{"title":"使用纳米镍金属催化剂在水介质中选择性加氢将二氧化碳转化为甲酸并获得更高产率:通过响应面方法(RSM)优化反应参数","authors":"Rajeev Ranjan, Prakash Biswas and K. K. Pant","doi":"10.1039/D4RE00194J","DOIUrl":null,"url":null,"abstract":"<p >A highly active mesoporous nano-nickel catalyst was synthesized by the sol–gel method for the selective conversion of CO<small><sub>2</sub></small> to formic acid (FA) in an aqueous medium. In this study, CO<small><sub>2</sub></small> hydrogenation reactions were performed in a high-pressure autoclave, and the experimental conditions were set by using the response surface methodology (RSM). The RSM analysis was done using a three-factor, one-response, and five-level central composite design (CCD) integrated with the desirability approach. Experiments revealed that under the optimized reaction conditions (200 °C, 60 bar), the obtained formic acid yield was significantly high (2245 μmol g<small><sup>−1</sup></small> h<small><sup>−1</sup></small>) with 100% catalyst selectivity. The obtained turnover number (TON) was ∼285, significantly higher in an aqueous medium and the presence of a non-noble nickel nano-metal catalyst. Mesoporous nano nickel particles (15–26 nm) facilitated the selective adsorption and splitting of hydrogen molecules to hydrogen radicals, which further reacted with the carbonate ions present in the reaction medium. Na<small><sub>2</sub></small>CO<small><sub>3</sub></small> acted as a promoter, which enhanced the CO<small><sub>2</sub></small> adsorption and the formic acid yield. The catalyst recyclability was confirmed by performing the experiments five times and a constant yield of formic acid was found.</p>","PeriodicalId":101,"journal":{"name":"Reaction Chemistry & Engineering","volume":" 10","pages":" 2635-2646"},"PeriodicalIF":3.4000,"publicationDate":"2024-07-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"Selective hydrogenation of CO2 to formic acid with higher yield in an aqueous medium with a nano-nickel-metal catalyst: reaction parameter optimization by response surface methodology (RSM)†\",\"authors\":\"Rajeev Ranjan, Prakash Biswas and K. K. Pant\",\"doi\":\"10.1039/D4RE00194J\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"<p >A highly active mesoporous nano-nickel catalyst was synthesized by the sol–gel method for the selective conversion of CO<small><sub>2</sub></small> to formic acid (FA) in an aqueous medium. In this study, CO<small><sub>2</sub></small> hydrogenation reactions were performed in a high-pressure autoclave, and the experimental conditions were set by using the response surface methodology (RSM). The RSM analysis was done using a three-factor, one-response, and five-level central composite design (CCD) integrated with the desirability approach. Experiments revealed that under the optimized reaction conditions (200 °C, 60 bar), the obtained formic acid yield was significantly high (2245 μmol g<small><sup>−1</sup></small> h<small><sup>−1</sup></small>) with 100% catalyst selectivity. The obtained turnover number (TON) was ∼285, significantly higher in an aqueous medium and the presence of a non-noble nickel nano-metal catalyst. Mesoporous nano nickel particles (15–26 nm) facilitated the selective adsorption and splitting of hydrogen molecules to hydrogen radicals, which further reacted with the carbonate ions present in the reaction medium. Na<small><sub>2</sub></small>CO<small><sub>3</sub></small> acted as a promoter, which enhanced the CO<small><sub>2</sub></small> adsorption and the formic acid yield. The catalyst recyclability was confirmed by performing the experiments five times and a constant yield of formic acid was found.</p>\",\"PeriodicalId\":101,\"journal\":{\"name\":\"Reaction Chemistry & Engineering\",\"volume\":\" 10\",\"pages\":\" 2635-2646\"},\"PeriodicalIF\":3.4000,\"publicationDate\":\"2024-07-09\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"Reaction Chemistry & Engineering\",\"FirstCategoryId\":\"92\",\"ListUrlMain\":\"https://pubs.rsc.org/en/content/articlelanding/2024/re/d4re00194j\",\"RegionNum\":3,\"RegionCategory\":\"化学\",\"ArticlePicture\":[],\"TitleCN\":null,\"AbstractTextCN\":null,\"PMCID\":null,\"EPubDate\":\"\",\"PubModel\":\"\",\"JCR\":\"Q2\",\"JCRName\":\"CHEMISTRY, MULTIDISCIPLINARY\",\"Score\":null,\"Total\":0}","platform":"Semanticscholar","paperid":null,"PeriodicalName":"Reaction Chemistry & Engineering","FirstCategoryId":"92","ListUrlMain":"https://pubs.rsc.org/en/content/articlelanding/2024/re/d4re00194j","RegionNum":3,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q2","JCRName":"CHEMISTRY, MULTIDISCIPLINARY","Score":null,"Total":0}
Selective hydrogenation of CO2 to formic acid with higher yield in an aqueous medium with a nano-nickel-metal catalyst: reaction parameter optimization by response surface methodology (RSM)†
A highly active mesoporous nano-nickel catalyst was synthesized by the sol–gel method for the selective conversion of CO2 to formic acid (FA) in an aqueous medium. In this study, CO2 hydrogenation reactions were performed in a high-pressure autoclave, and the experimental conditions were set by using the response surface methodology (RSM). The RSM analysis was done using a three-factor, one-response, and five-level central composite design (CCD) integrated with the desirability approach. Experiments revealed that under the optimized reaction conditions (200 °C, 60 bar), the obtained formic acid yield was significantly high (2245 μmol g−1 h−1) with 100% catalyst selectivity. The obtained turnover number (TON) was ∼285, significantly higher in an aqueous medium and the presence of a non-noble nickel nano-metal catalyst. Mesoporous nano nickel particles (15–26 nm) facilitated the selective adsorption and splitting of hydrogen molecules to hydrogen radicals, which further reacted with the carbonate ions present in the reaction medium. Na2CO3 acted as a promoter, which enhanced the CO2 adsorption and the formic acid yield. The catalyst recyclability was confirmed by performing the experiments five times and a constant yield of formic acid was found.
期刊介绍:
Reaction Chemistry & Engineering is a new journal reporting cutting edge research into all aspects of making molecules for the benefit of fundamental research, applied processes and wider society.
From fundamental, molecular-level chemistry to large scale chemical production, Reaction Chemistry & Engineering brings together communities of chemists and chemical engineers working to ensure the crucial role of reaction chemistry in today’s world.