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铁辅助在凝聚态一氧化碳上形成一氧化碳及其与星际化学的相关性。

Iron assisted formation of CO over condensed CO and its relevance to interstellar chemistry.

作者信息

Methikkalam Rabin Rajan J, Ghosh Jyotirmoy, Bhuin Radha Gobinda, Bag Soumabha, Ragupathy Gopi, Pradeep Thalappil

机构信息

DST Unit of Nanoscience (DST UNS) and Thematic Unit of Excellence (TUE), Department of Chemistry, Indian Institute of Technology Madras, Chennai 600 036, India.

出版信息

Phys Chem Chem Phys. 2020 Apr 28;22(16):8491-8498. doi: 10.1039/c9cp06983f. Epub 2020 Apr 15.

Abstract

Catalytic conversion of CO to CO has been investigated in ultrahigh vacuum (UHV) under cryogenic conditions (10 K). This cryogenic oxidation is assisted by iron upon its co-deposition with CO, on a substrate. The study shows that the interaction of Fe and CO results in a Fe-CO complex that reacts in the presence of excess CO at cryogenic conditions leading to CO. Here, the presence of CO on the surface is a prerequisite for the reaction to occur. Different control experiments confirm that the reaction takes place in the condensed phase and not in the gas phase. Surface sensitive reflection absorption infrared spectroscopy (RAIRS), temperature programmed desorption (TPD), and Cs based low energy ion scattering are utilized for this study. The iron assisted formation of CO may be proposed as another pathway relevant in interstellar ices, containing CO. This direct oxidation process, which occurs at extremely low temperatures and pressures, in the presence of a reactive metal species like iron (the most abundant metal in the interstellar medium) may have astrochemical importance. It does not require any external energy in the form of photo-irradiation or thermal processing. Such reactions are highly relevant in cold dense molecular clouds where interactions between neutral species are more favoured.

摘要

在超低温条件(10 K)下的超高真空(UHV)环境中,对一氧化碳(CO)催化转化为二氧化碳(CO₂)的过程进行了研究。在低温下,铁与CO共沉积在基底上时会辅助这种低温氧化反应。研究表明,Fe与CO的相互作用会形成一种Fe - CO络合物,该络合物在低温条件下,在过量CO存在时会发生反应生成CO₂。在此,表面存在CO是反应发生的前提条件。不同的对照实验证实该反应发生在凝聚相中而非气相中。本研究采用了表面灵敏的反射吸收红外光谱(RAIRS)、程序升温脱附(TPD)以及基于Cs的低能离子散射技术。铁辅助形成CO₂的过程可能是星际冰中与含CO相关的另一条反应途径。这种直接氧化过程在极低的温度和压力下,在像铁(星际介质中最丰富的金属)这样的活性金属物种存在时发生,可能具有天体化学意义。它不需要任何光辐照或热处理形式的外部能量。此类反应在冷致密分子云中高度相关,因为在其中中性物种之间的相互作用更为有利。

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