{"title":"气液反应器中的等离子体甲烷升级:一步甲醇生产过程的优化","authors":"Ekow Agyekum-Oduro, Ahmad Mukhtar, Sarah Wu","doi":"10.1016/j.jiec.2025.04.038","DOIUrl":null,"url":null,"abstract":"<div><div>In this work, methane (CH<sub>4</sub>) and ubiquitous water (H<sub>2</sub><span>O) were exploited as reactants in a continuous flow, catalyst-free, nonthermal plasma process to produce methanol at a rate of 21.28 mg/h with a specific yield of 1.46 mg</span><sub>MeOH</sub>/g<sub>CH4</sub><span> and selectivity of 90.8 % among other liquid products. A systematic investigation of process parameters through factorial design screened five process factors, i.e., applied power, gas flow rate<span><span>, liquid flow rate<span>, catalyst loading, and pH. While catalyst loading and pH showed minimal significance, gas flow rate, liquid flow rate, and applied power emerged as the significant factors affecting both production rate and specific yield, though with competing effects where </span></span>higher gas flow rates<span><span><span> enhanced production rates but reduced specific yields. Subsequent optimization using Box-Behnken design determined optimal conditions of 368 W applied power, 273 mL/min methane flow rate, and 51 mL/min water flow rate for maximizing methanol production rate while maintaining high selectivity. </span>OES and NMR analyses revealed a radical-mediated pathway primarily involving methyl and hydroxyl radical coupling for methanol formation. This catalyst-free process showed great promise for cleaner fuel production, reduced greenhouse gas emissions, and efficient utilization of natural gas and </span>biogas resources.</span></span></span></div></div>","PeriodicalId":363,"journal":{"name":"Journal of Industrial and Engineering Chemistry","volume":"151 ","pages":"Pages 682-691"},"PeriodicalIF":5.9000,"publicationDate":"2025-04-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"Plasma-enabled methane upgrading in a gas-liquid reactor: Optimizing a one-step methanol production process\",\"authors\":\"Ekow Agyekum-Oduro, Ahmad Mukhtar, Sarah Wu\",\"doi\":\"10.1016/j.jiec.2025.04.038\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"<div><div>In this work, methane (CH<sub>4</sub>) and ubiquitous water (H<sub>2</sub><span>O) were exploited as reactants in a continuous flow, catalyst-free, nonthermal plasma process to produce methanol at a rate of 21.28 mg/h with a specific yield of 1.46 mg</span><sub>MeOH</sub>/g<sub>CH4</sub><span> and selectivity of 90.8 % among other liquid products. A systematic investigation of process parameters through factorial design screened five process factors, i.e., applied power, gas flow rate<span><span>, liquid flow rate<span>, catalyst loading, and pH. While catalyst loading and pH showed minimal significance, gas flow rate, liquid flow rate, and applied power emerged as the significant factors affecting both production rate and specific yield, though with competing effects where </span></span>higher gas flow rates<span><span><span> enhanced production rates but reduced specific yields. Subsequent optimization using Box-Behnken design determined optimal conditions of 368 W applied power, 273 mL/min methane flow rate, and 51 mL/min water flow rate for maximizing methanol production rate while maintaining high selectivity. </span>OES and NMR analyses revealed a radical-mediated pathway primarily involving methyl and hydroxyl radical coupling for methanol formation. This catalyst-free process showed great promise for cleaner fuel production, reduced greenhouse gas emissions, and efficient utilization of natural gas and </span>biogas resources.</span></span></span></div></div>\",\"PeriodicalId\":363,\"journal\":{\"name\":\"Journal of Industrial and Engineering Chemistry\",\"volume\":\"151 \",\"pages\":\"Pages 682-691\"},\"PeriodicalIF\":5.9000,\"publicationDate\":\"2025-04-22\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"Journal of Industrial and Engineering Chemistry\",\"FirstCategoryId\":\"5\",\"ListUrlMain\":\"https://www.sciencedirect.com/science/article/pii/S1226086X25002734\",\"RegionNum\":3,\"RegionCategory\":\"工程技术\",\"ArticlePicture\":[],\"TitleCN\":null,\"AbstractTextCN\":null,\"PMCID\":null,\"EPubDate\":\"\",\"PubModel\":\"\",\"JCR\":\"Q1\",\"JCRName\":\"CHEMISTRY, MULTIDISCIPLINARY\",\"Score\":null,\"Total\":0}","platform":"Semanticscholar","paperid":null,"PeriodicalName":"Journal of Industrial and Engineering Chemistry","FirstCategoryId":"5","ListUrlMain":"https://www.sciencedirect.com/science/article/pii/S1226086X25002734","RegionNum":3,"RegionCategory":"工程技术","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q1","JCRName":"CHEMISTRY, MULTIDISCIPLINARY","Score":null,"Total":0}
Plasma-enabled methane upgrading in a gas-liquid reactor: Optimizing a one-step methanol production process
In this work, methane (CH4) and ubiquitous water (H2O) were exploited as reactants in a continuous flow, catalyst-free, nonthermal plasma process to produce methanol at a rate of 21.28 mg/h with a specific yield of 1.46 mgMeOH/gCH4 and selectivity of 90.8 % among other liquid products. A systematic investigation of process parameters through factorial design screened five process factors, i.e., applied power, gas flow rate, liquid flow rate, catalyst loading, and pH. While catalyst loading and pH showed minimal significance, gas flow rate, liquid flow rate, and applied power emerged as the significant factors affecting both production rate and specific yield, though with competing effects where higher gas flow rates enhanced production rates but reduced specific yields. Subsequent optimization using Box-Behnken design determined optimal conditions of 368 W applied power, 273 mL/min methane flow rate, and 51 mL/min water flow rate for maximizing methanol production rate while maintaining high selectivity. OES and NMR analyses revealed a radical-mediated pathway primarily involving methyl and hydroxyl radical coupling for methanol formation. This catalyst-free process showed great promise for cleaner fuel production, reduced greenhouse gas emissions, and efficient utilization of natural gas and biogas resources.
期刊介绍:
Journal of Industrial and Engineering Chemistry is published monthly in English by the Korean Society of Industrial and Engineering Chemistry. JIEC brings together multidisciplinary interests in one journal and is to disseminate information on all aspects of research and development in industrial and engineering chemistry. Contributions in the form of research articles, short communications, notes and reviews are considered for publication. The editors welcome original contributions that have not been and are not to be published elsewhere. Instruction to authors and a manuscript submissions form are printed at the end of each issue. Bulk reprints of individual articles can be ordered. This publication is partially supported by Korea Research Foundation and the Korean Federation of Science and Technology Societies.