武汉大学庄林团队报道了多维电化学解码氢氧化的运行机制。相关研究成果发表在2024年4月13日出版的国际学术期刊《德国应用化学》。

氢氧化反应（HOR）作为一种有效利用氢能的方法，在当前的碳中和时间内具有特别重要的意义。然而，HOR的机理仍然很模糊，主要是因为这种反应的基本步骤是快速且高度纠缠的，尤其是当偏离热力学平衡状态时。

该文中，研究人员报告了一种在运行条件下解码HOR机制的策略。除了使用气体扩散电极获得的宽电势范围I-V曲线外，还应用了交流阻抗谱来提供独立和互补的动力学信息。结合多维数据源使研究人员能够在数学上精确地拟合5-D数据空间中的核心动力学参数集。因此，作为过电势的函数的三个元素步骤（Tafel、Heyrovsky和Volmer反应）的反应速率可以单独蒸馏。这样一幅未记录的动力学图像详细揭示了HOR是如何由极化的基本步骤控制的。

该发现不仅为更好地理解HOR机制提供了依据，而且为开发改进的氢能利用系统奠定了基础。

附：英文原文

Title: Multidimensional electrochemistry decodes the operando mechanism of hydrogen oxidation

Author: Kaicong Yang, Hualong Ma, Renjie Ren, Li Xiao, Wenyong Jiang, Yu Xie, Gongwei Wang, Juntao Lu, Lin Zhuang

Issue&Volume: 2024-04-13

Abstract: Being an efficient approach to the utilization of hydrogen energy, the hydrogen oxidation reaction (HOR) is of particular significance in the current carbon-neutrality time. Yet the mechanistic picture of the HOR is still blurred, mostly because the elemental steps of this reaction are rapid and highly entangled, especially when deviating from the thermodynamic equilibrium state. Here we report a strategy for decoding the HOR mechanism under operando conditions. In addition to the wide-potential-range I-V curves obtained using gas diffusion electrodes, we have applied the AC impedance spectroscopy to provide independent and complementary kinetic information. Combining multidimensional data sources has enabled us to fit, in mathematical rigor, the core kinetic parameter set in a 5-D data space. The reaction rate of the three elemental steps (Tafel, Heyrovsky, and Volmer reactions), as a function of the overpotential, can thus be distilled individually. Such an undocumented kinetic picture unravels, in detail, how the HOR is controlled by the elemental steps on polarization. Our findings not only offer a better understanding of the HOR mechanism, but also lay the foundation for the development of improved hydrogen energy utilization systems.

DOI: 10.1002/anie.202318389

Source: https://onlinelibrary.wiley.com/doi/10.1002/anie.202318389