High Entropy Alloy Electrocatalytic Electrode toward Alkaline Glycerol Valorization Coupling with Acidic Hydrogen Production,Journal of the American Chemical Society

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High Entropy Alloy Electrocatalytic Electrode toward Alkaline Glycerol Valorization Coupling with Acidic Hydrogen Production
Journal of the American Chemical Society ( IF 14.4 ) Pub Date : 2022-04-11 , DOI: 10.1021/jacs.1c13740
Linfeng Fan ₁ , Yaxin Ji ₁ , Genxiang Wang ₁ , Junxiang Chen ₁ , Kai Chen ₁ , Xi Liu _{1,

2} , Zhenhai Wen ₁

Affiliation

Electrochemical glycerol oxidation reaction (GOR) is an attractive alternative anodic reaction to oxygen evolution reaction for a variety of electrolytic synthesis, thanks to the possibility of mass production of glycerol from biomass and the relative low thermodynamic potential of GOR. The development of high-activity cheap electrocatalysts toward GOR yet faces a daunting challenge. Herein, we experimentally prepare a new range of high entropy alloy (HEA) self-supported electrodes with uniform HEA nanoparticles grown on carbon cloth. The systematic electrochemical studies verify that the HEA-CoNiCuMnMo electrode exhibits attractive performance for GOR electrocatalysis with low overpotential and high selectivity toward formate products. The surface atomic configurations of HEA-CoNiCuMnMo are studied by a self-developed machine learning-based Monte Carlo simulation, which points out the catalytic active center to be Mo sites coordinated by Mn, Mo, and Ni. We further develop a hybrid alkali/acid flow electrolytic cell by pairing alkaline GOR with acidic hydrogen evolution reaction using the HEA-CoNiCuMnMo and the commercial RhIr/Ti as the anode and the cathode, respectively, which only requires an applied voltage of 0.55 V to reach an electrolytic current density of 10 mA cm^–2 and maintains long-term electrolysis stability over 12 days continuous running at 50 mA cm^–2 with Faraday efficiencies of over 99% for H₂ in the cathode and 92% for formate production in the anode.

中文翻译：

碱性甘油增值与酸性制氢耦合的高熵合金电催化电极

电化学甘油氧化反应 (GOR) 是用于各种电解合成的氧气析出反应的有吸引力的替代阳极反应，这要归功于从生物质中大量生产甘油的可能性和 GOR 相对较低的热力学势。开发用于 GOR 的高活性廉价电催化剂仍面临着艰巨的挑战。在此，我们通过实验制备了一系列新的高熵合金（HEA）自支撑电极，其具有在碳布上生长的均匀 HEA 纳米颗粒。系统的电化学研究证实了 HEA-CoNiCuMnMo 电极对 GOR 电催化表现出有吸引力的性能，具有低过电位和对甲酸盐产物的高选择性。HEA-CoNiCuMnMo的表面原子构型通过自主开发的基于机器学习的蒙特卡罗模拟研究，指出催化活性中心为Mn、Mo和Ni配位的Mo位点。我们进一步通过将碱性 GOR 与酸性析氢反应配对，使用 HEA-CoNiCuMnMo 和商用 RhIr/Ti 作为阳极和阴极，进一步开发了混合碱/酸流动电解池，只需施加 0.55 V 的电压即可达到 10 mA cm 的电解电流密度^{–2并在 50 mA cm}^–2下连续运行 12 天后保持长期电解稳定性，阴极中 H ₂的法拉第效率超过 99%，阳极中甲酸盐生产的法拉第效率超过 92%。

更新日期：2022-04-11

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