Jian Wang , Ying Shi , Chengxu Rong , Yulin Li , Zhuyin Sui , Xiufeng Xu
{"title":"自活化微孔碳具有定制的孔结构和表面极性,用于高效分离SF6/N2和NF3/N2","authors":"Jian Wang , Ying Shi , Chengxu Rong , Yulin Li , Zhuyin Sui , Xiufeng Xu","doi":"10.1016/j.carbon.2025.120647","DOIUrl":null,"url":null,"abstract":"<div><div>Adsorption-based separation of SF<sub>6</sub> and NF<sub>3</sub> from N<sub>2</sub> represents a promising strategy for resource recovery and environmental mitigation. However, the development of cost-effective adsorbents possessing precisely engineered structures for high efficiency remains challenging. This study introduces a straightforward, self-activation method for synthesizing microporous carbon adsorbents through the direct pyrolysis of polyvinylidene fluoride (PVDF) resin. This approach enables the simultaneous tailoring of micropore size distribution for size matching and the in-situ surface polarity modulation via polar oxygen and residual fluorine functional groups. By adjusting pyrolysis temperatures from 600 to 900 °C, we obtained an optimal PVDF-800 with a high concentration of micropores centered at ∼0.68 nm. The combination of tuned pore structure and enhanced polarity results in competitive static adsorption capacities for SF<sub>6</sub> (1.93 mmol g<sup>−1</sup>) and NF<sub>3</sub> (0.57 mmol g<sup>−1</sup>) at 298 K and 0.1 bar, coupled with moderate adsorption affinities for regeneration. Dynamic breakthrough experiments under binary mixtures confirm the effective separation performance and cyclic stability of PVDF-800. Critically, PVDF-800 demonstrates efficient desorption performance at 298 K, yielding 1.17 mmol g<sup>−1</sup> SF<sub>6</sub> and 0.13 mmol g<sup>−1</sup> NF<sub>3</sub> with ≥99.9 % purity. These results highlight the significance of concurrently optimizing pore size and surface polarity for developing high-performance porous adsorbents for F-gas separation.</div></div>","PeriodicalId":262,"journal":{"name":"Carbon","volume":"244 ","pages":"Article 120647"},"PeriodicalIF":11.6000,"publicationDate":"2025-07-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"Self-activated microporous carbon with tailored pore structures and surface polarity for efficient SF6/N2 and NF3/N2 separation\",\"authors\":\"Jian Wang , Ying Shi , Chengxu Rong , Yulin Li , Zhuyin Sui , Xiufeng Xu\",\"doi\":\"10.1016/j.carbon.2025.120647\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"<div><div>Adsorption-based separation of SF<sub>6</sub> and NF<sub>3</sub> from N<sub>2</sub> represents a promising strategy for resource recovery and environmental mitigation. However, the development of cost-effective adsorbents possessing precisely engineered structures for high efficiency remains challenging. This study introduces a straightforward, self-activation method for synthesizing microporous carbon adsorbents through the direct pyrolysis of polyvinylidene fluoride (PVDF) resin. This approach enables the simultaneous tailoring of micropore size distribution for size matching and the in-situ surface polarity modulation via polar oxygen and residual fluorine functional groups. By adjusting pyrolysis temperatures from 600 to 900 °C, we obtained an optimal PVDF-800 with a high concentration of micropores centered at ∼0.68 nm. The combination of tuned pore structure and enhanced polarity results in competitive static adsorption capacities for SF<sub>6</sub> (1.93 mmol g<sup>−1</sup>) and NF<sub>3</sub> (0.57 mmol g<sup>−1</sup>) at 298 K and 0.1 bar, coupled with moderate adsorption affinities for regeneration. Dynamic breakthrough experiments under binary mixtures confirm the effective separation performance and cyclic stability of PVDF-800. Critically, PVDF-800 demonstrates efficient desorption performance at 298 K, yielding 1.17 mmol g<sup>−1</sup> SF<sub>6</sub> and 0.13 mmol g<sup>−1</sup> NF<sub>3</sub> with ≥99.9 % purity. These results highlight the significance of concurrently optimizing pore size and surface polarity for developing high-performance porous adsorbents for F-gas separation.</div></div>\",\"PeriodicalId\":262,\"journal\":{\"name\":\"Carbon\",\"volume\":\"244 \",\"pages\":\"Article 120647\"},\"PeriodicalIF\":11.6000,\"publicationDate\":\"2025-07-21\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"Carbon\",\"FirstCategoryId\":\"88\",\"ListUrlMain\":\"https://www.sciencedirect.com/science/article/pii/S0008622325006633\",\"RegionNum\":2,\"RegionCategory\":\"材料科学\",\"ArticlePicture\":[],\"TitleCN\":null,\"AbstractTextCN\":null,\"PMCID\":null,\"EPubDate\":\"\",\"PubModel\":\"\",\"JCR\":\"Q1\",\"JCRName\":\"CHEMISTRY, PHYSICAL\",\"Score\":null,\"Total\":0}","platform":"Semanticscholar","paperid":null,"PeriodicalName":"Carbon","FirstCategoryId":"88","ListUrlMain":"https://www.sciencedirect.com/science/article/pii/S0008622325006633","RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q1","JCRName":"CHEMISTRY, PHYSICAL","Score":null,"Total":0}
Self-activated microporous carbon with tailored pore structures and surface polarity for efficient SF6/N2 and NF3/N2 separation
Adsorption-based separation of SF6 and NF3 from N2 represents a promising strategy for resource recovery and environmental mitigation. However, the development of cost-effective adsorbents possessing precisely engineered structures for high efficiency remains challenging. This study introduces a straightforward, self-activation method for synthesizing microporous carbon adsorbents through the direct pyrolysis of polyvinylidene fluoride (PVDF) resin. This approach enables the simultaneous tailoring of micropore size distribution for size matching and the in-situ surface polarity modulation via polar oxygen and residual fluorine functional groups. By adjusting pyrolysis temperatures from 600 to 900 °C, we obtained an optimal PVDF-800 with a high concentration of micropores centered at ∼0.68 nm. The combination of tuned pore structure and enhanced polarity results in competitive static adsorption capacities for SF6 (1.93 mmol g−1) and NF3 (0.57 mmol g−1) at 298 K and 0.1 bar, coupled with moderate adsorption affinities for regeneration. Dynamic breakthrough experiments under binary mixtures confirm the effective separation performance and cyclic stability of PVDF-800. Critically, PVDF-800 demonstrates efficient desorption performance at 298 K, yielding 1.17 mmol g−1 SF6 and 0.13 mmol g−1 NF3 with ≥99.9 % purity. These results highlight the significance of concurrently optimizing pore size and surface polarity for developing high-performance porous adsorbents for F-gas separation.
期刊介绍:
The journal Carbon is an international multidisciplinary forum for communicating scientific advances in the field of carbon materials. It reports new findings related to the formation, structure, properties, behaviors, and technological applications of carbons. Carbons are a broad class of ordered or disordered solid phases composed primarily of elemental carbon, including but not limited to carbon black, carbon fibers and filaments, carbon nanotubes, diamond and diamond-like carbon, fullerenes, glassy carbon, graphite, graphene, graphene-oxide, porous carbons, pyrolytic carbon, and other sp2 and non-sp2 hybridized carbon systems. Carbon is the companion title to the open access journal Carbon Trends. Relevant application areas for carbon materials include biology and medicine, catalysis, electronic, optoelectronic, spintronic, high-frequency, and photonic devices, energy storage and conversion systems, environmental applications and water treatment, smart materials and systems, and structural and thermal applications.