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甲酰胺在无定形二氧化硅表面的吸附:实验与计算相结合的方法

Formamide Adsorption at the Amorphous Silica Surface: A Combined Experimental and Computational Approach.

作者信息

Signorile Matteo, Salvini Clara, Zamirri Lorenzo, Bonino Francesca, Martra Gianmario, Sodupe Mariona, Ugliengo Piero

机构信息

Dipartimento di Chimica and NIS, Università di Torino, Via P. Giuria 7 - 10125 Torino and Via G. Quarello 15/A - 10135 Torino, Italy.

Departament de Química, Universitat Autònoma de Barcelona, 08193 Bellaterra, Catalogna, Spain.

出版信息

Life (Basel). 2018 Sep 23;8(4):42. doi: 10.3390/life8040042.

Abstract

Mineral surfaces have been demonstrated to play a central role in prebiotic reactions, which are understood to be at the basis of the origin of life. Among the various molecules proposed as precursors for these reactions, one of the most interesting is formamide. Formamide has been shown to be a pluripotent molecule, generating a wide distribution of relevant prebiotic products. In particular, the outcomes of its reactivity are strongly related to the presence of mineral phases acting as catalysts toward specific reaction pathways. While the mineral⁻products relationship has been deeply studied for a large pool of materials, the fundamental description of formamide reactivity over mineral surfaces at a microscopic level is missing in the literature. In particular, a key step of formamide chemistry at surfaces is adsorption on available interaction sites. This report aims to investigate the adsorption of formamide over a well-defined amorphous silica, chosen as a model mineral surface. An experimental IR investigation of formamide adsorption was carried out and its outcomes were interpreted on the basis of first principles simulation of the process, adopting a realistic model of amorphous silica.

摘要

矿物表面已被证明在益生元反应中起核心作用,而益生元反应被认为是生命起源的基础。在被提议作为这些反应前体的各种分子中,最有趣的一种是甲酰胺。甲酰胺已被证明是一种多能分子,能产生广泛分布的相关益生元产物。特别地,其反应活性的结果与作为特定反应途径催化剂的矿物相的存在密切相关。虽然对于大量材料,矿物与产物之间的关系已得到深入研究,但文献中缺少对甲酰胺在矿物表面微观层面反应活性的基本描述。特别地,甲酰胺在表面化学反应的一个关键步骤是吸附在可用的相互作用位点上。本报告旨在研究甲酰胺在一种明确界定的无定形二氧化硅上的吸附情况,该无定形二氧化硅被选作模型矿物表面。进行了甲酰胺吸附的红外实验研究,并基于该过程的第一性原理模拟,采用无定形二氧化硅的实际模型对实验结果进行了解释。

https://cdn.ncbi.nlm.nih.gov/pmc/blobs/5378/6316577/d2e10a586bf0/life-08-00042-g001.jpg

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