Pub Date : 2024-11-21DOI: 10.1016/j.cej.2024.157863
Kui Chen, Peng Zhao, Jingjing Chen, Chengtao Yang, Bin Tang
The rapid advancement of electronic technology has increased power consumption in integrated circuits, presenting significant challenges for efficient cooling. BaTiO3 (BT)-based ceramics offer promising electrocaloric (EC) cooling, providing a compact, efficient alternative to bulky, environmentally harmful vapor compression refrigeration, though temperature span (Tspan) and phase transitions limit their current practicality. This study explores a novel (0.5-x)Ba0.72Sr0.28TiO3-0.5BaTi0.8Sn0.2O3-xBa0.72Ca0.28TiO3 [(0.5-x)BST-BTS-xBCT] ceramic system, leveraging phase boundary engineering to achieve continuous and broad phase transitions. By optimizing grain size and enhancing the breakdown electric field (Eb) through a density adjustment strategy, the 0.2BCT ceramics demonstrated excellent EC performance at 38 °C, with a ΔT of 2.71 K and a Tspan of 49.1 °C. These findings establish (0.5-x)BST-BTS-xBCT ceramics as a promising lead-free material for EC applications with significant potential for improving microelectronic cooling solutions.
{"title":"Broad temperature span and large electrocaloric effect in lead-free ceramics via multi-strategy synergistic optimization","authors":"Kui Chen, Peng Zhao, Jingjing Chen, Chengtao Yang, Bin Tang","doi":"10.1016/j.cej.2024.157863","DOIUrl":"https://doi.org/10.1016/j.cej.2024.157863","url":null,"abstract":"The rapid advancement of electronic technology has increased power consumption in integrated circuits, presenting significant challenges for efficient cooling. BaTiO<sub>3</sub> (BT)-based ceramics offer promising electrocaloric (EC) cooling, providing a compact, efficient alternative to bulky, environmentally harmful vapor compression refrigeration, though temperature span (<em>T</em><sub>span</sub>) and phase transitions limit their current practicality. This study explores a novel (0.5-<em>x</em>)Ba<sub>0.72</sub>Sr<sub>0.28</sub>TiO<sub>3</sub>-0.5BaTi<sub>0.8</sub>Sn<sub>0.2</sub>O<sub>3</sub>-<em>x</em>Ba<sub>0.72</sub>Ca<sub>0.28</sub>TiO<sub>3</sub> [(0.5-<em>x</em>)BST-BTS-<em>x</em>BCT] ceramic system, leveraging phase boundary engineering to achieve continuous and broad phase transitions. By optimizing grain size and enhancing the breakdown electric field (<em>E</em><sub>b</sub>) through a density adjustment strategy, the 0.2BCT ceramics demonstrated excellent EC performance at 38 °C, with a Δ<em>T</em> of 2.71 K and a <em>T</em><sub>span</sub> of 49.1 °C. These findings establish (0.5-<em>x</em>)BST-BTS-<em>x</em>BCT ceramics as a promising lead-free material for EC applications with significant potential for improving microelectronic cooling solutions.","PeriodicalId":270,"journal":{"name":"Chemical Engineering Journal","volume":"14 1","pages":""},"PeriodicalIF":15.1,"publicationDate":"2024-11-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142679025","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"工程技术","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2024-11-21DOI: 10.1016/j.cej.2024.157860
Bo Han, Can Chen, Shuai Li, Ling Ran, Jie Li, Zhong Zou, Yongming Chen, Hongliang Zhang
The extraction performance of acid phosphate ester extractants (PEEs) decreases significantly as the acidity of the aqueous phase increases. Therefore, finding PEEs suitable for high-acid environments has become critical to addressing their performance attenuation. However, the unclear structure-performance relationship of PEEs has led to a lack of guidance in experimental synthesis, significantly impeding the emergence of new acid-resistant PEEs. To tackle these issues, ten novel phenyl phosphate ester extractants were designed based on the molecular formula of phosphodiester (R1R2P(=O)OH) and the conjugation effect of the benzene ring. The relationship between the intrinsic extraction performance of acid PEEs and substituent groups (phenoxy, alkoxy, and alkyl) was quantitatively established by calculating the Gibbs free energy changes of three primary reactions (dimer dissociation, monomer acid ionization, and metal coordination) during divalent cobalt ion extraction. Additionally, the impact of different substitution sites (para, meta, and ortho) of the benzene ring on the extraction performance of acid PEEs was studied. The results indicated that introducing phenoxy groups into traditional acid PEEs (P204 and P507) can effectively enhance the extractants’ acid ionization ability and thermodynamic driving force. The extraction performance of acid PEEs is positively correlated with the number of phenoxy groups, and carbon chain substitution at the meta-position of the benzene ring is the most advantageous. By screening five low-toxicity and low-cost phenolic hydroxyl reagents currently available on the market, design a phenyl phosphate ester extractant ([(CH3)3CCH2C(CH3)2C6H4O]2P(=O)OH, P-4TO) that combines cost and performance advantages. Furthermore, the transition state theory was used to confirm the feasibility of preparing/P-4(−|-)TO, which provided a comprehensive theoretical research method for the future design and synthesis of efficient PEEs.
{"title":"Structure-performance relationship and molecular structure optimization design of acid phosphate ester extractants","authors":"Bo Han, Can Chen, Shuai Li, Ling Ran, Jie Li, Zhong Zou, Yongming Chen, Hongliang Zhang","doi":"10.1016/j.cej.2024.157860","DOIUrl":"https://doi.org/10.1016/j.cej.2024.157860","url":null,"abstract":"The extraction performance of acid phosphate ester extractants (PEEs) decreases significantly as the acidity of the aqueous phase increases. Therefore, finding PEEs suitable for high-acid environments has become critical to addressing their performance attenuation. However, the unclear structure-performance relationship of PEEs has led to a lack of guidance in experimental synthesis, significantly impeding the emergence of new acid-resistant PEEs. To tackle these issues, ten novel phenyl phosphate ester extractants were designed based on the molecular formula of phosphodiester (R<sub>1</sub>R<sub>2</sub>P(=O)OH) and the conjugation effect of the benzene ring. The relationship between the intrinsic extraction performance of acid PEEs and substituent groups (phenoxy, alkoxy, and alkyl) was quantitatively established by calculating the Gibbs free energy changes of three primary reactions (dimer dissociation, monomer acid ionization, and metal coordination) during divalent cobalt ion extraction. Additionally, the impact of different substitution sites (para, meta, and ortho) of the benzene ring on the extraction performance of acid PEEs was studied. The results indicated that introducing phenoxy groups into traditional acid PEEs (P204 and P507) can effectively enhance the extractants’ acid ionization ability and thermodynamic driving force. The extraction performance of acid PEEs is positively correlated with the number of phenoxy groups, and carbon chain substitution at the <em>meta</em>-position of the benzene ring is the most advantageous. By screening five low-toxicity and low-cost phenolic hydroxyl reagents currently available on the market, design a phenyl phosphate ester extractant ([(CH<sub>3</sub>)<sub>3</sub>CCH<sub>2</sub>C(CH<sub>3</sub>)<sub>2</sub>C<sub>6</sub>H<sub>4</sub>O]<sub>2</sub>P(=O)OH, P-4TO) that combines cost and performance advantages. Furthermore, the transition state theory was used to confirm the feasibility of preparing/P<sup>-4</sup>(−|-)TO, which provided a comprehensive theoretical research method for the future design and synthesis of efficient PEEs.","PeriodicalId":270,"journal":{"name":"Chemical Engineering Journal","volume":"1 1","pages":""},"PeriodicalIF":15.1,"publicationDate":"2024-11-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142679081","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"工程技术","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2024-11-21DOI: 10.1016/j.cej.2024.157488
Li Yue Jing, Yang kai Fan, Bo Zhi Chen, De hui Li, Yu Ting He, Guo Liang Zhang, Ling Liang, Jie Du, Yuan Wang, Xin Dong Guo
Cortisol, known as the ’stress hormone’, plays a crucial role in the regulation of metabolism, the promotion of secondary sex characteristics, and the maintenance of normal biological functions. A conductive microneedle (MN)-based electrochemical biosensor modified with dendritic Au nanoparticles (AuNPs) was developed for real-time monitoring of cortisol levels in interstitial fluid (ISF) to address the current challenges of time-consuming and laborious cortisol detection. The dendritic AuNPs provide signal amplification due to their high surface area and abundance of active sites, and the amine group modification of the cortisol aptamer facilitates its connection to an Au MN electrode with surface-modified dendritic AuNPs. Through parameters optimization and utilization of differential pulse voltammetry (DPV), the MN biosensor exhibits a wide detection range (1–1000 nM) covering normal human cortisol levels. Notably, it demonstrates low computational detection limits of 0.17 nM and 0.22 nM in phosphate buffered saline (PBS) and simulated ISF respectively, along with exceptional stability, selectivity, and repeatability. Furthermore, the successful detection of cortisol in the healthy volunteers’ ISF reveals a significant circadian rhythm and a correlation between cortisol levels in the ISF and blood. Together these findings indicate the promise of aptamer-integrated microneedle biosensors for facilitating simple, sensitive, and disposable cortisol assays.
{"title":"An aptamer-integrated conductive microneedle biosensor for real-time transdermal cortisol monitoring","authors":"Li Yue Jing, Yang kai Fan, Bo Zhi Chen, De hui Li, Yu Ting He, Guo Liang Zhang, Ling Liang, Jie Du, Yuan Wang, Xin Dong Guo","doi":"10.1016/j.cej.2024.157488","DOIUrl":"https://doi.org/10.1016/j.cej.2024.157488","url":null,"abstract":"Cortisol, known as the ’stress hormone’, plays a crucial role in the regulation of metabolism, the promotion of secondary sex characteristics, and the maintenance of normal biological functions. A conductive microneedle (MN)-based electrochemical biosensor modified with dendritic Au nanoparticles (AuNPs) was developed for real-time monitoring of cortisol levels in interstitial fluid (ISF) to address the current challenges of time-consuming and laborious cortisol detection. The dendritic AuNPs provide signal amplification due to their high surface area and abundance of active sites, and the amine group modification of the cortisol aptamer facilitates its connection to an Au MN electrode with surface-modified dendritic AuNPs. Through parameters optimization and utilization of differential pulse voltammetry (DPV), the MN biosensor exhibits a wide detection range (1–1000 nM) covering normal human cortisol levels. Notably, it demonstrates low computational detection limits of 0.17 nM and 0.22 nM in phosphate buffered saline (PBS) and simulated ISF respectively, along with exceptional stability, selectivity, and repeatability. Furthermore, the successful detection of cortisol in the healthy volunteers’ ISF reveals a significant circadian rhythm and a correlation between cortisol levels in the ISF and blood. Together these findings indicate the promise of aptamer-integrated microneedle biosensors for facilitating simple, sensitive, and disposable cortisol assays.","PeriodicalId":270,"journal":{"name":"Chemical Engineering Journal","volume":"179 1","pages":""},"PeriodicalIF":15.1,"publicationDate":"2024-11-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142678709","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"工程技术","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2024-11-21DOI: 10.1016/j.cej.2024.157837
Yimeng Cai, Pochun Lin, Yuhan Li, Linfeng Liu, Shuqin Cao, Bin Zhao, Yueying Wang, Wei Song, Qian Wang, Xinyan Gan, Ke Xu, Qingheng Wu, Yuan Wang, Leixiao Yu, Quan Yuan
Healing of chronic wounds such as diabetic foot ulcers is a critical clinical challenge due to the failure management of excess exudates, persistent inflammatory responses, and vascular microcirculatory disturbances by most traditional wound dressings. To promote the wound healing under diabetic pathological environment, a supramolecular network, polyethyleneimine/polyacrylic acid/alpha-ketoglutarate (PEI/PAA/αKG) with bioactive and metabolic αKG was developed herein for exudates management and vascular microcirculatory reconstruction. Once deposited onto the wound area, the PEI/PAA/αKG supramolecular powder would quickly adsorb the exudates and in-situ gel to form a robust protective barrier for sustainably managing the wound exudates during the healing process. Owing to the reversible H-bonding and electrostatic interactions in the network, bioactive αKG monomer could responsively dissociate from the supramolecular network in a pH-dependent manner to promote the chronic diabetic wound healing. The collagen deposition, soft tissue regeneration, and neovascularization of the healing wound were all obviously enhanced under the mediation of PEI/PAA/αKG supramolecular hydrogel. It was further confirmed that the outstanding effect of PEI/PAA/αKG on angiogenesis under diabetic condition results from the function of αKG on cellular oxidative stress regulation. The present method of materializing therapeutic molecules provides a potential strategy to solve the problem of metabolic molecules in biomedical application.
{"title":"Alpha-ketoglutarate supramolecular network accelerates diabetic wound healing through exudates management and neovascularization","authors":"Yimeng Cai, Pochun Lin, Yuhan Li, Linfeng Liu, Shuqin Cao, Bin Zhao, Yueying Wang, Wei Song, Qian Wang, Xinyan Gan, Ke Xu, Qingheng Wu, Yuan Wang, Leixiao Yu, Quan Yuan","doi":"10.1016/j.cej.2024.157837","DOIUrl":"https://doi.org/10.1016/j.cej.2024.157837","url":null,"abstract":"Healing of chronic wounds such as diabetic foot ulcers is a critical clinical challenge due to the failure management of excess exudates, persistent inflammatory responses, and vascular microcirculatory disturbances by most traditional wound dressings. To promote the wound healing under diabetic pathological environment, a supramolecular network, polyethyleneimine/polyacrylic acid/alpha-ketoglutarate (PEI/PAA/αKG) with bioactive and metabolic αKG was developed herein for exudates management and vascular microcirculatory reconstruction. Once deposited onto the wound area, the PEI/PAA/αKG supramolecular powder would quickly adsorb the exudates and in-situ gel to form a robust protective barrier for sustainably managing the wound exudates during the healing process. Owing to the reversible H-bonding and electrostatic interactions in the network, bioactive αKG monomer could responsively dissociate from the supramolecular network in a pH-dependent manner to promote the chronic diabetic wound healing. The collagen deposition, soft tissue regeneration, and neovascularization of the healing wound were all obviously enhanced under the mediation of PEI/PAA/αKG supramolecular hydrogel. It was further confirmed that the outstanding effect of PEI/PAA/αKG on angiogenesis under diabetic condition results from the function of αKG on cellular oxidative stress regulation. The present method of materializing therapeutic molecules provides a potential strategy to solve the problem of metabolic molecules in biomedical application.","PeriodicalId":270,"journal":{"name":"Chemical Engineering Journal","volume":"74 1","pages":""},"PeriodicalIF":15.1,"publicationDate":"2024-11-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142679022","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"工程技术","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2024-11-21DOI: 10.1016/j.cej.2024.157858
Eleni D. Salonikidou, Karina Kowalska, Dimitrios A. Giannakoudakis, Antigoni Margellou, Evanthia Nanaki, Spyros Kiartzis, Mariusz Barczak, Piotr Borowski, Konstantinos S. Triantafyllidis
Experimental tests combined with theoretical calculations have yielded new insights into real diesel fuel desulfurization (rDeSulfur) using activated nanoporous carbons. The carbons were selected for their varying physicochemical properties and further were chemically treated to modify their surface chemistry, aiming to investigate the impact of the major physicochemical features on rDeSulfur. The experimental findings demonstrated that both porosity and surface chemistry play complex roles. Specifically, a high degree of graphitization and diverse pore size distributions enhanced adsorptive capabilities, with some carbon samples achieving ultra-deep desulfurization levels (<1 ppmwS). Theoretical calculations indicated that π-π stacking through dispersion forces was the primary mechanism of adsorption. While surface functionalities at the edges of graphene had minimal impact on interaction strength, structural defects, especially clusters of three quaternary nitrogen atoms or single defected vacancy with OH group, improved interaction energies, boosting adsorption effectiveness compared to pristine graphene. The study concludes that the effectiveness of carbons in diesel desulfurization depends heavily on graphitization levels, defects, and where specific functionalities are located. Lastly, although aromatic compounds in diesel, like benzene, toluene, and naphthalene, compete with thiophenics for adsorption, they have lower interaction energies, suggesting preferential adsorption of sulfur compounds over the aromatics.
{"title":"Merging experimental and theoretical approaches towards understanding real diesel fuel desulfurization by nanoporous carbons","authors":"Eleni D. Salonikidou, Karina Kowalska, Dimitrios A. Giannakoudakis, Antigoni Margellou, Evanthia Nanaki, Spyros Kiartzis, Mariusz Barczak, Piotr Borowski, Konstantinos S. Triantafyllidis","doi":"10.1016/j.cej.2024.157858","DOIUrl":"https://doi.org/10.1016/j.cej.2024.157858","url":null,"abstract":"Experimental tests combined with theoretical calculations have yielded new insights into real diesel fuel desulfurization (rDeSulfur) using activated nanoporous carbons. The carbons were selected for their varying physicochemical properties and further were chemically treated to modify their surface chemistry, aiming to investigate the impact of the major physicochemical features on rDeSulfur. The experimental findings demonstrated that both porosity and surface chemistry play complex roles. Specifically, a high degree of graphitization and diverse pore size distributions enhanced adsorptive capabilities, with some carbon samples achieving ultra-deep desulfurization levels (<1 ppmwS). Theoretical calculations indicated that π-π stacking through dispersion forces was the primary mechanism of adsorption. While surface functionalities at the edges of graphene had minimal impact on interaction strength, structural defects, especially clusters of three quaternary nitrogen atoms or single defected vacancy with OH group, improved interaction energies, boosting adsorption effectiveness compared to pristine graphene. The study concludes that the effectiveness of carbons in diesel desulfurization depends heavily on graphitization levels, defects, and where specific functionalities are located. Lastly, although aromatic compounds in diesel, like benzene, toluene, and naphthalene, compete with thiophenics for adsorption, they have lower interaction energies, suggesting preferential adsorption of sulfur compounds over the aromatics.","PeriodicalId":270,"journal":{"name":"Chemical Engineering Journal","volume":"18 1","pages":""},"PeriodicalIF":15.1,"publicationDate":"2024-11-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142679077","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"工程技术","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2024-11-21DOI: 10.1016/j.cej.2024.157856
Yuzhang Lei, Yating Sun, Yanda Li, Kai Han, Gonggang Liu, Shanshan Chang, Yuan Zhu, Xianjun Li, Yue Liu, Jinbo Hu
Due to low cost, renewability, high porosity and eco-friendliness, wood has been widely used to design solar steam generation devices, displaying great promise for clean water production in desalination and wastewater treatment. However, cleaner preparation processes and efficient structure design of wood based interfacial evaporators still need further exploration and development. Here, we reported an eco-friendly bio-incising method of wood microstructure modulation to fabricate high-performance wood-based solar steam generator by creating multi-level pumping water system. Self-growing Trametes versicolor (TV) which is a kind of bothersome wood fungus was skillfully used to increase porosity of wood and form interweaved mycelia fibers on wood surface, achieving the resegmentation and transmission of water bodies. These water-absorbing cell fibers and porous wood substrate collectively form a multi-level pumping water system ensuring effective heat management and high water evaporation area. Coupling with densely dispersed polydopamine nanoparticles (PDA NPs) on the surface of TV fiber for light absorption enhancement, the designed wood based solar steam generator with a smallest thickness of 1 mm shows outstanding evaporation rate (1.61 kg·m−2·h−1) and solar energy conversion efficiency (98.4 %) under simulated 1 sun irradiation. Moreover, the obtained clean water using as-prepared steam generator shows high removal rates both in simulated seawater and wastewater. This work presents a novel concept and green method for designing high-performance wood-based solar steam generator with multi-level pumping water system.
{"title":"Multi-level pumping water system from bioengineering wood microstructure by self-growing mycelium for boosting photothermal evaporation efficiency","authors":"Yuzhang Lei, Yating Sun, Yanda Li, Kai Han, Gonggang Liu, Shanshan Chang, Yuan Zhu, Xianjun Li, Yue Liu, Jinbo Hu","doi":"10.1016/j.cej.2024.157856","DOIUrl":"https://doi.org/10.1016/j.cej.2024.157856","url":null,"abstract":"Due to low cost, renewability, high porosity and eco-friendliness, wood has been widely used to design solar steam generation devices, displaying great promise for clean water production in desalination and wastewater treatment. However, cleaner preparation processes and efficient structure design of wood based interfacial evaporators still need further exploration and development. Here, we reported an eco-friendly bio-incising method of wood microstructure modulation to fabricate high-performance wood-based solar steam generator by creating multi-level pumping water system. Self-growing <em>Trametes versicolor</em> (TV) which is a kind of bothersome wood fungus was skillfully used to increase porosity of wood and form interweaved mycelia fibers on wood surface, achieving the resegmentation and transmission of water bodies. These water-absorbing cell fibers and porous wood substrate collectively form a multi-level pumping water system ensuring effective heat management and high water evaporation area. Coupling with densely dispersed polydopamine nanoparticles (PDA NPs) on the surface of TV fiber for light absorption enhancement, the designed wood based solar steam generator with a smallest thickness of 1 mm shows outstanding evaporation rate (1.61 kg·m<sup>−2</sup>·h<sup>−1</sup>) and solar energy conversion efficiency (98.4 %) under simulated 1 sun irradiation. Moreover, the obtained clean water using as-prepared steam generator shows high removal rates both in simulated seawater and wastewater. This work presents a novel concept and green method for designing high-performance wood-based solar steam generator with multi-level pumping water system.","PeriodicalId":270,"journal":{"name":"Chemical Engineering Journal","volume":"23 1","pages":""},"PeriodicalIF":15.1,"publicationDate":"2024-11-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142679079","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"工程技术","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2024-11-21DOI: 10.1016/j.cej.2024.157828
Yonglan Yang, Qianyu Cai, Liqiang Wang, Qiongmei Mai, Gang Ye, Jie Liu, Yanan Liu
Antibacterial Photocatalytic Therapy (APCT) is a promising therapeutic strategy for the treatment of bacterial infections, but it faces challenges such as low light utilization efficiency, insufficient reactive oxygen species (ROS) generation, and limited antibacterial efficacy. In this work, a novel Bi2MoO6@sRuO2@HA heterojunction (BMOsRH heterojunction) was constructed to address these limitations. The key innovation of this heterojunction lies in the introduction of sRuO2, which provides an effective charge carrier transfer interface for separated electrons and holes in Bi2MoO6, significantly delaying electron-hole recombination and promoting redox reactions that generate highly toxic ROS, thus enhancing antibacterial effects. Density functional theory (DFT) calculations indicated that BMOsRH possesses photocatalytic activity triply enhanced by near-infrared light absorption, defects, and the heterojunction. Consequently, under the combined action of near-infrared light and hydrogen peroxide, BMOsRH exhibited nearly 100 % antimicrobial activity against Escherichia coli (E. coli) and Methicillin-resistant Staphylococcus aureus (MRSA), and could also disrupt their biofilms. Furthermore, in mouse wound and abscess models of MRSA infection, BMOsRH effectively eliminated bacteria via mild photothermal therapy and significantly downregulated the inflammatory factors IL-1β and TNF-α, promoting rapid wound healing. In summary, this light-controlled therapeutic strategy shows great potential for antibacterial applications.
{"title":"Oxygen-Deficient Bi2MoO6@sRuO2@HA heterojunction for photocatalytic treatment of drug-resistant bacterial infections","authors":"Yonglan Yang, Qianyu Cai, Liqiang Wang, Qiongmei Mai, Gang Ye, Jie Liu, Yanan Liu","doi":"10.1016/j.cej.2024.157828","DOIUrl":"https://doi.org/10.1016/j.cej.2024.157828","url":null,"abstract":"Antibacterial Photocatalytic Therapy (APCT) is a promising therapeutic strategy for the treatment of bacterial infections, but it faces challenges such as low light utilization efficiency, insufficient reactive oxygen species (ROS) generation, and limited antibacterial efficacy. In this work, a novel Bi<sub>2</sub>MoO<sub>6</sub>@sRuO<sub>2</sub>@HA heterojunction (BMOsRH heterojunction) was constructed to address these limitations. The key innovation of this heterojunction lies in the introduction of sRuO<sub>2</sub>, which provides an effective charge carrier transfer interface for separated electrons and holes in Bi<sub>2</sub>MoO<sub>6</sub>, significantly delaying electron-hole recombination and promoting redox reactions that generate highly toxic ROS, thus enhancing antibacterial effects. Density functional theory (DFT) calculations indicated that BMOsRH possesses photocatalytic activity triply enhanced by near-infrared light absorption, defects, and the heterojunction. Consequently, under the combined action of near-infrared light and hydrogen peroxide, BMOsRH exhibited nearly 100 % antimicrobial activity against <em>Escherichia coli (E. coli)</em> and <em>Methicillin-resistant Staphylococcus aureus</em> (<em>MRSA</em>), and could also disrupt their biofilms. Furthermore, in mouse wound and abscess models of <em>MRSA</em> infection, BMOsRH effectively eliminated bacteria via mild photothermal therapy and significantly downregulated the inflammatory factors IL-1<em>β</em> and TNF-<em>α</em>, promoting rapid wound healing. In summary, this light-controlled therapeutic strategy shows great potential for antibacterial applications.","PeriodicalId":270,"journal":{"name":"Chemical Engineering Journal","volume":"110 1","pages":""},"PeriodicalIF":15.1,"publicationDate":"2024-11-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142678710","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"工程技术","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2024-11-21DOI: 10.1016/j.cej.2024.157814
Shalu Atri, Frantisek Zazimal, Sridhar Gowri Sankaran, Zuzana Dyrcikova, Maria Caplovicova, Tomas Roch, Dana Dvoranova, Tomas Homola, Gustav Plesch, Marcello Brigante, Olivier Monfort
In the frame of the environmental issues related to the efficiency of wastewaters treatment, the generation of advanced oxidation processes (AOPs) by 2D materials appears one of the most promising solutions. In this study, a novel catalytic system for peroxymonosulfate activation (PMS) was designed based on MXene (Ti3C2Tx) decorated with spinel oxides Co3O4, Fe3O4 and CoFe2O4 catalysts. Their efficiency in caffeine (CAF) degradation via PMS activation was assessed. The insertion of spinel oxides inside the multilayer structure of MXene along with their uniform surface decoration was demonstrated by SEM and TEM analyses and it also avoided the aggregation of the magnetic particles, thus increasing their efficiency. Among the different catalysts, the MXene/CoFe2O4 (MXCF) stood out as the most effective, mainly due to the Fe and Co redox cycles. The complete degradation of CAF was achieved in the dark within 10 min at natural pH using 0.2 g/L of MXCF and 0.5 mM of PMS. The novelty of current study lies in the efficient activation of PMS by, for the first time, MXCF in the dark along with mechanistic elucidation of PMS activation. The important role of Co3+/Co2+ and Fe3+/Fe2+ redox cycles alongside surface bound functional groups were highlighted. Radical scavenging and EPR experiments confirmed •OH and 1O2 as the main ROS involved in the CAF degradation. The CAF degradation pathways pointed to hydroxylation and imidazole ring opening mechanisms and MXCF catalyst also exhibited high efficiency in the degradation of sulfamethoxazole and phenol via PMS activation. To further highlight the relevance of the obtained results, treatment of tertiary effluents of wastewaters treatment plant (WWTP) in Bratislava contaminated by CAF exhibited a complete pollutant degradation after 3 h by supplying 0.2 g/L of catalyst and 2 mM PMS in the dark.
{"title":"Mxene-decorated spinel oxides as innovative activators of peroxymonosulfate for degradation of caffeine in WWTP effluents: Insights into mechanisms","authors":"Shalu Atri, Frantisek Zazimal, Sridhar Gowri Sankaran, Zuzana Dyrcikova, Maria Caplovicova, Tomas Roch, Dana Dvoranova, Tomas Homola, Gustav Plesch, Marcello Brigante, Olivier Monfort","doi":"10.1016/j.cej.2024.157814","DOIUrl":"https://doi.org/10.1016/j.cej.2024.157814","url":null,"abstract":"In the frame of the environmental issues related to the efficiency of wastewaters treatment, the generation of advanced oxidation processes (AOPs) by 2D materials appears one of the most promising solutions. In this study, a novel catalytic system for peroxymonosulfate activation (PMS) was designed based on MXene (Ti<sub>3</sub>C<sub>2</sub>T<sub>x</sub>) decorated with spinel oxides Co<sub>3</sub>O<sub>4</sub>, Fe<sub>3</sub>O<sub>4</sub> and CoFe<sub>2</sub>O<sub>4</sub> catalysts. Their efficiency in caffeine (CAF) degradation <em>via</em> PMS activation was assessed. The insertion of spinel oxides inside the multilayer structure of MXene along with their uniform surface decoration was demonstrated by SEM and TEM analyses and it also avoided the aggregation of the magnetic particles, thus increasing their efficiency. Among the different catalysts, the MXene/CoFe<sub>2</sub>O<sub>4</sub> (MXCF) stood out as the most effective, mainly due to the Fe and Co redox cycles. The complete degradation of CAF was achieved in the dark within 10 min at natural pH using 0.2 g/L of MXCF and 0.5 mM of PMS. The novelty of current study lies in the efficient activation of PMS by, for the first time, MXCF in the dark along with mechanistic elucidation of PMS activation. The important role of Co<sup>3+</sup>/Co<sup>2+</sup> and Fe<sup>3+</sup>/Fe<sup>2+</sup> redox cycles alongside surface bound functional groups were highlighted. Radical scavenging and EPR experiments confirmed <sup>•</sup>OH and <sup>1</sup>O<sub>2</sub> as the main ROS involved in the CAF degradation. The CAF degradation pathways pointed to hydroxylation and imidazole ring opening mechanisms and MXCF catalyst also exhibited high efficiency in the degradation of sulfamethoxazole and phenol <em>via</em> PMS activation. To further highlight the relevance of the obtained results, treatment of tertiary effluents of wastewaters treatment plant (WWTP) in Bratislava contaminated by CAF exhibited a complete pollutant degradation after 3 h by supplying 0.2 g/L of catalyst and 2 mM PMS in the dark.","PeriodicalId":270,"journal":{"name":"Chemical Engineering Journal","volume":"253 1","pages":""},"PeriodicalIF":15.1,"publicationDate":"2024-11-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142679023","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"工程技术","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2024-11-21DOI: 10.1016/j.cej.2024.157855
Yunyun Wei, Xinya Hou, Jiayi Liu, Ziqiang Han, Xiaolong Mao
Heavy metals bring a serious threat to human life because of their toxicity and non-biodegradability. Bioremediation is an effective and green strategy for the removal of hazardous substances by natural biological processes. However, the application of microorganisms has been largely limited because planktonic microorganisms have difficulty resisting harsh environments and are challenging to recover in nature. Herein, living probiotic Janus microparticles with magnetic property were prepared using droplet microfluidic and photo-crosslinking technology. Saccharomyces boulardii (S. boulardii), a probiotic fungus currently used in clinical treatment, was encapsulated in a hemisphere of Janus microparticles. The survival rates of S. boulardii encapsulated in the polyethylene glycol diacrylate hemisphere on day 10 and day 15 were above 90 %, and no S. boulardii was released from hydrogel hemisphere. Such living probiotic Janus microparticles could effectively remove copper ions (Cu2+) from wastewater, with the removal rate of Cu2+ reaching 64.78 % after 7 d. The adsorption capacity of S. boulardii in microparticles reached 51.83 mg/g. The cell viability of encapsulated S. boulardii was five times higher than that of free S. boulardii after exposed to Cu2+ for 5 d. Energy spectrum analysis showed that copper was accumulated in cytoplasm of S. boulardii. RNA-sequencing and western blotting results demonstrated the removal of Cu2+ by S. boulardii Janus microparticles mainly rely on copper/zinc superoxide dismutase-mediated biotransformation process. This work provides a green and sustainable strategy for the bioremediation of wastewater.
{"title":"Bioremediation of heavy metal ion (Cu2+) by live probiotic Janus microparticles using droplet-based microfluidic technique","authors":"Yunyun Wei, Xinya Hou, Jiayi Liu, Ziqiang Han, Xiaolong Mao","doi":"10.1016/j.cej.2024.157855","DOIUrl":"https://doi.org/10.1016/j.cej.2024.157855","url":null,"abstract":"Heavy metals bring a serious threat to human life because of their toxicity and non-biodegradability. Bioremediation is an effective and green strategy for the removal of hazardous substances by natural biological processes. However, the application of microorganisms has been largely limited because planktonic microorganisms have difficulty resisting harsh environments and are challenging to recover in nature. Herein, living probiotic Janus microparticles with magnetic property were prepared using droplet microfluidic and photo-crosslinking technology. <em>Saccharomyces boulardii (S. boulardii)</em>, a probiotic fungus currently used in clinical treatment, was encapsulated in a hemisphere of Janus microparticles. The survival rates of <em>S. boulardii</em> encapsulated in the polyethylene glycol diacrylate hemisphere on day 10 and day 15 were above 90 %, and no <em>S. boulardii</em> was released from hydrogel hemisphere. Such living probiotic Janus microparticles could effectively remove copper ions (Cu<sup>2+</sup>) from wastewater, with the removal rate of Cu<sup>2+</sup> reaching 64.78 % after 7 d. The adsorption capacity of <em>S. boulardii</em> in microparticles reached 51.83 mg/g. The cell viability of encapsulated <em>S. boulardii</em> was five times higher than that of free <em>S. boulardii</em> after exposed to Cu<sup>2+</sup> for 5 d. Energy spectrum analysis showed that copper was accumulated in cytoplasm of <em>S. boulardii</em>. RNA-sequencing and western blotting results demonstrated the removal of Cu<sup>2+</sup> by <em>S. boulardii</em> Janus microparticles mainly rely on copper/zinc superoxide dismutase-mediated biotransformation process. This work provides a green and sustainable strategy for the bioremediation of wastewater.","PeriodicalId":270,"journal":{"name":"Chemical Engineering Journal","volume":"8 1","pages":""},"PeriodicalIF":15.1,"publicationDate":"2024-11-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142678740","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"工程技术","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2024-11-21DOI: 10.1016/j.cej.2024.157864
Xuejiao Hu, Yuyuan Zhao, Qianwen Liu, Jin Bai, Xu Zhang, Zhihong Yu, Hongyuan Han, Li Wang
La-Y-Ni-based hydrogen storage alloys demonstrate tremendous application potential due to the superiority of hydrogen storage performance and manufacturing process. However, the insufficient research of La-Y-Ni-based hydrogen storage alloys in solid state hydrogen storage field compared with electrochemistry field limit their further development, especially for the effect of Y element in the alloys. Herein, in this work, a series of La-Y-Ni-based hydrogen storage alloys with various Y content were synthesized, and the structure/solid state hydrogen storage performance variation as well as structural stability, kinetics and thermodynamic properties of the alloys were explored systematically. The results exhibit La0.25Ce0.25Y5.5Ni22Mn0.8 alloy display the superior synthetic performance with a maximum hydrogen adsorption capacity of 1.54 wt% within 150 s and the dehydrogenation platform pressures of 0.40/1.80 MPa, and even better, a capacity retention ratio above 99 % after 100 cycles can be reached. Kinetic mechanism research reveals that the gas–solid reactions between hydrogen and La0.25Ce0.25Y5.5Ni22Mn0.8 alloy are controlled by branching nucleation, and the calculated thermodynamic parameters of alloys are well consistent with hydrogen storage properties.
La-Y-Ni 基储氢合金具有优异的储氢性能和制造工艺，因而具有巨大的应用潜力。然而，与电化学领域相比，La-Y-Ni 基储氢合金在固态储氢领域的研究不足，限制了其进一步发展，尤其是合金中 Y 元素的影响。因此，本研究合成了一系列不同 Y 元素含量的 La-Y-Ni 基储氢合金，并系统地探讨了合金的结构/固态储氢性能变化以及结构稳定性、动力学和热力学性质。结果表明，La0.25Ce0.25Y5.5Ni22Mn0.8合金具有优异的合成性能，150 s内最大吸氢容量为1.54 wt%，脱氢平台压力为0.40/1.80 MPa，更优异的是，100次循环后的容量保持率可达99%以上。动力学机理研究表明，氢与 La0.25Ce0.25Y5.5Ni22Mn0.8 合金之间的气固反应受支化成核控制，计算得到的合金热力学参数与储氢性能十分吻合。
{"title":"Investigation of La-Y-Ni based alloys with various Y content on gas–solid hydrogen storage performance","authors":"Xuejiao Hu, Yuyuan Zhao, Qianwen Liu, Jin Bai, Xu Zhang, Zhihong Yu, Hongyuan Han, Li Wang","doi":"10.1016/j.cej.2024.157864","DOIUrl":"https://doi.org/10.1016/j.cej.2024.157864","url":null,"abstract":"La-Y-Ni-based hydrogen storage alloys demonstrate tremendous application potential due to the superiority of hydrogen storage performance and manufacturing process. However, the insufficient research of La-Y-Ni-based hydrogen storage alloys in solid state hydrogen storage field compared with electrochemistry field limit their further development, especially for the effect of Y element in the alloys. Herein, in this work, a series of La-Y-Ni-based hydrogen storage alloys with various Y content were synthesized, and the structure/solid state hydrogen storage performance variation as well as structural stability, kinetics and thermodynamic properties of the alloys were explored systematically. The results exhibit La<sub>0.25</sub>Ce<sub>0.25</sub>Y<sub>5.5</sub>Ni<sub>22</sub>Mn<sub>0.8</sub> alloy display the superior synthetic performance with a maximum hydrogen adsorption capacity of 1.54 wt% within 150 s and the dehydrogenation platform pressures of 0.40/1.80 MPa, and even better, a capacity retention ratio above 99 % after 100 cycles can be reached. Kinetic mechanism research reveals that the gas–solid reactions between hydrogen and La<sub>0.25</sub>Ce<sub>0.25</sub>Y<sub>5.5</sub>Ni<sub>22</sub>Mn<sub>0.8</sub> alloy are controlled by branching nucleation, and the calculated thermodynamic parameters of alloys are well consistent with hydrogen storage properties.","PeriodicalId":270,"journal":{"name":"Chemical Engineering Journal","volume":"41 1","pages":""},"PeriodicalIF":15.1,"publicationDate":"2024-11-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142679024","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"工程技术","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
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