دورية أكاديمية
Atomic Three-Dimensional Investigations of Pd Nanocatalysts for Acetylene Semi-hydrogenation
| العنوان: | Atomic Three-Dimensional Investigations of Pd Nanocatalysts for Acetylene Semi-hydrogenation |
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| المؤلفون: | Fan Xue, Qiang Li, Mingxin Lv, Yuanfei Song, Tianxing Yang, Xiaoge Wang, Tianyi Li, Yang Ren, Koji Ohara, Yufei He, Dianqing Li, Qiheng Li, Xin Chen, Kun Lin, Xianran Xing |
| سنة النشر: | 2023 |
| مصطلحات موضوعية: | Biophysics, Biological Sciences not elsewhere classified, Chemical Sciences not elsewhere classified, Physical Sciences not elsewhere classified, Information Systems not elsewhere classified, reverse monte carlo, range ordered lattice, optimize chemical activity, heterogeneous catalysis process, unique compressed strain, ethylene adsorption energy, sph , complete acetylene conversion, atomic surface distribution, atomic 3d insight, surface strain, atomic level, performance catalysts, obvious weakening, new path, nanocatalyst surfaces, much higher, main factor, local structure, inherent insufficiency, ethylene selectivity, entailing shape, developing high, big challenge, better understanding |
| الوصف: | Deciphering the three-dimensional (3D) insight into nanocatalyst surfaces at the atomic level is crucial to understanding catalytic reaction mechanisms and developing high-performance catalysts. Nevertheless, better understanding the inherent insufficiency of a long-range ordered lattice in nanocatalysts is a big challenge. In this work, we report the local structure of Pd nanocatalysts, which is beneficial for demonstrating the shape–structure–adsorption relationship in acetylene hydrogenation. The 5.27 nm spherical Pd catalyst (Pd sph ) shows an ethylene selectivity of 88% at complete acetylene conversion, which is much higher than those of the Pd octahedron and Pd cube and superior to other reported monometallic Pd nanocatalysts so far. By virtue of the local structure revelation combined with the atomic pair distribution function (PDF) and reverse Monte Carlo (RMC) simulation, the atomic surface distribution of the unique compressed strain of Pd–Pd pairs in Pd sph was revealed. Density functional theory calculations verified the obvious weakening of the ethylene adsorption energy on account of the surface strain of Pd sph . It is the main factor to avoid the over-hydrogenation of acetylene. The present work, entailing shape-induced surface strain manipulation and atomic 3D insight, opens a new path to understand and optimize chemical activity and selectivity in the heterogeneous catalysis process. |
| نوع الوثيقة: | article in journal/newspaper |
| اللغة: | unknown |
| العلاقة: | https://figshare.com/articles/journal_contribution/Atomic_Three-Dimensional_Investigations_of_Pd_Nanocatalysts_for_Acetylene_Semi-hydrogenation/24649737Test |
| DOI: | 10.1021/jacs.3c08619.s001 |
| الإتاحة: | https://doi.org/10.1021/jacs.3c08619.s001Test https://figshare.com/articles/journal_contribution/Atomic_Three-Dimensional_Investigations_of_Pd_Nanocatalysts_for_Acetylene_Semi-hydrogenation/24649737Test |
| حقوق: | CC BY-NC 4.0 |
| رقم الانضمام: | edsbas.925D5F46 |
| قاعدة البيانات: | BASE |
| DOI: | 10.1021/jacs.3c08619.s001 |
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