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水热条件下铁催化一氧化碳自催化还原为甲酸的途径及动力学

Pathways and Kinetics for Autocatalytic Reduction of CO into Formic Acid with Fe under Hydrothermal Conditions.

作者信息

Jin Binbin, Luo Ligang, Xie Longfei

机构信息

School of Environmental Science and Engineering, Shanghai Jiao Tong University, 800 Dongchuan Road, Shanghai 200240, China.

College of Life Sciences, Shanghai Normal University, 100 Guilin Road, Shanghai 200240, China.

出版信息

ACS Omega. 2021 Apr 23;6(17):11280-11285. doi: 10.1021/acsomega.1c00119. eCollection 2021 May 4.

DOI:10.1021/acsomega.1c00119
PMID:34056283
原文链接:https://pmc.ncbi.nlm.nih.gov/articles/PMC8153913/
Abstract

The utilization of CO, as a cheap and abundant carbon source to produce useful chemicals or fuels, has been regarded as one of the promising ways to reduce CO emissions and minimize the green-house effect. Previous studies have demonstrated that CO (or HCO ) can be efficiently reduced to formic acid with metal Fe under hydrothermal conditions without additional hydrogen and any catalyst. However, the pathways and kinetics of the autocatalytic CO reduction remain unknown. In the present work, the reaction kinetics were carefully investigated according to the proposed reaction pathways, and a phenomenological kinetic model was developed for the first time. The results showed that the hydrothermal conversion of HCO into formic acid with Fe can be expressed as the first-order reaction, and the activation energy of HCO is 28 kJ/mol under hydrothermal conditions.

摘要

将一氧化碳(CO)作为一种廉价且丰富的碳源来生产有用的化学品或燃料,已被视为减少CO排放和将温室效应降至最低的一种有前景的方法。先前的研究表明,在水热条件下,无需额外的氢气和任何催化剂,CO(或HCO)就能与金属铁高效反应生成甲酸。然而,自催化CO还原的途径和动力学仍然未知。在本工作中,根据提出的反应途径对反应动力学进行了仔细研究,并首次建立了一个唯象动力学模型。结果表明,HCO与铁在水热条件下转化为甲酸的反应可表示为一级反应,且HCO在水热条件下的活化能为28 kJ/mol。

https://cdn.ncbi.nlm.nih.gov/pmc/blobs/c967/8153913/76f21f4a34f7/ao1c00119_0008.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/c967/8153913/b6720fb318f8/ao1c00119_0002.jpg
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https://cdn.ncbi.nlm.nih.gov/pmc/blobs/c967/8153913/7c9387acf2f9/ao1c00119_0005.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/c967/8153913/a3319e965c79/ao1c00119_0006.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/c967/8153913/f5ad01b89bbb/ao1c00119_0007.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/c967/8153913/76f21f4a34f7/ao1c00119_0008.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/c967/8153913/b6720fb318f8/ao1c00119_0002.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/c967/8153913/378858bd05b6/ao1c00119_0003.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/c967/8153913/2ea5f27ff8f6/ao1c00119_0004.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/c967/8153913/7c9387acf2f9/ao1c00119_0005.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/c967/8153913/a3319e965c79/ao1c00119_0006.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/c967/8153913/f5ad01b89bbb/ao1c00119_0007.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/c967/8153913/76f21f4a34f7/ao1c00119_0008.jpg

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