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Uncovering the active sites and demonstrating stable catalyst for the cost-effective conversion of ethanol to 1-butanol
Green Chemistry ( IF 9.8 ) Pub Date : 2021-08-24 , DOI: 10.1039/d1gc01979a
Mond F. Guo 1, 2 , Michel J. Gray 1 , Heather Job 1 , Carlos Alvarez-Vasco 1, 2 , Senthil Subramaniam 1, 2 , Xiao Zhang 1, 2 , Libor Kovarik 3 , Vijayakumar Murugesan 4 , Steven Phillips 1 , Karthikeyan K. Ramasamy 1
Affiliation  

The recent emergence of a robust renewable ethanol industry has provided a sustainable platform molecule toward the production of value-added chemicals and fuels; what is lacking now are viable conversion processes from ethanol that can displace the current production pathways from non-renewable pathways. Here in the work, we demonstrate the highly selective conversion of ethanol to higher alcohols over low copper loaded MgAl mixed oxide catalysts, with 50% improvement in higher alcohol yields over the current state of the art. At these copper concentrations, atomically dispersed Cu1+ were found to be stable even at highly reductive conditions and highly active towards higher alcohol products (e.g. butanol, hexanol) while suppressing side reaction pathways and leading to extended lifetimes of over 150 hours time on stream. Technoeconomic analysis conducted based on these experimental results demonstrate that this catalytic system is cost-competitive with the conventional process. This marks significant progress in the development of Guerbet coupling of ethanol as a viable renewable process and offers a pathway toward sustainable chemical and fuel production.

中文翻译:

发现活性位点并展示稳定的催化剂,用于经济有效地将乙醇转化为 1-丁醇

最近出现的强大的可再生乙醇产业为生产增值化学品和燃料提供了一个可持续的平台分子;现在缺乏的是可行的乙醇转化工艺,可以从不可再生途径取代当前的生产途径。在这项工作中,我们证明了与低铜负载的 MgAl 混合氧化物催化剂相比,乙醇高度选择性地转化为高级醇,与当前技术水平相比,高级醇的产率提高了 50%。在这些铜浓度下,发现原子分散的 Cu 1+即使在高度还原条件下也是稳定的,并且对高级醇产品(例如丁醇、己醇),同时抑制副反应途径并延长运行时间超过 150 小时。基于这些实验结果进行的技术经济分析表明,该催化系统与传统工艺相比具有成本竞争力。这标志着乙醇的 Guerbet 偶联作为一种可行的可再生工艺的发展取得了重大进展,并为可持续的化学品和燃料生产提供了途径。
更新日期:2021-09-08
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