Non-Oxidative Coupling of Methane via Plasma-Catalysis Over M/γ-Al2O3 Catalysts (M = Ni, Fe, Rh, Pt and Pd): Impact of Active Metal and Noble Gas Co-Feeding

IF 2.6 3区 物理与天体物理 Q3 ENGINEERING, CHEMICAL Plasma Chemistry and Plasma Processing Pub Date : 2024-09-10 DOI:10.1007/s11090-024-10507-2
Panagiotis N. Kechagiopoulos, James Rogers, Pierre-André Maitre, Alan J. McCue, Marcus N. Bannerman
{"title":"Non-Oxidative Coupling of Methane via Plasma-Catalysis Over M/γ-Al2O3 Catalysts (M = Ni, Fe, Rh, Pt and Pd): Impact of Active Metal and Noble Gas Co-Feeding","authors":"Panagiotis N. Kechagiopoulos,&nbsp;James Rogers,&nbsp;Pierre-André Maitre,&nbsp;Alan J. McCue,&nbsp;Marcus N. Bannerman","doi":"10.1007/s11090-024-10507-2","DOIUrl":null,"url":null,"abstract":"<div><p>Plasma-catalysis has attracted significant interest in recent years as an alternative for the direct upgrading of methane into higher-value products. Plasma-catalysis systems can enable the electrification of chemical processes; however, they are highly complex with many previous studies even reporting negative impacts on methane conversion. The present work focuses on the non-oxidative plasma-catalysis of pure methane in a Dielectric Barrier Discharge (DBD) reactor at atmospheric pressure and with no external heating. A range of transition and noble metals (Ni, Fe, Rh, Pt, Pd) supported on γ-Al<sub>2</sub>O<sub>3</sub> are studied, complemented by plasma-only and support-only experiments. All reactor packings are investigated either with pure methane or co-feeding of helium or argon to assess the role of noble gases in enhancing methane activation via energy transfer mechanisms. Electrical diagnostics and charge characteristics from Lissajous plots, and electron temperature and collision rates calculations via BOLSIG+ are used to support the findings with the aim of elucidating the impact of both active metal and noble gas on the reaction pathways and activity. The optimal combination of Pd catalyst and Ar co-feeding achieves a substantial improvement over non-catalytic pure methane results, with C<sub>2+</sub> yield rising from 30% to almost 45% at a concurrent reduction of energy cost from 2.4 to 1.7 <span>\\(\\:\\text{M}\\text{J}\\:{\\text{m}\\text{o}\\text{l}}_{\\text{C}{\\text{H}}_{4}}^{-1}\\)</span> and from 9 to 4.7 <span>\\(\\:\\text{M}\\text{J}\\:\\text{m}\\text{o}{\\text{l}}_{{\\text{C}}_{2+}}^{-1}\\)</span>. Pd, along with Pt, further displayed the lowest coke deposition rates among all packings with overall stable product composition during testing.</p></div>","PeriodicalId":734,"journal":{"name":"Plasma Chemistry and Plasma Processing","volume":"44 6","pages":"2057 - 2085"},"PeriodicalIF":2.6000,"publicationDate":"2024-09-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://link.springer.com/content/pdf/10.1007/s11090-024-10507-2.pdf","citationCount":"0","resultStr":null,"platform":"Semanticscholar","paperid":null,"PeriodicalName":"Plasma Chemistry and Plasma Processing","FirstCategoryId":"5","ListUrlMain":"https://link.springer.com/article/10.1007/s11090-024-10507-2","RegionNum":3,"RegionCategory":"物理与天体物理","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q3","JCRName":"ENGINEERING, CHEMICAL","Score":null,"Total":0}
引用次数: 0

Abstract

Plasma-catalysis has attracted significant interest in recent years as an alternative for the direct upgrading of methane into higher-value products. Plasma-catalysis systems can enable the electrification of chemical processes; however, they are highly complex with many previous studies even reporting negative impacts on methane conversion. The present work focuses on the non-oxidative plasma-catalysis of pure methane in a Dielectric Barrier Discharge (DBD) reactor at atmospheric pressure and with no external heating. A range of transition and noble metals (Ni, Fe, Rh, Pt, Pd) supported on γ-Al2O3 are studied, complemented by plasma-only and support-only experiments. All reactor packings are investigated either with pure methane or co-feeding of helium or argon to assess the role of noble gases in enhancing methane activation via energy transfer mechanisms. Electrical diagnostics and charge characteristics from Lissajous plots, and electron temperature and collision rates calculations via BOLSIG+ are used to support the findings with the aim of elucidating the impact of both active metal and noble gas on the reaction pathways and activity. The optimal combination of Pd catalyst and Ar co-feeding achieves a substantial improvement over non-catalytic pure methane results, with C2+ yield rising from 30% to almost 45% at a concurrent reduction of energy cost from 2.4 to 1.7 \(\:\text{M}\text{J}\:{\text{m}\text{o}\text{l}}_{\text{C}{\text{H}}_{4}}^{-1}\) and from 9 to 4.7 \(\:\text{M}\text{J}\:\text{m}\text{o}{\text{l}}_{{\text{C}}_{2+}}^{-1}\). Pd, along with Pt, further displayed the lowest coke deposition rates among all packings with overall stable product composition during testing.

Abstract Image

查看原文
分享 分享
微信好友 朋友圈 QQ好友 复制链接
本刊更多论文
在 M/γ-Al2O3 催化剂(M = Ni、Fe、Rh、Pt 和 Pd)上通过等离子催化进行甲烷的非氧化偶联:活性金属和惰性气体共馈的影响
近年来,等离子催化作为将甲烷直接升级为高附加值产品的一种替代方法,引起了人们的极大兴趣。等离子催化系统可以实现化学过程的电气化;然而,等离子催化系统非常复杂,之前的许多研究甚至报告了等离子催化系统对甲烷转化的负面影响。本研究的重点是在常压和无外部加热条件下,在介质势垒放电(DBD)反应器中对纯甲烷进行非氧化等离子催化。研究了一系列支撑在 γ-Al2O3 上的过渡金属和贵金属(镍、铁、铑、铂、钯),并辅以纯等离子体和纯支撑实验。对所有反应器填料都进行了研究,有的使用纯甲烷,有的同时使用氦气或氩气,以评估惰性气体在通过能量传递机制增强甲烷活化方面的作用。通过利萨如斯图得出的电学诊断和电荷特征,以及通过 BOLSIG+ 进行的电子温度和碰撞率计算都被用来支持研究结果,目的是阐明活性金属和惰性气体对反应途径和活性的影响。钯催化剂和氩气共馈的最佳组合比非催化的纯甲烷结果有了大幅提高,C2+ 收率从 30% 提高到近 45%,同时能源成本从 2.4 降至 1.7(\:\text{M}\text{J}\:{\text{m}\text{o}\text{l}}_{text{C}{text{H}}_{4}}^{-1}),能源成本从 9 降至 4.7(\:\text{M}\text{J}\:\text{m}\text{o}\text{l}}_{\text{C}}_{2+}}^{-1})。在所有填料中,钯和铂的焦炭沉积率最低,测试期间产品成分总体稳定。
本文章由计算机程序翻译,如有差异,请以英文原文为准。
求助全文
约1分钟内获得全文 去求助
来源期刊
Plasma Chemistry and Plasma Processing
Plasma Chemistry and Plasma Processing 工程技术-工程:化工
CiteScore
5.90
自引率
8.30%
发文量
73
审稿时长
6-12 weeks
期刊介绍: Publishing original papers on fundamental and applied research in plasma chemistry and plasma processing, the scope of this journal includes processing plasmas ranging from non-thermal plasmas to thermal plasmas, and fundamental plasma studies as well as studies of specific plasma applications. Such applications include but are not limited to plasma catalysis, environmental processing including treatment of liquids and gases, biological applications of plasmas including plasma medicine and agriculture, surface modification and deposition, powder and nanostructure synthesis, energy applications including plasma combustion and reforming, resource recovery, coupling of plasmas and electrochemistry, and plasma etching. Studies of chemical kinetics in plasmas, and the interactions of plasmas with surfaces are also solicited. It is essential that submissions include substantial consideration of the role of the plasma, for example, the relevant plasma chemistry, plasma physics or plasma–surface interactions; manuscripts that consider solely the properties of materials or substances processed using a plasma are not within the journal’s scope.
期刊最新文献
Chitosan Hydrogels with Antibacterial and Antifungal Properties: Enhanced Properties by Incorporating of Plasma Activated Water Dielectric Barrier Discharge Plasma Combined with Ce-Ni Mesoporous catalysts for CO2 splitting to CO Assessing the Preservation Effectiveness: A Comparative Study of Plasma Activated Water with Various Preservatives on Capsicum annuum L. (Jalapeño and Pusa Jwala) Recent Advances in Non-Thermal Plasma for Seed Germination, Plant Growth, and Secondary Metabolite Synthesis: A Promising Frontier for Sustainable Agriculture Non-Oxidative Coupling of Methane via Plasma-Catalysis Over M/γ-Al2O3 Catalysts (M = Ni, Fe, Rh, Pt and Pd): Impact of Active Metal and Noble Gas Co-Feeding
×
引用
GB/T 7714-2015
复制
MLA
复制
APA
复制
导出至
BibTeX EndNote RefMan NoteFirst NoteExpress
×
×
提示
您的信息不完整,为了账户安全,请先补充。
现在去补充
×
提示
您因"违规操作"
具体请查看互助需知
我知道了
×
提示
现在去查看 取消
×
提示
确定
0
微信
客服QQ
Book学术公众号 扫码关注我们
反馈
×
意见反馈
请填写您的意见或建议
请填写您的手机或邮箱
已复制链接
已复制链接
快去分享给好友吧!
我知道了
×
扫码分享
扫码分享
Book学术官方微信
Book学术文献互助
Book学术文献互助群
群 号:481959085
Book学术
文献互助 智能选刊 最新文献 互助须知 联系我们:info@booksci.cn
Book学术提供免费学术资源搜索服务,方便国内外学者检索中英文文献。致力于提供最便捷和优质的服务体验。
Copyright © 2023 Book学术 All rights reserved.
ghs 京公网安备 11010802042870号 京ICP备2023020795号-1