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Value-added formate production from selective ethylene glycol oxidation based on cost-effective self-supported MOF nanosheet arrays

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In order to realize electrochemical upgrading and improve the energy conversion efficiency, an ingenious strategy of constructing a thermodynamically favorable oxidation reaction to replace oxygen evolution reaction (OER) is proposed. Here we report the self-supported NiCo-based metal–organic framework (MOF) nanosheet arrays grown on a stainless-steel mesh (NiCo-SS), which can be used as a highly efficient and cost-effective electrocatalyst for ethylene glycol oxidation reaction (EGOR) coupling with hydrogen evolution reaction (HER) in the pair-electrolysis system to concurrently produce value-added formate and high-purity hydrogen. Impressively, the required potential for EGOR at the anode is 200 mV lower than that for OER to deliver the same current density of 100 mA·cm−2. In addition, the pair-electrolysis of selective ethylene glycol oxidation and hydrogen evolution only requires a quite low voltage of 1.68 V to achieve the current density of 50 mA·cm−2 in the membrane-free dual-electrode electrolytic cell, 200 mV smaller than that for overall water splitting. Moreover, Faradaic efficiencies of over 80% for formate production have been obtained. This work indicates that it is prospective to employ earth-abundant electrocatalysts to concurrently produce high-purity hydrogen and value-added formate, which would be a promising technology for supplying clean and renewable energy.

Graphical abstract

摘要

为了实现电化学升级和提高能量转换效率, 我们提出了一种构建热力学有利的氧化反应取代析氧反应 (OER) 的巧妙策略。在这里, 我们报道了在不锈钢网 (NiCo-SS) 上生长自支撑镍钴基金属有机框架 (MOF) 纳米片阵列, 作为乙二醇氧化反应 (EGOR) 与析氢反应 (HER) 电解对系统中的高效、经济的电催化剂, 同时产生高附加值甲酸和高纯氢气。令人印象深刻的是, 在100 mA·cm−2的相同电流密度下, EGOR在阳极上所需的电位比OER低200 mV。此外, 在无膜双电极电解池中, 乙二醇选择性氧化和析氢反应仅需1.68 V的较低电压即可达到50 mA·cm−2的电流密度, 比整体水分解的电压小200 mV。 此外, 还获得了超过80%的甲酸法拉第效率。研究结果表明, 利用廉价的电催化剂同时生产高纯氢和高附加值甲酸是一种很有前景的清洁可再生能源技术。

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Acknowledgements

This study was financially supported by the National Natural Science Foundation of China (Nos. 21901246 and 22175174) and the Natural Science Foundation of Fujian Province (Nos. 2020J01116 and 2021J06033).

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Authors and Affiliations

  1. College of Chemistry and Materials Science, Fujian Normal University, Fuzhou, 350007, China

    Lei Jiao

  2. State Key Laboratory of Structural Chemistry, Fujian Institute of Research on the Structure of Matter, Chinese Academy of Sciences (CAS), Fuzhou, 350002, China

    Lei Jiao, Wenbo Wei, Xiaofang Li, Cheng-Bin Hong, Shu-Guo Han, Muhammad Imran Khan & Qi-Long Zhu

  3. Fujian Science and Technology Innovation Laboratory for Optoelectronic Information of China, Fuzhou, 350108, China

    Qi-Long Zhu

  4. University of Chinese Academy of Sciences, Beijing, 100049, China

    Wenbo Wei, Shu-Guo Han & Qi-Long Zhu

  5. Research Institute of Sciences and Engineering (RISE), University of Sharjah, Sharjah, 27272, United Arab Emirates

    Muhammad Imran Khan

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Jiao, L., Wei, W., Li, X. et al. Value-added formate production from selective ethylene glycol oxidation based on cost-effective self-supported MOF nanosheet arrays. Rare Met. 41, 3654–3661 (2022). https://doi.org/10.1007/s12598-022-02072-4

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