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核壳结构的Ni/SiO@ZrO催化剂用于高选择性CO转化并提高反应稳定性。

Core-shell Ni/SiO@ZrO catalyst for highly selective CO conversion accompanied by enhancing reaction stability.

作者信息

Cui Sha, Wang Zhe, Zhao Honggang, Sun Houxiang, Wei Qinhong, Wang Luhui

机构信息

School of Petrochemical Engineering & Environment, Zhejiang Ocean University, Zhoushan, 316022, China.

Zhejiang Provincial Key Laboratory of Petrochemical Pollution Control, Zhejiang Ocean University, Zhoushan, 316022, China.

出版信息

Heliyon. 2024 Nov 27;10(23):e40697. doi: 10.1016/j.heliyon.2024.e40697. eCollection 2024 Dec 15.

Abstract

CO RWGS reaction was considered to be a promising process for carbon dioxide conversion, however it retained a big challenge owing to methanation and metal sintering. Therefore, it was desperately needed to devise highly selective and stable catalyst. Herein, core-shell Ni/SiO@ZrO catalyst was successfully prepared via a combination of the wet impregnation and in-situ hydrothermal synthesis method, with ZrO as the coating shell. The optimized Ni/SiO@4ZrO catalyst possessed enhanced metal-support interaction and rich oxygen vacancies as well as abundant medium-strength CO adsorption sites. As a result, under the GHSV of 120000 mL/g·h and 150000 mL/g·h, Ni/SiO@4ZrO displayed a considerable hydrogenation activity and significantly higher selectivity to CO, compared with the Ni/SiO catalyst as a reference. During stability tests, Ni/SiO@4ZrO also showed a superior catalytic stability with a steady 100 % CO selectivity, carried out at 600 °C for 72 h. This work provided a novel strategy of designing a core-shell catalyst for CO RWGS reaction, and was expected to be put into use in other multiphase reaction process.

摘要

CO逆水煤气变换反应被认为是一种很有前景的二氧化碳转化过程,然而由于甲烷化和金属烧结,它仍然面临巨大挑战。因此,迫切需要设计出高选择性和稳定性的催化剂。在此,通过湿浸渍法和原位水热合成法相结合,成功制备了以ZrO为包覆壳层的核壳结构Ni/SiO@ZrO催化剂。优化后的Ni/SiO@4ZrO催化剂具有增强的金属-载体相互作用、丰富的氧空位以及大量中等强度的CO吸附位点。结果,在120000 mL/g·h和150000 mL/g·h的气体时空速下,与作为参比的Ni/SiO催化剂相比,Ni/SiO@4ZrO表现出可观的加氢活性和对CO显著更高的选择性。在稳定性测试中,Ni/SiO@4ZrO在600℃下进行72小时的测试时,也表现出优异的催化稳定性,CO选择性稳定在100%。这项工作为设计用于CO逆水煤气变换反应的核壳催化剂提供了一种新策略,并有望应用于其他多相反应过程。

https://cdn.ncbi.nlm.nih.gov/pmc/blobs/a837/11648145/cf2bf346f67f/gr1.jpg

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