{"title":"过氧化氢处理的甘油源多孔碳与单质硫基硫磷共掺杂用于CO2捕获","authors":"Gerardo D.J. Guerrero Peña , Anish Mathai Varghese , Suresh Kuppireddy , Phil Hart , Rukayat S.B. Zakari , Nahla Alamoodi , Georgios N. Karanikolos , Abhijeet Raj , Mirella Elkadi","doi":"10.1016/j.scitotenv.2025.178967","DOIUrl":null,"url":null,"abstract":"<div><div>In this work, glycerol and elemental sulfur-based porous carbon adsorbents with sulfur‑phosphorus co-doping and subsequent H<sub>2</sub>O<sub>2</sub> treatment were developed for CO<sub>2</sub> capture. The best adsorbent for capturing CO<sub>2</sub> among the developed adsorbents was P‑carbon-2000mgS-H<sub>2</sub>O<sub>2</sub>, which had surface area of 652 m<sup>2</sup>/g, a total pore volume of 0.446 cm<sup>3</sup>/g, an average pore size of 2.74 nm, narrow micropore distribution, X-ray photoelectron spectroscopy (XPS)-based sulfur content of 5.7 at.% and phosphorus content of 3.7 at.%, Raman-based average PAHs size of 24.9 Å and a defect density of 4.47 × 10<sup>11</sup> cm<sup>−2</sup>, and X-ray diffraction (XRD)-based nano-crystallite height of 11.15 Å and length of 23.35 Å. The CO<sub>2</sub> adsorption capacity of P‑carbon-2000mgS-H<sub>2</sub>O<sub>2</sub> was 1.95 mmol/g at 25 °C and 1 bar (3.02 mmol/g at 0 °C), and it also demonstrated an impressive CO<sub>2</sub> selectivity over N<sub>2</sub> at 25 °C, with 15.24 at 0.5 bar and 12.03 at 1 bar. In addition to cyclic performance, the isosteric heat of CO<sub>2</sub> adsorption, which was found to be between 22 and 23 kJ/mol, suggested that a physical mechanism predominated the CO<sub>2</sub> interaction with active sites. These findings suggest that employing elemental sulfur to produce glycerol-derived porous carbon with sulfur-phosphorus co-doping and subsequent H<sub>2</sub>O<sub>2</sub> treatment is an effective method to produce CO<sub>2</sub> capture adsorbents, facilitating the usage of glycerol and elemental sulfur - based products for large-scale applications.</div></div>","PeriodicalId":422,"journal":{"name":"Science of the Total Environment","volume":"969 ","pages":"Article 178967"},"PeriodicalIF":8.0000,"publicationDate":"2025-02-27","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"Hydrogen peroxide-treated glycerol sourced porous carbon with elemental sulfur-based sulfur-phosphorus co-doping for CO2 capture\",\"authors\":\"Gerardo D.J. Guerrero Peña , Anish Mathai Varghese , Suresh Kuppireddy , Phil Hart , Rukayat S.B. Zakari , Nahla Alamoodi , Georgios N. Karanikolos , Abhijeet Raj , Mirella Elkadi\",\"doi\":\"10.1016/j.scitotenv.2025.178967\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"<div><div>In this work, glycerol and elemental sulfur-based porous carbon adsorbents with sulfur‑phosphorus co-doping and subsequent H<sub>2</sub>O<sub>2</sub> treatment were developed for CO<sub>2</sub> capture. The best adsorbent for capturing CO<sub>2</sub> among the developed adsorbents was P‑carbon-2000mgS-H<sub>2</sub>O<sub>2</sub>, which had surface area of 652 m<sup>2</sup>/g, a total pore volume of 0.446 cm<sup>3</sup>/g, an average pore size of 2.74 nm, narrow micropore distribution, X-ray photoelectron spectroscopy (XPS)-based sulfur content of 5.7 at.% and phosphorus content of 3.7 at.%, Raman-based average PAHs size of 24.9 Å and a defect density of 4.47 × 10<sup>11</sup> cm<sup>−2</sup>, and X-ray diffraction (XRD)-based nano-crystallite height of 11.15 Å and length of 23.35 Å. The CO<sub>2</sub> adsorption capacity of P‑carbon-2000mgS-H<sub>2</sub>O<sub>2</sub> was 1.95 mmol/g at 25 °C and 1 bar (3.02 mmol/g at 0 °C), and it also demonstrated an impressive CO<sub>2</sub> selectivity over N<sub>2</sub> at 25 °C, with 15.24 at 0.5 bar and 12.03 at 1 bar. In addition to cyclic performance, the isosteric heat of CO<sub>2</sub> adsorption, which was found to be between 22 and 23 kJ/mol, suggested that a physical mechanism predominated the CO<sub>2</sub> interaction with active sites. These findings suggest that employing elemental sulfur to produce glycerol-derived porous carbon with sulfur-phosphorus co-doping and subsequent H<sub>2</sub>O<sub>2</sub> treatment is an effective method to produce CO<sub>2</sub> capture adsorbents, facilitating the usage of glycerol and elemental sulfur - based products for large-scale applications.</div></div>\",\"PeriodicalId\":422,\"journal\":{\"name\":\"Science of the Total Environment\",\"volume\":\"969 \",\"pages\":\"Article 178967\"},\"PeriodicalIF\":8.0000,\"publicationDate\":\"2025-02-27\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"Science of the Total Environment\",\"FirstCategoryId\":\"93\",\"ListUrlMain\":\"https://www.sciencedirect.com/science/article/pii/S0048969725006023\",\"RegionNum\":1,\"RegionCategory\":\"环境科学与生态学\",\"ArticlePicture\":[],\"TitleCN\":null,\"AbstractTextCN\":null,\"PMCID\":null,\"EPubDate\":\"\",\"PubModel\":\"\",\"JCR\":\"Q1\",\"JCRName\":\"ENVIRONMENTAL SCIENCES\",\"Score\":null,\"Total\":0}","platform":"Semanticscholar","paperid":null,"PeriodicalName":"Science of the Total Environment","FirstCategoryId":"93","ListUrlMain":"https://www.sciencedirect.com/science/article/pii/S0048969725006023","RegionNum":1,"RegionCategory":"环境科学与生态学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q1","JCRName":"ENVIRONMENTAL SCIENCES","Score":null,"Total":0}
Hydrogen peroxide-treated glycerol sourced porous carbon with elemental sulfur-based sulfur-phosphorus co-doping for CO2 capture
In this work, glycerol and elemental sulfur-based porous carbon adsorbents with sulfur‑phosphorus co-doping and subsequent H2O2 treatment were developed for CO2 capture. The best adsorbent for capturing CO2 among the developed adsorbents was P‑carbon-2000mgS-H2O2, which had surface area of 652 m2/g, a total pore volume of 0.446 cm3/g, an average pore size of 2.74 nm, narrow micropore distribution, X-ray photoelectron spectroscopy (XPS)-based sulfur content of 5.7 at.% and phosphorus content of 3.7 at.%, Raman-based average PAHs size of 24.9 Å and a defect density of 4.47 × 1011 cm−2, and X-ray diffraction (XRD)-based nano-crystallite height of 11.15 Å and length of 23.35 Å. The CO2 adsorption capacity of P‑carbon-2000mgS-H2O2 was 1.95 mmol/g at 25 °C and 1 bar (3.02 mmol/g at 0 °C), and it also demonstrated an impressive CO2 selectivity over N2 at 25 °C, with 15.24 at 0.5 bar and 12.03 at 1 bar. In addition to cyclic performance, the isosteric heat of CO2 adsorption, which was found to be between 22 and 23 kJ/mol, suggested that a physical mechanism predominated the CO2 interaction with active sites. These findings suggest that employing elemental sulfur to produce glycerol-derived porous carbon with sulfur-phosphorus co-doping and subsequent H2O2 treatment is an effective method to produce CO2 capture adsorbents, facilitating the usage of glycerol and elemental sulfur - based products for large-scale applications.
期刊介绍:
The Science of the Total Environment is an international journal dedicated to scientific research on the environment and its interaction with humanity. It covers a wide range of disciplines and seeks to publish innovative, hypothesis-driven, and impactful research that explores the entire environment, including the atmosphere, lithosphere, hydrosphere, biosphere, and anthroposphere.
The journal's updated Aims & Scope emphasizes the importance of interdisciplinary environmental research with broad impact. Priority is given to studies that advance fundamental understanding and explore the interconnectedness of multiple environmental spheres. Field studies are preferred, while laboratory experiments must demonstrate significant methodological advancements or mechanistic insights with direct relevance to the environment.