Pub Date : 2025-02-04DOI: 10.1016/j.cej.2025.159503
Kexing Li, Zhao-tie Liu, Zhong-wen Liu, Jinqiang Jiang, Guo Li
Metal-organic frameworks (MOFs) emerge as promising candidates for developing stimuli-responsive actuators. However, currently reported MOF-loading actuators rely on the reversible volume change of MOF crystal lattice upon stimulation, which requires a much longer time than other types of hygroscopic fillers to accomplish the actuating process. In this work, we report the use of Zr-Fc to develop NIR light and moisture responsive actuators. Zr-Fc possesses a rigid structure and is prepared by a conventional solvent-thermal approach using ZrCl4 and Fc(COOH)2 as raw materials, and the composite is developed by introducing Zr-Fc into polyvinyl alcohol with a gradient distribution. The developed composite can reversibly bend toward different sides upon the stimulation of NIR light or moisture, and the actuation processes can be completed within seconds due to structural rigidity of Zr-Fc. Further by inducing the formation of chemical crosslinking between polyvinyl alcohol chains, the composite can be programmed into intricate 3D shapes, which enables the exhibition of different modes of deformation and motion upon stimulation. This work enriches the design and preparation of actuators by MOF-loading with advanced actuating behaviors.
{"title":"Fast photo- and Moisture-Driven bidirectional actuation of a Shape-Programmable MOFLoading composite","authors":"Kexing Li, Zhao-tie Liu, Zhong-wen Liu, Jinqiang Jiang, Guo Li","doi":"10.1016/j.cej.2025.159503","DOIUrl":"https://doi.org/10.1016/j.cej.2025.159503","url":null,"abstract":"Metal-organic frameworks (MOFs) emerge as promising candidates for developing stimuli-responsive actuators. However, currently reported MOF-loading actuators rely on the reversible volume change of MOF crystal lattice upon stimulation, which requires a much longer time than other types of hygroscopic fillers to accomplish the actuating process. In this work, we report the use of Zr-Fc to develop NIR light and moisture responsive actuators. Zr-Fc possesses a rigid structure and is prepared by a conventional solvent-thermal approach using ZrCl<sub>4</sub> and Fc(COOH)<sub>2</sub> as raw materials, and the composite is developed by introducing Zr-Fc into polyvinyl alcohol with a gradient distribution. The developed composite can reversibly bend toward different sides upon the stimulation of NIR light or moisture, and the actuation processes can be completed within seconds due to structural rigidity of Zr-Fc. Further by inducing the formation of chemical crosslinking between polyvinyl alcohol chains, the composite can be programmed into intricate 3D shapes, which enables the exhibition of different modes of deformation and motion upon stimulation. This work enriches the design and preparation of actuators by MOF-loading with advanced actuating behaviors.","PeriodicalId":270,"journal":{"name":"Chemical Engineering Journal","volume":"136 1","pages":""},"PeriodicalIF":15.1,"publicationDate":"2025-02-04","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143124936","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 high sensitivity and precise detection of trace ammonia (NH3) remains a critical focus of research in the fields of air pollution, agriculture/industrial process control, polar-region environment research and extraterrestrial life search. Herein, we proposed a bionic trace fluid preconcentration strategy to promote miniature trace gas sensing performance. This strategy leverages the selective adsorption behavior from atmosphere of novel phosphine oxide functionalized porous aromatic frameworks (PAFs), alongside the bionic fluid control theory modeled after the Pike’s nasal structure and the Squid’s sine function-shaped fins. A wireless bionic olfactory system (WBOS) is developed to achieve the wide range accurate monitoring of 5 ppb-300 ppm with an actual detection limit of 100 ppt facilitated by advanced preconcentration up to 37,000 times. The high sensing performance is also discussed by density functional theory (DFT), computational fluid dynamics (CFD) simulations and machine learning-genetic algorithms. Our work provides new inspiration for developing miniature bionic sensing devices based on advanced materials for synergistic trace gas preconcentration and detection.
{"title":"Phosphine oxide functionalized porous aromatic frameworks enabled wireless bionic olfactory system with preconcentration capability for trace ammonia monitoring","authors":"Shuai Zhao, Hongyang Jin, Zihao Chen, Yonglai Zhang, Xiaoqin Zou, Lin Xu, Shaolei Wang, Zhenglei Yu, Zhiyong Chang","doi":"10.1016/j.cej.2025.160282","DOIUrl":"https://doi.org/10.1016/j.cej.2025.160282","url":null,"abstract":"The high sensitivity and precise detection of trace ammonia (NH<sub>3</sub>) remains a critical focus of research in the fields of air pollution, agriculture/industrial process control, polar-region environment research and extraterrestrial life search. Herein, we proposed a bionic trace fluid preconcentration strategy to promote miniature trace gas sensing performance. This strategy leverages the selective adsorption behavior from atmosphere of novel phosphine oxide functionalized porous aromatic frameworks (PAFs), alongside the bionic fluid control theory modeled after the Pike’s nasal structure and the Squid’s sine function-shaped fins. A wireless bionic olfactory system (WBOS) is developed to achieve the wide range accurate monitoring of 5 ppb-300 ppm with an actual detection limit of 100 ppt facilitated by advanced preconcentration up to 37,000 times. The high sensing performance is also discussed by density functional theory (DFT), computational fluid dynamics (CFD) simulations and machine learning-genetic algorithms. Our work provides new inspiration for developing miniature bionic sensing devices based on advanced materials for synergistic trace gas preconcentration and detection.","PeriodicalId":270,"journal":{"name":"Chemical Engineering Journal","volume":"15 1","pages":""},"PeriodicalIF":15.1,"publicationDate":"2025-02-04","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143124361","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 : 2025-02-04DOI: 10.1016/j.cej.2025.160232
Flor Louage, Stijn W.H. Van Hulle, Diederik P.L. Rousseau
The single well push–pull test (SWPPT) involves injecting a solution into a well and later extracting it to assess reaction rates by analyzing changes in concentration over time. This study first optimized the conditions for conducting SWPPTs in a horizontal subsurface flow constructed wetland (HSSFCW) and then determined in situ heterotrophic aerobic and anoxic reaction rates in the influent zone of the HSSFCW. The optimal tracer concentration and injection solution volume for the SWPPT were determined to be 0.3 g NaCl L-1 and 10 L, respectively. Rate constants were derived using two different models: well-mixed and plug-flow. The average well-mixed and plug-flow first-order oxygen rate constants were 0.95 ± 0.20 and 0.66 ± 0.14 min−1, respectively. After adding an easily degradable carbon source to the aerated injection solution, the heterotrophic yield coefficient was calculated to be 0.50 gCOD gCOD-1. First-order denitrification rate constants varied across the HSSFCW influent zone, ranging between 0.005–0.035 min−1 for the well-mixed model and 0.004–0.027 min−1 for the plug-flow model. The heterotrophic denitrification yield coefficient YdH values averaged at 0.55 ± 0.33. Different oxygen utilization routes were identified, with the bulk consumed in multiple biological processes, a small portion lost to trapped gas bubbles and an insignificant amount to chemical reactions. The results of this study demonstrate the potential of using SWPPTs to measure heterotrophic aerobic and denitrifying degradation rate constants and yield in situ in HSSFCWs.
{"title":"Development of single well push–pull tests for measuring local rate constants in horizontal subsurface flow constructed wetlands","authors":"Flor Louage, Stijn W.H. Van Hulle, Diederik P.L. Rousseau","doi":"10.1016/j.cej.2025.160232","DOIUrl":"https://doi.org/10.1016/j.cej.2025.160232","url":null,"abstract":"The single well push–pull test (SWPPT) involves injecting a solution into a well and later extracting it to assess reaction rates by analyzing changes in concentration over time. This study first optimized the conditions for conducting SWPPTs in a horizontal subsurface flow constructed wetland (HSSFCW) and then determined in situ heterotrophic aerobic and anoxic reaction rates in the influent zone of the HSSFCW. The optimal tracer concentration and injection solution volume for the SWPPT were determined to be 0.3 g NaCl L<sup>-1</sup> and 10 L, respectively. Rate constants were derived using two different models: well-mixed and plug-flow. The average well-mixed and plug-flow first-order oxygen rate constants were 0.95 ± 0.20 and 0.66 ± 0.14 min<sup>−1</sup>, respectively. After adding an easily degradable carbon source to the aerated injection solution, the heterotrophic yield coefficient was calculated to be 0.50 gCOD gCOD<sup>-1</sup>. First-order denitrification rate constants varied across the HSSFCW influent zone, ranging between 0.005–0.035 min<sup>−1</sup> for the well-mixed model and 0.004–0.027 min<sup>−1</sup> for the plug-flow model. The heterotrophic denitrification yield coefficient <em>Yd<sub>H</sub></em> values averaged at 0.55 ± 0.33. Different oxygen utilization routes were identified, with the bulk consumed in multiple biological processes, a small portion lost to trapped gas bubbles and an insignificant amount to chemical reactions. The results of this study demonstrate the potential of using SWPPTs to measure heterotrophic aerobic and denitrifying degradation rate constants and yield in situ in HSSFCWs.","PeriodicalId":270,"journal":{"name":"Chemical Engineering Journal","volume":"82 1","pages":""},"PeriodicalIF":15.1,"publicationDate":"2025-02-04","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143124362","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 excessive usage of value-added sacrificial agents and poor carrier separation constrain the development of photocatalytic H2 production. To address these challenges, we propose a waste-to-energy conception by utilizing pollutants as sacrificial agents in heterojunctions with potent carrier separation. Herein, a dual Z-scheme ZnCo2O4/C-TiO2/ZnIn2S4 (ZCO/CTO/ZIS) heterojunction was successfully constructed from MOFs with effective carrier separation to integrate H2 production and organic pollutants degradation in a single photo-redox process. When ciprofloxacin (CIP), a prevalent aquatic contaminant, was substituted for the sacrificial agents to utilize the energy of holes, the dual Z-scheme photocatalyst exhibited excellent hydrogen production performance (∼4.93 ). Concurrently, the degradation of CIP was up to 92.21 %, with a 66.71 % mineralization rate. The experimental results combined with theoretical calculations revealed that the interfacial electron field formed at dual Z-scheme ZCO/CTO/ZIS affords fast pathways for charge transfer to achieve the high performance of simultaneous reactions. Additionally, the low toxicity of the degradation intermediates during the bifunctional photocatalysis process implies that this is an environment-friendly route to obtain clean energy. This study provides a feasible strategy for constructing dual Z-scheme photocatalysts from MOFs to alleviate energy crises and environmental pollution.
{"title":"Integrating photocatalytic hydrogen evolution with antibiotic degradation over a dual Z-scheme heterojunction","authors":"Churu Zhang, Shuai Hu, Weigang Cui, Shuangjiang Li, Long Tian, Xinggen Yuan, Waseem Tariq, Kaili Yao, Yunfei Zhi, Tianding Hu, Shaoyun Shan","doi":"10.1016/j.cej.2025.160317","DOIUrl":"https://doi.org/10.1016/j.cej.2025.160317","url":null,"abstract":"The excessive usage of value-added sacrificial agents and poor carrier separation constrain the development of photocatalytic H<sub>2</sub> production. To address these challenges, we propose a waste-to-energy conception by utilizing pollutants as sacrificial agents in heterojunctions with potent carrier separation. Herein, a dual Z-scheme ZnCo<sub>2</sub>O<sub>4</sub>/C-TiO<sub>2</sub>/ZnIn<sub>2</sub>S<sub>4</sub> (ZCO/CTO/ZIS) heterojunction was successfully constructed from MOFs with effective carrier separation to integrate H<sub>2</sub> production and organic pollutants degradation in a single photo-redox process. When ciprofloxacin (CIP), a prevalent aquatic contaminant, was substituted for the sacrificial agents to utilize the energy of holes, the dual Z-scheme photocatalyst exhibited excellent hydrogen production performance (∼4.93 <span><math><mrow is=\"true\"><msup is=\"true\"><mrow is=\"true\"><mtext is=\"true\">mmol g</mtext></mrow><mrow is=\"true\"><mspace is=\"true\" width=\"0.333333em\"></mspace><mtext is=\"true\">- 1</mtext></mrow></msup><msup is=\"true\"><mrow is=\"true\"><mspace is=\"true\" width=\"0.333333em\"></mspace><mtext is=\"true\">h</mtext></mrow><mrow is=\"true\"><mspace is=\"true\" width=\"0.333333em\"></mspace><mtext is=\"true\">- 1</mtext></mrow></msup></mrow></math></span>). Concurrently, the degradation of CIP was up to 92.21 %, with a 66.71 % mineralization rate. The experimental results combined with theoretical calculations revealed that the interfacial electron field formed at dual Z-scheme ZCO/CTO/ZIS affords fast pathways for charge transfer to achieve the high performance of simultaneous reactions. Additionally, the low toxicity of the degradation intermediates during the bifunctional photocatalysis process implies that this is an environment-friendly route to obtain clean energy. This study provides a feasible strategy for constructing dual Z-scheme photocatalysts from MOFs to alleviate energy crises and environmental pollution.","PeriodicalId":270,"journal":{"name":"Chemical Engineering Journal","volume":"61 1","pages":""},"PeriodicalIF":15.1,"publicationDate":"2025-02-04","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143124364","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 : 2025-02-04DOI: 10.1016/j.cej.2025.160293
Dandan Che, Yao Xiao, Xiaoyong Zhang, Kai Zhu, Wanyi Chen, Guoxing You, Yongming Yao, Hong Zhou, Gan Chen
Acute liver injury is a common complication of sepsis, making it one of the most challenging problems in intensive clinical care. Currently, no specific therapies are available for sepsis and sepsis-induced liver injury. Herein, we developed novel multifunctional polyphenol-copper nanozymes (Cu-CA NZs) with excellent biocompatibility and explored their therapeutic effect in sepsis and sepsis-induced acute liver injury. The Cu-CA NZs exhibited broad-spectrum non-antibiotic antibacterial and robust cascade superoxide dismutase- and catalase-mimicking activities. Further, the Cu-CA NZs diminished the lipopolysaccharide-induced inflammatory response and decreased mitochondrial damage in an in vitro macrophage inflammatory model. Moreover, Cu-CA NZs treatment dramatically mitigated liver injury biomarkers in the plasma, reduced hepatic oxidative stress and inflammatory responses, stimulated hepatic M1-type to M2 macrophage polarization, and improved the survival rate of septic mice. Mechanistically, the therapeutic effect of Cu-CA NZs may be mediated by alleviating excessive endoplasmic reticulum stress in the liver via the eIF2α/ATF4/CHOP pathway during sepsis. Thus, Cu-CA NZs are promising therapeutic candidates for treating sepsis and other inflammatory diseases.
{"title":"Multifunctional integrated polyphenol-copper nanozymes for sepsis-induced acute liver injury via ameliorating endoplasmic reticulum stress and reprogramming inflammatory microenvironment","authors":"Dandan Che, Yao Xiao, Xiaoyong Zhang, Kai Zhu, Wanyi Chen, Guoxing You, Yongming Yao, Hong Zhou, Gan Chen","doi":"10.1016/j.cej.2025.160293","DOIUrl":"https://doi.org/10.1016/j.cej.2025.160293","url":null,"abstract":"Acute liver injury is a common complication of sepsis, making it one of the most challenging problems in intensive clinical care. Currently, no specific therapies are available for sepsis and sepsis-induced liver injury. Herein, we developed novel multifunctional polyphenol-copper nanozymes (Cu-CA NZs) with excellent biocompatibility and explored their therapeutic effect in sepsis and sepsis-induced acute liver injury. The Cu-CA NZs exhibited broad-spectrum non-antibiotic antibacterial and robust cascade superoxide dismutase- and catalase-mimicking activities. Further, the Cu-CA NZs diminished the lipopolysaccharide-induced inflammatory response and decreased mitochondrial damage in an <em>in vitro</em> macrophage inflammatory model. Moreover, Cu-CA NZs treatment dramatically mitigated liver injury biomarkers in the plasma, reduced hepatic oxidative stress and inflammatory responses, stimulated hepatic M1-type to M2 macrophage polarization, and improved the survival rate of septic mice. Mechanistically, the therapeutic effect of Cu-CA NZs may be mediated by alleviating excessive endoplasmic reticulum stress in the liver via the eIF2α/ATF4/CHOP pathway during sepsis. Thus, Cu-CA NZs are promising therapeutic candidates for treating sepsis and other inflammatory diseases.","PeriodicalId":270,"journal":{"name":"Chemical Engineering Journal","volume":"136 1","pages":""},"PeriodicalIF":15.1,"publicationDate":"2025-02-04","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143124724","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 : 2025-02-04DOI: 10.1016/j.cej.2025.160285
Jinwu Bai, Kai Li, Zihang Zhang, Zhenzhong Hu, Mengmeng Zhen
Lithium–sulfur batteries (LSBs) with various advantages including high energy density, low costs and environmental friendliness, have been considered as one of the most promising advanced rechargeable batteries. Although great achievements have been realized in recent years, these test conditions are generally carried out under excess electrolyte (electrolyte-to-sulfur (E/S) ratio > 10.0 µL mg−1), significantly hindering practical energy density improvements of LSBs. The lean electrolyte is a key factor for improving the energy density of LSBs, yet several tough issues under lean electrolyte, such as shuttle effect, sluggish reaction kinetics and side reaction, seriously hinder the improvement of battery performances. Transition metals@MXenes have been considered as ideal electrocatalysts for regulating redox reaction of LSBs due to their metallic conductivity, large polar surface and abundant active sites. Nevertheless, a in-depth overview of transition metals@MXenes electrocatalysts for lean electrolyte LSBs is still lacking. This review aims to fill this gap by providing a detailed analysis of the mechanisms, challenges, and solutions associated with lean electrolyte LSBs. It focuses on the role of transition metals@MXenes in regulating redox reactions and improving lithium plating/stripping behaviors, particularly in high-concentration lithium polysulfide (LiPS) environments. The review also discusses the structure–activity relationship of these electrocatalysts, highlighting their potential to mitigate the shuttle effect and enhance reaction kinetics. Furthermore, the review presents the latest advancements in the application of transition metals@MXenes for high-performance lean electrolyte LSBs and proposes future research directions to advance their development in the energy storage field.
{"title":"Transition Metals@MXenes electrocatalysts for high-performance Lithium–Sulfur batteries under lean electrolyte: A comprehensive review","authors":"Jinwu Bai, Kai Li, Zihang Zhang, Zhenzhong Hu, Mengmeng Zhen","doi":"10.1016/j.cej.2025.160285","DOIUrl":"https://doi.org/10.1016/j.cej.2025.160285","url":null,"abstract":"Lithium–sulfur batteries (LSBs) with various advantages including high energy density, low costs and environmental friendliness, have been considered as one of the most promising advanced rechargeable batteries. Although great achievements have been realized in recent years, these test conditions are generally carried out under excess electrolyte (electrolyte-to-sulfur (E/S) ratio > 10.0 µL mg<sup>−1</sup>), significantly hindering practical energy density improvements of LSBs. The lean electrolyte is a key factor for improving the energy density of LSBs, yet several tough issues under lean electrolyte, such as shuttle effect, sluggish reaction kinetics and side reaction, seriously hinder the improvement of battery performances. Transition metals@MXenes have been considered as ideal electrocatalysts for regulating redox reaction of LSBs due to their metallic conductivity, large polar surface and abundant active sites. Nevertheless, a in-depth overview of transition metals@MXenes electrocatalysts for lean electrolyte LSBs is still lacking. This review aims to fill this gap by providing a detailed analysis of the mechanisms, challenges, and solutions associated with lean electrolyte LSBs. It focuses on the role of transition metals@MXenes in regulating redox reactions and improving lithium plating/stripping behaviors, particularly in high-concentration lithium polysulfide (LiPS) environments. The review also discusses the structure–activity relationship of these electrocatalysts, highlighting their potential to mitigate the shuttle effect and enhance reaction kinetics. Furthermore, the review presents the latest advancements in the application of transition metals@MXenes for high-performance lean electrolyte LSBs and proposes future research directions to advance their development in the energy storage field.","PeriodicalId":270,"journal":{"name":"Chemical Engineering Journal","volume":"76 1","pages":""},"PeriodicalIF":15.1,"publicationDate":"2025-02-04","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143124777","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 : 2025-02-04DOI: 10.1016/j.cej.2025.160182
Yuxia Tang, Meng Dang, Yang Li, Xuan Sha, Ziqing Xu, Jie Zhang, Feiyun Wu, Shouju Wang
Disulfiram (DSF) has gained interest for its anti-cancer potential, but its clinical application is hindered by its poor solubility, short half-life, and lack of tumor targeting. Nanotechnology has been employed to address these challenges, with various strategies developed for DSF delivery. However, these methods face issues such as low drug loading and complex synthesis. We present an in situ activatable Disulfiram-Rhodium (III) nanocomplex that surmounts these obstacles. Our nanocomplex self-assembles DSF with Rhodium (III) complexes, offering high drug loading, tumor microenvironment activation, and copper ion chelation. It also inhibits the STAT3 pathway, activating the immune environment and enhancing the anti-tumor immune response. Additionally, loading with Ce6 potentiates photodynamic and immunotherapy, providing synergistic effects. This novel nanocomplex holds promise for improved cancer treatment through enhanced targeting, activation, and therapeutic synergy.
{"title":"In situ activatable Disulfiram-Rhodium(III) nanocomplex for Cu chelation and STAT3 inhibition to Potentiate photodynamic and immunotherapy","authors":"Yuxia Tang, Meng Dang, Yang Li, Xuan Sha, Ziqing Xu, Jie Zhang, Feiyun Wu, Shouju Wang","doi":"10.1016/j.cej.2025.160182","DOIUrl":"https://doi.org/10.1016/j.cej.2025.160182","url":null,"abstract":"Disulfiram (DSF) has gained interest for its anti-cancer potential, but its clinical application is hindered by its poor solubility, short half-life, and lack of tumor targeting. Nanotechnology has been employed to address these challenges, with various strategies developed for DSF delivery. However, these methods face issues such as low drug loading and complex synthesis. We present an in situ activatable Disulfiram-Rhodium (III) nanocomplex that surmounts these obstacles. Our nanocomplex self-assembles DSF with Rhodium (III) complexes, offering high drug loading, tumor microenvironment activation, and copper ion chelation. It also inhibits the STAT3 pathway, activating the immune environment and enhancing the anti-tumor immune response. Additionally, loading with Ce6 potentiates photodynamic and immunotherapy, providing synergistic effects. This novel nanocomplex holds promise for improved cancer treatment through enhanced targeting, activation, and therapeutic synergy.","PeriodicalId":270,"journal":{"name":"Chemical Engineering Journal","volume":"134 1","pages":""},"PeriodicalIF":15.1,"publicationDate":"2025-02-04","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143124351","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 : 2025-02-04DOI: 10.1016/j.cej.2025.160191
Donghyeok Kim, Myeung-Jin Lee, Yejin Choi, Jongkyoung Kim, Bora Jeong, Bora Ye, Seungho Cho, Hong-Dae Kim
NOx emissions are a major environmental issue, and NH3-SCR is a key method for their control. V-based catalysts perform well at high temperatures; however, SO2-poisoning remains a critical issue for NH3-SCR catalysts under low-temperature conditions. In this study, we develop an effective strategy of loading a stable sulfide two-dimensional (2D) material, WS2, to enhance the SO2 resistance of existing commercial V/Ti catalysts. In-situ DRIFTS analysis and spent SO2-poisoning catalyst analyses are conducted to clarify the enhanced SO2 resistance mechanism. These findings demonstrate that the superior SO2 resistance can be attributed to the suppression of SO2 by WS2. Therefore, WS2 loading inhibits the SO2 adsorption and protects the NH3 species adsorption, thereby enhancing the SO2 resistance and low-temperature activity. This research can be utilized without changing the catalyst synthesis process, allowing it to be applied to current commercial catalysts, thereby underscoring its remarkable potential for industrial applications.
{"title":"Enhancing SO2 resistance in vanadium catalysts with tungsten disulfide for NH3-SCR","authors":"Donghyeok Kim, Myeung-Jin Lee, Yejin Choi, Jongkyoung Kim, Bora Jeong, Bora Ye, Seungho Cho, Hong-Dae Kim","doi":"10.1016/j.cej.2025.160191","DOIUrl":"https://doi.org/10.1016/j.cej.2025.160191","url":null,"abstract":"NO<sub>x</sub> emissions are a major environmental issue, and NH<sub>3</sub>-SCR is a key method for their control. V-based catalysts perform well at high temperatures; however, SO<sub>2</sub>-poisoning remains a critical issue for NH<sub>3</sub>-SCR catalysts under low-temperature conditions. In this study, we develop an effective strategy of loading a stable sulfide two-dimensional (2D) material, WS<sub>2</sub>, to enhance the SO<sub>2</sub> resistance of existing commercial V/Ti catalysts. In-situ DRIFTS analysis and spent SO<sub>2</sub>-poisoning catalyst analyses are conducted to clarify the enhanced SO<sub>2</sub> resistance mechanism. These findings demonstrate that the superior SO<sub>2</sub> resistance can be attributed to the suppression of SO<sub>2</sub> by WS<sub>2</sub>. Therefore, WS<sub>2</sub> loading inhibits the SO<sub>2</sub> adsorption and protects the NH<sub>3</sub> species adsorption, thereby enhancing the SO<sub>2</sub> resistance and low-temperature activity. This research can be utilized without changing the catalyst synthesis process, allowing it to be applied to current commercial catalysts, thereby underscoring its remarkable potential for industrial applications.","PeriodicalId":270,"journal":{"name":"Chemical Engineering Journal","volume":"37 1","pages":""},"PeriodicalIF":15.1,"publicationDate":"2025-02-04","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143124359","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 : 2025-02-04DOI: 10.1016/j.cej.2025.160294
Yunhao Wang, Lei Ding, Ziguo Lin, Baolong Li, Di Hu, Shichen Zhang, Shujun Zhou, Yuxiang Ning, Fei Xin, Yunfei Ying, Fukai Zhu, Peiyuan Wang, Yanfeng Wang
Immune checkpoint inhibitors (ICIs) are among the most prominent immunotherapies for cancer and have been approved as first-line treatments for various tumors. Although some patients experience long-lasting responses, the objective response rate (ORR) of ICIs as monotherapy is relatively low due to the complexity of the tumor microenvironment and the heterogeneity of tumors. Maximizing the benefits of this novel therapeutic approach for a greater number of patients remains a research focus in the field of anticancer treatment. Here, we have investigated a novel Pt/Cu Dual-Atom Nanozyme (Pt/Cu DAzyme) which is engineered by the successive growth of metal-nanocrystals on the assembled surfactant templates. This DAzyme can significantly enhance the intracellular copper ion levels in tumor cells, inducing cuproptosis. Additionally, the Pt/Cu DAzyme exhibits excellent dual enzyme catalytic activity as both glutathione oxidase (GSHOx) and peroxidase (POD) activity, which not only reduces glutathione (GSH) levels in tumors to enhance cuproptosis but also converts intracellular H2O2 into •OH to kill tumor cells. Furthermore, the Pt/Cu DAzyme demonstrates a strong photothermal effect, with its enzymatic reactions being enhanced at mildly elevated temperatures. This DAzyme effectively kills tumors and activates the body’s robust immune system, reshaping the tumor immune-suppressive microenvironment and significantly increasing the therapeutic response rate to αPD-L1. It not only achieves complete ablation of primary tumors but also markedly inhibits the progression of distal tumors and distant metastasis. This study aims to develop new combination therapy strategies to enhance the efficacy of ICIs and promote their advancement in the field of cancer immunotherapy.
{"title":"Mesoporous dual-atom nanozyme induced cuproptosis and apoptosis for boosting immunogenic cell death along with reprogramming tumor immune-suppressive microenvironment","authors":"Yunhao Wang, Lei Ding, Ziguo Lin, Baolong Li, Di Hu, Shichen Zhang, Shujun Zhou, Yuxiang Ning, Fei Xin, Yunfei Ying, Fukai Zhu, Peiyuan Wang, Yanfeng Wang","doi":"10.1016/j.cej.2025.160294","DOIUrl":"https://doi.org/10.1016/j.cej.2025.160294","url":null,"abstract":"Immune checkpoint inhibitors (ICIs) are among the most prominent immunotherapies for cancer and have been approved as first-line treatments for various tumors. Although some patients experience long-lasting responses, the objective response rate (ORR) of ICIs as monotherapy is relatively low due to the complexity of the tumor microenvironment and the heterogeneity of tumors. Maximizing the benefits of this novel therapeutic approach for a greater number of patients remains a research focus in the field of anticancer treatment. Here, we have investigated a novel Pt/Cu Dual-Atom Nanozyme (Pt/Cu DAzyme) which is engineered by the successive growth of metal-nanocrystals on the assembled surfactant templates. This DAzyme can significantly enhance the intracellular copper ion levels in tumor cells, inducing cuproptosis. Additionally, the Pt/Cu DAzyme exhibits excellent dual enzyme catalytic activity as both glutathione oxidase (GSHOx) and peroxidase (POD) activity, which not only reduces glutathione (GSH) levels in tumors to enhance cuproptosis but also converts intracellular H<sub>2</sub>O<sub>2</sub> into •OH to kill tumor cells. Furthermore, the Pt/Cu DAzyme demonstrates a strong photothermal effect, with its enzymatic reactions being enhanced at mildly elevated temperatures. This DAzyme effectively kills tumors and activates the body’s robust immune system, reshaping the tumor immune-suppressive microenvironment and significantly increasing the therapeutic response rate to αPD-L1. It not only achieves complete ablation of primary tumors but also markedly inhibits the progression of distal tumors and distant metastasis. This study aims to develop new combination therapy strategies to enhance the efficacy of ICIs and promote their advancement in the field of cancer immunotherapy.","PeriodicalId":270,"journal":{"name":"Chemical Engineering Journal","volume":"40 1","pages":""},"PeriodicalIF":15.1,"publicationDate":"2025-02-04","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143124360","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 : 2025-02-04DOI: 10.1016/j.cej.2025.160305
Kexin Xu, Li Wang, Xinghua Zhang, Xuehai Wang, Yimin Zhu
High efficient NO adsorption on zeolites not only accelerates catalytic NO to N2 by concentrating, but also figures out the difficulty of removing NO with low temperature and low concentration. This study evaluates the dynamic NO adsorption–desorption behaviors on 12 commercial zeolites, demonstrating 13X and 5A zeolites as excellent adsorbents with high NO adsorption capacity and low regeneration temperature. Based on extensive characterizations including N2-physisorption, NH3-TPD, CO2-TPD, on-line MS and in-situ DRIFTS, the pore structure-performance relationship, acidity-performance relationship and basicity-performance relationship have been thoroughly investigated and discussed upon NO adsorption–desorption behaviors, together with the gaseous and surface species. NO directly coordinates to the strong Lewis acid sites and strong base sites (i.e., strong Lewis acid-base pairs), leading to coordinately bonded NOδ+ and NOδ- species, respectively. Besides, NO also directly disproportionates to N2O and NO2, followed by in-situ conversion of NO2 into nitrate species. Thus, the coordination and disproportionation mechanisms have been identified for high-efficient NO adsorption on 13X and 5A zeolites, which supplements the current understandings of NO adsorption on zeolites and provides a new strategy to strengthen NO adsorption on zeolites with strong Lewis acid-base pairs.
{"title":"Disproportionation and coordination driven high-efficient NO adsorption on FAU-and LTA-type zeolites","authors":"Kexin Xu, Li Wang, Xinghua Zhang, Xuehai Wang, Yimin Zhu","doi":"10.1016/j.cej.2025.160305","DOIUrl":"https://doi.org/10.1016/j.cej.2025.160305","url":null,"abstract":"High efficient NO adsorption on zeolites not only accelerates catalytic NO to N<sub>2</sub> by concentrating, but also figures out the difficulty of removing NO with low temperature and low concentration. This study evaluates the dynamic NO adsorption–desorption behaviors on 12 commercial zeolites, demonstrating 13X and 5A zeolites as excellent adsorbents with high NO adsorption capacity and low regeneration temperature. Based on extensive characterizations including N<sub>2</sub>-physisorption, NH<sub>3</sub>-TPD, CO<sub>2</sub>-TPD, <em>on-line</em> MS and <em>in-situ</em> DRIFTS, the pore structure-performance relationship, acidity-performance relationship and basicity-performance relationship have been thoroughly investigated and discussed upon NO adsorption–desorption behaviors, together with the gaseous and surface species. NO directly coordinates to the strong Lewis acid sites and strong base sites (i.e., strong Lewis acid-base pairs), leading to coordinately bonded NO<sup>δ+</sup> and NO<sup>δ-</sup> species, respectively. Besides, NO also directly disproportionates to N<sub>2</sub>O and NO<sub>2</sub>, followed by in-situ conversion of NO<sub>2</sub> into nitrate species. Thus, the coordination and disproportionation mechanisms have been identified for high-efficient NO adsorption on 13X and 5A zeolites, which supplements the current understandings of NO adsorption on zeolites and provides a new strategy to strengthen NO adsorption on zeolites with strong Lewis acid-base pairs.","PeriodicalId":270,"journal":{"name":"Chemical Engineering Journal","volume":"11 1","pages":""},"PeriodicalIF":15.1,"publicationDate":"2025-02-04","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143124723","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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