Guizhou Provincial Key Laboratory of Computational Nano-Material Science, Guizhou Education University, Guiyang 550018, P. R. China.
Hefei National Research Center for Physical Sciences at the Microscale, University of Science and Technology of China, Hefei 230026, Anhui, P. R. China.
ACS Appl Mater Interfaces. 2023 Jun 7;15(22):26852-26862. doi: 10.1021/acsami.3c04342. Epub 2023 May 24.
Hydrazine oxidation-assisted water electrolysis provides a promising way for the energy-efficient electrochemical hydrogen (H) and synchronous decomposition of hydrazine-rich wastewater, but the development of highly active catalysts still remains a great challenge. Here, we demonstrate the robust and highly active Ru nanoparticles supported on the hollow N-doped carbon microtube (denoted as Ru NPs/H-NCMT) composite structure as HER and HzOR bifunctional electrocatalysts. Thanks to such unique hierarchical architectures, the as-synthesized Ru NPs/H-NCMTs exhibit prominent electrocatalytic activity in the alkaline condition, which needs a low overpotential of 29 mV at 10 mA cm for HER and an ultrasmall working potential of -0.06 V (vs RHE) to attain the same current density for HzOR. In addition, assembling a two-electrode hybrid electrolyzer using as-prepared Ru NPs/H-NCMT catalysts shows a small cell voltage of mere 0.108 V at 100 mA cm, as well as the remarkable long-term stability. Density functional theory calculations further reveal that the Ru NPs serve as the active sites for both the HER and HzOR in the nanocomposite, which facilitates the adsorption of H atoms and hydrazine dehydrogenation kinetics, thus enhancing the performances of HER and HzOR. This work paves a novel avenue to develop efficient and stable electrocatalysts toward HER and HzOR that promises energy-saving hybrid water electrolysis electrochemical H production.
水肼氧化辅助水电解为节能的电化学析氢(HER)和富水肼废水的同步分解提供了一种很有前途的方法,但开发高活性催化剂仍然是一个巨大的挑战。在这里,我们展示了负载在中空氮掺杂碳微管(表示为 Ru NPs/H-NCMT)复合材料结构上的稳定且高活性的 Ru 纳米颗粒作为 HER 和 HzOR 双功能电催化剂。由于这种独特的分层结构,所合成的 Ru NPs/H-NCMTs 在碱性条件下表现出突出的电催化活性,在 HER 中需要 29 mV 的低过电势即可达到 10 mA cm 的电流密度,而对于 HzOR,则需要超小的工作电势为-0.06 V(相对于 RHE)。此外,使用制备的 Ru NPs/H-NCMT 催化剂组装的两电极混合电解槽在 100 mA cm 时仅需 0.108 V 的小电池电压,并且具有出色的长期稳定性。密度泛函理论计算进一步表明,Ru NPs 纳米复合材料中的 HER 和 HzOR 均为活性位点,有利于 H 原子的吸附和水肼脱氢动力学,从而提高了 HER 和 HzOR 的性能。这项工作为开发高效稳定的电催化剂开辟了一条新途径,有望实现节能的混合水电解电化学析氢。