Active Center Size-Dependent Fenton-Like Chemistry for Sustainable Water Decontamination

Wu，Zelin1,2; Xiong，Zhaokun1,2; Liu，Wen3; Liu，Rui4; Feng，Xuezhen5; Huang，Bingkun1,2; Wang，Xinhao1,2; Gao，Yixuan3; Chen，Hong5; Yao，Gang2,6; Lai，Bo1,2

2023-12-19

10.1021/acs.est.3c06887

Environmental Science and Technology   影响因子和分区

0013-936X

1520-5851

Accurately controlling catalytic activity and mechanism as well as identifying structure-activity-selectivity correlations in Fenton-like chemistry is essential for designing high-performance catalysts for sustainable water decontamination. Herein, active center size-dependent catalysts with single cobalt atoms (CoSA), atomic clusters (CoAC), and nanoparticles (CoNP) were fabricated to realize the changeover of catalytic activity and mechanism in peroxymonosulfate (PMS)-based Fenton-like chemistry. Catalytic activity and durability vary with the change in metal active center sizes. Besides, reducing the metal size from nanoparticles to single atoms significantly modulates contributions of radical and nonradical mechanisms, thus achieving selective/nonselective degradation. Density functional theory calculations reveal evolutions in catalytic mechanisms of size-dependent catalytic systems over different Gibbs free energies for reactive oxygen species generation. Single-atom site contact with PMS is preferred to induce nonradical mechanisms, while PMS dissociates and generates radicals on clusters and nanoparticles. Differences originating from reaction mechanisms endow developed systems with size-dependent selectivity and mineralization for treating actual hospital wastewater in column reactors. This work brings an in-depth understanding of metal size effects in Fenton-like chemistry and guides the design of intelligent catalysts to fulfill the demand of specific scenes for water purification.

DFT calculations Fenton-like catalysis reaction activity and mechanism single-atom catalysts size-dependent

EI ; SCI

英语

NI论文

其他

20235115246149

Atoms ; Catalyst selectivity ; Degradation ; Density functional theory ; Design for testability ; Metal nanoparticles ; Nanocatalysts ; Oxidation ; Quantum chemistry ; Wastewater reclamation ; Wastewater treatment

Industrial Wastes Treatment and Disposal:452.4 ; Nanotechnology:761 ; Physical Chemistry:801.4 ; Chemical Reactions:802.2 ; Chemical Agents and Basic Industrial Chemicals:803 ; Chemical Products Generally:804 ; Probability Theory:922.1 ; Atomic and Molecular Physics:931.3 ; Quantum Theory; Quantum Mechanics:931.4

ENVIRONMENT/ECOLOGY

2-s2.0-85180077645

Scopus

1.State Key Laboratory of Hydraulics and Mountain River Engineering,College of Architecture and Environment,Sichuan University,Chengdu,610065,China
2.Sino-German Centre for Water and Health Research,Sichuan University,Chengdu,610065,China
3.College of Environmental Sciences and Engineering,Peking University,The Key Laboratory of Water and Sediment Sciences,Ministry of Education,Beijing,100871,China
4.State Key Laboratory of Environmental Chemistry and Ecotoxicology,Research Center for Eco-Environmental Sciences,Chinese Academy of Sciences,Beijing,100085,China
5.Shenzhen Key Laboratory of Interfacial Science and Engineering of Materials,State Environmental Protection Key Laboratory of Integrated Surface Water-Groundwater Pollution Control,Southern University of Science and Technology,Shenzhen,518055,China
6.Sino-German Centre for innovative Environmental Technologies (WATCH e.V.),Aachen,52078,Germany

Wu，Zelin,Xiong，Zhaokun,Liu，Wen,et al. Active Center Size-Dependent Fenton-Like Chemistry for Sustainable Water Decontamination[J]. Environmental Science and Technology,2023,57(50):21416-21427.

Wu，Zelin.,Xiong，Zhaokun.,Liu，Wen.,Liu，Rui.,Feng，Xuezhen.,...&Lai，Bo.(2023).Active Center Size-Dependent Fenton-Like Chemistry for Sustainable Water Decontamination.Environmental Science and Technology,57(50),21416-21427.

Wu，Zelin,et al."Active Center Size-Dependent Fenton-Like Chemistry for Sustainable Water Decontamination".Environmental Science and Technology 57.50(2023):21416-21427.