Xinran Jiao , Chaoqun Ma , Biao Huang , Dengke Zhao , Fukai Feng , Sumei Han , Nailiang Yang , Qipeng Lu , Yiyao Ge , Qian Xu
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Specifically, Pd-Ru MNSs demonstrate excellent HER performance in alkaline electrolyte, requiring an overpotential of only 16 mV to reach 10 mA cm<sup>−2</sup>, significantly outperforming Pd mesoporous nanosheets and commercial catalysts. Density functional theory calculations reveal that the Ru sites in Pd-Ru MNSs could facilitate the water adsorption, accelerate the water dissociation, and optimize the hydrogen desorption, leading to the superior HER activity. Pd-Ru MNSs also exhibit high mass activities of 11.19 A mg<sup>−1</sup><sub>Pd</sub> for EGOR and 8.84 A mg<sup>−1</sup><sub>Pd</sub> for EOR, which is 7.8 and 9.6 times than that of commercial Pd/C, respectively. The EGOR reaction pathway over Pd-Ru MNSs was further investigated by using <em>in situ</em> Fourier-transform infrared spectroscopy.</div></div>","PeriodicalId":7283,"journal":{"name":"Advanced Powder Materials","volume":"4 5","pages":"Article 100320"},"PeriodicalIF":0.0000,"publicationDate":"2025-07-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"Submonolayered Ru-modified Pd mesoporous nanosheets as multifunctional electrocatalyst for hydrogen evolution and alcohol oxidation reactions\",\"authors\":\"Xinran Jiao , Chaoqun Ma , Biao Huang , Dengke Zhao , Fukai Feng , Sumei Han , Nailiang Yang , Qipeng Lu , Yiyao Ge , Qian Xu\",\"doi\":\"10.1016/j.apmate.2025.100320\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"<div><div>The structural modulation of metal-based heterostructure plays a vital role in achieving enhanced performances for highly efficient electrocatalysis. Here we design submonolayered Ru-modified Pd mesoporous nanosheets (Pd-Ru MNSs) with the exposure of both Pd and Ru active sites as well as the high atomic utilization of two-dimensional structure. The obtained Pd-Ru MNSs can act as a highly efficient multifunctional catalyst for hydrogen evolution reaction (HER) and alcohol oxidation reactions including ethylene glycol oxidation (EGOR) and ethanol oxidation (EOR), offering new opportunities towards the alcohol oxidation assisted hydrogen production. Specifically, Pd-Ru MNSs demonstrate excellent HER performance in alkaline electrolyte, requiring an overpotential of only 16 mV to reach 10 mA cm<sup>−2</sup>, significantly outperforming Pd mesoporous nanosheets and commercial catalysts. Density functional theory calculations reveal that the Ru sites in Pd-Ru MNSs could facilitate the water adsorption, accelerate the water dissociation, and optimize the hydrogen desorption, leading to the superior HER activity. Pd-Ru MNSs also exhibit high mass activities of 11.19 A mg<sup>−1</sup><sub>Pd</sub> for EGOR and 8.84 A mg<sup>−1</sup><sub>Pd</sub> for EOR, which is 7.8 and 9.6 times than that of commercial Pd/C, respectively. 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引用次数: 0
摘要
金属基异质结构的结构调制对于提高高效电催化性能起着至关重要的作用。在这里,我们设计了亚单层的Ru修饰Pd介孔纳米片(Pd-Ru MNSs),同时暴露了Pd和Ru的活性位点,并且具有二维结构的高原子利用率。所制得的Pd-Ru MNSs可作为析氢反应(HER)和醇氧化反应(EGOR)、乙醇氧化(EOR)的高效多功能催化剂,为醇氧化辅助制氢提供了新的机遇。具体来说,Pd- ru MNSs在碱性电解质中表现出优异的HER性能,只需要16 mV的过电位就可以达到10 mA cm - 2,明显优于Pd介孔纳米片和商用催化剂。密度泛函理论计算表明,Pd-Ru MNSs中的Ru位点可以促进水吸附,加速水解离,优化氢脱附,从而使其具有较好的HER活性。Pd- ru MNSs的EGOR质量活性为11.19 A mg - 1Pd, EOR质量活性为8.84 A mg - 1Pd,分别是商业Pd/C的7.8倍和9.6倍。利用原位傅里叶变换红外光谱进一步研究了Pd-Ru MNSs上的EGOR反应途径。
Submonolayered Ru-modified Pd mesoporous nanosheets as multifunctional electrocatalyst for hydrogen evolution and alcohol oxidation reactions
The structural modulation of metal-based heterostructure plays a vital role in achieving enhanced performances for highly efficient electrocatalysis. Here we design submonolayered Ru-modified Pd mesoporous nanosheets (Pd-Ru MNSs) with the exposure of both Pd and Ru active sites as well as the high atomic utilization of two-dimensional structure. The obtained Pd-Ru MNSs can act as a highly efficient multifunctional catalyst for hydrogen evolution reaction (HER) and alcohol oxidation reactions including ethylene glycol oxidation (EGOR) and ethanol oxidation (EOR), offering new opportunities towards the alcohol oxidation assisted hydrogen production. Specifically, Pd-Ru MNSs demonstrate excellent HER performance in alkaline electrolyte, requiring an overpotential of only 16 mV to reach 10 mA cm−2, significantly outperforming Pd mesoporous nanosheets and commercial catalysts. Density functional theory calculations reveal that the Ru sites in Pd-Ru MNSs could facilitate the water adsorption, accelerate the water dissociation, and optimize the hydrogen desorption, leading to the superior HER activity. Pd-Ru MNSs also exhibit high mass activities of 11.19 A mg−1Pd for EGOR and 8.84 A mg−1Pd for EOR, which is 7.8 and 9.6 times than that of commercial Pd/C, respectively. The EGOR reaction pathway over Pd-Ru MNSs was further investigated by using in situ Fourier-transform infrared spectroscopy.