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Enhanced CO2 hydrogenation to methanol over La oxide-modified Cu nanoparticles socketed on Cu phyllosilicate nanotubes
Journal of CO2 Utilization ( IF 7.2 ) Pub Date : 2021-09-01 , DOI: 10.1016/j.jcou.2021.101699
Jiachang Zuo 1 , Kun Chen 1, 2 , Jianwei Zheng 1 , Linmin Ye 1 , Youzhu Yuan 1
Affiliation  

The use of Cu-based catalysts in CO2 hydrogenation to methanol (MeOH) has attracted considerable attention due to their low reaction temperature, low cost, and high activity. However, Cu nanoparticles are usually sintered under high-H2 atmosphere. The difficulty in keeping the Cu+/Cu0 ratio stable during the reaction leads to the instability of Cu-based catalysts. In this work, La oxide-doped Cu nanoparticles socketed into parent Cu phyllosilicate nanotubes (La/CuSi-NT) are synthesized by exsolution in situ under a reducing atmosphere at elevated temperatures. They are used to catalyze CO2 hydrogenation to MeOH. Catalytic results show that the La/CuSi-NT catalyst is more stable than intact CuSi-NT and Cu-based catalysts prepared via traditional methods. Among the prepared catalysts, the 0.2La/CuSi-NT catalyst with the La/Cu molar ratio of 0.2 exhibits the highest MeOH yield of up to 428 mg gcat−1 h−1 and performance that remains stable for at least 200 h. Characteristic studies indicate that introducing a La promoter helps increase Cu+/Cu0 ratios and confirm that LaOx species favor generating the formate species of CO2 hydrogenation. Therefore, MeOH synthesis through CO2 hydrogenation is intensified over the La/CuSi-NT catalyst.



中文翻译:

嵌入在铜页硅酸盐纳米管上的氧化镧修饰的铜纳米颗粒增强 CO2 加氢制甲醇

Cu基催化剂在CO 2加氢制甲醇(MeOH)中的应用由于其反应温度低、成本低和活性高而受到广泛关注。然而,Cu纳米颗粒通常在高H 2气氛下烧结。在反应过程中保持Cu + /Cu 0比稳定的困难导致Cu基催化剂的不稳定性。在这项工作中,通过在还原气氛下在升高的温度下原位外溶合成了嵌入母体铜页硅酸盐纳米管 (La/CuSi-NT) 中的 La 氧化物掺杂的 Cu 纳米粒子。它们用于催化 CO 2加氢为甲醇。催化结果表明,La/CuSi-NT催化剂比通过传统方法制备的完整CuSi-NT和Cu基催化剂更稳定。在制备的催化剂中,La/Cu 摩尔比为 0.2 的 0.2La/CuSi-NT 催化剂表现出最高的 MeOH 产率,高达 428 mg g cat -1 h -1并且性能保持稳定至少 200 h。特征研究表明,引入 La 促进剂有助于提高 Cu + /Cu 0比率,并证实 LaO x物质有利于生成 CO 2氢化的甲酸盐物质。因此,在 La/CuSi-NT 催化剂上,通过 CO 2氢化反应的甲醇合成得到加强。

更新日期:2021-09-01
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