Wang Zhao-Di, Han Ye, Wang Ying-Ying, Zang Shuang-Quan, Peng Peng
Henan Key Laboratory of Crystalline Molecular Functional Materials and College of Chemistry, Zhengzhou University, Zhengzhou, 450001, China.
Angew Chem Int Ed Engl. 2025 Jan 27;64(5):e202416973. doi: 10.1002/anie.202416973. Epub 2024 Nov 19.
Constructing catalysts that simultaneously contain single atom/metal nanocluster active sites is a promising strategy to enhance the original catalytic behavior and accelerate the catalysis involving multi-electron reactions or multi-intermediates. Herein, the pyrolysis-free synthetic method is developed to integrate single atoms and nanoclusters towards highly satisfactory catalytic performances for both acidic and alkaline hydrogen electrocatalysis. The controllable pyrolysis-free strategy allows the precise modulation of the active centers, realizing the optimization of the adsorption energy and the regulation of the synergistic active components. Specially, the as-prepared catalysts with hybrid single-atom/nanocluster sites exhibited superior catalytic activities for hydrogen evolution in both acidic and alkaline media with low over-potentials at -10 mA cm of 25 mV and 8.6 mV, respectively, combining with outstanding durability towards high current density and methanol poisoning. This work developed a universal synthetic strategy for the single atom/nanocluster synergy systems and addressed the superiority of hybrid single-atom/nanocluster sites.
构建同时包含单原子/金属纳米团簇活性位点的催化剂是一种很有前景的策略，可增强原始催化性能并加速涉及多电子反应或多中间体的催化过程。在此，开发了一种无热解合成方法，将单原子和纳米团簇整合在一起，以实现对酸性和碱性氢电催化均高度令人满意的催化性能。可控的无热解策略允许对活性中心进行精确调控，实现吸附能的优化和协同活性组分的调节。特别地，所制备的具有单原子/纳米团簇混合位点的催化剂在酸性和碱性介质中均表现出优异的析氢催化活性，在 -10 mA cm时的过电位分别低至25 mV和8.6 mV，同时对高电流密度和甲醇中毒具有出色的耐久性。这项工作为单原子/纳米团簇协同体系开发了一种通用的合成策略，并揭示了单原子/纳米团簇混合位点的优势。
