Jing Nie, Subrata Chandra Roy, Sital Dhami, Taohedul Islam, Ruhul Amin, Xianchun Zhu, Kathryn Taylor-Pashow, Fengxiang Han, Saiful Muhammad Islam
{"title":"K-Co-Mo-Sx Chalcogel - 高容量去除 Pb2+ 和 Ag+ 及其基本机制","authors":"Jing Nie, Subrata Chandra Roy, Sital Dhami, Taohedul Islam, Ruhul Amin, Xianchun Zhu, Kathryn Taylor-Pashow, Fengxiang Han, Saiful Muhammad Islam","doi":"10.1039/d4ta05158k","DOIUrl":null,"url":null,"abstract":"Chalcogenide-based aerogels, known as chalcogels, represent a novel class of nanoparticle-based porous amorphous materials characterized by high surface polarizability, substantial surface area, and Lewis base properties, exhibiting promising applications in clean energy and separation science. This work presents K-Co-Mo-S<small><sub>x</sub></small> (KCMS) chalcogel as a highly efficient sorbent for heavy metal ions and details its sorption mechanisms. Its incoherent structure comprises Mo<small><sub>2</sub></small><small><sup>V</sup></small>(S<small><sub>2</sub></small>)<small><sub>6</sub></small> and Mo<small><sub>3</sub></small><small><sup>IV</sup></small>S(S<small><sub>6</sub></small>)<small><sub>2</sub></small> anionic clusters and four- and six-coordinated Co─S polyhedra, forming a Co-Mo-S covalent network that hosts K+ ions through electrostatic attraction. Interactions of KCMS with heavy metal ions, particularly Pb<small><sup>2+</sup></small> and Ag<small><sup>+</sup></small>, revealed that KCMS is exceptionally effective in removing these ions from ppm concentrations down to trace levels (≤5 ppb). KCMS rapidly removes Ag<small><sup>+</sup></small> (≈81.7%) and Pb<small><sup>2+</sup></small> (≈99.5%) within five minutes, achieving >99.9% removal within an hour, with a distribution constant, K<small><sub>d</sub></small> ≥108 mL/g. KCMS exhibits an impressive removal capacity of 1378 mg/g for Ag<small><sup>+</sup></small> and 1146 mg/g for Pb<small><sup>2+</sup></small>, establishing it as one of the most effective materials known to date for heavy metal removal. This material is also effective for the removal of Ag<small><sup>+</sup></small> and Pb<small><sup>2+</sup></small> along with Hg<small><sup>2+</sup></small>, Ni<small><sup>2+</sup></small>, Cu<small><sup>2+</sup></small>, and Cd<small><sup>2+</sup></small> from various waters even in the presence of highly concentrated and chemically diverse cations, anions, and organic species. Analysis of the post-interacted KCMS by synchrotron pair distribution functions (PDF), X-ray photoelectron spectroscopy (XPS) and energy dispersive X-ray spectroscopy (EDS) revealed the sorption of Pb<small><sup>2+</sup></small>, Ag<small><sup>+</sup></small>, and Hg<small><sup>2+</sup></small> mainly occurs by the exchange of K<small><sup>+</sup></small> and Co<small><sup>2+</sup></small>. Despite being amorphous, this material exhibits unprecedented ion-exchange mechanisms both for the ionically and covalently bound K<small><sup>+</sup></small> and Co<small><sup>2+</sup></small>, respectively. This discovery advances our knowledge of amorphous gels and guides material synthesis principles for the highly selective and efficient removal of heavy metal ions from water.","PeriodicalId":82,"journal":{"name":"Journal of Materials Chemistry A","volume":null,"pages":null},"PeriodicalIF":10.7000,"publicationDate":"2024-10-08","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"K-Co-Mo-Sx Chalcogel ─ High Capacity Removal of Pb2+ and Ag+ and their Underlying Mechanisms\",\"authors\":\"Jing Nie, Subrata Chandra Roy, Sital Dhami, Taohedul Islam, Ruhul Amin, Xianchun Zhu, Kathryn Taylor-Pashow, Fengxiang Han, Saiful Muhammad Islam\",\"doi\":\"10.1039/d4ta05158k\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"Chalcogenide-based aerogels, known as chalcogels, represent a novel class of nanoparticle-based porous amorphous materials characterized by high surface polarizability, substantial surface area, and Lewis base properties, exhibiting promising applications in clean energy and separation science. This work presents K-Co-Mo-S<small><sub>x</sub></small> (KCMS) chalcogel as a highly efficient sorbent for heavy metal ions and details its sorption mechanisms. Its incoherent structure comprises Mo<small><sub>2</sub></small><small><sup>V</sup></small>(S<small><sub>2</sub></small>)<small><sub>6</sub></small> and Mo<small><sub>3</sub></small><small><sup>IV</sup></small>S(S<small><sub>6</sub></small>)<small><sub>2</sub></small> anionic clusters and four- and six-coordinated Co─S polyhedra, forming a Co-Mo-S covalent network that hosts K+ ions through electrostatic attraction. Interactions of KCMS with heavy metal ions, particularly Pb<small><sup>2+</sup></small> and Ag<small><sup>+</sup></small>, revealed that KCMS is exceptionally effective in removing these ions from ppm concentrations down to trace levels (≤5 ppb). KCMS rapidly removes Ag<small><sup>+</sup></small> (≈81.7%) and Pb<small><sup>2+</sup></small> (≈99.5%) within five minutes, achieving >99.9% removal within an hour, with a distribution constant, K<small><sub>d</sub></small> ≥108 mL/g. KCMS exhibits an impressive removal capacity of 1378 mg/g for Ag<small><sup>+</sup></small> and 1146 mg/g for Pb<small><sup>2+</sup></small>, establishing it as one of the most effective materials known to date for heavy metal removal. This material is also effective for the removal of Ag<small><sup>+</sup></small> and Pb<small><sup>2+</sup></small> along with Hg<small><sup>2+</sup></small>, Ni<small><sup>2+</sup></small>, Cu<small><sup>2+</sup></small>, and Cd<small><sup>2+</sup></small> from various waters even in the presence of highly concentrated and chemically diverse cations, anions, and organic species. Analysis of the post-interacted KCMS by synchrotron pair distribution functions (PDF), X-ray photoelectron spectroscopy (XPS) and energy dispersive X-ray spectroscopy (EDS) revealed the sorption of Pb<small><sup>2+</sup></small>, Ag<small><sup>+</sup></small>, and Hg<small><sup>2+</sup></small> mainly occurs by the exchange of K<small><sup>+</sup></small> and Co<small><sup>2+</sup></small>. Despite being amorphous, this material exhibits unprecedented ion-exchange mechanisms both for the ionically and covalently bound K<small><sup>+</sup></small> and Co<small><sup>2+</sup></small>, respectively. This discovery advances our knowledge of amorphous gels and guides material synthesis principles for the highly selective and efficient removal of heavy metal ions from water.\",\"PeriodicalId\":82,\"journal\":{\"name\":\"Journal of Materials Chemistry A\",\"volume\":null,\"pages\":null},\"PeriodicalIF\":10.7000,\"publicationDate\":\"2024-10-08\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"Journal of Materials Chemistry A\",\"FirstCategoryId\":\"88\",\"ListUrlMain\":\"https://doi.org/10.1039/d4ta05158k\",\"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":"Journal of Materials Chemistry A","FirstCategoryId":"88","ListUrlMain":"https://doi.org/10.1039/d4ta05158k","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}
K-Co-Mo-Sx Chalcogel ─ High Capacity Removal of Pb2+ and Ag+ and their Underlying Mechanisms
Chalcogenide-based aerogels, known as chalcogels, represent a novel class of nanoparticle-based porous amorphous materials characterized by high surface polarizability, substantial surface area, and Lewis base properties, exhibiting promising applications in clean energy and separation science. This work presents K-Co-Mo-Sx (KCMS) chalcogel as a highly efficient sorbent for heavy metal ions and details its sorption mechanisms. Its incoherent structure comprises Mo2V(S2)6 and Mo3IVS(S6)2 anionic clusters and four- and six-coordinated Co─S polyhedra, forming a Co-Mo-S covalent network that hosts K+ ions through electrostatic attraction. Interactions of KCMS with heavy metal ions, particularly Pb2+ and Ag+, revealed that KCMS is exceptionally effective in removing these ions from ppm concentrations down to trace levels (≤5 ppb). KCMS rapidly removes Ag+ (≈81.7%) and Pb2+ (≈99.5%) within five minutes, achieving >99.9% removal within an hour, with a distribution constant, Kd ≥108 mL/g. KCMS exhibits an impressive removal capacity of 1378 mg/g for Ag+ and 1146 mg/g for Pb2+, establishing it as one of the most effective materials known to date for heavy metal removal. This material is also effective for the removal of Ag+ and Pb2+ along with Hg2+, Ni2+, Cu2+, and Cd2+ from various waters even in the presence of highly concentrated and chemically diverse cations, anions, and organic species. Analysis of the post-interacted KCMS by synchrotron pair distribution functions (PDF), X-ray photoelectron spectroscopy (XPS) and energy dispersive X-ray spectroscopy (EDS) revealed the sorption of Pb2+, Ag+, and Hg2+ mainly occurs by the exchange of K+ and Co2+. Despite being amorphous, this material exhibits unprecedented ion-exchange mechanisms both for the ionically and covalently bound K+ and Co2+, respectively. This discovery advances our knowledge of amorphous gels and guides material synthesis principles for the highly selective and efficient removal of heavy metal ions from water.
期刊介绍:
The Journal of Materials Chemistry A, B & C covers a wide range of high-quality studies in the field of materials chemistry, with each section focusing on specific applications of the materials studied. Journal of Materials Chemistry A emphasizes applications in energy and sustainability, including topics such as artificial photosynthesis, batteries, and fuel cells. Journal of Materials Chemistry B focuses on applications in biology and medicine, while Journal of Materials Chemistry C covers applications in optical, magnetic, and electronic devices. Example topic areas within the scope of Journal of Materials Chemistry A include catalysis, green/sustainable materials, sensors, and water treatment, among others.