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Single-atom catalysis for advanced oxidation and reduction systems in water decontamination

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Abstract

Water scarcity is an escalating global crisis, posing a severe threat to populations worldwide. Consequently, exploring various materials to remove emerging contaminants from freshwater sources has garnered significant attention. In this regard, single-atom catalysis (SACs) has emerged as a catalyst of scientific progress in water purification and treatment methodologies during recent decades. SACs exhibit exceptional catalytic activity, selectivity and stability, due to their near-perfect atom utilization, highly unsaturated coordination environment and uniform reaction centers. However, a comprehensive and critical review encompassing the successful integration of SACs into water purification processes needs to be completed. This review aims to accentuate recent trends by presenting the synthesis, structure, and environment and energy application-relevant properties of SACs. The results show that a comprehensive and multi-perspective summary of the advantages of SACs in environmental remediation can have significant benefits, such as fast kinetics, cost-effectiveness, selectivity. The oxidation and reduction processes of SACs and functional SACs materials in water purification were emphasized. Furthermore, the last section is devoted to the current research gaps and further perspectives on the application of SACs in water treatment, which are summarized and analyzed.

Graphical Abstract

摘要

水资源匮乏是一种日益加剧的全球危机，对全球人口构成严重威胁。因此，探索用于水体净化的材料已引起广泛关注，基于此，单原子催化剂在近几十年的水净化方法中已成为重要的纳米材料。由于其高效的原子利用率、高度不饱和的配位环境和均匀的反应中心，单原子催化剂表现出卓越的催化活性、选择性和稳定性。本综述旨在通过介绍SACs的合成、结构特性以及在环境和能源领域的相关应用，来强调其发展趋势。对单原子催化剂在环境修复中的优势进行全面和多角度的总结，并阐明其在水处理过程中的显著优势，包括快速的动力学、成本效益、选择性等。进而强调了功能性单原子催化剂在水净化中的氧化和还原过程。最后，总结和分析了单原子催化剂在水处理中的应用和当前的研究壁垒，并为后续研究进行了展望。

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Fig. 1

Reproduced with permission from Ref. [42]. Copyright 2022, American Chemical Society. b Preparation and model structure of noble-SACs. Reproduced with permission from Ref. [43]. Copyright 2019, American Association for the Advancement of Science. c Schematic diagram of synthesis process of Cu–SACs membranes functionalized by thiol groups. Reproduced with permission from Ref. [44]. Copyright 2022, American Chemical Society. d Robot synthesis platform photo and scheme flowchart, comparison of metal content between automatic and manual synthesis of Ni-nitrogen-doped carbon catalysts. Reproduced with permission from Ref. [45]. Copyright 2022, Springer Nature

Fig. 2

Reproduced with permission from Ref. [52]. Copyright 2022, Springer Nature

Fig. 3

Reproduced with permission from Ref. [65]. Copyright 2017, American Chemical Society. b Schematic diagram of pyrolysis process of C-g-C3N4–Fe. Reproduced with permission from Ref. [66]. Copyright 2020, Wiley. c Universal synthesis procedure of Metal-SACs in two steps. Reproduced with permission from Ref. [67]. Copyright 2019, Springer Nature

Fig. 4

Reproduced with permission from Ref. [73]. Copyright 2021, Wiley. b Schematic illustration of preparation of Cu–SACs support on nitrogen-doped carbon. Reproduced with permission from Ref. [74]. Copyright 2018, Springer Nature

Fig. 5

Reproduced with permission from Ref. [34]. Copyright 2011, Springer Nature. c Atomic resolution image showing a Pt single atom located in clean region of MoS2; d enlarged image from boxed area in c, and e corresponding DFT relax atomic model. Reproduced with permission from Ref. [83]. Copyright 2017, American Chemical Society. f Low-temperature STM image of FeN4/graphene and g simulated STM image; h dl/dV spectra and (inset) image acquired along white line. Reproduced with permission from Ref. [80]. Copyright 2015, American Association for the Advancement of Science. i Atom-resolved STM image and j ball model of Co-Mo-S. Reproduced with permission from Ref. [84]. Copyright 2007, Elsevier

Fig. 6

Reproduced with permission from Ref. [89]. Copyright 2015, American Association for the Advancement of Science. c EXAFS, d Fourier transforms and e wavelet transform for Co-nitrogen-doped graphene oxide and Co-graphene, respectively. Reproduced with permission from Ref. [90]. Copyright 2015, Springer Nature. XANES and EXAFS spectra of f, h Co K-edge and g, i Bi L3-edge. Reproduced with permission from Ref. [91]. Copyright 2019, Springer Nature. j Comparison XPS spectra of Pd–SACs on mesoporous support; k, l BET surface area and Pd2+/Pd4+ ratio correlation with different Pd surface concentrations. Reproduced with permission from Ref. [92]. Copyright 2017, Royal Society of Chemistry

Fig. 7

Reproduced with permission from Ref. [93]. Copyright 2016, Wiley. d Positron lifetime spectrum of BiOCl nanosheets and BiOCl nanoplates, respectively. e, f schematic diagrammatic of positrons captured by VBi‴ defect and VBi‴VO•VBi‴ vacancy associates, respectively. Reproduced with permission from Ref. [95]. Copyright 2013, American Chemical Society

Fig. 8

Reproduced with permission from Ref. [86]. Copyright 2018, Springer Nature. b Geometric structures and c calculated formation energy (Ef) of Fe-graphene and Fe-nitrogen-graphene. Reproduced with permission from Ref. [98]. Copyright 2019, Elsevier

Fig. 9

Reproduced with permission from Ref. [102]. Copyright 2019, Springer Nature. b Six typical configurations of [PtCl6]2– on different supports and corresponding calculated free energies. Reproduced with permission from Ref. [103]. Copyright 2019, Springer Nature. c Optimized structures for Pt–MoN and Pt–α–MoC; d free energy profiles for ORR over Pt–SACs at various potentials. Reproduced with permission from Ref. [104]. Copyright 2019, American Chemical Society. e Proposed mechanism of O2 evolution over HCM@Ni–N; f free energy diagram at 0 V for OER over HCM, HCM@N, HCM@Ni–N. Reproduced with permission from Ref. [105]. Copyright 2019, Wiley

Fig. 10

Reproduced with permission from Ref. [113]. Copyright 2017, Elsevier

Fig. 11

Reproduced with permission from Ref. [118]. Copyright 2021, Elsevier

Fig. 12

Reproduced with permission from Ref. [122]. Copyright 2019, American Chemical Society

Fig. 13

Reproduced with permission from Ref. [44]. Copyright 2022, American Chemical Society. b Fabrication scheme of C–MOF–ACs and mechanism of sulfite activation. Reproduced with permission from Ref. [112]. Copyright 2020, American Chemical Society

Fig. 14

Reproduced with permission from Ref. [133]. Copyright 2017, Elsevier

Fig. 15

Reproduced with permission from Ref. [139]. Copyright 2021, Springer Nature

Fig. 16

Reproduced with permission from Ref. [152]. Copyright 2020, Elsevier. c Schematic mechanism of hydrodefluorination activation on Pt–SACs. Reproduced with permission from Ref. [155]. Copyright 2018, American Chemical Society

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Acknowledgements

This study was financially supported by the National Natural Science Foundation of China (No. 52200055), the Natural Science Foundation of Jiangsu Province (No. BK20210483), China Postdoctoral Science Foundation (No. 2022T150271) and the Natural Science Research of Jiangsu Higher Education Institutions of China (No. 23KJB610001).

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  1. School of Urban Construction, Changzhou University, Changzhou, 213164, China

    Jie Teng, Jin-Hui Xu, Xue-Feng Liu & Xia Xu

  2. School of Environmental and Civil Engineering, Jiangnan University, Wuxi, 214122, China

    Wen-Xin Sun & Guo-Shuai Liu

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  1. Jie Teng
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Teng, J., Xu, JH., Sun, WX. et al. Single-atom catalysis for advanced oxidation and reduction systems in water decontamination. Rare Met. (2024). https://doi.org/10.1007/s12598-024-02709-6

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