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气态二氧化碳和甲烷的等离子体辅助催化转化为增值平台化学品和燃料的综述。

A review of plasma-assisted catalytic conversion of gaseous carbon dioxide and methane into value-added platform chemicals and fuels.

作者信息

Puliyalil Harinarayanan, Lašič Jurković Damjan, Dasireddy Venkata D B C, Likozar Blaž

机构信息

Department of Catalysis and Chemical Reaction Engineering, National Institute of Chemistry Hajdrihova 19 1001 Ljubljana Slovenia

出版信息

RSC Adv. 2018 Aug 2;8(48):27481-27508. doi: 10.1039/c8ra03146k. eCollection 2018 Jul 30.

Abstract

CO and CH contribute to greenhouse gas emissions, while the production of industrial base chemicals from natural gas resources is emerging as well. Such conversion processes, however, are energy-intensive and introducing a renewable and sustainable electric activation seems optimal, at least for intermediate-scale modular operation. The review thus analyses such valorisation by plasma reactor technologies and heterogeneous catalysis application, largely into higher hydrocarbon molecules, that is ethane, ethylene, acetylene, propane, , and organic oxygenated compounds, methanol, formaldehyde, formic acid and dimethyl ether. Focus is given to reaction pathway mechanisms, related to the partial oxidation steps of CH with O, HO and CO, CO reduction with H, CH or other paraffin species, and to a lesser extent, to mixtures' dry reforming to syngas. Dielectric barrier discharge, corona, spark and gliding arc sources are considered, combined with (noble) metal materials. Carbon (C), silica (SiO) and alumina (AlO) as well as various catalytic supports are examined as precious critical raw materials ( platinum, palladium and rhodium) or transition metal ( manganese, iron, cobalt, nickel and copper) substrates. These are applied for turnover, such as that pertinent to reformer, (reverse) water-gas shift (WGS or RWGS) and CHOH synthesis. Time-on-stream catalyst deactivation or reactivation is also overviewed from the viewpoint of individual transient moieties and their adsorption or desorption characteristics, as well as reactivity.

摘要

一氧化碳和甲烷会导致温室气体排放,同时利用天然气资源生产工业基础化学品的情况也日益兴起。然而,此类转化过程能源密集,引入可再生且可持续的电活化方式似乎是最佳选择,至少对于中等规模的模块化操作而言是这样。因此,本综述分析了通过等离子体反应器技术和多相催化应用实现的这种增值过程,主要是转化为更高碳氢化合物分子,即乙烷、乙烯、乙炔、丙烷等,以及有机氧化合物,如甲醇、甲醛、甲酸和二甲醚。重点关注与甲烷与氧气、羟基和一氧化碳的部分氧化步骤、一氧化碳与氢气、甲烷或其他链烷烃物种的还原反应相关的反应途径机制,以及在较小程度上关注混合物干重整制合成气的反应途径机制。研究考虑了介质阻挡放电、电晕、火花和滑动弧等放电源,并结合了(贵金属)金属材料。研究了碳(C)、二氧化硅(SiO₂)和氧化铝(Al₂O₃)以及各种催化载体,它们作为关键的珍贵原材料(铂、钯和铑)或过渡金属(锰、铁、钴、镍和铜)载体。这些材料被用于催化转化,例如与重整器、(逆)水煤气变换(WGS或RWGS)以及甲醇合成相关的催化转化。还从单个瞬态部分及其吸附或解吸特性以及反应活性的角度概述了催化剂随时间的失活或再活化情况。

https://cdn.ncbi.nlm.nih.gov/pmc/blobs/032f/9083801/ba9b5d80c771/c8ra03146k-f1.jpg

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