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用于中温水煤气变换反应的具有高效催化活性的镍-氧化镍-氧化钇界面

Catalytically efficient Ni-NiO-YO interface for medium temperature water-gas shift reaction.

作者信息

Xu Kai, Ma Chao, Yan Han, Gu Hao, Wang Wei-Wei, Li Shan-Qing, Meng Qing-Lu, Shao Wei-Peng, Ding Guo-Heng, Wang Feng Ryan, Jia Chun-Jiang

机构信息

Key Laboratory for Colloid and Interface Chemistry, Key Laboratory of Special Aggregated Materials, School of Chemistry and Chemical Engineering, Shandong University, Jinan, 250100, China.

College of Materials Science and Engineering, Hunan University, Changsha, 410082, China.

出版信息

Nat Commun. 2022 May 4;13(1):2443. doi: 10.1038/s41467-022-30138-5.

Abstract

The metal-support interfaces between metals and oxide supports have long been studied in catalytic applications, thanks to their significance in structural stability and efficient catalytic activity. The metal-rare earth oxide interface is particularly interesting because these early transition cations have high electrophilicity, and therefore good binding strength with Lewis basic molecules, such as HO. Based on this feature, here we design a highly efficient composite Ni-YO catalyst, which forms abundant active Ni-NiO-YO interfaces under the water-gas shift (WGS) reaction condition, achieving 140.6 μmol g s rate at 300 °C, which is the highest activity for Ni-based catalysts. A combination of theory and ex/in situ experimental study suggests that YO helps HO dissociation at the Ni-NiO-YO interfaces, promoting this rate limiting step in the WGS reaction. Construction of such new interfacial structure for molecules activation holds great promise in many catalytic systems.

摘要

由于金属与氧化物载体之间的金属-载体界面在结构稳定性和高效催化活性方面具有重要意义,因此在催化应用中一直受到研究。金属-稀土氧化物界面尤其引人关注,因为这些早期过渡阳离子具有较高的亲电性,因此与Lewis碱性分子(如HO)具有良好的结合强度。基于这一特性,我们在此设计了一种高效复合Ni-YO催化剂,该催化剂在水煤气变换(WGS)反应条件下形成了丰富的活性Ni-NiO-YO界面,在300°C时实现了140.6 μmol g s的反应速率,这是镍基催化剂的最高活性。理论与原位/非原位实验研究相结合表明,YO有助于在Ni-NiO-YO界面上使HO解离,从而促进WGS反应中的这一速率限制步骤。构建这种用于分子活化的新型界面结构在许多催化体系中具有广阔的前景。

https://cdn.ncbi.nlm.nih.gov/pmc/blobs/eaf1/9068818/0404be387220/41467_2022_30138_Fig1_HTML.jpg

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