Pub Date : 2024-07-23DOI: 10.1021/acsestengg.4c0023910.1021/acsestengg.4c00239
Chenqi Gao, Yang Yue, Wenying Li, Qing Zhang, Lingen Zhang* and Guangren Qian*,
Low-temperature thermal degradation of PCDD/Fs in incineration fly ash (IFA) has attracted widespread attention with the advantages of low energy consumption and high efficiency. However, in the process of industrialization, the inevitable O2 leakage in the system has always been a technical bottleneck. Based on the characteristics of IFA and the mechanism of PCDD/F regeneration, this study first proposes a dual-strategy LTTD of predechlorination and reduction atmosphere-keeping. Predechlorination removes soluble chlorine and soluble metals while hydrolyzing CaClOH in IFA into Ca(OH)2 to accelerate the detoxication of PCDD/Fs, and deep reduction atmosphere-keeping is created by introducing activated carbon to inhibit the possible PCDD/F regeneration. Compared with typical LTTD, synergistic application of dual-strategy LTTD can obtain 99.4 and 97.4% detoxification efficiencies of PCDD/Fs in the presence of 1 and 2% O2, respectively. Based on the identification of congener distribution and density functional theory calculations, the dechlorination mechanism of acid chloride group-containing PCDD/F intermediates with the participation of CO and Ca(OH)2 was proposed. Finally, the reproducibility of dual-strategy LTTD after optimization of working parameters was well verified and the proposed dual strategies are expected to provide a new direction for the industrialization of LTTD.
{"title":"Dual Positive Effects of Pre-Dechlorine and Low-Temperature Deep Reduction-Keeping on the PCDD/F Removal of Incineration Fly Ash","authors":"Chenqi Gao, Yang Yue, Wenying Li, Qing Zhang, Lingen Zhang* and Guangren Qian*, ","doi":"10.1021/acsestengg.4c0023910.1021/acsestengg.4c00239","DOIUrl":"https://doi.org/10.1021/acsestengg.4c00239https://doi.org/10.1021/acsestengg.4c00239","url":null,"abstract":"<p >Low-temperature thermal degradation of PCDD/Fs in incineration fly ash (IFA) has attracted widespread attention with the advantages of low energy consumption and high efficiency. However, in the process of industrialization, the inevitable O<sub>2</sub> leakage in the system has always been a technical bottleneck. Based on the characteristics of IFA and the mechanism of PCDD/F regeneration, this study first proposes a dual-strategy LTTD of predechlorination and reduction atmosphere-keeping. Predechlorination removes soluble chlorine and soluble metals while hydrolyzing CaClOH in IFA into Ca(OH)<sub>2</sub> to accelerate the detoxication of PCDD/Fs, and deep reduction atmosphere-keeping is created by introducing activated carbon to inhibit the possible PCDD/F regeneration. Compared with typical LTTD, synergistic application of dual-strategy LTTD can obtain 99.4 and 97.4% detoxification efficiencies of PCDD/Fs in the presence of 1 and 2% O<sub>2</sub>, respectively. Based on the identification of congener distribution and density functional theory calculations, the dechlorination mechanism of acid chloride group-containing PCDD/F intermediates with the participation of CO and Ca(OH)<sub>2</sub> was proposed. Finally, the reproducibility of dual-strategy LTTD after optimization of working parameters was well verified and the proposed dual strategies are expected to provide a new direction for the industrialization of LTTD.</p>","PeriodicalId":7008,"journal":{"name":"ACS ES&T engineering","volume":null,"pages":null},"PeriodicalIF":7.4,"publicationDate":"2024-07-23","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142228099","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2024-07-23DOI: 10.1021/acsestengg.4c00281
Dong Jin Kim, Jiyeon Park, Gayoung Ham, Hyojung Cha, Dong Suk Han, Minho Kim, Hyunwoong Park
Heterojunctioning anatase (A) and rutile (R) TiO2 is considered a benchmark strategy for high photocatalytic activity. In this study, we synthesized heterojunctions of anatase (A) and bronze (B) TiO2 via hydrothermal and annealing processes using low-cost commercial A-TiO2. The as-synthesized AB-TiO2 shows remarkable activity for toluene mineralization and a strong tolerance to deactivation. The activity and durability of AB-TiO2 far exceed those of A-, R-, B-, and AR-TiO2, which are bare and even Pt-deposited (a total of 10 TiO2 samples). AB-TiO2 exhibits highly active {001} facets for the generation of hydroxyl radicals and oxygen vacancies beneficial for O2 adsorption. Transient absorption and time-resolved photoluminescence spectroscopies reveal the characteristic lifetimes of electrons and holes. Density functional theory calculations demonstrate facile charge separation and identify the catalytically active surface for oxidation as the anatase surface in AB-TiO2. The observed high activity and durability are analyzed in terms of photochemical and catalytic factors.
{"title":"Deactivation-Tolerance of Heterojunction Anatase and Bronze TiO2 in the Photocatalytic Mineralization of Toluene","authors":"Dong Jin Kim, Jiyeon Park, Gayoung Ham, Hyojung Cha, Dong Suk Han, Minho Kim, Hyunwoong Park","doi":"10.1021/acsestengg.4c00281","DOIUrl":"https://doi.org/10.1021/acsestengg.4c00281","url":null,"abstract":"Heterojunctioning anatase (A) and rutile (R) TiO<sub>2</sub> is considered a benchmark strategy for high photocatalytic activity. In this study, we synthesized heterojunctions of anatase (A) and bronze (B) TiO<sub>2</sub> via hydrothermal and annealing processes using low-cost commercial A-TiO<sub>2</sub>. The as-synthesized AB-TiO<sub>2</sub> shows remarkable activity for toluene mineralization and a strong tolerance to deactivation. The activity and durability of AB-TiO<sub>2</sub> far exceed those of A-, R-, B-, and AR-TiO<sub>2</sub>, which are bare and even Pt-deposited (a total of 10 TiO<sub>2</sub> samples). AB-TiO<sub>2</sub> exhibits highly active {001} facets for the generation of hydroxyl radicals and oxygen vacancies beneficial for O<sub>2</sub> adsorption. Transient absorption and time-resolved photoluminescence spectroscopies reveal the characteristic lifetimes of electrons and holes. Density functional theory calculations demonstrate facile charge separation and identify the catalytically active surface for oxidation as the anatase surface in AB-TiO<sub>2</sub>. The observed high activity and durability are analyzed in terms of photochemical and catalytic factors.","PeriodicalId":7008,"journal":{"name":"ACS ES&T engineering","volume":null,"pages":null},"PeriodicalIF":7.1,"publicationDate":"2024-07-23","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141774969","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Chlorophenols (CPs) pose significant risks to human health due to their toxicity and carcinogenic properties. The direct oxidative breakdown of CPs can produce even more harmful byproducts, resulting in secondary pollution. There is a pressing need for a technology capable of both reducing and oxidizing CPs for their removal. For this research, we utilized commercially accessible organic polymer fluorinated ethylene propylene (FEP) as a catalyst, activated through ultrasound to kickstart a contact-electro-catalysis process to degrade pentachlorophenol (PCP). A proposed mechanism is presented for the reduction and oxidative breakdown of PCP relying on contact electrification-induced electron transfer that creates reactive species. Experimental findings demonstrate that PCP can be completely degraded with only 1.0 mg of FEP. Experiments on identifying and quenching reactive oxygen species indicate that •O2−, •OH, and 1O2 play a role in the degradation process. The degradation of PCP involves four pathways: direct dechlorination, hydroxylation dechlorination, oxidation, and polymerization. Toxicity assessment reveals that the dechlorination process notably decreases the toxicity of intermediates. Furthermore, characterization and cycling experiments demonstrate the outstanding stability and recyclability of FEP, making it suitable for real environmental water applications. Ultrasound-driven contact-electro-catalysis system offers a straightforward, economical, and eco-friendly approach to degrade PCP. It offers valuable insights for potentially treating stubborn CPs effectively.
{"title":"Contact-Electro-Catalysis for the Degradation of Pentachlorophenol Using Inert Fluorinated Ethylene Propylene Powders","authors":"Keyi Li, Yue Lai, Senpei Lin, Lihua Zhou, Minghao He, Huayue Lin, Yong Yuan","doi":"10.1021/acsestengg.4c00284","DOIUrl":"https://doi.org/10.1021/acsestengg.4c00284","url":null,"abstract":"Chlorophenols (CPs) pose significant risks to human health due to their toxicity and carcinogenic properties. The direct oxidative breakdown of CPs can produce even more harmful byproducts, resulting in secondary pollution. There is a pressing need for a technology capable of both reducing and oxidizing CPs for their removal. For this research, we utilized commercially accessible organic polymer fluorinated ethylene propylene (FEP) as a catalyst, activated through ultrasound to kickstart a contact-electro-catalysis process to degrade pentachlorophenol (PCP). A proposed mechanism is presented for the reduction and oxidative breakdown of PCP relying on contact electrification-induced electron transfer that creates reactive species. Experimental findings demonstrate that PCP can be completely degraded with only 1.0 mg of FEP. Experiments on identifying and quenching reactive oxygen species indicate that <sup>•</sup>O<sub>2</sub><sup>−</sup>, <sup>•</sup>OH, and <sup>1</sup>O<sub>2</sub> play a role in the degradation process. The degradation of PCP involves four pathways: direct dechlorination, hydroxylation dechlorination, oxidation, and polymerization. Toxicity assessment reveals that the dechlorination process notably decreases the toxicity of intermediates. Furthermore, characterization and cycling experiments demonstrate the outstanding stability and recyclability of FEP, making it suitable for real environmental water applications. Ultrasound-driven contact-electro-catalysis system offers a straightforward, economical, and eco-friendly approach to degrade PCP. It offers valuable insights for potentially treating stubborn CPs effectively.","PeriodicalId":7008,"journal":{"name":"ACS ES&T engineering","volume":null,"pages":null},"PeriodicalIF":7.1,"publicationDate":"2024-07-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141774971","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2024-07-21DOI: 10.1021/acsestengg.4c00295
Saurabh N. Misal, Donglin Li, Sangil Kim, Brian P. Chaplin
This study investigated the material and ion transport properties of TiO2 nanopores as a function of solution conditions and applied electrode potentials. Zeta potential measurements revealed that the TiO2 surface charge was highly dependent on solution conditions, which was attributed to protonation/deprotonation of surface functional groups and adsorption of ions. Ion rejection followed the absolute magnitude of the membrane surface charge and was pH-dependent, reflecting the amphoteric nature of TiO2. The rejection of NaCl was approximately symmetrical about the point of zero charge of the membrane, with the highest rejection at acidic and basic conditions. Specific adsorption of SO42– and Mg2+ under acidic and basic conditions, respectively, neutralized the membrane charge and significantly reduced ion rejection. A mathematical transport model was fit to experimental data, and the model-determined membrane charge densities as a function of solution conditions agreed with experimental zeta potential measurements. Model results also revealed that rejection was primarily attributed to the Donnan exclusion mechanism. The application of both anodic and cathodic potentials directly to the TiO2 membrane caused permselective transport under specific solution conditions.
{"title":"Effect of Solution Conditions and Applied Potential on Ion Transport in TiO2 Nanopores","authors":"Saurabh N. Misal, Donglin Li, Sangil Kim, Brian P. Chaplin","doi":"10.1021/acsestengg.4c00295","DOIUrl":"https://doi.org/10.1021/acsestengg.4c00295","url":null,"abstract":"This study investigated the material and ion transport properties of TiO<sub>2</sub> nanopores as a function of solution conditions and applied electrode potentials. Zeta potential measurements revealed that the TiO<sub>2</sub> surface charge was highly dependent on solution conditions, which was attributed to protonation/deprotonation of surface functional groups and adsorption of ions. Ion rejection followed the absolute magnitude of the membrane surface charge and was pH-dependent, reflecting the amphoteric nature of TiO<sub>2</sub>. The rejection of NaCl was approximately symmetrical about the point of zero charge of the membrane, with the highest rejection at acidic and basic conditions. Specific adsorption of SO<sub>4</sub><sup>2–</sup> and Mg<sup>2+</sup> under acidic and basic conditions, respectively, neutralized the membrane charge and significantly reduced ion rejection. A mathematical transport model was fit to experimental data, and the model-determined membrane charge densities as a function of solution conditions agreed with experimental zeta potential measurements. Model results also revealed that rejection was primarily attributed to the Donnan exclusion mechanism. The application of both anodic and cathodic potentials directly to the TiO<sub>2</sub> membrane caused permselective transport under specific solution conditions.","PeriodicalId":7008,"journal":{"name":"ACS ES&T engineering","volume":null,"pages":null},"PeriodicalIF":7.1,"publicationDate":"2024-07-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141745683","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
With the sharp increase in electronic and electrical equipment as well as concomitant electronic waste, it is imperative to recover precious metals from secondary resources from the perspective of environment protection and sustainable development. Herein, a free-standing, dual-cross-linking polydopamine (PDA) in conjunction with poly(imide dioxime) (PIDO) porous membrane (denoted as PDA/PIDO) is fabricated via a facile interfacial polymerization method for gold recovery. As expected, the constructed PDA/PIDO membrane features a hierarchical porous structure, ample active sites, and excellent hydrophilicity, endowing it with an ultrahigh gold capture capacity (3368 mg g–1), fast equilibrium time (35 min), superior recovery selectivity (separation factor of Au/Cu = 5.4 × 105, Au/Ni = 3.9 × 105), high flux (1050 L m2 h–1), and high retention rate (98%). Furthermore, the proposed PDA/PIDO membrane is also competent for selective gold recovery from the central processing unit leachate with remarkable efficiency in a continuous-flowing filtration system, highlighting its huge potential in practical large-scale gold recovery from e-waste.
{"title":"Dual-Crosslinking Polydopamine/Poly(imide dioxime) Porous Network Membrane Enables Efficient and Selective Gold Recovery from e-Waste","authors":"Xueqin Zhang, Huaimeng Li, Zhenzhen Liu, Zhen Fu, Haimin Zhang, Guozhong Wang, Yunxia Zhang","doi":"10.1021/acsestengg.4c00263","DOIUrl":"https://doi.org/10.1021/acsestengg.4c00263","url":null,"abstract":"With the sharp increase in electronic and electrical equipment as well as concomitant electronic waste, it is imperative to recover precious metals from secondary resources from the perspective of environment protection and sustainable development. Herein, a free-standing, dual-cross-linking polydopamine (PDA) in conjunction with poly(imide dioxime) (PIDO) porous membrane (denoted as PDA/PIDO) is fabricated via a facile interfacial polymerization method for gold recovery. As expected, the constructed PDA/PIDO membrane features a hierarchical porous structure, ample active sites, and excellent hydrophilicity, endowing it with an ultrahigh gold capture capacity (3368 mg g<sup>–1</sup>), fast equilibrium time (35 min), superior recovery selectivity (separation factor of Au/Cu = 5.4 × 10<sup>5</sup>, Au/Ni = 3.9 × 10<sup>5</sup>), high flux (1050 L m<sup>2</sup> h<sup>–1</sup>), and high retention rate (98%). Furthermore, the proposed PDA/PIDO membrane is also competent for selective gold recovery from the central processing unit leachate with remarkable efficiency in a continuous-flowing filtration system, highlighting its huge potential in practical large-scale gold recovery from e-waste.","PeriodicalId":7008,"journal":{"name":"ACS ES&T engineering","volume":null,"pages":null},"PeriodicalIF":7.1,"publicationDate":"2024-07-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141745681","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Recent progress has brought carbon-confined transition metal catalysts to the forefront as effective agents for Fenton-like reactions. However, achieving a stable integration of densely loaded and well-dispersed transition metals onto carbon support poses significant challenges. Herein, we introduce a plant polyphenol-driven polymerization-confinement method for the synthesis of a highly dispersed FeCo bimetallic catalyst (FeCo@NGB). Utilizing the chelating effect of tea polyphenols with metal ions and their subsequent polymerization and confinement offers a durable solution for stabilizing the FeCo bimetallic sites. The resulting FeCo@NGB demonstrates exceptional performance in activating peroxymonosulfate (PMS) for the swift degradation of tetracycline (TC), with a 99.5% reduction achieved in just 30 min, predominantly through a singlet oxygen (1O2)-driven pathway. Experimental and theoretical calculations highlight the pivotal role of atomically dispersed FeN4–CoN3 sites in facilitating rapid electron transfer between the catalyst and PMS, thereby enhancing 1O2 production. This work not only advances the development of high-performance multiphase catalysts but also introduces a compelling strategy for water purification leveraging nonradical oxidative pathways.
{"title":"Plant Polyphenol-Driven Polymerization-Confinement Strategy toward Ultrahighly Loaded Atomically Dispersed FeCo Bimetallic Catalysts for Singlet Oxygen-Dominated Fenton-like Reactions","authors":"Yue Wang, Zhenglong Liu, Weilu Kang, Tielong Li* and Haitao Wang*, ","doi":"10.1021/acsestengg.4c0023710.1021/acsestengg.4c00237","DOIUrl":"https://doi.org/10.1021/acsestengg.4c00237https://doi.org/10.1021/acsestengg.4c00237","url":null,"abstract":"<p >Recent progress has brought carbon-confined transition metal catalysts to the forefront as effective agents for Fenton-like reactions. However, achieving a stable integration of densely loaded and well-dispersed transition metals onto carbon support poses significant challenges. Herein, we introduce a plant polyphenol-driven polymerization-confinement method for the synthesis of a highly dispersed FeCo bimetallic catalyst (FeCo@NGB). Utilizing the chelating effect of tea polyphenols with metal ions and their subsequent polymerization and confinement offers a durable solution for stabilizing the FeCo bimetallic sites. The resulting FeCo@NGB demonstrates exceptional performance in activating peroxymonosulfate (PMS) for the swift degradation of tetracycline (TC), with a 99.5% reduction achieved in just 30 min, predominantly through a singlet oxygen (<sup>1</sup>O<sub>2</sub>)-driven pathway. Experimental and theoretical calculations highlight the pivotal role of atomically dispersed FeN<sub>4</sub>–CoN<sub>3</sub> sites in facilitating rapid electron transfer between the catalyst and PMS, thereby enhancing <sup>1</sup>O<sub>2</sub> production. This work not only advances the development of high-performance multiphase catalysts but also introduces a compelling strategy for water purification leveraging nonradical oxidative pathways.</p>","PeriodicalId":7008,"journal":{"name":"ACS ES&T engineering","volume":null,"pages":null},"PeriodicalIF":7.4,"publicationDate":"2024-07-18","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142228021","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2024-07-18DOI: 10.1021/acsestengg.4c00237
Yue Wang, Zhenglong Liu, Weilu Kang, Tielong Li, Haitao Wang
Recent progress has brought carbon-confined transition metal catalysts to the forefront as effective agents for Fenton-like reactions. However, achieving a stable integration of densely loaded and well-dispersed transition metals onto carbon support poses significant challenges. Herein, we introduce a plant polyphenol-driven polymerization-confinement method for the synthesis of a highly dispersed FeCo bimetallic catalyst (FeCo@NGB). Utilizing the chelating effect of tea polyphenols with metal ions and their subsequent polymerization and confinement offers a durable solution for stabilizing the FeCo bimetallic sites. The resulting FeCo@NGB demonstrates exceptional performance in activating peroxymonosulfate (PMS) for the swift degradation of tetracycline (TC), with a 99.5% reduction achieved in just 30 min, predominantly through a singlet oxygen (1O2)-driven pathway. Experimental and theoretical calculations highlight the pivotal role of atomically dispersed FeN4–CoN3 sites in facilitating rapid electron transfer between the catalyst and PMS, thereby enhancing 1O2 production. This work not only advances the development of high-performance multiphase catalysts but also introduces a compelling strategy for water purification leveraging nonradical oxidative pathways.
{"title":"Plant Polyphenol-Driven Polymerization-Confinement Strategy toward Ultrahighly Loaded Atomically Dispersed FeCo Bimetallic Catalysts for Singlet Oxygen-Dominated Fenton-like Reactions","authors":"Yue Wang, Zhenglong Liu, Weilu Kang, Tielong Li, Haitao Wang","doi":"10.1021/acsestengg.4c00237","DOIUrl":"https://doi.org/10.1021/acsestengg.4c00237","url":null,"abstract":"Recent progress has brought carbon-confined transition metal catalysts to the forefront as effective agents for Fenton-like reactions. However, achieving a stable integration of densely loaded and well-dispersed transition metals onto carbon support poses significant challenges. Herein, we introduce a plant polyphenol-driven polymerization-confinement method for the synthesis of a highly dispersed FeCo bimetallic catalyst (FeCo@NGB). Utilizing the chelating effect of tea polyphenols with metal ions and their subsequent polymerization and confinement offers a durable solution for stabilizing the FeCo bimetallic sites. The resulting FeCo@NGB demonstrates exceptional performance in activating peroxymonosulfate (PMS) for the swift degradation of tetracycline (TC), with a 99.5% reduction achieved in just 30 min, predominantly through a singlet oxygen (<sup>1</sup>O<sub>2</sub>)-driven pathway. Experimental and theoretical calculations highlight the pivotal role of atomically dispersed FeN<sub>4</sub>–CoN<sub>3</sub> sites in facilitating rapid electron transfer between the catalyst and PMS, thereby enhancing <sup>1</sup>O<sub>2</sub> production. This work not only advances the development of high-performance multiphase catalysts but also introduces a compelling strategy for water purification leveraging nonradical oxidative pathways.","PeriodicalId":7008,"journal":{"name":"ACS ES&T engineering","volume":null,"pages":null},"PeriodicalIF":7.1,"publicationDate":"2024-07-18","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141745682","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2024-07-18DOI: 10.1021/acsestengg.4c00111
Qi Liu, Xiaoqi Zhu, Baoliang Chen, Xiaoying Zhu
Atomic force microscopy (AFM), as a type of scanning probe microscopy (SPM), possesses formidable capabilities for nanoscale imaging and force spectroscopy. Due to its advantages such as high resolution, nondestructive detection, minimal environmental restrictions, strong versatility, and real-time in situ analysis, AFM has become an indispensable tool in surface science and materials research, finding extensive applications in the study of the membrane separation and fouling processes. The tremendous advantages of AFM in characterization applications stem from its diverse tip functionalization techniques. This review encompasses the preparation of AFM probe tips and the modification techniques of special tips, including carbon nanotube (CNT) probes, metal nanowire probes, colloidal probes, and single-cell/molecule probes. Furthermore, it highlights the applications and advancements of AFM and probe modification techniques in membrane technology research. With the continuous development of tip modification techniques, the analytical capabilities of AFM will be further expanded, promising broader prospects for its application in the study of membrane fouling mechanisms and the development of antifouling membrane materials.
{"title":"Applications of AFM in Membrane Characterization and Fouling Analysis","authors":"Qi Liu, Xiaoqi Zhu, Baoliang Chen, Xiaoying Zhu","doi":"10.1021/acsestengg.4c00111","DOIUrl":"https://doi.org/10.1021/acsestengg.4c00111","url":null,"abstract":"Atomic force microscopy (AFM), as a type of scanning probe microscopy (SPM), possesses formidable capabilities for nanoscale imaging and force spectroscopy. Due to its advantages such as high resolution, nondestructive detection, minimal environmental restrictions, strong versatility, and real-time in situ analysis, AFM has become an indispensable tool in surface science and materials research, finding extensive applications in the study of the membrane separation and fouling processes. The tremendous advantages of AFM in characterization applications stem from its diverse tip functionalization techniques. This review encompasses the preparation of AFM probe tips and the modification techniques of special tips, including carbon nanotube (CNT) probes, metal nanowire probes, colloidal probes, and single-cell/molecule probes. Furthermore, it highlights the applications and advancements of AFM and probe modification techniques in membrane technology research. With the continuous development of tip modification techniques, the analytical capabilities of AFM will be further expanded, promising broader prospects for its application in the study of membrane fouling mechanisms and the development of antifouling membrane materials.","PeriodicalId":7008,"journal":{"name":"ACS ES&T engineering","volume":null,"pages":null},"PeriodicalIF":7.1,"publicationDate":"2024-07-18","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141737372","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2024-07-18DOI: 10.1021/acsestengg.4c0011110.1021/acsestengg.4c00111
Qi Liu, Xiaoqi Zhu, Baoliang Chen and Xiaoying Zhu*,
Atomic force microscopy (AFM), as a type of scanning probe microscopy (SPM), possesses formidable capabilities for nanoscale imaging and force spectroscopy. Due to its advantages such as high resolution, nondestructive detection, minimal environmental restrictions, strong versatility, and real-time in situ analysis, AFM has become an indispensable tool in surface science and materials research, finding extensive applications in the study of the membrane separation and fouling processes. The tremendous advantages of AFM in characterization applications stem from its diverse tip functionalization techniques. This review encompasses the preparation of AFM probe tips and the modification techniques of special tips, including carbon nanotube (CNT) probes, metal nanowire probes, colloidal probes, and single-cell/molecule probes. Furthermore, it highlights the applications and advancements of AFM and probe modification techniques in membrane technology research. With the continuous development of tip modification techniques, the analytical capabilities of AFM will be further expanded, promising broader prospects for its application in the study of membrane fouling mechanisms and the development of antifouling membrane materials.
{"title":"Applications of AFM in Membrane Characterization and Fouling Analysis","authors":"Qi Liu, Xiaoqi Zhu, Baoliang Chen and Xiaoying Zhu*, ","doi":"10.1021/acsestengg.4c0011110.1021/acsestengg.4c00111","DOIUrl":"https://doi.org/10.1021/acsestengg.4c00111https://doi.org/10.1021/acsestengg.4c00111","url":null,"abstract":"<p >Atomic force microscopy (AFM), as a type of scanning probe microscopy (SPM), possesses formidable capabilities for nanoscale imaging and force spectroscopy. Due to its advantages such as high resolution, nondestructive detection, minimal environmental restrictions, strong versatility, and real-time in situ analysis, AFM has become an indispensable tool in surface science and materials research, finding extensive applications in the study of the membrane separation and fouling processes. The tremendous advantages of AFM in characterization applications stem from its diverse tip functionalization techniques. This review encompasses the preparation of AFM probe tips and the modification techniques of special tips, including carbon nanotube (CNT) probes, metal nanowire probes, colloidal probes, and single-cell/molecule probes. Furthermore, it highlights the applications and advancements of AFM and probe modification techniques in membrane technology research. With the continuous development of tip modification techniques, the analytical capabilities of AFM will be further expanded, promising broader prospects for its application in the study of membrane fouling mechanisms and the development of antifouling membrane materials.</p>","PeriodicalId":7008,"journal":{"name":"ACS ES&T engineering","volume":null,"pages":null},"PeriodicalIF":7.4,"publicationDate":"2024-07-18","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141957685","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2024-07-17DOI: 10.1021/acsestengg.4c00142
Sung Il Yu, Junbeom Jeon, Yong-Uk Shin, Hyokwan Bae
Flow-electrode capacitive deionization (FCDI) has created a breakthrough toward a more stable desalination performance by adopting a flow-electrode compared to existing capacitive deionization and membrane capacitive deionization as a promising electrochemical water treatment technology. However, the FCDI technology requires investigation of various mechanisms pertaining to flow-electrode materials to achieve system optimization. Further, studies on applying machine learning to the FCDI technology have been scarcely reported. Our study aims to explore optimal algorithms via machine learning for predicting the salt adsorption capacity of FCDI processes and evaluate the feasibility of optimization applications. Concurrently, a comparative analysis was conducted through the performance model indicators of mean absolute error (MAE), mean squared error, and R2 for support vector machine, random forest, and artificial neural network (ANN) algorithms. Herein, we demonstrated that the optimal ANN-based model exhibited the highest predictive performance, achieving R2 and MAE values of 0.996 and 0.21 mg/g, respectively. Additionally, the Shapley additive explanations (SHAP) confirmed a trend in the contribution of influent concentration, aligning closely with the results of statistical analysis. Specifically, the change in voltage of the FCDI process serves as a key factor in determining salt adsorption efficiency. Moreover, a parallel comparison of the Pearson correlation coefficient and SHAP analyses suggests that the impact of voltage entails a nonlinear contribution within the realm of machine learning. Finally, to deploy a machine learning-driven ANN model system, we present multiple factors (e.g., weight of flow-electrodes, influent concentration, and voltages) as a reinforcement learning model for decision-making. This offers valuable insights and guidance for future operations of the FCDI process.
{"title":"Optimal Management Strategy for Salt Adsorption Capacity in Machine Learning-Based Flow-Electrode Capacitive Deionization Process","authors":"Sung Il Yu, Junbeom Jeon, Yong-Uk Shin, Hyokwan Bae","doi":"10.1021/acsestengg.4c00142","DOIUrl":"https://doi.org/10.1021/acsestengg.4c00142","url":null,"abstract":"Flow-electrode capacitive deionization (FCDI) has created a breakthrough toward a more stable desalination performance by adopting a flow-electrode compared to existing capacitive deionization and membrane capacitive deionization as a promising electrochemical water treatment technology. However, the FCDI technology requires investigation of various mechanisms pertaining to flow-electrode materials to achieve system optimization. Further, studies on applying machine learning to the FCDI technology have been scarcely reported. Our study aims to explore optimal algorithms via machine learning for predicting the salt adsorption capacity of FCDI processes and evaluate the feasibility of optimization applications. Concurrently, a comparative analysis was conducted through the performance model indicators of mean absolute error (MAE), mean squared error, and <i>R</i><sup>2</sup> for support vector machine, random forest, and artificial neural network (ANN) algorithms. Herein, we demonstrated that the optimal ANN-based model exhibited the highest predictive performance, achieving <i>R</i><sup>2</sup> and MAE values of 0.996 and 0.21 mg/g, respectively. Additionally, the Shapley additive explanations (SHAP) confirmed a trend in the contribution of influent concentration, aligning closely with the results of statistical analysis. Specifically, the change in voltage of the FCDI process serves as a key factor in determining salt adsorption efficiency. Moreover, a parallel comparison of the Pearson correlation coefficient and SHAP analyses suggests that the impact of voltage entails a nonlinear contribution within the realm of machine learning. Finally, to deploy a machine learning-driven ANN model system, we present multiple factors (e.g., weight of flow-electrodes, influent concentration, and voltages) as a reinforcement learning model for decision-making. This offers valuable insights and guidance for future operations of the FCDI process.","PeriodicalId":7008,"journal":{"name":"ACS ES&T engineering","volume":null,"pages":null},"PeriodicalIF":7.1,"publicationDate":"2024-07-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141737374","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}