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Polyoxometalates-derived nanostructures for electrocatalysis application

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Abstract

The conversion of intermittent renewable electrical energy to chemical energy is of great importance, which can not only mitigate current energy and environmental crisis but also contribute to the ongoing carbon neutrality national strategy. Electrocatalysis is serving as a low-carbon conversion technology that enables green and efficient energy conversion mainly through hydrogen evolution reaction (HER), carbon dioxide reduction reaction (CO2RR), and nitrogen reduction reaction (NRR). The core of electrocatalysis is the design and construction of low-cost, high-activity and high-stability electrocatalyst to drive reaction thermodynamics and kinetics. The employment of polyoxometalates (POMs) as platforms or precursors to construct different types of electrocatalysts has been widely reported. Herein, we systematically summarized the recent advances in POM-derived nanostructures for electrocatalysis application. The strategies for precursor design and electrocatalyst synthesis were briefly introduced. The morphology control, phase control, composite modulation, and heterostructure engineering in POM-derived nanostructures were presented in detail. The structure–activity relationship of POM-derived nanostructures is fully discussed for HER, CO2RR, and NRR applications. Finally, the current challenges and future outlooks of POM-derived nanostructures are summarized to provide insights toward high-efficiency electrocatalysts for energy conversion technologies.

Graphical abstract

摘要

将间歇性可再生电能转化为化学能具有重要意义，不仅可以缓解当前的能源和环境危机，而且有助于我国碳中和国家战略的实现。电催化是一种低碳转化技术，主要通过析氢反应(HER)、二氧化碳还原反应(CO2RR)和氮还原反应(NRR)实现绿色高效的能源转化。电催化的核心是设计和构建低成本、高活性、高稳定性的电催化剂来驱动反应。多金属氧酸盐(POMs)是一类具有精确原子结构的金属氧化物(V、Mo、Nb、Ta、Mo和W)聚阴离子簇。利用POMs作为平台或前体构建不同类型的电催化剂已被广泛报道。在此，我们系统地总结了近年来POMs衍生的纳米结构在电催化方面的应用进展；简要介绍了前驱体设计和电催化剂合成的策略；详细介绍了POMs纳米结构的形貌控制、晶相控制、组成调控和异质结构设计；充分讨论了POMs衍生纳米结构在HER、CO2RR和NRR应用中的构效关系；最后对POMs衍生纳米结构的当前挑战和未来展望进行总结，期望启发高效电催化剂的设计和制备。

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Scheme 1
Fig. 1

Reproduced with permission from Ref. [41]. Copyright 2019, Springer Nature. f Preparation route and g XRD pattern of super-Co3S4/P-WS2/Co9S8; polarization curves in h alkaline, i acid and j neutral HER; k, l calculated free energy; m electron density at WS2/Co3S4 interfaces. Reproduced with permission from Ref. [42]. Copyright 2022, Wiley-VCH

Fig. 2

Reproduced with permission from Ref. [46]. Copyright 2015, Wiley-VCH. d Illustration for synthesis of AlO@Mo2N–NrGO; e calculated reaction pathways for AlO@Mo2N–NrGO in alkaline and acid HER; f SEM and g TEM images of sample; polarization curves h with and i without IR compensation; j long-term durability test. Reproduced with permission from Ref. [47]. Copyright 2023, Wiley-VCH

Fig. 3

Reproduced with permission from Ref. [55]. Copyright 2016, The Royal Society of Chemistry. f Schematic illustration and g, h TEM images of N@Mo2C preparation; polarization curves of i in 0.5 mol·L−1 H2SO4 and j in 1 mol·L−1 KOH; k free energy diagram; l relationship of Ed-band and ΔGH* with number of N atoms doping. Reproduced with permission from Ref. [51]. Copyright 2018, Wiley-VCH

Fig. 4

Reproduced with permission from Ref. [59]. Copyright 2018, The Royal Society of Chemistry. g Synthesis procedure, h XRD pattern and i TEM images of MoP@PC; j polarization curves; k Tafel plot; l stability test. Reproduced with permission from Ref. [60]. Copyright 2018, American Chemical Society

Fig. 5

Reproduced with permission from Ref. [62]. Copyright 2018, Wiley-VCH. h Illustration of Mo2N–Mo2C synthesis; i, l high-resolution HAADF-STEM images; j, k SEM images of Mo2N–Mo2C; m polarization curves in 1 mol·L−1 KOH solution; n polarization curves and o overpotentials at different current densities in artificial seawater. Reproduced with permission from Ref. [68]. Copyright 2022, Wiley-VCH

Fig. 6

Reproduced with permission from Ref. [70]. Copyright 2021, Elsevier B.V. g Three-dimensional supramolecular network of PMo12/BPE; h XRD patterns and i polarization curves of Mo2C@NC for HER; j polarization curve of MoO2@NC for OER; k, l polarization curve of overall water splitting with Mo2C@NC as cathode and MoO2@NC as anode. Reproduced with permission from Ref. [71]. Copyright 2018, The Royal Society of Chemistry

Fig. 7

Reproduced with permission from Ref. [75]. Copyright 2018, The Royal Society of Chemistry. f Schematic illustration, g SEM image and h XRD pattern of FeS2/MoS2@RGO composite; i corresponding NRR activity and j mechanism. Reproduced with permission from Ref. [76]. Copyright 2022, Elsevier B.V. k Illustration and l NRR activity of CoS2/MoS2 synthesis. Reproduced with permission from Ref. [77]. Copyright 2022, Elsevier B.V

Fig. 8

Copyright 2018, Springer Nature. f Schematic diagram of Mo8@Cu/TNA for CO2RR; g SEM image, h, i electrochemical activity (cyan: hydrogen, red: ethanol, green: acetate, yellow: methane, blue: ethylene, purple: ethane) and j reaction mechanism of Mo8@Cu/TNA in CO2RR. Reproduced with permission from Ref. [95]. Copyright 2021, Elsevier B.V

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Acknowledgements

This study was financially supported by Shandong Provincial Natural Science Foundation (No. ZR2019BB025).

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  1. Chao-Yue Sun and Wen Li have contributed equally to this work.

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  1. Institute for Advanced Interdisciplinary Research (iAIR), College of Chemistry and Chemical Engineering, University of Jinan, Jinan, 250022, China

    Chao-Yue Sun, Wen Li, Wei-Jia Zhou & Hai-Qing Wang

  2. Shandong Electrical Engineering and Equipment Group Intelligent Electric Co., Ltd., Jinan, 250022, China

    Kai Wang

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  1. Chao-Yue Sun
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Sun, CY., Li, W., Wang, K. et al. Polyoxometalates-derived nanostructures for electrocatalysis application. Rare Met. 43, 1845–1866 (2024). https://doi.org/10.1007/s12598-023-02567-8

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