Efficient hydrogen production through water splitting relies on the development of high-performance catalysts for the hydrogen evolution reaction (HER). In this study, we synthesized the CoNi SAs@NPs-NC catalyst using multi-metal single-crystal ordered macroporous metal-organic frameworks (MOFs) as precursors. This catalyst features a hierarchical porous structure with ordered macropores and micropores, which not only provides a high specific surface area but also promotes efficient mass diffusion. Furthermore, the incorporation of bimetallic components, coupled with synergistic interactions between single atoms (SAs) and nanoparticles (NPs), significantly enhances its catalytic activity. The CoNi SAs@NPs-NC nanocatalysts demonstrated exceptional activity in the HER, recording overpotentials of 90 mV in 1 M KOH and 61 mV in 0.5 M H₂SO₄, both at a current density of 10 mA cm^-2. In addition, density functional theory (DFT) analysis was employed to investigate the synergistic interactions among CoNi NPs, SAs, and nitrogen dopants. Our finding highlights the promising potential of the CoNi SAs@NPs-NC catalyst for efficient hydrogen evolution, making it a valuable candidate for advancing the field of water splitting.

摘要

本研究中, 我们使用多金属单晶有序大孔金属-有机框架(MOFs) 作为前体, 合成了CoNi SAs@NPs-NC催化剂. 该催化剂具有大孔和微 孔的多级孔结构, 该结构不仅提供了高比表面积, 还提供了快速的物质 扩散通道. 此外, 该催化剂具有的双金属组分, 以及单原子(SAs)和纳米 颗粒(NPs)之间的协同作用显著增强了其催化活性. CoNi SAs@NPs-NC 纳米催化剂在析氢反应中展示了卓越的活性, 在1 M的KOH和0.5 M的 H₂SO₄中分别具有90和61 mV的过电势(电流密度10 mA cm⁻²). 此外, 我们还使用密度泛函理论(DFT)分析研究了CoNi NPs与SAs之间的协 同作用. 本工作展示了CoNi SAs@NPs-NC催化剂在高效析氢中的潜力.