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Kinetic diffusion–controlled synthesis of twinned intermetallic nanocrystals for CO-resistant catalysis
Science Advances ( IF 13.6 ) Pub Date : 2022-06-22 , DOI: 10.1126/sciadv.abo4599
Kun Wang 1 , Lei Wang 1 , Zhen Yao 1 , Lei Zhang 1 , Luyao Zhang 1 , Xusheng Yang 1 , Yingbo Li 1 , Yang-Gang Wang 1 , Yan Li 2, 3, 4 , Feng Yang 1
Affiliation  

Intermetallic catalysts are of immense interest, but how heterometals diffuse and related interface structure remain unclear when there exists a strong metal-support interaction. Here, we developed a kinetic diffusion–controlled method and synthesized intermetallic Pt 2 Mo nanocrystals with twin boundaries on mesoporous carbon (Pt 2 Mo/C). The formation of small-sized twinned intermetallic nanocrystals is associated with the strong Mo-C interaction–induced slow Mo diffusion and the heterogeneity of alloying, which is revealed by an in situ aberration-corrected transmission electron microscope (TEM) at high temperature. The twinned Pt 2 Mo/C constitutes a promising CO-resistant catalyst for highly selective hydrogenation of nitroarenes. Theoretical calculations and environmental TEM suggest that the weakened CO adsorption over Pt sites of Pt 2 Mo twin boundaries and their local region endows them with high CO resistance, selectivity, and reusability. The present strategy paves the way for tailoring the interface structure of high–melting point Mo/W-based intermetallic nanocrystals that proved to be important for the industrially viable reactions.

中文翻译:

用于抗 CO 催化的孪晶金属间化合物纳米晶体的动力学扩散控制合成

金属间化合物催化剂引起了极大的兴趣,但是当存在强金属-载体相互作用时,异质金属如何扩散以及相关的界面结构仍不清楚。在这里,我们开发了一种动力学扩散控制方法并合成了金属间化合物 Pt2介孔碳(Pt)上具有孪晶界的 Mo 纳米晶体2月/日)。高温下原位像差校正透射电子显微镜 (TEM) 揭示了小尺寸孪晶金属间化合物纳米晶体的形成与强 Mo-C 相互作用诱导的慢 Mo 扩散和合金化的异质性有关。双胞胎 Pt2Mo/C 是一种很有前途的耐 CO 催化剂,可用于硝基芳烃的高选择性加氢。理论计算和环境 TEM 表明,在 Pt 的 Pt 位点上减弱的 CO 吸附2Mo孪晶边界及其局部区域赋予它们高CO阻力、选择性和可重复使用性。目前的策略为定制高熔点 Mo/W 基金属间化合物纳米晶体的界面结构铺平了道路,这被证明对工业上可行的反应很重要。
更新日期:2022-06-22
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