Gabriel D. Reske , Hercules A. Pereira , Guilherme L. Dotto , Fernanda De Castilhos
{"title":"在高压和高温条件下使用浸渍了沸石 LTA 的氧化石墨增强银离子的连续吸附能力","authors":"Gabriel D. Reske , Hercules A. Pereira , Guilherme L. Dotto , Fernanda De Castilhos","doi":"10.1016/j.molliq.2025.127380","DOIUrl":null,"url":null,"abstract":"<div><div>This study explores the potential of zeolite-impregnated graphite oxide (GOIZ) as a highly efficient adsorbent for the continuous removal of silver ions (Ag(I)) under elevated temperature and pressure conditions in a fixed-bed column. Adsorption performance significantly improved at higher temperatures (100–200 °C), with the best results obtained at 200 °C and 25 MPa. Under these conditions, the maximum stoichiometric adsorption capacity reached 407 mg/g, a substantial increase compared to 47 mg/g under normal conditions (25 °C and 0.101 MPa). This improvement is attributed to enhanced activation of adsorption sites, reduced mass transfer resistance, and progressive desolvation of Ag(I) ions under elevated temperatures, as well as liquid compression effects at high pressure. Interestingly, only at 200 °C and 25 MPa pressure did play a synergistic role, likely due to conditions approaching the subcritical state of water, altering the interaction between adsorbent and adsorbate. Mathematical modeling using the Dose-Response model demonstrated superior predictive accuracy (R<sup>2</sup> ≥ 0.954) compared to the Thomas model, accurately describing Ag(I) adsorption behavior under varying experimental conditions. Mechanistic analysis revealed a adsorption process governed by redox reactions, where Ag<sup>+</sup> ions were reduced to Ag<sup>0</sup> on the adsorbent surface, electrostatic interactions between Ag<sup>+</sup> ions and the negatively charged functional groups of GOIZ and cationic-exchange. The formation of Ag<sup>0</sup> on the adsorbent surface was confirmed, with further adsorption hindered by the resulting silver layer. These findings underscore the exceptional capability of GOIZ for Ag(I) removal in wastewater treatment, particularly under extreme temperature and pressure conditions.</div></div>","PeriodicalId":371,"journal":{"name":"Journal of Molecular Liquids","volume":"426 ","pages":"Article 127380"},"PeriodicalIF":5.3000,"publicationDate":"2025-03-12","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"Enhanced continuous adsorption of silver ions using graphite oxide impregnated with zeolite LTA under high pressure and temperature conditions\",\"authors\":\"Gabriel D. Reske , Hercules A. Pereira , Guilherme L. Dotto , Fernanda De Castilhos\",\"doi\":\"10.1016/j.molliq.2025.127380\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"<div><div>This study explores the potential of zeolite-impregnated graphite oxide (GOIZ) as a highly efficient adsorbent for the continuous removal of silver ions (Ag(I)) under elevated temperature and pressure conditions in a fixed-bed column. Adsorption performance significantly improved at higher temperatures (100–200 °C), with the best results obtained at 200 °C and 25 MPa. Under these conditions, the maximum stoichiometric adsorption capacity reached 407 mg/g, a substantial increase compared to 47 mg/g under normal conditions (25 °C and 0.101 MPa). This improvement is attributed to enhanced activation of adsorption sites, reduced mass transfer resistance, and progressive desolvation of Ag(I) ions under elevated temperatures, as well as liquid compression effects at high pressure. Interestingly, only at 200 °C and 25 MPa pressure did play a synergistic role, likely due to conditions approaching the subcritical state of water, altering the interaction between adsorbent and adsorbate. Mathematical modeling using the Dose-Response model demonstrated superior predictive accuracy (R<sup>2</sup> ≥ 0.954) compared to the Thomas model, accurately describing Ag(I) adsorption behavior under varying experimental conditions. Mechanistic analysis revealed a adsorption process governed by redox reactions, where Ag<sup>+</sup> ions were reduced to Ag<sup>0</sup> on the adsorbent surface, electrostatic interactions between Ag<sup>+</sup> ions and the negatively charged functional groups of GOIZ and cationic-exchange. The formation of Ag<sup>0</sup> on the adsorbent surface was confirmed, with further adsorption hindered by the resulting silver layer. These findings underscore the exceptional capability of GOIZ for Ag(I) removal in wastewater treatment, particularly under extreme temperature and pressure conditions.</div></div>\",\"PeriodicalId\":371,\"journal\":{\"name\":\"Journal of Molecular Liquids\",\"volume\":\"426 \",\"pages\":\"Article 127380\"},\"PeriodicalIF\":5.3000,\"publicationDate\":\"2025-03-12\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"Journal of Molecular Liquids\",\"FirstCategoryId\":\"92\",\"ListUrlMain\":\"https://www.sciencedirect.com/science/article/pii/S0167732225005471\",\"RegionNum\":2,\"RegionCategory\":\"化学\",\"ArticlePicture\":[],\"TitleCN\":null,\"AbstractTextCN\":null,\"PMCID\":null,\"EPubDate\":\"\",\"PubModel\":\"\",\"JCR\":\"Q2\",\"JCRName\":\"CHEMISTRY, PHYSICAL\",\"Score\":null,\"Total\":0}","platform":"Semanticscholar","paperid":null,"PeriodicalName":"Journal of Molecular Liquids","FirstCategoryId":"92","ListUrlMain":"https://www.sciencedirect.com/science/article/pii/S0167732225005471","RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q2","JCRName":"CHEMISTRY, PHYSICAL","Score":null,"Total":0}
Enhanced continuous adsorption of silver ions using graphite oxide impregnated with zeolite LTA under high pressure and temperature conditions
This study explores the potential of zeolite-impregnated graphite oxide (GOIZ) as a highly efficient adsorbent for the continuous removal of silver ions (Ag(I)) under elevated temperature and pressure conditions in a fixed-bed column. Adsorption performance significantly improved at higher temperatures (100–200 °C), with the best results obtained at 200 °C and 25 MPa. Under these conditions, the maximum stoichiometric adsorption capacity reached 407 mg/g, a substantial increase compared to 47 mg/g under normal conditions (25 °C and 0.101 MPa). This improvement is attributed to enhanced activation of adsorption sites, reduced mass transfer resistance, and progressive desolvation of Ag(I) ions under elevated temperatures, as well as liquid compression effects at high pressure. Interestingly, only at 200 °C and 25 MPa pressure did play a synergistic role, likely due to conditions approaching the subcritical state of water, altering the interaction between adsorbent and adsorbate. Mathematical modeling using the Dose-Response model demonstrated superior predictive accuracy (R2 ≥ 0.954) compared to the Thomas model, accurately describing Ag(I) adsorption behavior under varying experimental conditions. Mechanistic analysis revealed a adsorption process governed by redox reactions, where Ag+ ions were reduced to Ag0 on the adsorbent surface, electrostatic interactions between Ag+ ions and the negatively charged functional groups of GOIZ and cationic-exchange. The formation of Ag0 on the adsorbent surface was confirmed, with further adsorption hindered by the resulting silver layer. These findings underscore the exceptional capability of GOIZ for Ag(I) removal in wastewater treatment, particularly under extreme temperature and pressure conditions.
期刊介绍:
The journal includes papers in the following areas:
– Simple organic liquids and mixtures
– Ionic liquids
– Surfactant solutions (including micelles and vesicles) and liquid interfaces
– Colloidal solutions and nanoparticles
– Thermotropic and lyotropic liquid crystals
– Ferrofluids
– Water, aqueous solutions and other hydrogen-bonded liquids
– Lubricants, polymer solutions and melts
– Molten metals and salts
– Phase transitions and critical phenomena in liquids and confined fluids
– Self assembly in complex liquids.– Biomolecules in solution
The emphasis is on the molecular (or microscopic) understanding of particular liquids or liquid systems, especially concerning structure, dynamics and intermolecular forces. The experimental techniques used may include:
– Conventional spectroscopy (mid-IR and far-IR, Raman, NMR, etc.)
– Non-linear optics and time resolved spectroscopy (psec, fsec, asec, ISRS, etc.)
– Light scattering (Rayleigh, Brillouin, PCS, etc.)
– Dielectric relaxation
– X-ray and neutron scattering and diffraction.
Experimental studies, computer simulations (MD or MC) and analytical theory will be considered for publication; papers just reporting experimental results that do not contribute to the understanding of the fundamentals of molecular and ionic liquids will not be accepted. Only papers of a non-routine nature and advancing the field will be considered for publication.