Chemistry of Materials最新文献_第6页

Fermi-Level Interstitial Electron Contributions: A Key Mechanism Driving Magnetism in Electrides

IF 7.2 2区材料科学

Chemistry of Materials Pub Date : 2025-03-12 DOI: 10.1021/acs.chemmater.5c0015810.1021/acs.chemmater.5c00158

Jiahao Yu, Kun Li, Hideo Hosono and Junjie Wang*,

{"title":"Fermi-Level Interstitial Electron Contributions: A Key Mechanism Driving Magnetism in Electrides","authors":"Jiahao Yu, Kun Li, Hideo Hosono and Junjie Wang*, ","doi":"10.1021/acs.chemmater.5c0015810.1021/acs.chemmater.5c00158","DOIUrl":"https://doi.org/10.1021/acs.chemmater.5c00158https://doi.org/10.1021/acs.chemmater.5c00158","url":null,"abstract":"Electrides, a unique class of ionic materials, are distinguished by their exceptional properties, such as low work functions, making them highly versatile for a broad range of applications. Remarkably, some electrides exhibit magnetism, even in the absence of conventional magnetic elements. However, the underlying mechanisms governing their magnetic properties require further investigation, which will enable the development of magnetic electrides that are not primarily limited to modifying materials with magnetic elements. In this study, we demonstrate that the proportion of interstitial electrons contributing to states near the Fermi level is a critical factor in the emergence of magnetism in electrides. Leveraging this insight, we successfully designed and identified a series of magnetic electrides, including Ca3YNbSi3 and Sr24P15F, without reliance on known magnetic prototypes. This strategy and the accompanying theoretical framework present a flexible and powerful approach, potentially expanding the frontiers of magnetic electrides research.","PeriodicalId":33,"journal":{"name":"Chemistry of Materials","volume":"37 6","pages":"2339–2348 2339–2348"},"PeriodicalIF":7.2,"publicationDate":"2025-03-12","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143678451","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Driving Thermoelectric Optimization in AgSbTe2 via Design of Experiments and Machine Learning

IF 8.6 2区材料科学

Chemistry of Materials Pub Date : 2025-03-12 DOI: 10.1021/acs.chemmater.5c00022

Jan-Hendrik Pöhls, Chun-Wan Timothy Lo, Marissa MacIver, Yu-Chih Tseng, Yurij Mozharivskyj

引用次数: 0

Regulating the Co-Spin State in a CoP/Co2P Heterojunction by Phosphorus Vacancies for Efficient Seawater Hydrogen Evolution

IF 8.6 2区材料科学

Chemistry of Materials Pub Date : 2025-03-11 DOI: 10.1021/acs.chemmater.4c02773

Jiang-Bo Chen, Huan Wang, Yu-Xuan Xiao, Jie Ying

{"title":"Regulating the Co-Spin State in a CoP/Co2P Heterojunction by Phosphorus Vacancies for Efficient Seawater Hydrogen Evolution","authors":"Jiang-Bo Chen, Huan Wang, Yu-Xuan Xiao, Jie Ying","doi":"10.1021/acs.chemmater.4c02773","DOIUrl":"https://doi.org/10.1021/acs.chemmater.4c02773","url":null,"abstract":"Hydrogen energy production through seawater splitting is an essential route for a sustainable energy society; however, it is impeded by chlorine corrosion. Therefore, the rational design of highly efficient electrocatalysts for hydrogen evolution by repelling chlorine ion effects is key to unlocking its wide operation. Herein, we report the facile construction of a cobalt phosphide heterojunction with phosphorus vacancies for efficient hydrogen evolution, which needs overpotentials of 82/287 mV and 75/237 mV to achieve a current density of 10/100 mA cm–2 in 1 M KOH and simulated seawater (1 M KOH + 0.5 M NaCl), respectively, outperforming numerous reported non-noble-metal-based electrocatalysts in water/seawater systems. Additionally, the catalyst demonstrates long-time stability over a 120 h period in simulated seawater. More profoundly, both experimental and computational results demonstrate that phosphorus vacancies induce a higher spin state in cobalt atoms within phosphides, which accelerates the desorption of hydrogen species and creates a significant repulsive effect on Cl–, consequently contributing to significantly enhanced hydrogen evolution in simulated seawater.","PeriodicalId":33,"journal":{"name":"Chemistry of Materials","volume":"22 1","pages":""},"PeriodicalIF":8.6,"publicationDate":"2025-03-11","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143599624","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Regulating the Co-Spin State in a CoP/Co2P Heterojunction by Phosphorus Vacancies for Efficient Seawater Hydrogen Evolution

IF 7.2 2区材料科学

Chemistry of Materials Pub Date : 2025-03-11 DOI: 10.1021/acs.chemmater.4c0277310.1021/acs.chemmater.4c02773

Jiang-Bo Chen, Huan Wang, Yu-Xuan Xiao and Jie Ying*,

{"title":"Regulating the Co-Spin State in a CoP/Co2P Heterojunction by Phosphorus Vacancies for Efficient Seawater Hydrogen Evolution","authors":"Jiang-Bo Chen, Huan Wang, Yu-Xuan Xiao and Jie Ying*, ","doi":"10.1021/acs.chemmater.4c0277310.1021/acs.chemmater.4c02773","DOIUrl":"https://doi.org/10.1021/acs.chemmater.4c02773https://doi.org/10.1021/acs.chemmater.4c02773","url":null,"abstract":"Hydrogen energy production through seawater splitting is an essential route for a sustainable energy society; however, it is impeded by chlorine corrosion. Therefore, the rational design of highly efficient electrocatalysts for hydrogen evolution by repelling chlorine ion effects is key to unlocking its wide operation. Herein, we report the facile construction of a cobalt phosphide heterojunction with phosphorus vacancies for efficient hydrogen evolution, which needs overpotentials of 82/287 mV and 75/237 mV to achieve a current density of 10/100 mA cm–2 in 1 M KOH and simulated seawater (1 M KOH + 0.5 M NaCl), respectively, outperforming numerous reported non-noble-metal-based electrocatalysts in water/seawater systems. Additionally, the catalyst demonstrates long-time stability over a 120 h period in simulated seawater. More profoundly, both experimental and computational results demonstrate that phosphorus vacancies induce a higher spin state in cobalt atoms within phosphides, which accelerates the desorption of hydrogen species and creates a significant repulsive effect on Cl–, consequently contributing to significantly enhanced hydrogen evolution in simulated seawater.","PeriodicalId":33,"journal":{"name":"Chemistry of Materials","volume":"37 6","pages":"2145–2154 2145–2154"},"PeriodicalIF":7.2,"publicationDate":"2025-03-11","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143678454","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Engineering the Artificial Cathode-Electrolyte Interphase Coating for Solid-State Batteries via Tailored Annealing

IF 7.2 2区材料科学

Chemistry of Materials Pub Date : 2025-03-11 DOI: 10.1021/acs.chemmater.4c0308610.1021/acs.chemmater.4c03086

Maximilian Kissel, Felix Walther, Jonas Hertle, Thomas Demuth, Ruizhuo Zhang, Philipp Brüner, Torsten Brezesinski, Kerstin Volz and Jürgen Janek*,

{"title":"Engineering the Artificial Cathode-Electrolyte Interphase Coating for Solid-State Batteries via Tailored Annealing","authors":"Maximilian Kissel, Felix Walther, Jonas Hertle, Thomas Demuth, Ruizhuo Zhang, Philipp Brüner, Torsten Brezesinski, Kerstin Volz and Jürgen Janek*, ","doi":"10.1021/acs.chemmater.4c0308610.1021/acs.chemmater.4c03086","DOIUrl":"https://doi.org/10.1021/acs.chemmater.4c03086https://doi.org/10.1021/acs.chemmater.4c03086","url":null,"abstract":"Solid-state batteries with nickel-rich layered oxide cathode active materials (CAMs) and sulfide-based solid electrolytes (SEs) are emerging as promising candidates for next-generation energy-storage systems. However, both active and electrolyte materials suffer from poor (electro)chemical compatibility, leading to severe degradation at the SE|CAM interface which is highly detrimental to the long-term cycling stability. Inspired by the natural cathode-electrolyte interphase (CEI), a novel coating concept involves formation of a protective, artificial CEI coating prior to cell assembly. Here, we investigate the oxidative annealing process after coating Li3PS4 as precursor onto polycrystalline LiNi0.85Co0.10Mn0.05O2 (NCM85). A combination of microscopic (scanning transmission electron microscopy, STEM), spectroscopic/spectrometric (X-ray photoelectron spectroscopy, XPS, low energy ion scattering, LEIS, and time-of-flight secondary ion mass spectrometry, ToF-SIMS), and electrochemical methods reveals that the composition, morphology, and performance of the coating can be tailored by controlled annealing in oxidizing atmosphere. The effect on coating quality and its stabilizing effect on the SE|CAM interface are examined. Only a morphologically and compositionally optimized coating can successfully prevent interfacial degradation, highlighting the need for tailored process parameters to fully exploit the coating potential. The optimization is supported by an efficient benchmarking framework combining electrochemical and analytical methods, which can serve as a basis for further systematic coating studies.","PeriodicalId":33,"journal":{"name":"Chemistry of Materials","volume":"37 6","pages":"2192–2203 2192–2203"},"PeriodicalIF":7.2,"publicationDate":"2025-03-11","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.acs.org/doi/epdf/10.1021/acs.chemmater.4c03086","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143678642","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Engineering the Artificial Cathode-Electrolyte Interphase Coating for Solid-State Batteries via Tailored Annealing

IF 8.6 2区材料科学

Chemistry of Materials Pub Date : 2025-03-11 DOI: 10.1021/acs.chemmater.4c03086

Maximilian Kissel, Felix Walther, Jonas Hertle, Thomas Demuth, Ruizhuo Zhang, Philipp Brüner, Torsten Brezesinski, Kerstin Volz, Jürgen Janek

{"title":"Engineering the Artificial Cathode-Electrolyte Interphase Coating for Solid-State Batteries via Tailored Annealing","authors":"Maximilian Kissel, Felix Walther, Jonas Hertle, Thomas Demuth, Ruizhuo Zhang, Philipp Brüner, Torsten Brezesinski, Kerstin Volz, Jürgen Janek","doi":"10.1021/acs.chemmater.4c03086","DOIUrl":"https://doi.org/10.1021/acs.chemmater.4c03086","url":null,"abstract":"Solid-state batteries with nickel-rich layered oxide cathode active materials (CAMs) and sulfide-based solid electrolytes (SEs) are emerging as promising candidates for next-generation energy-storage systems. However, both active and electrolyte materials suffer from poor (electro)chemical compatibility, leading to severe degradation at the SE|CAM interface which is highly detrimental to the long-term cycling stability. Inspired by the natural cathode-electrolyte interphase (CEI), a novel coating concept involves formation of a protective, artificial CEI coating prior to cell assembly. Here, we investigate the oxidative annealing process after coating Li3PS4 as precursor onto polycrystalline LiNi0.85Co0.10Mn0.05O2 (NCM85). A combination of microscopic (scanning transmission electron microscopy, STEM), spectroscopic/spectrometric (X-ray photoelectron spectroscopy, XPS, low energy ion scattering, LEIS, and time-of-flight secondary ion mass spectrometry, ToF-SIMS), and electrochemical methods reveals that the composition, morphology, and performance of the coating can be tailored by controlled annealing in oxidizing atmosphere. The effect on coating quality and its stabilizing effect on the SE|CAM interface are examined. Only a morphologically and compositionally optimized coating can successfully prevent interfacial degradation, highlighting the need for tailored process parameters to fully exploit the coating potential. The optimization is supported by an efficient benchmarking framework combining electrochemical and analytical methods, which can serve as a basis for further systematic coating studies.","PeriodicalId":33,"journal":{"name":"Chemistry of Materials","volume":"31 1","pages":""},"PeriodicalIF":8.6,"publicationDate":"2025-03-11","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143590132","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

A Flexible Interpenetrated Diamondoid Metal–Organic Framework with Aromatic-Enriched Channels as a Preconcentrator for the Detection of Fluorinated Anesthetics

IF 8.6 2区材料科学

Chemistry of Materials Pub Date : 2025-03-11 DOI: 10.1021/acs.chemmater.4c03221

Danilo Marchetti, Nicolò Riboni, A. Ken Inge, Ocean Cheung, Mauro Gemmi, Enrico Dalcanale, Federica Bianchi, Chiara Massera, Alessandro Pedrini

{"title":"A Flexible Interpenetrated Diamondoid Metal–Organic Framework with Aromatic-Enriched Channels as a Preconcentrator for the Detection of Fluorinated Anesthetics","authors":"Danilo Marchetti, Nicolò Riboni, A. Ken Inge, Ocean Cheung, Mauro Gemmi, Enrico Dalcanale, Federica Bianchi, Chiara Massera, Alessandro Pedrini","doi":"10.1021/acs.chemmater.4c03221","DOIUrl":"https://doi.org/10.1021/acs.chemmater.4c03221","url":null,"abstract":"Flexible metal–organic frameworks (MOFs) are dynamic materials that combine long-range structural order with reversible stimulus-responsive phase transitions. In this study, we report the synthesis and characterization of two isoreticular flexible MOFs, TPPM-CPW(Me) and TPPM-CPW(Ph), constructed by combining the ligand tetra-4-(4-pyridyl)phenylmethane (TPPM) with specific Cu(II) paddle-wheel (CPW) secondary building units (SBUs). These MOFs exhibit reversible transitions between open- and closed-pore forms triggered by external stimuli, such as temperature- and pressure-induced guest removal and uptake. The stability of these frameworks is influenced by the residual equatorial groups on the Cu(II) SBUs, with phenyl-functionalized TPPM-CPW(Ph) displaying dynamic behavior characteristic of third-generation soft porous crystals. Notably, TPPM-CPW(Ph) exhibited high adsorption affinity toward fluorinated guests, including SF6 and volatile anesthetics (VAs) such as desflurane and sevoflurane. This material, when used in solid-phase microextraction (SPME) as fiber coating for the preconcentration of these VAs in air, outperformed commercial CAR/PDMS fibers, underscoring the potential of these versatile flexible MOFs in addressing environmental challenges associated with the use of volatile fluorinated compounds.","PeriodicalId":33,"journal":{"name":"Chemistry of Materials","volume":"3 1","pages":""},"PeriodicalIF":8.6,"publicationDate":"2025-03-11","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143590128","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

A Flexible Interpenetrated Diamondoid Metal–Organic Framework with Aromatic-Enriched Channels as a Preconcentrator for the Detection of Fluorinated Anesthetics

IF 7.2 2区材料科学

Chemistry of Materials Pub Date : 2025-03-11 DOI: 10.1021/acs.chemmater.4c0322110.1021/acs.chemmater.4c03221

Danilo Marchetti, Nicolò Riboni, A. Ken Inge, Ocean Cheung, Mauro Gemmi, Enrico Dalcanale, Federica Bianchi, Chiara Massera* and Alessandro Pedrini*,

{"title":"A Flexible Interpenetrated Diamondoid Metal–Organic Framework with Aromatic-Enriched Channels as a Preconcentrator for the Detection of Fluorinated Anesthetics","authors":"Danilo Marchetti, Nicolò Riboni, A. Ken Inge, Ocean Cheung, Mauro Gemmi, Enrico Dalcanale, Federica Bianchi, Chiara Massera* and Alessandro Pedrini*, ","doi":"10.1021/acs.chemmater.4c0322110.1021/acs.chemmater.4c03221","DOIUrl":"https://doi.org/10.1021/acs.chemmater.4c03221https://doi.org/10.1021/acs.chemmater.4c03221","url":null,"abstract":"Flexible metal–organic frameworks (MOFs) are dynamic materials that combine long-range structural order with reversible stimulus-responsive phase transitions. In this study, we report the synthesis and characterization of two isoreticular flexible MOFs, TPPM-CPW(Me) and TPPM-CPW(Ph), constructed by combining the ligand tetra-4-(4-pyridyl)phenylmethane (TPPM) with specific Cu(II) paddle-wheel (CPW) secondary building units (SBUs). These MOFs exhibit reversible transitions between open- and closed-pore forms triggered by external stimuli, such as temperature- and pressure-induced guest removal and uptake. The stability of these frameworks is influenced by the residual equatorial groups on the Cu(II) SBUs, with phenyl-functionalized TPPM-CPW(Ph) displaying dynamic behavior characteristic of third-generation soft porous crystals. Notably, TPPM-CPW(Ph) exhibited high adsorption affinity toward fluorinated guests, including SF6 and volatile anesthetics (VAs) such as desflurane and sevoflurane. This material, when used in solid-phase microextraction (SPME) as fiber coating for the preconcentration of these VAs in air, outperformed commercial CAR/PDMS fibers, underscoring the potential of these versatile flexible MOFs in addressing environmental challenges associated with the use of volatile fluorinated compounds.","PeriodicalId":33,"journal":{"name":"Chemistry of Materials","volume":"37 6","pages":"2230–2240 2230–2240"},"PeriodicalIF":7.2,"publicationDate":"2025-03-11","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.acs.org/doi/epdf/10.1021/acs.chemmater.4c03221","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143678641","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Chemically Robust Urea-Tethered Adaptable Ionic Porous Nanotrap: Ultrafast Organic and Inorganic Arsenic Water Decontamination

IF 7.2 2区材料科学

Chemistry of Materials Pub Date : 2025-03-10 DOI: 10.1021/acs.chemmater.5c0030410.1021/acs.chemmater.5c00304

Gourab K. Dam, Sumanta Let, Vidha Bhasin, Sahel Fajal, Kishalay Biswas, Mandar M. Shirolkar, Dibyendu Bhattacharyya and Sujit K. Ghosh*,

{"title":"Chemically Robust Urea-Tethered Adaptable Ionic Porous Nanotrap: Ultrafast Organic and Inorganic Arsenic Water Decontamination","authors":"Gourab K. Dam, Sumanta Let, Vidha Bhasin, Sahel Fajal, Kishalay Biswas, Mandar M. Shirolkar, Dibyendu Bhattacharyya and Sujit K. Ghosh*, ","doi":"10.1021/acs.chemmater.5c0030410.1021/acs.chemmater.5c00304","DOIUrl":"https://doi.org/10.1021/acs.chemmater.5c00304https://doi.org/10.1021/acs.chemmater.5c00304","url":null,"abstract":"The poultry industry widely makes use of organoarsenic compounds as feed additives. Consequently, their release into wastewater can be the genesis of serious poisoning of the ecosystem. Roxarsone (ROX), a typical aromatic organoarsenical, on account of being an emerging micropollutant, is imperative to remove from water as it can be degraded into extremely toxic inorganic arsenic compounds poisoning the ecosystem. Therefore, it is topical to design and develop potent materials with high affinity toward organic and inorganic arsenic species, which still remains very challenging. Herein, we report the amalgamation of ionicity and anchoring-adaptable functionality tethered covalently to ensure structural robustness in a single material. IPiPOP-3U bearing a urea functionality-based “nano-trap” displayed outstanding organoarsenic adsorption competence in terms of ultrafast uptake (up to 99% removal in 30 s) and an excellent capacity (833 mg g–1 for ROX). The practical applicability of IPiPOP-3U was verified with trace concentration studies and flow-through experiments. It also displayed unaltered sorption efficiency in various real-world water samples, while the mechanistic aspects were expressed with the aid of an extended X-ray absorption fine structure (EXAFS) in combination with theoretical studies. The thermodynamic feasibility of ROX capture by IPiPOP-3U was further probed by isothermal titration calorimetry (ITC). Additionally, IPiPOP-3U also showed remarkable performance toward the removal of inorganic arsenic, i.e., arsenate (HAsO42–), with a high uptake capacity (264 mg g–1) and excellent cycling performance (up to 10 cycles).","PeriodicalId":33,"journal":{"name":"Chemistry of Materials","volume":"37 6","pages":"2367–2378 2367–2378"},"PeriodicalIF":7.2,"publicationDate":"2025-03-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143678637","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Chemically Robust Urea-Tethered Adaptable Ionic Porous Nanotrap: Ultrafast Organic and Inorganic Arsenic Water Decontamination

IF 8.6 2区材料科学

Chemistry of Materials Pub Date : 2025-03-10 DOI: 10.1021/acs.chemmater.5c00304

Gourab K. Dam, Sumanta Let, Vidha Bhasin, Sahel Fajal, Kishalay Biswas, Mandar M. Shirolkar, Dibyendu Bhattacharyya, Sujit K. Ghosh

{"title":"Chemically Robust Urea-Tethered Adaptable Ionic Porous Nanotrap: Ultrafast Organic and Inorganic Arsenic Water Decontamination","authors":"Gourab K. Dam, Sumanta Let, Vidha Bhasin, Sahel Fajal, Kishalay Biswas, Mandar M. Shirolkar, Dibyendu Bhattacharyya, Sujit K. Ghosh","doi":"10.1021/acs.chemmater.5c00304","DOIUrl":"https://doi.org/10.1021/acs.chemmater.5c00304","url":null,"abstract":"The poultry industry widely makes use of organoarsenic compounds as feed additives. Consequently, their release into wastewater can be the genesis of serious poisoning of the ecosystem. Roxarsone (ROX), a typical aromatic organoarsenical, on account of being an emerging micropollutant, is imperative to remove from water as it can be degraded into extremely toxic inorganic arsenic compounds poisoning the ecosystem. Therefore, it is topical to design and develop potent materials with high affinity toward organic and inorganic arsenic species, which still remains very challenging. Herein, we report the amalgamation of ionicity and anchoring-adaptable functionality tethered covalently to ensure structural robustness in a single material. IPiPOP-3U bearing a urea functionality-based “nano-trap” displayed outstanding organoarsenic adsorption competence in terms of ultrafast uptake (up to 99% removal in 30 s) and an excellent capacity (833 mg g–1 for ROX). The practical applicability of IPiPOP-3U was verified with trace concentration studies and flow-through experiments. It also displayed unaltered sorption efficiency in various real-world water samples, while the mechanistic aspects were expressed with the aid of an extended X-ray absorption fine structure (EXAFS) in combination with theoretical studies. The thermodynamic feasibility of ROX capture by IPiPOP-3U was further probed by isothermal titration calorimetry (ITC). Additionally, IPiPOP-3U also showed remarkable performance toward the removal of inorganic arsenic, i.e., arsenate (HAsO42–), with a high uptake capacity (264 mg g–1) and excellent cycling performance (up to 10 cycles).","PeriodicalId":33,"journal":{"name":"Chemistry of Materials","volume":"87 1","pages":""},"PeriodicalIF":8.6,"publicationDate":"2025-03-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143590135","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0