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Graphene oxide-derived single-atom catalysts for electrochemical energy conversion

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Abstract

Sustainable electrochemical energy conversion is considered as a promising solution to energy crises and environmental issues. Owing to their maximized utilization efficiency and excellent catalytic performance, single-atom catalysts (SACs) have obtained tremendous attention in the field of electrochemical energy conversion. In the last few years, graphene oxide (GO) has been considered to be a promising precursor for fabricating graphene-supported SACs due to its advantageous features such as large surface area, high density of intrinsic defects, and scalability. In this review, the recent advances in the preparation of graphene oxide-derived single-atom catalysts (GO-SACs) and their diverse electrochemical applications are summarized. Firstly, the synthetic strategies of GO-SACs are discussed with focuses on the advantages and shortages of each method. Subsequently, the electrochemical applications of GO-SACs in various energy conversion processes, including the oxygen reduction reaction (ORR), oxygen evolution reaction (OER), hydrogen evolution reaction (HER), nitrogen reduction reaction (NRR), and carbon dioxide reduction reaction (CO2RR), are discussed in detail. Finally, the remaining challenges and future prospects in the fabrication and application of GO-SACs are presented.

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摘要

可持续的电化学能量转换被认为是解决能源危机和环境问题的理想方案。单原子催化剂由于其最大的原子利用率和优异的催化性能, 在电化学能量转换领域引起了极大的关注。在过去的几年中, 氧化石墨烯由于其具有大表面积、高密度的本征缺陷和可大批量制备等优点, 被认为是制备石墨烯负载单原子催化剂的重要前驱体。此综述中, 我们总结了氧化石墨烯衍生的单原子催化剂的制备及其各种电化学应用的最新进展。首先, 讨论了氧化石墨烯衍生的单原子催化剂的合成策略, 重点介绍了每种方法的优缺点。随后, 介绍了该类催化剂在各种能量转换过程中的电化学应用, 包括氧还原反应、析氧反应、析氢反应、氮还原反应和二氧化碳还原反应等。最后, 我们总结了该类催化剂在制备和应用中面临的挑战和具有的前景。

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Fig. 1
Fig. 2

Copyright 2013, Nature Publishing Group. b Schematic illustration of single-atom Pd1/graphene catalyst synthesis; c low-magnification HAADF-STEM images of Pd1/graphene; d high-magnification HAADF-STEM images of Pd1/graphene, where atomically dispersed Pd atoms are highlighted by white circles. Reproduced with permission Ref. [66]. Copyright 2015, American Chemical Society

Fig. 3

Reproduced with permission from Ref. [70]. Copyright 2017, American Chemical Society. b Preparation route to synthesize various monodispersed atomic metals embedded in 3D holey graphene frameworks. Reproduced with permission from Ref. [79]. Copyright 2018, Nature Publishing Group. c Schematic illustration showing that FePc molecules supported on 3D hollow graphene nanospheres facilitated formation of Fe single atoms. Reproduced with permission from Ref. [81]. Copyright 2018, Wiley–VCH. d Schematic illustration of synthesis process of Fe–N/GNs, which used GO-supported Fe/ZIF-8 as precursors. Reproduced with permission from Ref. [82]. Copyright 2020, Wiley–VCH

Fig. 4

Reproduced with permission from Ref. [87]. Copyright 2018, Wiley–VCH

Fig. 5

Reproduced with permission from Ref. [88]. Copyright 2018, Royal Society of Chemistry. c Schematic illustration of preparation of Co2+/GO hybrids; d EXAFS-FT analysis of Co2+/GO (blue), CoCO3 (red), and metallic cobalt (black). Reproduced with permission from Ref. [89]. Copyright 2017, American Chemical Society

Fig. 6

Reproduced with permission from Ref. [71]. Copyright 2019, American Chemical Society

Fig. 7

Reproduced with permission from Ref. [51]. Copyright 2015, Nature Publishing Group. e EXAFS-FT spectra of Co-SAC; f LSV curves of Ni-SAC, W-SAC Co-SAC for HER along with control sample of metal-free NG; g scheme of orbital hybridization of catalysts active sites with hydrogen (σ = bonding and σ* = antibonding state orbital); h Gibbs free energy (ΔGH*) diagram for hydrogen adsorption step (Volmer reaction) for a series of transition metals-based SACs. Reproduced with permission from Ref. [110]. Copyright 2019, Wiley–VCH

Fig. 8

Reproduced with permission from Ref. [82]. Copyright 2020, Wiley–VCH. d EXAFS-FT spectra of CoNG-350 and reference samples; e ORR polarization curves of CoNG-350 at rotation speed of 1600 r·min−1 with the scan rate of 5 mV·s−1; f discharge polarization curves and corresponding power density of CoNG-350 and Pt/C, respectively, in primary Zn-air batteries. Reproduced with permission from Ref. [93]. Copyright 2019, The Royal Society of Chemistry. g HAADF-STEM image of Sc@NG; h polarization curves of Sc@NG-750 and control samples at a rotation speed of 1600 r·min−1 in 0.1 mol·L−1 KOH; i K-L plots of Sc@NG-750 measured using a RDE in O2-saturated 0.1 mol·L−1 KOH. Reproduced with permission from Ref. [76]. Copyright 2019, Elsevier Ltd

Fig. 9

Reproduced with permission from Ref. [120]. Copyright 2019, American Chemical Society. b Schematic diagram of synthesis route for Co1–NG(O); c deconvoluted O 1s spectra of Co1–NG(O) and Co1–NG(R); d comparison of ORR performance at 1,600 r·min−1 (solid lines) and simultaneous H2O2 detection current densities at ring electrode (dashed lines) for NG(O), Co1–NG(O) and Co1–NG(R) in 0.1 mol·L−1 KOH; e calculated H2O2 selectivity as a function of applied potential; f mass activity at 0.65 V (vs. RHE); g chronoamperometry stability test of Co1–NG(O). Reproduced with permission from Ref. [96]. Copyright 2020, Nature Publishing Group. h Schematic illustration of synthesis of Ni-SA/G; i RRDE measurements of Ni-SA/G and control samples at 1600 r·min−1 under 10 mV·s−1; j electron transfer number (n) and H2O2 selectivity of Ni-SA/G and control samples. Reproduced with permission from Ref. [97]. Copyright 2020, American Chemical Society

Fig. 10

Reproduced with permission from Ref. [77]. Copyright 2018, Nature Publishing Group. d HAADF-STEM of Ni-NHGF, Co-NHGF and Fe-NHGF with scale bars: 5 nm (A), 2 nm (B), 0.5 nm (C–E); e OER polarization curves of Ni-NHGF along with control samples; f Tafel plots for Ni-NHGF and control samples. Reproduced with permission from Ref. [79]. Copyright 2018, Nature Publishing Group

Fig. 11

Reproduced with permission from Ref. [75]. Copyright 2018, The Royal Society of Chemistry. f HAADF-STEM images of Fe/NG-750 catalyst; g LSV curves of Fe/NG-750 catalyst on glassy carbon electrodes in Ar- or CO2-saturated 0.1 mol·L−1 KHCO3; h potential- dependent FE of CO for electrochemical CO2 reduction on Fe/NG catalysts prepared at different annealing temperatures; i partial current densities of CO on Fe/NG catalysts derived by corresponding potential-dependent FE data. Reproduced with permission from Ref. [78]. Copyright 2018, Wiley–VCH

Fig. 12

Reproduced with permission from Ref. [102]. Copyright 2021, Wiley–VCH

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Acknowledgements

This study was financially supported by National Natural Science Foundation of China (No. 51902099), Hunan High-Level Talent Gathering Project (No. 2019RS1021), the Fundamental Research Funds for the Central Universities (No. 531119200087) and the Natural Science Foundation of Hunan Province (No. 2020JJ4204).

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  1. State Key Laboratory of Chemo/Biosensing and Chemometrics, College of Chemistry and Chemical Engineering, Hunan University, Changsha, 410082, China

    Jian-Bin Liu, Hai-Sheng Gong, Gong-Lan Ye & Hui-Long Fei

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Liu, JB., Gong, HS., Ye, GL. et al. Graphene oxide-derived single-atom catalysts for electrochemical energy conversion. Rare Met. 41, 1703–1726 (2022). https://doi.org/10.1007/s12598-021-01904-z

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