{"title":"在非贵金属 Cu-Fe 催化剂上低温高效催化将一氧化氮转化为 N2","authors":"Jianqiang Zhang, Yanyan Li, Lifang Cai, Yakun Li, Xuzhao Yang, Yingying Zhang, Jingli Han, Shide Wu","doi":"10.1134/S0023158423600955","DOIUrl":null,"url":null,"abstract":"<p>Nitrous oxide (N<sub>2</sub>O) is a long-lived stratospheric ozone-depleting substance with an atmospheric lifetime of 116 years. It is also a greenhouse gas with a global warming potential value of about 310. Due to its high kinetic stability and thermal decomposition temperature exceeding 1000°C, the treatment and recovery of nitrous oxide pose significant engineering and climate challenges. In this study, we introduce a Cu–Fe oxide catalyst that demonstrates efficient and low-temperature conversion of N<sub>2</sub>O to N<sub>2</sub> using readily available reductant CO. The oxide catalyst was synthesized by a solvothermal method and a “from bottom to top” technique. Characterizations by X-ray diffraction (XRD), CO temperature-programmed desorption (C-O‑TPD), scanning electron microscopy (SEM), and BET indicate that the catalyst with weaker CO adsorption sites, fewer strong CO adsorption sites, suitable particle size, good dispersion and high specific surface area performs excellent reaction activity in the reduction of N<sub>2</sub>O to N<sub>2</sub> by CO. The active site of Cu is stronger, and the addition of Fe can promote dispersion of the Cu active site and increase the exposure to the active site. A new approach has been proposed to address nitrous oxide emissions, a greenhouse gas with high thermodynamic stability, in the chemical industrial process that generates nitrous oxide as a byproduct.</p>","PeriodicalId":682,"journal":{"name":"Kinetics and Catalysis","volume":"65 3","pages":"261 - 270"},"PeriodicalIF":1.3000,"publicationDate":"2024-08-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"Low-Temperature and High-Efficiency Catalytic Conversion N2O to N2 in the Presence of CO over Nonnoble Metal Cu–Fe Catalyst\",\"authors\":\"Jianqiang Zhang, Yanyan Li, Lifang Cai, Yakun Li, Xuzhao Yang, Yingying Zhang, Jingli Han, Shide Wu\",\"doi\":\"10.1134/S0023158423600955\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"<p>Nitrous oxide (N<sub>2</sub>O) is a long-lived stratospheric ozone-depleting substance with an atmospheric lifetime of 116 years. It is also a greenhouse gas with a global warming potential value of about 310. Due to its high kinetic stability and thermal decomposition temperature exceeding 1000°C, the treatment and recovery of nitrous oxide pose significant engineering and climate challenges. In this study, we introduce a Cu–Fe oxide catalyst that demonstrates efficient and low-temperature conversion of N<sub>2</sub>O to N<sub>2</sub> using readily available reductant CO. The oxide catalyst was synthesized by a solvothermal method and a “from bottom to top” technique. Characterizations by X-ray diffraction (XRD), CO temperature-programmed desorption (C-O‑TPD), scanning electron microscopy (SEM), and BET indicate that the catalyst with weaker CO adsorption sites, fewer strong CO adsorption sites, suitable particle size, good dispersion and high specific surface area performs excellent reaction activity in the reduction of N<sub>2</sub>O to N<sub>2</sub> by CO. The active site of Cu is stronger, and the addition of Fe can promote dispersion of the Cu active site and increase the exposure to the active site. A new approach has been proposed to address nitrous oxide emissions, a greenhouse gas with high thermodynamic stability, in the chemical industrial process that generates nitrous oxide as a byproduct.</p>\",\"PeriodicalId\":682,\"journal\":{\"name\":\"Kinetics and Catalysis\",\"volume\":\"65 3\",\"pages\":\"261 - 270\"},\"PeriodicalIF\":1.3000,\"publicationDate\":\"2024-08-15\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"Kinetics and Catalysis\",\"FirstCategoryId\":\"92\",\"ListUrlMain\":\"https://link.springer.com/article/10.1134/S0023158423600955\",\"RegionNum\":4,\"RegionCategory\":\"化学\",\"ArticlePicture\":[],\"TitleCN\":null,\"AbstractTextCN\":null,\"PMCID\":null,\"EPubDate\":\"\",\"PubModel\":\"\",\"JCR\":\"Q4\",\"JCRName\":\"CHEMISTRY, PHYSICAL\",\"Score\":null,\"Total\":0}","platform":"Semanticscholar","paperid":null,"PeriodicalName":"Kinetics and Catalysis","FirstCategoryId":"92","ListUrlMain":"https://link.springer.com/article/10.1134/S0023158423600955","RegionNum":4,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q4","JCRName":"CHEMISTRY, PHYSICAL","Score":null,"Total":0}
引用次数: 0
摘要
摘要一氧化二氮(N2O)是一种长效平流层臭氧消耗物质,在大气中的寿命长达 116 年。它也是一种温室气体,全球变暖潜势值约为 310。由于其动力学稳定性高,热分解温度超过 1000°C,氧化亚氮的处理和回收对工程和气候都构成了重大挑战。在本研究中,我们介绍了一种 Cu-Fe 氧化物催化剂,该催化剂可利用现成的还原剂 CO 将一氧化二氮高效低温转化为二氧化氮。该氧化物催化剂是通过溶热法和 "自下而上 "技术合成的。X 射线衍射 (XRD)、CO 温度编程解吸 (C-O-TPD)、扫描电子显微镜 (SEM) 和 BET 表征表明,催化剂具有较弱的 CO 吸附位点、较少的强 CO 吸附位点、合适的粒度、良好的分散性和较高的比表面积,在 CO 将 N2O 还原成 N2 的过程中具有优异的反应活性。Cu 的活性位点较强,加入 Fe 可以促进 Cu 活性位点的分散,增加活性位点的暴露量。一氧化二氮是一种热力学稳定性很高的温室气体,在化学工业过程中会产生一氧化二氮作为副产品。
Low-Temperature and High-Efficiency Catalytic Conversion N2O to N2 in the Presence of CO over Nonnoble Metal Cu–Fe Catalyst
Nitrous oxide (N2O) is a long-lived stratospheric ozone-depleting substance with an atmospheric lifetime of 116 years. It is also a greenhouse gas with a global warming potential value of about 310. Due to its high kinetic stability and thermal decomposition temperature exceeding 1000°C, the treatment and recovery of nitrous oxide pose significant engineering and climate challenges. In this study, we introduce a Cu–Fe oxide catalyst that demonstrates efficient and low-temperature conversion of N2O to N2 using readily available reductant CO. The oxide catalyst was synthesized by a solvothermal method and a “from bottom to top” technique. Characterizations by X-ray diffraction (XRD), CO temperature-programmed desorption (C-O‑TPD), scanning electron microscopy (SEM), and BET indicate that the catalyst with weaker CO adsorption sites, fewer strong CO adsorption sites, suitable particle size, good dispersion and high specific surface area performs excellent reaction activity in the reduction of N2O to N2 by CO. The active site of Cu is stronger, and the addition of Fe can promote dispersion of the Cu active site and increase the exposure to the active site. A new approach has been proposed to address nitrous oxide emissions, a greenhouse gas with high thermodynamic stability, in the chemical industrial process that generates nitrous oxide as a byproduct.
期刊介绍:
Kinetics and Catalysis Russian is a periodical that publishes theoretical and experimental works on homogeneous and heterogeneous kinetics and catalysis. Other topics include the mechanism and kinetics of noncatalytic processes in gaseous, liquid, and solid phases, quantum chemical calculations in kinetics and catalysis, methods of studying catalytic processes and catalysts, the chemistry of catalysts and adsorbent surfaces, the structure and physicochemical properties of catalysts, preparation and poisoning of catalysts, macrokinetics, and computer simulations in catalysis. The journal also publishes review articles on contemporary problems in kinetics and catalysis. The journal welcomes manuscripts from all countries in the English or Russian language.