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用于二胺与醇脱氢偶联合成苯并咪唑和喹喔啉的生物源δ-MnO纳米颗粒的室温合成:一种用于电化学应用的高效催化剂

Room-Temperature Synthesis of Biogenic δ-MnO NPs for the Dehydrogenative Coupling of Diamines with Alcohols for Benzimidazole and Quinoxaline Synthesis: An Efficient Catalyst for Electrochemical Applications.

作者信息

R Thrilokraj, Yhobu Zhoveta, Budagumpi Srinivasa, Małecki Jan Grzegorz, Ghosh Arnab, Limaye Akshay S, R Nandini, Dateer Ramesh B

机构信息

Centre for Nano and Material Sciences, JAIN (Deemed to be University), Jain Global Campus, Bangalore 562112, India.

Institute of Chemistry, University of Silesia, 40-006 Katowice, Poland.

出版信息

Langmuir. 2023 Nov 7;39(44):15474-15486. doi: 10.1021/acs.langmuir.3c01749. Epub 2023 Oct 24.

Abstract

An efficient, unique, and eco-friendly biogenic synthesis of single-crystalline δ-phase manganese oxide nanoparticles (MnO NPs) using leaves (GSL) extract at room temperature has been revealed for the first time. The active chemicals present in the GSL extract were found to serve as both reducing and stabilizing agents. The catalyst shows an excellent surface area of 301.13 m g, a mean pore diameter of 4.01 nm, and 39.97% w/w of active metal content. The reactivity of the synthesized catalyst was demonstrated by achieving a one-pot synthesis of benzimidazoles and quinoxalines via an acceptorless dehydrogenative coupling strategy utilizing biorenewable alcohols. The release of hydrogen gas was observed as the only side product and proven by its successful utilization for alkene reduction which supports the mechanistic elucidation. The release of hydrogen gas as a useful byproduct highlights the scientific importance of the present methodology. Additionally, gram-scale synthesis and catalyst recyclability studies are deliberated. Importantly, the δ-MnO NP catalyst exhibited superior catalytic activity and high durability toward hydrogen evolution reaction in alkaline media, highlighting the dual use of the catalyst. The δ-MnO NPs attain the current density of 10 mA/cm at an overpotential of 154 mV with a Tafel slope of 119 mV/dec.

摘要

首次揭示了一种在室温下使用香叶天竺葵(GSL)叶提取物高效、独特且环保的单晶δ相锰氧化物纳米颗粒(MnO NPs)的生物合成方法。发现GSL提取物中存在的活性化学物质可作为还原剂和稳定剂。该催化剂具有301.13 m²/g的优异比表面积、4.01 nm的平均孔径和39.97% w/w的活性金属含量。通过利用生物可再生醇的无受体脱氢偶联策略实现苯并咪唑和喹喔啉的一锅法合成,证明了合成催化剂的反应活性。观察到氢气作为唯一的副产物释放,并通过其成功用于烯烃还原得到证实,这支持了机理阐释。氢气作为有用副产物的释放突出了本方法的科学重要性。此外,还讨论了克级合成和催化剂可回收性研究。重要的是,δ-MnO NP催化剂在碱性介质中对析氢反应表现出优异的催化活性和高耐久性,突出了该催化剂的双重用途。δ-MnO NPs在154 mV的过电位下达到10 mA/cm²的电流密度,塔菲尔斜率为119 mV/dec。

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