Ma Yi, Li Luming, Zhang Yong, Jian Ning, Pan Huiyan, Deng Jie, Li Junshan
School of Mechanical Engineering, Chengdu University, Chengdu 610106, China; Institute for Advanced Study, Chengdu University, Chengdu 610106, China.
Institute for Advanced Study, Chengdu University, Chengdu 610106, China; College of Food and Biological Engineering, Chengdu University, Chengdu 610106, China.
J Colloid Interface Sci. 2024 Jun;663:971-980. doi: 10.1016/j.jcis.2024.02.191. Epub 2024 Feb 29.
Electrochemical upgrading methanol into value-added formate at the anode in alkaline media enables the boosting production of hydrogen fuel at the cathode with saved energy. To achieve such a cost-effective and efficient electrocatalytic process, herein this work presents a Mn-doped nickel iron layered double hydroxides supported on nickel foam, derived from a simple hydrothermal synthesis. This developed electrocatalyst could act as an efficient bifunctional electrocatalyst for methanol-to-formate with a high faradaic efficiency of nearly 100 %, and for hydrogen evolution reaction, at an external potential of 1.5 V versus reversible hydrogen electrode. Additionally, a current density of 131.1 mA cm with a decay of merely 12.2 % over 120 h continuous long-term testing was generated in co-electrocatalysis of water/methanol solution. Further density functional theoretical calculations were used to unravel the methanol-to-formate reaction mechanism arising from the doping of Fe and/or Mn. This work offers a good example of co-electrocatalysis to produce formate and green hydrogen fuel using a bifunctional electrocatalyst.
在碱性介质中，通过电化学方法将甲醇在阳极升级为增值甲酸盐，能够在阴极节省能源的情况下提高氢燃料的产量。为了实现这种具有成本效益且高效的电催化过程，本文介绍了一种通过简单水热合成法制备的负载在泡沫镍上的锰掺杂镍铁层状双氢氧化物。这种开发的电催化剂可作为一种高效的双功能电催化剂，用于甲醇制甲酸盐，法拉第效率接近100%，并且在相对于可逆氢电极1.5 V的外部电势下用于析氢反应。此外，在水/甲醇溶液的共电催化中，连续120小时的长期测试产生了131.1 mA cm的电流密度，衰减仅为12.2%。进一步的密度泛函理论计算用于揭示由铁和/或锰掺杂引起的甲醇制甲酸盐反应机理。这项工作为使用双功能电催化剂共电催化生产甲酸盐和绿色氢燃料提供了一个很好的例子。
