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Breaking Highly Ordered PtPbBi Intermetallic with Disordered Amorphous Phase for Boosting Electrocatalytic Hydrogen Evolution and Alcohol Oxidation
Angewandte Chemie International Edition ( IF 16.6 ) Pub Date : 2024-04-16 , DOI: 10.1002/anie.202405173
Fukai Feng 1 , Chaoqun Ma 1 , Sumei Han 1 , Xiao Ma 2 , Caihong He 3 , Huaifang Zhang 3 , Wenbin Cao 3 , Xiangmin Meng 4 , Jing Xia 4 , Lijie Zhu 5 , Yahui Tian 6 , Qi Wang 1 , Qinbai Yun 7 , Qipeng Lu 3
Affiliation  

Constructing amorphous/intermetallic (A/IMC) heterophase structures by breaking the highly ordered IMC phase with disordered amorphous phase is an effective way to improve the electrocatalytic performance of noble metal‐based IMC electrocatalysts because of the optimized electronic structure and abundant heterophase boundaries as active sites. In this study, we report the synthesis of ultrathin A/IMC PtPbBi nanosheets (NSs) for boosting hydrogen evolution reaction (HER) and alcohol oxidation reactions. The resulting A/IMC PtPbBi NSs exhibit a remarkably low overpotential of only 25 mV at 10 mA cm‐2 for the HER in an acidic electrolyte, together with outstanding stability for 100 h. In addition, the PtPbBi NSs show high mass activities for methanol oxidation reaction (MOR) and ethanol oxidation reaction (EOR), which are 13.2 and 14.5 times higher than those of commercial Pt/C, respectively. Density functional theory calculations demonstrate that the synergistic effect of amorphous/intermetallic components and multimetallic composition facilitate the electron transfer from the catalyst to key intermediates, thus improving the catalytic activity of MOR. This work establishes a novel pathway for the synthesis of heterophase two‐dimensional nanomaterials with high electrocatalytic performance across a wide range of electrochemical applications.

中文翻译:

用无序非晶相打破高度有序的 PtPbBi 金属间化合物,促进电催化析氢和醇氧化

通过用无序非晶相打破高度有序的IMC相来构建非晶/金属间化合物(A/IMC)异相结构是提高贵金属基IMC电催化剂电催化性能的有效方法,因为优化的电子结构和丰富的异相边界作为活性网站。在这项研究中,我们报道了超薄 A/IMC PtPbBi 纳米片 (NSs) 的合成,用于促进析氢反应 (HER) 和醇氧化反应。所得的 A/IMC PtPbBi NS 在酸性电解质中的 HER 中表现出极低的过电势,在 10 mA cm-2 下仅为 25 mV,并且具有 100 小时的出色稳定性。此外,PtPbBi NSs对甲醇氧化反应(MOR)和乙醇氧化反应(EOR)表现出较高的质量活性,分别比商业Pt/C高13.2和14.5倍。密度泛函理论计算表明,非晶/金属间化合物和多金属成分的协同作用促进了电子从催化剂转移到关键中间体,从而提高了MOR的催化活性。这项工作为合成在广泛的电化学应用中具有高电催化性能的异相二维纳米材料建立了一条新的途径。
更新日期:2024-04-16
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