Oxygen
Oxides
Oxygen
Anti-Bacterial Agents
Metals, Rare Earth