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High‐Density and Thermally Stable Palladium Single‐Atom Catalysts for Chemoselective Hydrogenations
Angewandte Chemie International Edition ( IF 16.1 ) Pub Date : 2020-08-12 , DOI: 10.1002/anie.202007707
Ying Ma 1, 2 , Yujing Ren 1 , Yanan Zhou 3, 4 , Wei Liu 1 , Walid Baaziz 5 , Ovidiu Ersen 5 , Cuong Pham‐Huu 6 , Mark Greiner 7 , Wei Chu 4 , Aiqin Wang 1 , Tao Zhang 1 , Yuefeng Liu 1
Affiliation  

Single‐atom catalysts (SACs) have shown superior activity and/or selectivity for many energy‐ and environment‐related reactions, but their stability at high site density and under reducing atmosphere remains unresolved. Herein, we elucidate the intrinsic driving force of a Pd single atom with high site density (up to 5 wt %) under reducing atmosphere, and its unique catalytic performance for hydrogenation reactions. In situ experiments and calculations reveal that Pd atoms tend to migrate into the surface vacancy‐enriched MoC surface during the carburization process by transferring oxide crystals to carbide crystals, leading to the surface enrichment of atomic Pd instead of formation of particles. The Pd1/α‐MoC catalyst exhibits high activity and excellent selectivity for liquid‐phase hydrogenation of substituted nitroaromatics (>99 %) and gas‐phase hydrogenation of CO2 to CO (>98 %). The Pd1/α‐MoC catalyst could endure up to 400 °C without any observable aggregation of single atoms.

中文翻译:

用于化学选择性加氢的高密度热稳定钯单原子催化剂

单原子催化剂(SAC)对许多与能源和环境有关的反应均显示出优异的活性和/或选择性,但在高位密度和还原性气氛下的稳定性仍未解决。在本文中,我们阐明了还原气氛下具有高位点密度(最高5 wt%)的Pd单原子的固有驱动力,以及其对氢化反应的独特催化性能。原位实验和计算表明,在渗碳过程中,Pd原子倾向于通过将氧化物晶体转移到碳化物晶体中而迁移到表面空位富集的MoC表面,从而导致原子Pd的表面富集而不是形成颗粒。钯1/α-MoC催化剂对取代的硝基芳烃进行液相加氢(> 99%)和将CO 2气相转化为CO(> 98%)具有很高的活性和优异的选择性。Pd 1 /α-MoC催化剂可承受高达400°C的温度,而没有任何可观察到的单个原子聚集。
更新日期:2020-08-12
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