Bin Meng , Erping Cao , Liwei Jia , Yuhua Zheng , Yanbin Cui
{"title":"na2co3改性活性炭负载Cu-Fe氧化物促进低温脱除H2S","authors":"Bin Meng , Erping Cao , Liwei Jia , Yuhua Zheng , Yanbin Cui","doi":"10.1016/j.seppur.2025.131415","DOIUrl":null,"url":null,"abstract":"<div><div>A variety of Cu-Fe oxide supported on Na<sub>2</sub>CO<sub>3</sub>-modified activated carbon (CuFeNaAC-X) catalysts were prepared via the impregnation and calcination methods and their desulfurization performance was evaluated at low-temperature. By optimizing the loading content of Cu-Fe, the sulfur capacity of the CuFeNaAC-5 reached a maximum of 430.09 mg/g, surpassing most activated carbon (AC) catalysts. EPR testing revealed that the loading of Cu-Fe oxide can activate oxygen to form superoxide radicals (<span><math><msubsup><mtext>O</mtext><mrow><mtext>2</mtext></mrow><mtext>-</mtext></msubsup></math></span>·), thereby promoting the catalytic oxidation of H<sub>2</sub>S. XPS testing revealed that upon loading of Cu-Fe oxide, the formation of FeOOH can facilitate the catalytic oxidation of H<sub>2</sub>S to sulfur (S) through a chain reaction. Combining EPR and XPS analyses, Na<sub>2</sub>CO<sub>3</sub> modification modulates the content of <span><math><msubsup><mtext>O</mtext><mrow><mtext>2</mtext></mrow><mtext>-</mtext></msubsup></math></span>·, directing the formation of S and then significantly improving the catalyst’s desulfurization efficiency. Furthermore, CO<sub>2</sub>-TPD testing revealed that Na<sub>2</sub>CO<sub>3</sub> modification promotes the ionization of H<sub>2</sub>S to HS<sup>-</sup>, thereby enhancing the catalyst’s desulfurization performance. Based on the distribution of sulfur species in used catalysts, and the results of characterizations, a possible desulfurization mechanism of CuFeNaAC-X has been proposed.</div></div>","PeriodicalId":427,"journal":{"name":"Separation and Purification Technology","volume":"361 ","pages":"Article 131415"},"PeriodicalIF":9.0000,"publicationDate":"2025-01-03","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"Cu-Fe oxide supported on Na2CO3-modified activated carbon boost H2S removal at low temperature\",\"authors\":\"Bin Meng , Erping Cao , Liwei Jia , Yuhua Zheng , Yanbin Cui\",\"doi\":\"10.1016/j.seppur.2025.131415\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"<div><div>A variety of Cu-Fe oxide supported on Na<sub>2</sub>CO<sub>3</sub>-modified activated carbon (CuFeNaAC-X) catalysts were prepared via the impregnation and calcination methods and their desulfurization performance was evaluated at low-temperature. By optimizing the loading content of Cu-Fe, the sulfur capacity of the CuFeNaAC-5 reached a maximum of 430.09 mg/g, surpassing most activated carbon (AC) catalysts. EPR testing revealed that the loading of Cu-Fe oxide can activate oxygen to form superoxide radicals (<span><math><msubsup><mtext>O</mtext><mrow><mtext>2</mtext></mrow><mtext>-</mtext></msubsup></math></span>·), thereby promoting the catalytic oxidation of H<sub>2</sub>S. XPS testing revealed that upon loading of Cu-Fe oxide, the formation of FeOOH can facilitate the catalytic oxidation of H<sub>2</sub>S to sulfur (S) through a chain reaction. Combining EPR and XPS analyses, Na<sub>2</sub>CO<sub>3</sub> modification modulates the content of <span><math><msubsup><mtext>O</mtext><mrow><mtext>2</mtext></mrow><mtext>-</mtext></msubsup></math></span>·, directing the formation of S and then significantly improving the catalyst’s desulfurization efficiency. Furthermore, CO<sub>2</sub>-TPD testing revealed that Na<sub>2</sub>CO<sub>3</sub> modification promotes the ionization of H<sub>2</sub>S to HS<sup>-</sup>, thereby enhancing the catalyst’s desulfurization performance. Based on the distribution of sulfur species in used catalysts, and the results of characterizations, a possible desulfurization mechanism of CuFeNaAC-X has been proposed.</div></div>\",\"PeriodicalId\":427,\"journal\":{\"name\":\"Separation and Purification Technology\",\"volume\":\"361 \",\"pages\":\"Article 131415\"},\"PeriodicalIF\":9.0000,\"publicationDate\":\"2025-01-03\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"Separation and Purification Technology\",\"FirstCategoryId\":\"5\",\"ListUrlMain\":\"https://www.sciencedirect.com/science/article/pii/S1383586625000127\",\"RegionNum\":1,\"RegionCategory\":\"工程技术\",\"ArticlePicture\":[],\"TitleCN\":null,\"AbstractTextCN\":null,\"PMCID\":null,\"EPubDate\":\"\",\"PubModel\":\"\",\"JCR\":\"Q1\",\"JCRName\":\"ENGINEERING, CHEMICAL\",\"Score\":null,\"Total\":0}","platform":"Semanticscholar","paperid":null,"PeriodicalName":"Separation and Purification Technology","FirstCategoryId":"5","ListUrlMain":"https://www.sciencedirect.com/science/article/pii/S1383586625000127","RegionNum":1,"RegionCategory":"工程技术","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q1","JCRName":"ENGINEERING, CHEMICAL","Score":null,"Total":0}
Cu-Fe oxide supported on Na2CO3-modified activated carbon boost H2S removal at low temperature
A variety of Cu-Fe oxide supported on Na2CO3-modified activated carbon (CuFeNaAC-X) catalysts were prepared via the impregnation and calcination methods and their desulfurization performance was evaluated at low-temperature. By optimizing the loading content of Cu-Fe, the sulfur capacity of the CuFeNaAC-5 reached a maximum of 430.09 mg/g, surpassing most activated carbon (AC) catalysts. EPR testing revealed that the loading of Cu-Fe oxide can activate oxygen to form superoxide radicals (·), thereby promoting the catalytic oxidation of H2S. XPS testing revealed that upon loading of Cu-Fe oxide, the formation of FeOOH can facilitate the catalytic oxidation of H2S to sulfur (S) through a chain reaction. Combining EPR and XPS analyses, Na2CO3 modification modulates the content of ·, directing the formation of S and then significantly improving the catalyst’s desulfurization efficiency. Furthermore, CO2-TPD testing revealed that Na2CO3 modification promotes the ionization of H2S to HS-, thereby enhancing the catalyst’s desulfurization performance. Based on the distribution of sulfur species in used catalysts, and the results of characterizations, a possible desulfurization mechanism of CuFeNaAC-X has been proposed.
期刊介绍:
Separation and Purification Technology is a premier journal committed to sharing innovative methods for separation and purification in chemical and environmental engineering, encompassing both homogeneous solutions and heterogeneous mixtures. Our scope includes the separation and/or purification of liquids, vapors, and gases, as well as carbon capture and separation techniques. However, it's important to note that methods solely intended for analytical purposes are not within the scope of the journal. Additionally, disciplines such as soil science, polymer science, and metallurgy fall outside the purview of Separation and Purification Technology. Join us in advancing the field of separation and purification methods for sustainable solutions in chemical and environmental engineering.