Suppr超能文献

定制用于CO加氢的L型沸石负载铜催化剂:对CHOH和CO形成机理的见解。

Tailoring Zeolite L-Supported-Cu Catalysts for CO Hydrogenation: Insights into the Mechanism of CHOH and CO Formation.

作者信息

Yang Xiaoli, Duan Hongmin, Wang Ruifeng, Zhao Fengwang, Jin Fayi, Jiang Wei, Han Guangting, Guan Qingxin, Ben Haoxi

机构信息

College of Textiles and Clothing, State Key Laboratory of BioFibers and Eco-textiles, Qingdao University, Qingdao 266071, China.

State Key Laboratory of Catalysis, Dalian Institute of Chemical Physics, Chinese Academy of Sciences, Dalian 116023, China.

出版信息

Inorg Chem. 2023 Aug 21;62(33):13419-13427. doi: 10.1021/acs.inorgchem.3c01763. Epub 2023 Aug 8.

Abstract

The utilization of Cu-based catalysts in CO conversion into valuable chemicals is of significant interest due to their potential in mitigating greenhouse gas emissions. However, the controllable design of Cu-based catalysts and the regulation of their mechanism remain challenging. In this study, a series of efficient Cu/L catalysts were prepared for this process, and the intrinsic influencing factors on the reaction routes were systematically revealed. Various techniques revealed that Cu particles in L-supported catalysts exhibited higher dispersion and formed Cu-O(OH)-K interfacial sites. However, with increasing Cu loading, the dispersion of Cu particles and the percentage of Cu-O(OH)-K interfaces decreased. Kinetic investigations revealed that the adsorption configuration and electronic structure of Cu species codetermined the reaction pathways and resulting selectivity. Cu/L catalysts possessing Cu-O(OH)-K interfaces and small particles demonstrated the preferential formation of formate species, promoting methanol formation. However, larger Cu particles generated carboxylate intermediates, resulting in higher CO selectivity..

摘要

由于铜基催化剂在减少温室气体排放方面的潜力,其在将CO转化为有价值化学品中的应用备受关注。然而,铜基催化剂的可控设计及其机理调控仍然具有挑战性。在本研究中,制备了一系列用于该过程的高效Cu/L催化剂,并系统地揭示了影响反应路径的内在因素。各种技术表明,负载在L上的催化剂中的铜颗粒表现出更高的分散性,并形成了Cu-O(OH)-K界面位点。然而,随着铜负载量的增加,铜颗粒的分散性和Cu-O(OH)-K界面的百分比降低。动力学研究表明,铜物种的吸附构型和电子结构共同决定了反应路径和产物选择性。具有Cu-O(OH)-K界面和小颗粒的Cu/L催化剂表现出优先形成甲酸盐物种,促进甲醇生成。然而,较大的铜颗粒产生羧酸盐中间体,导致CO选择性更高。

文献检索

告别复杂PubMed语法,用中文像聊天一样搜索,搜遍4000万医学文献。AI智能推荐,让科研检索更轻松。

立即免费搜索

文件翻译

保留排版,准确专业,支持PDF/Word/PPT等文件格式,支持 12+语言互译。

免费翻译文档

深度研究

AI帮你快速写综述,25分钟生成高质量综述,智能提取关键信息,辅助科研写作。

立即免费体验