Lei Hang, Zhou Yifan, Huangfu Zhuowen, Chen Liangjun, Cao Jin, Yang Xuelin, Mai Wenjie, Wang Zilong
Hubei Provincial Collaborative Innovation Center for New Energy Microgrid, College of Electrical Engineering & New Energy, China Three Gorges University, Yichang, Hubei, 443002, P. R. China.
Key Laboratory of Advanced Energy Materials Chemistry (Ministry of Education), Nankai University, Tianjin, 300071, P. R. China.
Adv Sci (Weinh). 2025 Jul;12(27):e2504462. doi: 10.1002/advs.202504462. Epub 2025 Apr 30.
Constructing electrocatalysts with high activity and low precious metal content is essential for achieving efficient hydrogen production in pH-universal overall water splitting. Herein, five types of noble metal anchored transition metal phosphides are analyzed by theoretical derivation. Based on the calculation results, a suitable hybrid is screened out of Pt nanoparticles anchored on CoP nanowires (Pt─CoP) via robust Pt─P─Co bonds. This strong synergy between Pt and CoP through interfacial Pt─P─Co bonds optimizes the adsorption of key intermediates for hydrogen evolution reaction (HER) in a wide pH range from 0 to 14. Furthermore, strong interaction between Pt and CoP accompanied by a delicate structure reduces interfacial charge transfer resistance, creates abundant active sites, and enhances catalyst durability, while facilitating active site exposure and electron/mass transfer during the HER process. Accordingly, the synthesized Pt─CoP exhibits low overpotentials of 79, 26, and 18 mV at 10 mA cm in acidic, neutral, and alkaline media for HER, respectively, superior to commercial Pt/C benchmarks and most reported electrocatalysts. This work paves a new clue to exploit electrocatalysts with low-Pt-loading for pH-universal HER.
构建具有高活性和低贵金属含量的电催化剂对于在pH通用的全水解中实现高效产氢至关重要。在此,通过理论推导分析了五种类型的贵金属锚定过渡金属磷化物。基于计算结果,通过坚固的Pt─P─Co键从锚定在CoP纳米线上的Pt纳米颗粒(Pt─CoP)中筛选出合适的杂化物。Pt与CoP之间通过界面Pt─P─Co键的这种强协同作用在0至14的宽pH范围内优化了析氢反应(HER)关键中间体的吸附。此外,Pt与CoP之间的强相互作用伴随着精细的结构降低了界面电荷转移电阻,创造了丰富的活性位点,增强了催化剂的耐久性,同时在HER过程中促进了活性位点的暴露以及电子/质量转移。因此,合成的Pt─CoP在酸性、中性和碱性介质中,对于HER在10 mA cm时分别表现出79、26和18 mV的低过电位,优于商业Pt/C基准和大多数报道的电催化剂。这项工作为开发用于pH通用HER的低Pt负载电催化剂提供了新的线索。