Citation: Xin Feng, Kexin Guo, Chunguang Jia, Bowen Liu, Suqin Ci, Junxiang Chen, Zhenhai Wen. 耦合甘油高选择性转化为甲酸盐与制氢的酸碱双电解液流动电解器[J]. Acta Physico-Chimica Sinica, ;2024, 40(5): 230305. doi: 10.3866/PKU.WHXB202303050 shu

耦合甘油高选择性转化为甲酸盐与制氢的酸碱双电解液流动电解器

1.
Key Laboratory of Jiangxi Province for Persistent Pollutants Control and Resources Recycle, Nanchang Hangkong University, Nanchang 330063, China;
2.
CAS Key Laboratory of Design and Assembly of Functional Nanostructures, Fujian Provincial Key Laboratory of Nanomaterials, Fujian Institute of Research on the Structure of Matter, Chinese Academy of Sciences, Fuzhou 350002, China

Received Date: 28 March 2023
Revised Date: 31 May 2023
Accepted Date: 1 June 2023

Fund Project: The project was supported by the National Natural Science Foundation of China (22168025) and the Natural Science Foundation of Jiangxi Province (20192BAB203013, 20202ACBL203003).

氢气因其高能量密度、可持续性和燃烧后无污染等优点，被认为是取代传统化石燃料的最具前途的新兴能源载体之一。其中，电解水制氢技术因为其高效和绿色的特性而备受关注。然而电解水制氢过程通常受到阳极析氧反应(Oxygen Evolution Reaction，OER)的限制，因此这种方法的大规模应用面临重大挑战。克服这一难题的一个有前途的解决方法是在阳极上使用电催化甘油氧化反应(Glycerol Oxidation Reaction，GOR)代替OER，这种替代反应可以实现节能降耗的同时提高电解水制氢的效率，进一步推动氢气作为清洁能源的发展。然而，这一目标的实现需要高效、低成本且高选择性的GOR电催化剂。在这篇文章中，我们报告了一种新型的酸碱双电解质流电解器(AADEF-electrolyzer)，用于在碱性阳极GOR耦合酸性阴极析氢反应(Hydrogen Evolution Reaction，HER)。我们通过一种简单的水热煅烧方法制备了一种在镍泡沫(NF)上原位生长的自支撑的NiCo₂O₄纳米针电极材料(NiCo₂O₄/NF)。该电极在GOR中表现出优异的电催化性能，在低电位下实现了高的电解电流密度，对甲酸盐的生产表现出优异的选择性，法拉第效率超过85%。密度泛函理论计算表明，NiCo₂O₄对GOR具有较低的反应能垒，Ni的存在有利于降低Co的电子态密度，从而实现NiCo₂O₄与中间体的高效解离，促进甲酸的生成。基于NiCo₂O₄/NF出色的GOR性能和电化学中和能(ENE)理论，我们构建了一个新型的AADEF-electrolyzer，利用NiCo₂O₄/NF作为GOR的阳极，配合酸性阴极进行析氢反应(HER)。实验结果表明，AADEF-electrolyzer对GOR具有低过电位和高选择性产甲酸的优异性能，仅需0.36 V的电压即可实现10 mA·cm^-2的电流密度，平均产甲酸的法拉第效率为85%。同时该电解槽表现出良好的长期稳定性和辅助产氢性能，阴极产氢的法拉第效率接近100%。这种低成本、易于制备的自支撑电极材料和新型酸碱双电解质流动电解器为促进化学品的增值转化和开发新型混合电解系统或其他相关电化学反应的混合电解装置提供了创新策略。
- Hydrogen production,
- Glycerol oxidation,
- Electrocatalysis,
- Electrolyzer
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