Liu Siyu, Liu Shangheng, Bao Jingliang, Huang Zhongliang, Wei Licheng, Chen Nanjun, Hu Zhiwei, Huang Wei-Hsiang, Pao Chih-Wen, Kong Qingyu, Han Jiajia, Li Leigang, Huang Xiaoqing
State Key Laboratory of Physical Chemistry of Solid Surfaces, College of Chemistry and Chemical Engineering, Xiamen University, Xiamen, 361005, China.
Max Planck Institute for Chemical Physics of Solids, Nothnitzer Strasse 40, Dresden, 01187, Germany.
Angew Chem Int Ed Engl. 2025 Mar 17;64(12):e202421013. doi: 10.1002/anie.202421013. Epub 2025 Jan 7.
PtRu-based catalysts toward hydrogen oxidation reaction (HOR) suffer from low efficiency, CO poisoning and over-oxidation at high potentials. In this work, an amorphization strategy is adopted for preparation of amorphous SrRuPtOH nanobelts (a-SrRuPtOH NBs). The a-SrRuPtOH NBs has optimized adsorption of intermediates (H and OH), increased number of active sites, highly weakened CO poisoning and enhanced anti-oxidation ability owing to the special amorphous structure. Consequently, a-SrRuPtOH NBs displays superior HOR performance with a mass activity of 7.5 A/mg, 25 and 5 times of that of SrRuPt(OH) NBs and commercial PtRu/C, respectively, and long-lasting stability. Besides, a peak power density of 750 mW/cm and a specific power of 14.8 W/mg have been achieved for a-SrRuPtOH NBs at a low loading of 0.05 mg/cm, surpassing many reported HOR catalysts. Mechanism investigation indicates that Pt and Ru are present in oxide/hydroxide forms and H in a-SrRuPtOH NBs participates in HOR. Ab initio molecular dynamics (AIMD) simulations and density functional theory (DFT) calculations show that there are three catalytic mechanisms participating in a-SrRuPtOH NBs, which all exhibit low catalytic barrier and highly improved HOR efficiency. This work provides a new strategy for designing high-performance catalysts towards fuel cells.
基于PtRu的氢氧化反应(HOR)催化剂存在效率低、CO中毒以及在高电位下过度氧化等问题。在这项工作中,采用非晶化策略制备了非晶态SrRuPtOH纳米带(a-SrRuPtOH NBs)。由于特殊的非晶结构,a-SrRuPtOH NBs对中间体(H和OH)具有优化的吸附,活性位点数量增加,CO中毒高度减弱且抗氧化能力增强。因此,a-SrRuPtOH NBs表现出优异的HOR性能,质量活性为7.5 A/mg,分别是SrRuPt(OH) NBs和商业PtRu/C的25倍和5倍,并且具有持久的稳定性。此外,在0.05 mg/cm的低负载量下,a-SrRuPtOH NBs实现了750 mW/cm的峰值功率密度和14.8 W/mg的比功率,超过了许多报道的HOR催化剂。机理研究表明,Pt和Ru以氧化物/氢氧化物形式存在,a-SrRuPtOH NBs中的H参与HOR。从头算分子动力学(AIMD)模拟和密度泛函理论(DFT)计算表明,a-SrRuPtOH NBs中存在三种催化机制,均表现出低催化势垒和高度提高的HOR效率。这项工作为设计用于燃料电池的高性能催化剂提供了一种新策略。