Satyam Gupta*, Saumya Tiwari, Vaibhav Kumar Arghode and Goutam Deo,
{"title":"用于甲烷烟气转化的γ-Al2O3支撑镍钴催化剂的钴促进和镍钴负载效应","authors":"Satyam Gupta*, Saumya Tiwari, Vaibhav Kumar Arghode and Goutam Deo, ","doi":"10.1021/acs.energyfuels.4c01317","DOIUrl":null,"url":null,"abstract":"<p >In this study, we synthesize a series of active Ni<sub>3</sub>Co–Al<sub>2</sub>O<sub>3</sub> catalysts, calcined at 850 °C for 5 h, to examine the effects of (i) substituting Ni with Co on the catalytic performance of the Ni–Al<sub>2</sub>O<sub>3</sub> catalyst and (ii) the total metal amount on the catalytic activity of Ni<sub>3</sub>Co–Al for the flue gas reforming of methane (FGRM) reaction at 600 °C. We maintain high calcination temperatures to ensure strong alloy–support interactions. We also synthesize a Co–Al<sub>2</sub>O<sub>3</sub> catalyst and use the data of a previously synthesized Ni–Al<sub>2</sub>O<sub>3</sub> catalyst to analyze the effect of cobalt promotion. In the Ni<sub>3</sub>Co–Al catalysts, we maintain the Ni/Co ratio to be 3 and increase the Ni+Co amount from 5 to 25 wt % to examine the effect of total metal loading. The H<sub>2</sub>-reduction profiles reveal that the temperature where the consumption of H<sub>2</sub> was maximum, <i>T</i><sub>max</sub> temperature, is a function of the total metal loading. Comparison of the catalytic activities appears to suggest that in situ reduction of the catalyst at <i>T</i><sub>max</sub> was better than the reduction at higher temperatures, since a larger number of surface active sites are available. The CH<sub>4</sub> and CO<sub>2</sub> conversions and H<sub>2</sub> and CO yields increase when nickel is substituted with cobalt due to Ni–Co nanoalloy formation. However, the dispersion of the nanoalloy varies with the metal loading, and the optimum dispersion is when Ni+Co = 10 wt %. This 10Ni<sub>3</sub>Co–Al catalyst exhibits optimum CH<sub>4</sub> (89%) and CO<sub>2</sub> (30%) conversions and H<sub>2</sub> (79%) and CO (46%) yields for the FGRM reaction at 600 °C for a GHSV of 120,000 mL g<sup>–1</sup> h<sup>–1</sup>. The conversions, yields, and particle size of the alloy of this 10Ni<sub>3</sub>Co–Al catalyst do not change significantly, and an insignificant amount of carbon is formed during 24 h of operation. Thus, after using a promoter, it is necessary to optimize the loading of the active phase to obtain the best catalyst for FGRM.</p>","PeriodicalId":35,"journal":{"name":"Energy & Fuels","volume":"38 12","pages":"11022–11036"},"PeriodicalIF":5.3000,"publicationDate":"2024-06-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"Cobalt Promotion and Ni+Co Loading Effects of γ-Al2O3-Supported Ni–Co Catalysts for the Flue Gas Reforming of Methane\",\"authors\":\"Satyam Gupta*, Saumya Tiwari, Vaibhav Kumar Arghode and Goutam Deo, \",\"doi\":\"10.1021/acs.energyfuels.4c01317\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"<p >In this study, we synthesize a series of active Ni<sub>3</sub>Co–Al<sub>2</sub>O<sub>3</sub> catalysts, calcined at 850 °C for 5 h, to examine the effects of (i) substituting Ni with Co on the catalytic performance of the Ni–Al<sub>2</sub>O<sub>3</sub> catalyst and (ii) the total metal amount on the catalytic activity of Ni<sub>3</sub>Co–Al for the flue gas reforming of methane (FGRM) reaction at 600 °C. We maintain high calcination temperatures to ensure strong alloy–support interactions. We also synthesize a Co–Al<sub>2</sub>O<sub>3</sub> catalyst and use the data of a previously synthesized Ni–Al<sub>2</sub>O<sub>3</sub> catalyst to analyze the effect of cobalt promotion. In the Ni<sub>3</sub>Co–Al catalysts, we maintain the Ni/Co ratio to be 3 and increase the Ni+Co amount from 5 to 25 wt % to examine the effect of total metal loading. The H<sub>2</sub>-reduction profiles reveal that the temperature where the consumption of H<sub>2</sub> was maximum, <i>T</i><sub>max</sub> temperature, is a function of the total metal loading. Comparison of the catalytic activities appears to suggest that in situ reduction of the catalyst at <i>T</i><sub>max</sub> was better than the reduction at higher temperatures, since a larger number of surface active sites are available. The CH<sub>4</sub> and CO<sub>2</sub> conversions and H<sub>2</sub> and CO yields increase when nickel is substituted with cobalt due to Ni–Co nanoalloy formation. However, the dispersion of the nanoalloy varies with the metal loading, and the optimum dispersion is when Ni+Co = 10 wt %. This 10Ni<sub>3</sub>Co–Al catalyst exhibits optimum CH<sub>4</sub> (89%) and CO<sub>2</sub> (30%) conversions and H<sub>2</sub> (79%) and CO (46%) yields for the FGRM reaction at 600 °C for a GHSV of 120,000 mL g<sup>–1</sup> h<sup>–1</sup>. The conversions, yields, and particle size of the alloy of this 10Ni<sub>3</sub>Co–Al catalyst do not change significantly, and an insignificant amount of carbon is formed during 24 h of operation. Thus, after using a promoter, it is necessary to optimize the loading of the active phase to obtain the best catalyst for FGRM.</p>\",\"PeriodicalId\":35,\"journal\":{\"name\":\"Energy & Fuels\",\"volume\":\"38 12\",\"pages\":\"11022–11036\"},\"PeriodicalIF\":5.3000,\"publicationDate\":\"2024-06-02\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"Energy & Fuels\",\"FirstCategoryId\":\"5\",\"ListUrlMain\":\"https://pubs.acs.org/doi/10.1021/acs.energyfuels.4c01317\",\"RegionNum\":3,\"RegionCategory\":\"工程技术\",\"ArticlePicture\":[],\"TitleCN\":null,\"AbstractTextCN\":null,\"PMCID\":null,\"EPubDate\":\"\",\"PubModel\":\"\",\"JCR\":\"Q2\",\"JCRName\":\"ENERGY & FUELS\",\"Score\":null,\"Total\":0}","platform":"Semanticscholar","paperid":null,"PeriodicalName":"Energy & Fuels","FirstCategoryId":"5","ListUrlMain":"https://pubs.acs.org/doi/10.1021/acs.energyfuels.4c01317","RegionNum":3,"RegionCategory":"工程技术","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q2","JCRName":"ENERGY & FUELS","Score":null,"Total":0}
Cobalt Promotion and Ni+Co Loading Effects of γ-Al2O3-Supported Ni–Co Catalysts for the Flue Gas Reforming of Methane
In this study, we synthesize a series of active Ni3Co–Al2O3 catalysts, calcined at 850 °C for 5 h, to examine the effects of (i) substituting Ni with Co on the catalytic performance of the Ni–Al2O3 catalyst and (ii) the total metal amount on the catalytic activity of Ni3Co–Al for the flue gas reforming of methane (FGRM) reaction at 600 °C. We maintain high calcination temperatures to ensure strong alloy–support interactions. We also synthesize a Co–Al2O3 catalyst and use the data of a previously synthesized Ni–Al2O3 catalyst to analyze the effect of cobalt promotion. In the Ni3Co–Al catalysts, we maintain the Ni/Co ratio to be 3 and increase the Ni+Co amount from 5 to 25 wt % to examine the effect of total metal loading. The H2-reduction profiles reveal that the temperature where the consumption of H2 was maximum, Tmax temperature, is a function of the total metal loading. Comparison of the catalytic activities appears to suggest that in situ reduction of the catalyst at Tmax was better than the reduction at higher temperatures, since a larger number of surface active sites are available. The CH4 and CO2 conversions and H2 and CO yields increase when nickel is substituted with cobalt due to Ni–Co nanoalloy formation. However, the dispersion of the nanoalloy varies with the metal loading, and the optimum dispersion is when Ni+Co = 10 wt %. This 10Ni3Co–Al catalyst exhibits optimum CH4 (89%) and CO2 (30%) conversions and H2 (79%) and CO (46%) yields for the FGRM reaction at 600 °C for a GHSV of 120,000 mL g–1 h–1. The conversions, yields, and particle size of the alloy of this 10Ni3Co–Al catalyst do not change significantly, and an insignificant amount of carbon is formed during 24 h of operation. Thus, after using a promoter, it is necessary to optimize the loading of the active phase to obtain the best catalyst for FGRM.
期刊介绍:
Energy & Fuels publishes reports of research in the technical area defined by the intersection of the disciplines of chemistry and chemical engineering and the application domain of non-nuclear energy and fuels. This includes research directed at the formation of, exploration for, and production of fossil fuels and biomass; the properties and structure or molecular composition of both raw fuels and refined products; the chemistry involved in the processing and utilization of fuels; fuel cells and their applications; and the analytical and instrumental techniques used in investigations of the foregoing areas.