Pub Date : 2025-04-23DOI: 10.1016/j.cej.2025.163006
Xiuzhen Zhang, Xiyu Wang, Xiaohuan Zhang, Yuanyuan Zhang, Yongxiu Sun, Lili Liu, Wei Yan, Ning Zhang, Changyuan Zhang, Linxing Shi
In the two-step method for perovskite film fabrication, insufficient reaction between organic ammonium salts and PbI2 affects the active layer quality, resulting in poor power conversion efficiency (PCE). In this work, we introduce pentanamine acetic acid (PenAAc) and 5-aminovaleric acid iodine (5-AVAI) as two efficient additives to modify PbI2 layer during perovskite films fabrication via the two-step method in an air environment. After additive modifications, the quality of both PbI2 layers is improved: PenAAc enhances crystallinity and increases PbI2 grain size, while 5-AVAI induces a uniform and smooth PbI2 layer. The optimized PbI2 films facilitate the reaction between PbI2 and organic salts, yielding a high-quality perovskite layer with enhanced crystallinity and reduced defect density. In contrast, the macromolecule structure of 5-AVAI does not diffuse after annealing, remaining in the PbI2 layer and exerting minimal influence on the perovskite surface. However, dissociative CH3COO− groups in PenAAc molecules diffuse from the PbI2 layer to the perovskite surface during annealing, forming strong interactions between I- and Pb2+ with CH3COO− groups. This further improves perovskite film quality and accelerates charge carrier extraction/transport in devices. Consequently, additive-modified perovskite solar cells achieve excellent PCEs of 24.50 % (5-AVAI) and 24.65 % (PenAAc), significantly surpassing the control device (22.84 %). Moreover, hysteresis index is reduced from 4.20 % (control) to 0.33 % (5-AVAI) and 0.08 % (PenAAc). Additionally, the modified devices also demonstrated enhanced environmental stability across humidity, light, and thermal stress conditions.
{"title":"Additive strategy toward PbI2 film modifications for efficient perovskite solar cells fabricated in an air environment","authors":"Xiuzhen Zhang, Xiyu Wang, Xiaohuan Zhang, Yuanyuan Zhang, Yongxiu Sun, Lili Liu, Wei Yan, Ning Zhang, Changyuan Zhang, Linxing Shi","doi":"10.1016/j.cej.2025.163006","DOIUrl":"https://doi.org/10.1016/j.cej.2025.163006","url":null,"abstract":"In the two-step method for perovskite film fabrication, insufficient reaction between organic ammonium salts and PbI<sub>2</sub> affects the active layer quality, resulting in poor power conversion efficiency (PCE). In this work, we introduce pentanamine acetic acid (PenAAc) and 5-aminovaleric acid iodine (5-AVAI) as two efficient additives to modify PbI<sub>2</sub> layer during perovskite films fabrication via the two-step method in an air environment. After additive modifications, the quality of both PbI<sub>2</sub> layers is improved: PenAAc enhances crystallinity and increases PbI<sub>2</sub> grain size, while 5-AVAI induces a uniform and smooth PbI<sub>2</sub> layer. The optimized PbI<sub>2</sub> films facilitate the reaction between PbI<sub>2</sub> and organic salts, yielding a high-quality perovskite layer with enhanced crystallinity and reduced defect density. In contrast, the macromolecule structure of 5-AVAI does not diffuse after annealing, remaining in the PbI<sub>2</sub> layer and exerting minimal influence on the perovskite surface. However, dissociative CH<sub>3</sub>COO<sup>−</sup> groups in PenAAc molecules diffuse from the PbI<sub>2</sub> layer to the perovskite surface during annealing, forming strong interactions between I<sup>-</sup> and Pb<sup>2+</sup> with CH<sub>3</sub>COO<sup>−</sup> groups. This further improves perovskite film quality and accelerates charge carrier extraction/transport in devices. Consequently, additive-modified perovskite solar cells achieve excellent PCEs of 24.50 % (5-AVAI) and 24.65 % (PenAAc), significantly surpassing the control device (22.84 %). Moreover, hysteresis index is reduced from 4.20 % (control) to 0.33 % (5-AVAI) and 0.08 % (PenAAc). Additionally, the modified devices also demonstrated enhanced environmental stability across humidity, light, and thermal stress conditions.","PeriodicalId":270,"journal":{"name":"Chemical Engineering Journal","volume":"22 1","pages":""},"PeriodicalIF":15.1,"publicationDate":"2025-04-23","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143866744","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 : 2025-04-23DOI: 10.1016/j.cej.2025.163011
Weichao Wang, Liuying Wang, Jie Huang, Qi Gu, Yanyan Lu, Chaoqun Ge, Gu Liu
The rapid advancement of aerospace technology has subjected high-speed aircraft to increasingly severe high-temperature conditions, thereby substantially increasing the demand for high-temperature electromagnetic wave (EMW) absorbing materials. However, due to the temperature dependence of the permittivity, high-temperature EMW absorbing materials still face the challenge of maintaining consistent impedance matching performance at different temperatures. This study proposes a novel approach by in-situ constructing Si-Co alloys in amorphous SiOCN ceramics, taking advantage of the inverse temperature-dependent resistivity behavior among components to dynamically equilibrate the overall conductivity of the ceramics, thereby achieving temperature-insensitive permittivity. This strategy significantly enhances the robustness of dielectric properties against temperature fluctuations and enables effective EMW absorption within a temperature range from ambient to 800 °C at low thickness. By using the self-sacrificing template method, a porous structure was formed while ensuring the precise shaping, thereby further achieving the lightweighting of the ceramics. This lightweight dielectric ceramic with temperature-insensitive permittivity provides novel perspectives for the development of wide-temperature-range EMW absorbing materials.
{"title":"Leveraging counteractive temperature-dependent resistivity among components for temperature-insensitive electromagnetic characteristics in lightweight SiOCN ceramics","authors":"Weichao Wang, Liuying Wang, Jie Huang, Qi Gu, Yanyan Lu, Chaoqun Ge, Gu Liu","doi":"10.1016/j.cej.2025.163011","DOIUrl":"https://doi.org/10.1016/j.cej.2025.163011","url":null,"abstract":"The rapid advancement of aerospace technology has subjected high-speed aircraft to increasingly severe high-temperature conditions, thereby substantially increasing the demand for high-temperature electromagnetic wave (EMW) absorbing materials. However, due to the temperature dependence of the permittivity, high-temperature EMW absorbing materials still face the challenge of maintaining consistent impedance matching performance at different temperatures. This study proposes a novel approach by in-situ constructing Si-Co alloys in amorphous SiOCN ceramics, taking advantage of the inverse temperature-dependent resistivity behavior among components to dynamically equilibrate the overall conductivity of the ceramics, thereby achieving temperature-insensitive permittivity. This strategy significantly enhances the robustness of dielectric properties against temperature fluctuations and enables effective EMW absorption within a temperature range from ambient to 800 °C at low thickness. By using the self-sacrificing template method, a porous structure was formed while ensuring the precise shaping, thereby further achieving the lightweighting of the ceramics. This lightweight dielectric ceramic with temperature-insensitive permittivity provides novel perspectives for the development of wide-temperature-range EMW absorbing materials.","PeriodicalId":270,"journal":{"name":"Chemical Engineering Journal","volume":"35 1","pages":""},"PeriodicalIF":15.1,"publicationDate":"2025-04-23","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143866288","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}
Ammonium ion batteries (AIBs) have emerged as a promising technology for large-scale energy storage due to their low cost, high safety, and excellent electrochemical performance. However, the development of suitable anode materials has been a major challenge. In this study, we report a novel p-π conjugated cross-linked quinone-amine polymer (PQDAB) that exhibits remarkable capacity and cycling stability as an anode material for reversible storage of NH4+. The p-π conjugated polymer framework creates an internal electric field at heteroatom sites, facilitating efficient electron transfer during charge and discharge processes, achieving a high capacity of 158.85mAh g−1 at 0.5 A g−1 and an excellent cycle stability of 77.1 % capacity retention over 16,000 cycles. Additionally, a “rocking-chair” AIB based on PQDAB//CuFe-PBA delivers a high capacity of 124.75mAh g−1 at 0.5 A g−1 and excellent cycle stability over 3,000 cycles at 3 A g−1. Furthermore, we also explore the NH4+ storage process through a novel reversibly carbonyl conversion reaction using in-situ/ex-situ characterization and theoretical simulation. Molecular Dynamics (MD) simulations reveal that the solvation layer structures of PQDAB in (NH4)2SO4 electrolyte contribute to its superior stability. This work provides valuable insights for designing high-capacity and stable anode materials for AIBs.
{"title":"p-π Conjugated quinone-amine polymer metal-free anode for high-performance reversible NH4+ charge storage","authors":"Fuyao Huang, Yuhang Jia, Wenkai Zhao, Yongqi Mi, Yujia Guo, Sehrish Gull, Guankui Long, Pengcheng Du","doi":"10.1016/j.cej.2025.163027","DOIUrl":"https://doi.org/10.1016/j.cej.2025.163027","url":null,"abstract":"Ammonium ion batteries (AIBs) have emerged as a promising technology for large-scale energy storage due to their low cost, high safety, and excellent electrochemical performance. However, the development of suitable anode materials has been a major challenge. In this study, we report a novel p-π conjugated cross-linked quinone-amine polymer (PQDAB) that exhibits remarkable capacity and cycling stability as an anode material for reversible storage of NH<sub>4</sub><sup>+</sup>. The p-π conjugated polymer framework creates an internal electric field at heteroatom sites, facilitating efficient electron transfer during charge and discharge processes, achieving a high capacity of 158.85mAh g<sup>−1</sup> at 0.5 A g<sup>−1</sup> and an excellent cycle stability of 77.1 % capacity retention over 16,000 cycles. Additionally, a “rocking-chair” AIB based on PQDAB//CuFe-PBA delivers a high capacity of 124.75mAh g<sup>−1</sup> at 0.5 A g<sup>−1</sup> and excellent cycle stability over 3,000 cycles at 3 A g<sup>−1</sup>. Furthermore, we also explore the NH<sub>4</sub><sup>+</sup> storage process through a novel reversibly carbonyl conversion reaction using in-situ/ex-situ characterization and theoretical simulation. Molecular Dynamics (MD) simulations reveal that the solvation layer structures of PQDAB in (NH<sub>4</sub>)<sub>2</sub>SO<sub>4</sub> electrolyte contribute to its superior stability. This work provides valuable insights for designing high-capacity and stable anode materials for AIBs.","PeriodicalId":270,"journal":{"name":"Chemical Engineering Journal","volume":"70 1","pages":""},"PeriodicalIF":15.1,"publicationDate":"2025-04-23","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143866290","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}
At present, selecting suitable fluorescent molecules to design low-cost, stable and sensitive ammonia response sensors is an important topic in the field of meat quality detection. In this work, a solid–liquid applicable ammonia-responsive fluorescent molecule (2-(benzo[d]thiazol-2-yl)-4-chlorophenol acetate, BTCP-Ac), was designed by enhancing the aggregation-induced emission (AIE)/excited state intramolecular proton transfer (ESIPT) luminescence properties of 2-(Benzo[d]thiazol-2-yl) phenol (HBT) molecules. BTCP-Ac combined the advantages of the red luminescence (colorimetric intrinsic parameter) and the confinement effect (enhanced aggregation of fluorescent molecules) of the metal–organic framework (Eu-MOF) to prepare fluorescent probes (BTCP-Ac@Eu-MOF). The sensor (BTCP-Ac@Eu-MOF film) was prepared using bacterial cellulose (BC) as a fluorescent probe loading platform. The sensor achieves specific detection of amines by “switching: the intramolecular proton transfer process of fluorescent molecules. The experimental results showed that the sensor reacted significantly with ammonia compared to BTCP-Ac (LOD = 2.24 ppm), with a low detection limit (LOD = 0.68 ppm) and stable luminescence (no decay for 30 d). The sensor with high temperature resistance and strong hydrophobicity (121.64°) successfully monitored the freshness of chicken meat, which changed color from red to blue-green and was easily visible to the consumer’s eye. This method encapsulates specially designed AIE molecules in a luminescent metal–organic framework to prepare ammonia-responsive sensors with selectivity, high sensitivity and stability, providing a novel and practical strategy for designing gas-responsive solid-state sensors.
{"title":"Preparation of an ammonia-responsive sensor based on bacterial cellulose film with enhanced AIE/ESIPT emission of fluorescent molecules bound to europium-based metal–organic framework","authors":"Yanlan Ma, Yuehui Li, Tianran Huang, Xinyi Yang, Jichao Huang, Ming Huang","doi":"10.1016/j.cej.2025.163034","DOIUrl":"https://doi.org/10.1016/j.cej.2025.163034","url":null,"abstract":"At present, selecting suitable fluorescent molecules to design low-cost, stable and sensitive ammonia response sensors is an important topic in the field of meat quality detection. In this work, a solid–liquid applicable ammonia-responsive fluorescent molecule (2-(benzo[<em>d</em>]thiazol-2-yl)-4-chlorophenol acetate, BTCP-Ac), was designed by enhancing the aggregation-induced emission (AIE)/excited state intramolecular proton transfer (ESIPT) luminescence properties of 2-(Benzo[<em>d</em>]thiazol-2-yl) phenol (HBT) molecules. BTCP-Ac combined the advantages of the red luminescence (colorimetric intrinsic parameter) and the confinement effect (enhanced aggregation of fluorescent molecules) of the metal–organic framework (Eu-MOF) to prepare fluorescent probes (BTCP-Ac@Eu-MOF). The sensor (BTCP-Ac@Eu-MOF film) was prepared using bacterial cellulose (BC) as a fluorescent probe loading platform. The sensor achieves specific detection of amines by “switching: the intramolecular proton transfer process of fluorescent molecules. The experimental results showed that the sensor reacted significantly with ammonia compared to BTCP-Ac (LOD = 2.24 ppm), with a low detection limit (LOD = 0.68 ppm) and stable luminescence (no decay for 30 d). The sensor with high temperature resistance and strong hydrophobicity (121.64°) successfully monitored the freshness of chicken meat, which changed color from red to blue-green and was easily visible to the consumer’s eye. This method encapsulates specially designed AIE molecules in a luminescent metal–organic framework to prepare ammonia-responsive sensors with selectivity, high sensitivity and stability, providing a novel and practical strategy for designing gas-responsive solid-state sensors.","PeriodicalId":270,"journal":{"name":"Chemical Engineering Journal","volume":"53 1","pages":""},"PeriodicalIF":15.1,"publicationDate":"2025-04-23","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143866515","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 : 2025-04-23DOI: 10.1016/j.cej.2025.163026
Shengfei Bao, Aodi Jiang, Li Peng, Fuying Liao, Ga Liu, Li Chen, Peng Zhou, Zhen Zhu, Rui L. Reis, Subhas C. Kundu, Lian Duan, Bo Xiao, Xiao Yang
Continuous invasion and infection of drug-resistant bacteria leads to chronic inflammation and ulcers in skin wounds, which hinders wound healing and even results in sepsis. Here, we constructed a multifunctional injectable hydrogel (GA/PIOP/SF) that was composed of a synthesized porous ionic organic polymer (PIOP) with photothermal and photodynamic therapy (PDT/PTT) capacities to kill bacteria, a bioactive small molecule glycyrrhizinic acid (GA) to trigger macrophage polarization towards M2-type, and silk fibroin (SF) with excellent biocompatibility to facilitate cell proliferation. In vitro antibacterial and cellular experiments revealed that the GA/PIOP/SF hydrogel exhibited excellent bactericidal activity and induced M2-type macrophage polarization, promoting L929 fibroblast migration. In the methicillin-resistant Staphylococcus aureus (MRSA) infected wound model, GA/PIOP/SF hydrogel created a sterile microenvironment at the wound site by activating the PDT/PTT properties of PIOP through 660 nm laser irradiation, which could destroy the MRSA structure, and combined GA to regulate the immune microenvironment of the wound site. Moreover, in chronic diabetic wound models, the photothermal activity of PIOP promoted the disintegration of self-assembled GA nanofibers. It released the GA small molecules from the GA/PIOP/SF double network, facilitating macrophage polarization from M1-type to M2-type and alleviating inflammation. There two animal experimental results presented that the GA/PIOP/SF hydrogel could accelerate the recovery of both MRSA-infected wound and diabetic wounds through its antibacterial activity and improved fibroblast migration, M2-type macrophage polarization, as well as angiogenesis, demonstrating its excellent application potential as wound dressing in the treatment of chronic infected diabetic wound.
{"title":"Injectable dual-network hydrogel for phototherapy and immunomodulation in the treatment of MRSA-infected and diabetic wound","authors":"Shengfei Bao, Aodi Jiang, Li Peng, Fuying Liao, Ga Liu, Li Chen, Peng Zhou, Zhen Zhu, Rui L. Reis, Subhas C. Kundu, Lian Duan, Bo Xiao, Xiao Yang","doi":"10.1016/j.cej.2025.163026","DOIUrl":"https://doi.org/10.1016/j.cej.2025.163026","url":null,"abstract":"Continuous invasion and infection of drug-resistant bacteria leads to chronic inflammation and ulcers in skin wounds, which hinders wound healing and even results in sepsis. Here, we constructed a multifunctional injectable hydrogel (GA/PIOP/SF) that was composed of a synthesized porous ionic organic polymer (PIOP) with photothermal and photodynamic therapy (PDT/PTT) capacities to kill bacteria, a bioactive small molecule glycyrrhizinic acid (GA) to trigger macrophage polarization towards M2-type, and silk fibroin (SF) with excellent biocompatibility to facilitate cell proliferation. In vitro antibacterial and cellular experiments revealed that the GA/PIOP/SF hydrogel exhibited excellent bactericidal activity and induced M2-type macrophage polarization, promoting L929 fibroblast migration. In the methicillin-resistant <em>Staphylococcus aureus</em> (MRSA) infected wound model, GA/PIOP/SF hydrogel created a sterile microenvironment at the wound site by activating the PDT/PTT properties of PIOP through 660 nm laser irradiation, which could destroy the MRSA structure, and combined GA to regulate the immune microenvironment of the wound site. Moreover, in chronic diabetic wound models, the photothermal activity of PIOP promoted the disintegration of self-assembled GA nanofibers. It released the GA small molecules from the GA/PIOP/SF double network, facilitating macrophage polarization from M1-type to M2-type and alleviating inflammation. There two animal experimental results presented that the GA/PIOP/SF hydrogel could accelerate the recovery of both MRSA-infected wound and diabetic wounds through its antibacterial activity and improved fibroblast migration, M2-type macrophage polarization, as well as angiogenesis, demonstrating its excellent application potential as wound dressing in the treatment of chronic infected diabetic wound.","PeriodicalId":270,"journal":{"name":"Chemical Engineering Journal","volume":"33 1","pages":""},"PeriodicalIF":15.1,"publicationDate":"2025-04-23","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143866522","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}
The photocatalysts studied for hydrogen production from seawater have not been very effective in hydrogen production. In this paper, simple ZnIn2S4 (ZIS) and ZnIn2S4 with S defects (Sd-ZIS) were prepared by hydrothermal method, the presence of S defects provides unsaturated S atoms for the in situ growth of 0D WSe2 QDs at the defects of 3D Sd-ZIS by the secondary hydrothermal method to obtain the 3D/0D Sd-ZIS/WSe2 QDs complex (SZWx, x = 1,2,3). The formation of W-S bonds with strong coupling effects at their interfaces provides a channel for the fast separation of carriers. The seawater hydrogen production performance (6.40 mmol/g/h) of the best-performing SZW2 is 53.33 and 26.67 times higher than that of ZIS and Sd-ZIS, which tested with 0.10 M ascorbic acid as the sacrificial agents. The carrier dynamics mechanism of SZWx was further investigated by tests such as TRPL, TPV, and DFT calculations. This paper provides some ideas for future research on ZIS-based photocatalysts for efficient heterojunction interfacial carrier dynamics and seawater hydrogen production.
{"title":"Defect-assisted strong interfacial interaction in ZnIn2S4/WSe2 heterojunction for efficient Photohydrogen production from seawater","authors":"Caifeng Huang, Li Xiang, Yun Zhou, Wangping Xu, Huihuang Mao, Fugang Qi, Xiaoping Ouyang","doi":"10.1016/j.cej.2025.162918","DOIUrl":"https://doi.org/10.1016/j.cej.2025.162918","url":null,"abstract":"The photocatalysts studied for hydrogen production from seawater have not been very effective in hydrogen production. In this paper, simple ZnIn<sub>2</sub>S<sub>4</sub> (ZIS) and ZnIn<sub>2</sub>S<sub>4</sub> with S defects (S<sub>d</sub>-ZIS) were prepared by hydrothermal method, the presence of S defects provides unsaturated S atoms for the in situ growth of 0D WSe<sub>2</sub> QDs at the defects of 3D S<sub>d</sub>-ZIS by the secondary hydrothermal method to obtain the 3D/0D S<sub>d</sub>-ZIS/WSe<sub>2</sub> QDs complex (SZWx, x = 1,2,3). The formation of W-S bonds with strong coupling effects at their interfaces provides a channel for the fast separation of carriers. The seawater hydrogen production performance (6.40 mmol/g/h) of the best-performing SZW2 is 53.33 and 26.67 times higher than that of ZIS and S<sub>d</sub>-ZIS, which tested with 0.10 M ascorbic acid as the sacrificial agents. The carrier dynamics mechanism of SZWx was further investigated by tests such as TRPL, TPV, and DFT calculations. This paper provides some ideas for future research on ZIS-based photocatalysts for efficient heterojunction interfacial carrier dynamics and seawater hydrogen production.","PeriodicalId":270,"journal":{"name":"Chemical Engineering Journal","volume":"18 1","pages":""},"PeriodicalIF":15.1,"publicationDate":"2025-04-23","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143862825","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 : 2025-04-23DOI: 10.1016/j.cej.2025.162937
Xiaoming Wang, Zehua Huang, Mengge Li, Hongzheng Lu, Mengting Sun, Yuanmei Song, Xiaolin Wang, Huifang Li, Yan He, Fei Wang
The use of carbon nanotubes (CNTs) to enhance methane hydrate formation for energy storage has garnered attention. However, their promotion efficiency remains inferior to that of traditional promoters (e.g., surfactants), highlighting the necessity of re-evaluation on the feasibility of CNTs as effective promoters for methane hydrate formation. Here, the promotion of CNTs to methane hydrate formation was comprehensively evaluated via both experimental and simulation methods, with the scales from macro to micro and status from suspension, to serum and water-saturated powder. It was revealed for the first time that there was a contradiction between the CNTs status and the promotion efficiency in different periods (nucleation and growth). With the increase in CNTs concentration, transitioning from suspension to serum and water-saturated powder, the enhancement of hydrate nucleation was attributed to the increase in nucleation sites within the liquid phase. The initial stage of hydrate formation was significantly shortened, dropping from 148 min to 14 min, and nearly to 0 min. However, the promotion of hydrate growth was reduced, as the final methane storage capacity decreased from 141 to 132 and then to 90 v/v. This reduction was due to the high dosage of CNTs, which adsorbed water and hindered its migration during the hydrate growth period. Regarding the inner cavity of CNTs, molecular simulations confirmed that methane hydrates could not form in this special space, indicating that pristine CNTs have limited potential as standalone methane hydrate promoters. Therefore, promising research directions may include the combination of CNTs with other promoters, the functionalization of CNT surfaces with active groups, the synergistic enhancement of heat and mass transfer in CNT-based fluids, and the application of CNTs in the industrialization of hydrate-based technologies.
{"title":"Re-evaluation of using carbon nanotubes as the kinetic promoters for methane hydrate formation","authors":"Xiaoming Wang, Zehua Huang, Mengge Li, Hongzheng Lu, Mengting Sun, Yuanmei Song, Xiaolin Wang, Huifang Li, Yan He, Fei Wang","doi":"10.1016/j.cej.2025.162937","DOIUrl":"https://doi.org/10.1016/j.cej.2025.162937","url":null,"abstract":"The use of carbon nanotubes (CNTs) to enhance methane hydrate formation for energy storage has garnered attention. However, their promotion efficiency remains inferior to that of traditional promoters (<em>e.g.</em>, surfactants), highlighting the necessity of re-evaluation on the feasibility of CNTs as effective promoters for methane hydrate formation. Here, the promotion of CNTs to methane hydrate formation was comprehensively evaluated via both experimental and simulation methods, with the scales from macro to micro and status from suspension, to serum and water-saturated powder. It was revealed for the first time that there was a contradiction between the CNTs status and the promotion efficiency in different periods (nucleation and growth). With the increase in CNTs concentration, transitioning from suspension to serum and water-saturated powder, the enhancement of hydrate nucleation was attributed to the increase in nucleation sites within the liquid phase. The initial stage of hydrate formation was significantly shortened, dropping from 148 min to 14 min, and nearly to 0 min. However, the promotion of hydrate growth was reduced, as the final methane storage capacity decreased from 141 to 132 and then to 90 v/v. This reduction was due to the high dosage of CNTs, which adsorbed water and hindered its migration during the hydrate growth period. Regarding the inner cavity of CNTs, molecular simulations confirmed that methane hydrates could not form in this special space, indicating that pristine CNTs have limited potential as standalone methane hydrate promoters. Therefore, promising research directions may include the combination of CNTs with other promoters, the functionalization of CNT surfaces with active groups, the synergistic enhancement of heat and mass transfer in CNT-based fluids, and the application of CNTs in the industrialization of hydrate-based technologies.","PeriodicalId":270,"journal":{"name":"Chemical Engineering Journal","volume":"40 1","pages":""},"PeriodicalIF":15.1,"publicationDate":"2025-04-23","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143866525","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 : 2025-04-23DOI: 10.1016/j.cej.2025.162917
Xin Zhao, Jun Xiao, Dingxian Jia, Pengfei Qi, Mingjie Wei, Shuang Hao, Yunxia Hu
Thin-film composite (TFC) nanofiltration (NF) membranes fabricated via conventional interfacial polymerization (IP) inherently suffer from the permeability-selectivity trade-off due to diffusion-limited monomer transport. Here, we unveil an ionic liquid (IL)-based surfactants ([C12mim][Cl]) as a dynamic bidirectional regulator of piperazine (PIP) and trimesoyl chloride (TMC) that uniquely reengineers IP kinetics to fabricate high-performance NF membranes with simultaneous enhancement in both water permeability and ion selectivity. Unlike existing additives that often passively decelerate amine diffusion, [C12mim][Cl] establishes a critical diffusion asymmetry (DTMC > DPIP) by simultaneously accelerating TMC mobility while spatially confining PIP through intermolecular binding and viscosity modulation. This diffusion-driven instability triggers spontaneous Turing patterning, yielding an ultrathin (≈24 nm) polyamide (PA) layer with a loosely packed hierarchical network and enhanced carboxyl density (59.8 mM m−2). The synergistic interplay of Turing structure and intensified Donnan exclusion achieves unprecedented performance of NF membrane: water permeance (19.3 LMH bar−1, +210 %) and mono-/divalent ion selectivity (83), surpassing over current leading benchmarks. This work establishes a universal strategy to fabricate high-performance NF membranes with large permeable surface and enhanced carboxyl density through an ionic liquid‐based surfactants-mediated IP, breaking the permeability-selectivity trade-off and offering transformative potential for precision separations.
{"title":"Ionic liquid‐based surfactants-mediated turing patterning in nanofiltration membranes via bidirectional diffusion control of piperazine and trimesoyl chloride for synergistic permselectivity enhancement","authors":"Xin Zhao, Jun Xiao, Dingxian Jia, Pengfei Qi, Mingjie Wei, Shuang Hao, Yunxia Hu","doi":"10.1016/j.cej.2025.162917","DOIUrl":"https://doi.org/10.1016/j.cej.2025.162917","url":null,"abstract":"Thin-film composite (TFC) nanofiltration (NF) membranes fabricated <em>via</em> conventional interfacial polymerization (IP) inherently suffer from the permeability-selectivity trade-off due to diffusion-limited monomer transport. Here, we unveil an ionic liquid (IL)-based surfactants ([C<sub>12</sub>mim][Cl]) as a dynamic bidirectional regulator of piperazine (PIP) and trimesoyl chloride (TMC) that uniquely reengineers IP kinetics to fabricate high-performance NF membranes with simultaneous enhancement in both water permeability and ion selectivity. Unlike existing additives that often passively decelerate amine diffusion, [C<sub>12</sub>mim][Cl] establishes a critical diffusion asymmetry (<em>D</em><sub>TMC</sub> > <em>D</em><sub>PIP</sub>) by simultaneously accelerating TMC mobility while spatially confining PIP through intermolecular binding and viscosity modulation. This diffusion-driven instability triggers spontaneous Turing patterning, yielding an ultrathin (≈24 nm) polyamide (PA) layer with a loosely packed hierarchical network and enhanced carboxyl density (59.8 mM m<sup>−2</sup>). The synergistic interplay of Turing structure and intensified Donnan exclusion achieves unprecedented performance of NF membrane: water permeance (19.3 LMH bar<sup>−1</sup>, +210 %) and mono-/divalent ion selectivity (83), surpassing over current leading benchmarks. This work establishes a universal strategy to fabricate high-performance NF membranes with large permeable surface and enhanced carboxyl density through an ionic liquid‐based surfactants-mediated IP, breaking the permeability-selectivity trade-off and offering transformative potential for precision separations.","PeriodicalId":270,"journal":{"name":"Chemical Engineering Journal","volume":"261 1","pages":""},"PeriodicalIF":15.1,"publicationDate":"2025-04-23","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143866292","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 : 2025-04-23DOI: 10.1016/j.cej.2025.162919
Seon Yeong Chae, Geun Young Kim, Hyun-Seok Choe, Young Woo Kwon, Suck Won Hong, Jae-Hyuk Kim
Synergistic chemo-photothermal therapy is a robust and reliable strategy for the effective elimination of cancer cells. In this study, we introduce a developed therapeutic approach that integrates photothermal therapy (PTT) via yolk-shell gold nanoparticles (YS-GNP) with doxorubicin (DOX)-mediated chemotherapy to enhance anticancer efficacy. YS-GNP was meticulously engineered as a highly efficient photothermal agent, utilizing the localized surface plasmon resonance of gold nanoparticles within the yolk-shell structure. Upon near-infrared laser irradiation, YS-GNP effectively induced cancer cell death under mild hyperthermic condition. In vitro studies on HeLa and YD10B cancer cell lines demonstrated that the combination therapy (YS-GNP/DOX/Laser) significantly improved therapeutic outcomes compared to monotherapies, selectively targeting cancer cells while minimizing damage to normal cells. The enhanced anticancer effects were attributed to the complementary mechanisms of DOX-induced reactive oxygen species generation and YS-GNP-mediated lysosomal disruption. Furthermore, inhibition of heat shock proteins (HSPs) substantially amplified cancer cell death, highlighting the multifaceted mechanisms underlying the PTT approach. In particular, significant reductions in HSP70 expression (1.45-fold in YD10B, 1.96-fold in HeLa) and HSP90 expression (1.58-fold in YD10B, 5.88-fold in HeLa), support the synergistic anticancer effect and mechanism of DOX and PTT. This dual approach, which combines photothermal therapy and chemotherapy, enhances treatment precision and pathological site-specific accumulation, presenting strong potential for clinical translation.
{"title":"Photothermal cancer treatment with laser-activated yolk-shell nanoparticles and synergistic combination of chemotherapy","authors":"Seon Yeong Chae, Geun Young Kim, Hyun-Seok Choe, Young Woo Kwon, Suck Won Hong, Jae-Hyuk Kim","doi":"10.1016/j.cej.2025.162919","DOIUrl":"https://doi.org/10.1016/j.cej.2025.162919","url":null,"abstract":"Synergistic chemo-photothermal therapy is a robust and reliable strategy for the effective elimination of cancer cells. In this study, we introduce a developed therapeutic approach that integrates photothermal therapy (PTT) via yolk-shell gold nanoparticles (YS-GNP) with doxorubicin (DOX)-mediated chemotherapy to enhance anticancer efficacy. YS-GNP was meticulously engineered as a highly efficient photothermal agent, utilizing the localized surface plasmon resonance of gold nanoparticles within the yolk-shell structure. Upon near-infrared laser irradiation, YS-GNP effectively induced cancer cell death under mild hyperthermic condition. In vitro studies on HeLa and YD10B cancer cell lines demonstrated that the combination therapy (YS-GNP/DOX/Laser) significantly improved therapeutic outcomes compared to monotherapies, selectively targeting cancer cells while minimizing damage to normal cells. The enhanced anticancer effects were attributed to the complementary mechanisms of DOX-induced reactive oxygen species generation and YS-GNP-mediated lysosomal disruption. Furthermore, inhibition of heat shock proteins (HSPs) substantially amplified cancer cell death, highlighting the multifaceted mechanisms underlying the PTT approach. In particular, significant reductions in HSP70 expression (1.45-fold in YD10B, 1.96-fold in HeLa) and HSP90 expression (1.58-fold in YD10B, 5.88-fold in HeLa), support the synergistic anticancer effect and mechanism of DOX and PTT. This dual approach, which combines photothermal therapy and chemotherapy, enhances treatment precision and pathological site-specific accumulation, presenting strong potential for clinical translation.","PeriodicalId":270,"journal":{"name":"Chemical Engineering Journal","volume":"153 1","pages":""},"PeriodicalIF":15.1,"publicationDate":"2025-04-23","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143866362","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 : 2025-04-23DOI: 10.1016/j.cej.2025.163020
Zhexiang Wang, Xinyi Li, Rui Lv, Ruochen Guo, Qinglei Shu, Tianjin Ge, Jun Yan, Zhihao Zhao, Guanghui Wang, Jian Liu
The click chemistry catalyzed by transition metals is the research front line for bioorthogonal therapeutics. However, it demands the use of external ligands to form transition metal–ligand complexes for the catalytic enhancement, thus leading to biosafety concerns on the undesired side effects of the complexes or the additional ligands themselves during therapies. Here we report a pH/GSH-driven inside-out nanoreactor initiating Cu(I)-precursor chelation-promoted bioorthogonal catalysis against malignant tumors. It comparts the precursors (Azide and Alkyne) and Cu(II) safely with disulfide-functionalized hyaluronic acid-polycarprolactone (abbr. PCHP1) polymersome structure. Once sensing the pH/GSH changes typically in tumor microenvironment, our nanoreactor starts with a unique programed releasing, allowing for the inside-out translocation of Azide with the highest priority. Subsequently the Cu(I)-Azide chelation can promote the catalytic reaction to generate drug molecules in a highly efficient, ligand-free manner. The PCHP1 nanoreactor can suppress malignant tumors significantly better than the other control groups in the in vitro and in vivo experiments, while inducing minimal side effects. Our strategy of ligand-free Cu(I)-precursor chelation promoted click chemistry will facilitate the development of bioorthogonal catalytic therapies for clinical translation.
{"title":"pH/GSH-Driven inside-out nanoreactor initiating copper(I)-precursor chelation-promoted bioorthogonal therapy","authors":"Zhexiang Wang, Xinyi Li, Rui Lv, Ruochen Guo, Qinglei Shu, Tianjin Ge, Jun Yan, Zhihao Zhao, Guanghui Wang, Jian Liu","doi":"10.1016/j.cej.2025.163020","DOIUrl":"https://doi.org/10.1016/j.cej.2025.163020","url":null,"abstract":"The click chemistry catalyzed by transition metals is the research front line for bioorthogonal therapeutics. However, it demands the use of external ligands to form transition metal–ligand complexes for the catalytic enhancement, thus leading to biosafety concerns on the undesired side effects of the complexes or the additional ligands themselves during therapies. Here we report a pH/GSH-driven inside-out nanoreactor initiating Cu(I)-precursor chelation-promoted bioorthogonal catalysis against malignant tumors. It comparts the precursors (Azide and Alkyne) and Cu(II) safely with disulfide-functionalized hyaluronic acid-polycarprolactone (abbr. PCHP1) polymersome structure. Once sensing the pH/GSH changes typically in tumor microenvironment, our nanoreactor starts with a unique programed releasing, allowing for the inside-out translocation of Azide with the highest priority. Subsequently the Cu(I)-Azide chelation can promote the catalytic reaction to generate drug molecules in a highly efficient, ligand-free manner. The PCHP1 nanoreactor can suppress malignant tumors significantly better than the other control groups in the <em>in vitro</em> and <em>in vivo</em> experiments, while inducing minimal side effects. Our strategy of ligand-free Cu(I)-precursor chelation promoted click chemistry will facilitate the development of bioorthogonal catalytic therapies for clinical translation.","PeriodicalId":270,"journal":{"name":"Chemical Engineering Journal","volume":"91 1","pages":""},"PeriodicalIF":15.1,"publicationDate":"2025-04-23","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143866527","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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