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使用简单、可回收且高效的多相催化剂将 CO 加氢转化为甲酸盐。

Hydrogenation of CO to Formate using a Simple, Recyclable, and Efficient Heterogeneous Catalyst.

机构信息

Department of Applied Chemistry , Kookmin University , 861-1 Jeongneung-dong , Seongbuk-gu, Seoul 136-702 , Republic of Korea.

Clean Energy Research Centre , Korea Institute of Science and Technology , P.O. Box 131, Cheongryang , Republic of Korea.

出版信息

Inorg Chem. 2019 Mar 18;58(6):3717-3723. doi: 10.1021/acs.inorgchem.8b03336. Epub 2019 Mar 1.

Abstract

Today, one of the most imperative targets to realize the conversions of CO in industry is the development of practically viable catalytic systems that demonstrate excellent activity, selectivity, and durability. Herein, a simple heterogeneous Ru(III) catalyst is prepared by immobilizing commercially available RuCl· xHO onto a bipyridine-functionalized covalent triazine framework, [bpy-CTF-RuCl], for the first time. This novel catalyst efficiently hydrogenates CO into formate with an unprecedented turnover frequency (38800 h) and selectivity. In addition, the catalyst excellently maintains its efficiency over successive runs and produces a maximum final formate concentration of ∼2.1 M in just 2.5 h with a conversion of 12% in regard to CO feed. The apparent advantages of air stability, ease of handling, simplicity, the use of a readily available metal precursor, and the outstanding catalytic performance make [bpy-CTF-RuCl] one of the possible candidates for realizing the large-scale production of formic acid/formate by CO hydrogenation.

摘要

如今,实现工业中 CO 转化的最紧迫目标之一是开发具有出色活性、选择性和耐久性的实用可行的催化体系。在此,首次通过将市售 RuCl·xH2O 固定在联吡啶功能化共价三嗪骨架[bpy-CTF-RuCl]上,制备了一种简单的非均相 Ru(III)催化剂。该新型催化剂可高效地将 CO 氢化生成甲酸盐,其周转频率(38800 h)和选择性前所未有。此外,该催化剂在连续运行中表现出优异的稳定性,并在短短 2.5 小时内以 12%的 CO 进料转化率产生了最大的最终甲酸盐浓度约 2.1 M。空气稳定性、易于处理、简单、使用易得的金属前体以及出色的催化性能等明显优势,使 [bpy-CTF-RuCl]成为通过 CO 氢化实现甲酸/甲酸盐大规模生产的可能候选者之一。

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