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非热等离子体对CuO-FeO的原位改性:对CO加氢制CHOH反应的见解

In Situ Modification of CuO-FeO by Nonthermal Plasma: Insights into the CO-to-CHOH Hydrogenation Reaction.

作者信息

Joshi Nitesh, Loganathan Sivachandiran

机构信息

Laboratory of Plasma Chemistry and Physics (LPCP), Department of Chemistry, Faculty of Engineering and Technology, SRM Institute of Science and Technology, SRM Nagar, Kattankulathur, Chennai 603203, India.

Plasma Research Laboratory, Department of Chemical and Biomolecular Engineering, and Center for Air and Aquatic Resources Engineering & Science, Clarkson University, Potsdam, New York 13699, United States.

出版信息

ACS Omega. 2023 Mar 29;8(14):13410-13420. doi: 10.1021/acsomega.3c00915. eCollection 2023 Apr 11.

DOI:10.1021/acsomega.3c00915
PMID:37065016
原文链接:https://pmc.ncbi.nlm.nih.gov/articles/PMC10099434/
Abstract

The hydrogenation of CO to CHOH on the binary mixed metal oxides of CuO-FeO under nonthermal plasma discharge has been reported in this study. The catalysts are synthesized using the sol-gel route and characterized by XRD, FTIR, SEM, and XPS techniques. The impact of CuO mixing with FeO on CO conversion and CHOH yield has been investigated. Herein, we have compared two distinct techniques, namely thermal and plasma catalytic processes. The overall outcome shows that the CO conversion and CHOH production increase with an increase in CuO mixing with FeO. The synthesized catalyst does not show significant CO conversion and CHOH formation in the thermal catalytic process (100-250 °C). Interestingly, when plasma discharge is combined with thermal heating, CO conversion and CHOH production significantly improve. The plasma discharges in the CO/H gas stream, at low temperatures (<200 °C), reduce Cu to Cu and Fe to Fe, which could probably enhance the CO conversion and CHOH production. Among the catalysts prepared, 15% CuO-FeO exhibited the best catalytic activity with 13.2% CO conversion, 7.3% CHOH yield, and a space-time yield of 13 mmol/h g, with 4.67 kJ/L of specific input energy (SIE). The CHOH space-time yield is 2.9-fold higher than that of the commercial catalyst Cu/ZnO/AlO, which is operated at 30 °C with 45.45 kJ/L SIE.

摘要

本研究报道了在非热等离子体放电条件下,CO在CuO-FeO二元混合金属氧化物上氢化生成CHOH的过程。催化剂采用溶胶-凝胶法合成,并通过XRD、FTIR、SEM和XPS技术进行表征。研究了CuO与FeO混合对CO转化率和CHOH产率的影响。在此,我们比较了两种不同的技术,即热催化和等离子体催化过程。总体结果表明,随着CuO与FeO混合比例的增加,CO转化率和CHOH产量增加。在热催化过程(100-250°C)中,合成的催化剂未显示出显著的CO转化率和CHOH生成。有趣的是,当等离子体放电与热加热相结合时,CO转化率和CHOH产量显著提高。在CO/H气流中,低温(<200°C)下的等离子体放电将Cu还原为Cu,将Fe还原为Fe,这可能会提高CO转化率和CHOH产量。在所制备的催化剂中,15% CuO-FeO表现出最佳的催化活性,CO转化率为13.2%,CHOH产率为7.3%,时空产率为13 mmol/h g,比输入能量(SIE)为4.67 kJ/L。CHOH时空产率比在30°C、SIE为45.45 kJ/L下运行的商业催化剂Cu/ZnO/AlO高2.9倍。

https://cdn.ncbi.nlm.nih.gov/pmc/blobs/0edd/10099434/d65ef044a8be/ao3c00915_0008.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/0edd/10099434/276b1a95ee7a/ao3c00915_0002.jpg
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https://cdn.ncbi.nlm.nih.gov/pmc/blobs/0edd/10099434/37121b995d28/ao3c00915_0007.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/0edd/10099434/d65ef044a8be/ao3c00915_0008.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/0edd/10099434/276b1a95ee7a/ao3c00915_0002.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/0edd/10099434/ddd3997a9dcc/ao3c00915_0003.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/0edd/10099434/78f48089f4fb/ao3c00915_0004.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/0edd/10099434/44fd998fbb36/ao3c00915_0005.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/0edd/10099434/b86b047fa60d/ao3c00915_0006.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/0edd/10099434/37121b995d28/ao3c00915_0007.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/0edd/10099434/d65ef044a8be/ao3c00915_0008.jpg

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