Zhou Wenbo, Huang Yichao, Cai Hanqing, Wang Tao, Li Haitao, Zhang Chao, Zhao Lianming, Chen Lulu, Liao Meihong, Tang Zhiqing, Chen Kai, Gu Jing, Gao Wenpei, Fan Zhuangjun, Wen Zhenhai
State Key Laboratory of Chemical Safety, Shandong Key Laboratory of Intelligent Energy Materials, School of Materials Science and Engineering, China University of Petroleum (East China), Qingdao, 266580, People's Republic of China.
State Key Laboratory of Metal Matrix Composites, School of Materials Science and Engineering, Future Material Innovation Center, Zhangjiang Institute for Advanced Study, Shanghai Jiao Tong University, Shanghai, 200240, People's Republic of China.
Nanomicro Lett. 2025 Jun 13;17(1):296. doi: 10.1007/s40820-025-01798-x.
Creating strongly coupled heterostructures with favorable catalytic activities is crucial for promoting the performance of catalytic reactions, especially those involve multiple intermediates. Herein, we fabricated a strongly coupled platinum/molybdenum nitrides nanocluster heterostructure on nitrogen-doped reduced graphene oxide (Pt/Mo₂N-NrGO) for alkaline hydrogen evolution reaction. The well-defined Pt-containing Anderson-type polyoxometalates promote strong interfacial Pt-N-Mo bonding in Pt/MoN-NrGO, which exhibits a remarkably low overpotential, high mass activity, and exceptional long-term durability (> 500 h at 1500 mA cm⁻) in an anion-exchange membrane water electrolyzer (AEMWE). Operando Raman spectroscopy and density functional theory reveal that pronounced electronic coupling at the Pt/Mo₂N cluster interface facilitates the catalytic decomposition of HO through synergistic stabilization of intermediates (Pt-H* and Mo-OH*), thereby enhancing the kinetics of the rate-determining Volmer step. Techno-economic analysis indicates a levelized hydrogen production cost of $2.02 kg⁻, meeting the US DOE targets. Our strategy presents a viable pathway to designing next-generation catalysts for industrial AEMWE for green hydrogen production.
创建具有良好催化活性的强耦合异质结构对于提高催化反应性能至关重要，尤其是那些涉及多种中间体的反应。在此，我们在氮掺杂还原氧化石墨烯（Pt/Mo₂N-NrGO）上制备了一种用于碱性析氢反应的强耦合铂/氮化钼纳米团簇异质结构。明确的含铂安德森型多金属氧酸盐促进了Pt/MoN-NrGO中强的界面Pt-N-Mo键合，该异质结构在阴离子交换膜水电解槽（AEMWE）中表现出极低的过电位、高质量活性和出色的长期耐久性（在1500 mA cm⁻下超过500小时）。原位拉曼光谱和密度泛函理论表明，Pt/Mo₂N团簇界面处明显的电子耦合通过中间体（Pt-H和Mo-OH）的协同稳定促进了HO的催化分解，从而增强了速率决定步骤Volmer步骤的动力学。技术经济分析表明，平准化制氢成本为2.02美元/千克，符合美国能源部的目标。我们的策略为设计用于绿色制氢的工业AEMWE的下一代催化剂提供了一条可行的途径。
