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用于将废物转化为高附加值化学品的酸性石墨烯有机催化剂。

Acidic graphene organocatalyst for the superior transformation of wastes into high-added-value chemicals.

机构信息

Regional Centre of Advanced Technologies and Materials, Czech Advanced Technology and Research Institute (CATRIN), Palacký University in Olomouc, Šlechtitelů 27, 783 71, Olomouc, Czech Republic.

Department of Chemistry, Faculty of Natural Sciences, Matej Bel University, Tajovského 40, 974 01, Banská Bystrica, Slovak Republic.

出版信息

Nat Commun. 2023 Mar 13;14(1):1373. doi: 10.1038/s41467-023-36602-0.

Abstract

Our dependence on finite fossil fuels and the insecure energy supply chains have stimulated intensive research for sustainable technologies. Upcycling glycerol, produced from biomass fermentation and as a biodiesel formation byproduct, can substantially contribute in circular carbon economy. Here, we report glycerol's solvent-free and room-temperature conversion to high-added-value chemicals via a reusable graphene catalyst (G-ASA), functionalized with a natural amino acid (taurine). Theoretical studies unveil that the superior performance of the catalyst (surpassing even homogeneous, industrial catalysts) is associated with the dual role of the covalently linked taurine, boosting the catalyst's acidity and affinity for the reactants. Unlike previous catalysts, G-ASA exhibits excellent activity (7508 mmol g h) and selectivity (99.9%) for glycerol conversion to solketal, an additive for improving fuels' quality and a precursor of commodity and fine chemicals. Notably, the catalyst is also particularly active in converting oils to biodiesel, demonstrating its general applicability.

摘要

我们对有限的化石燃料的依赖和能源供应链的不安全性刺激了对可持续技术的深入研究。从生物量发酵中产生的甘油以及生物柴油形成的副产物,可以通过一种可重复使用的石墨烯催化剂(G-ASA)在循环碳经济中做出重大贡献,该催化剂用天然氨基酸(牛磺酸)进行了功能化。理论研究表明,催化剂的卓越性能(甚至超过均相、工业催化剂)与共价连接的牛磺酸的双重作用有关,这增强了催化剂的酸度和对反应物的亲和力。与以前的催化剂不同,G-ASA 表现出优异的活性(7508mmolgh)和选择性(99.9%),可将甘油转化为缩醛,缩醛是一种提高燃料质量的添加剂,也是商品和精细化学品的前体。值得注意的是,该催化剂在将油转化为生物柴油方面也特别活跃,证明了其普遍适用性。

https://cdn.ncbi.nlm.nih.gov/pmc/blobs/9824/10011376/96e082e85547/41467_2023_36602_Fig1_HTML.jpg

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