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Improvement of the oxidation efficiency of photogenerated holes at ferric single-atom catalysts via ferric-nitrogen co-sculpted carbon defect engineering
IF 15.1 1区 工程技术 Q1 ENGINEERING, CHEMICAL Pub Date : 2025-01-27 DOI: 10.1016/j.cej.2025.159996
Faze Chen, Zilian Liu, Rongrong Miao, Huajing Zhou, Liang He, Sheng Liang, Xin Lei, Qingqing Guan
Direct oxidation of organic pollutants by visible-light-generated holes is considered a promising technique for remediating contaminated water bodies. However, random and rapid recombination of photogenerated holes and electrons hampers the accumulation of holes on catalyst surface. To address this challenge, a strategy involving the co-etching of bagasse pith parenchyma cells with iron and nitrogen was proposed, creating an Fe-N-C catalyst with a web-like fibrous structure and abundant carbon defects. This iron and nitrogen co-etching strategy endowed the Fe-N-C catalyst with not only ultrafast photogenerated electron transfer and capture capabilities but also enabled it to have abundant and accessible surface-active sites, co-facilitating rapid and efficient electron transfer between pollutants and holes. Thus, compared to pure bagasse pith carbon or nitrogen-doped carbon, the optimized Fe-N-C single-atom catalysts (SACs) exhibited a significant enhancement in the photocatalytic oxidation kinetics of tetracycline (TC) by 16.47 and 5.38 times, respectively, with the maximum degradation efficiency increasing from 25.6% and 48.6% to 99.6%. Based on theoretical and experimental analyses, the toxicity of TC-contaminated water was significantly reduced after treatment with the Fe-N-C catalyst. Through analyzing the material characterization and photocatalytic behavior, a structure-performance correlation that links intrinsic carbon defects to effective surface hole transfer in Fe-N-C was established and validated. From the perspective of holes as the primary active sites, this work offered a promising approach to enhancing the overall photocatalytic oxidation efficiency of Fe-N-C SACs.
{"title":"Improvement of the oxidation efficiency of photogenerated holes at ferric single-atom catalysts via ferric-nitrogen co-sculpted carbon defect engineering","authors":"Faze Chen, Zilian Liu, Rongrong Miao, Huajing Zhou, Liang He, Sheng Liang, Xin Lei, Qingqing Guan","doi":"10.1016/j.cej.2025.159996","DOIUrl":"https://doi.org/10.1016/j.cej.2025.159996","url":null,"abstract":"Direct oxidation of organic pollutants by visible-light-generated holes is considered a promising technique for remediating contaminated water bodies. However, random and rapid recombination of photogenerated holes and electrons hampers the accumulation of holes on catalyst surface. To address this challenge, a strategy involving the co-etching of bagasse pith parenchyma cells with iron and nitrogen was proposed, creating an Fe-N-C catalyst with a web-like fibrous structure and abundant carbon defects. This iron and nitrogen co-etching strategy endowed the Fe-N-C catalyst with not only ultrafast photogenerated electron transfer and capture capabilities but also enabled it to have abundant and accessible surface-active sites, co-facilitating rapid and efficient electron transfer between pollutants and holes. Thus, compared to pure bagasse pith carbon or nitrogen-doped carbon, the optimized Fe-N-C single-atom catalysts (SACs) exhibited a significant enhancement in the photocatalytic oxidation kinetics of tetracycline (TC) by 16.47 and 5.38 times, respectively, with the maximum degradation efficiency increasing from 25.6% and 48.6% to 99.6%. Based on theoretical and experimental analyses, the toxicity of TC-contaminated water was significantly reduced after treatment with the Fe-N-C catalyst. Through analyzing the material characterization and photocatalytic behavior, a structure-performance correlation that links intrinsic carbon defects to effective surface hole transfer in Fe-N-C was established and validated. From the perspective of holes as the primary active sites, this work offered a promising approach to enhancing the overall photocatalytic oxidation efficiency of Fe-N-C SACs.","PeriodicalId":270,"journal":{"name":"Chemical Engineering Journal","volume":"35 1","pages":""},"PeriodicalIF":15.1,"publicationDate":"2025-01-27","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143050570","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}
引用次数: 0
Selective removal of microcystin from eutrophic water by a nanobody-metal hybrid photocatalyst
IF 15.1 1区 工程技术 Q1 ENGINEERING, CHEMICAL Pub Date : 2025-01-27 DOI: 10.1016/j.cej.2025.159993
Xiao Dai, Qi Chen, Jia Hu, Yunkai Fan, Ying Xiong, Xiaoyang Li
Microcystin-LR (MC-LR) is a major contaminant in food and the environment, posing a significant public health risk. However, targeted degradation of MC-LR in complex systems remains a challenging task. In this study, we rationally designed a hierarchically structured nanobody-metal hybrid photocatalyst with both high affinity for MC-LR and excellent photocatalytic activity. Due to the synergistic and proximity effects between nanobody and photocatalyst, the degradation efficiency of Ag/AgCl/BSA-Nb hybrid catalyst achieved a degradation rate 2.3 times higher than that of Ag/AgCl/BSA in eutrophic water. Nearly 100% degradation of MC-LR was achieved within 30 min under visible light irradiation. The degradation pathways of MC-LR were analyzed using UPLC-Q-TOF MS. The hepatotoxicity of the MC-LR transformation products was significantly reduced compared to that of MC-LR. Ag/AgCl/BSA-Nb demonstrated excellent reusability and a good industrial application prospect.
{"title":"Selective removal of microcystin from eutrophic water by a nanobody-metal hybrid photocatalyst","authors":"Xiao Dai, Qi Chen, Jia Hu, Yunkai Fan, Ying Xiong, Xiaoyang Li","doi":"10.1016/j.cej.2025.159993","DOIUrl":"https://doi.org/10.1016/j.cej.2025.159993","url":null,"abstract":"Microcystin-LR (MC-LR) is a major contaminant in food and the environment, posing a significant public health risk. However, targeted degradation of MC-LR in complex systems remains a challenging task. In this study, we rationally designed a hierarchically structured nanobody-metal hybrid photocatalyst with both high affinity for MC-LR and excellent photocatalytic activity. Due to the synergistic and proximity effects between nanobody and photocatalyst, the degradation efficiency of Ag/AgCl/BSA-Nb hybrid catalyst achieved a degradation rate 2.3 times higher than that of Ag/AgCl/BSA in eutrophic water. Nearly 100% degradation of MC-LR was achieved within 30 min under visible light irradiation. The degradation pathways of MC-LR were analyzed using UPLC-Q-TOF MS. The hepatotoxicity of the MC-LR transformation products was significantly reduced compared to that of MC-LR. Ag/AgCl/BSA-Nb demonstrated excellent reusability and a good industrial application prospect.","PeriodicalId":270,"journal":{"name":"Chemical Engineering Journal","volume":"6 1","pages":""},"PeriodicalIF":15.1,"publicationDate":"2025-01-27","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143050571","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}
引用次数: 0
Silk fibroin for cosmetic dermatology
IF 15.1 1区 工程技术 Q1 ENGINEERING, CHEMICAL Pub Date : 2025-01-27 DOI: 10.1016/j.cej.2025.159986
Songjie Li, Han Chen, Xin Dan, Yikun Ju, Tong Li, Bo Liu, Yang Li, Lanjie Lei, Xing Fan
People are increasingly focusing on skin health and maintenance because of improvements in living standards. Skin damage and defects caused by various factors and skin aging, spots, and pigmentation due to the passage of time and improper maintenance can be improved and restored via the beautification of the skin. A plethora of additives are used in cosmetic dermatology applications including silk fibroin (SF), which is increasingly being used due to its significant role in enhancing skin luster and elasticity, reducing pigmentation, combating skin aging, and promoting scalp care owing to its unique moisturizing, anti-inflammatory, and antioxidant properties. Additionally, SF is a low-cost, easy-to-use biomaterial that displays high biocompatibility, controllable biodegradability, and adjustable mechanical properties, which facilitate its application in the field of cosmetic dermatology. SF may offer superior solutions to skin problems. This review describes the compositional structure of SF and introduces its relevant properties in the context of cosmetic dermatology. The sources and cross-linked forms of SF, along with several extraction methods are summarized, and several SF application strategies are listed, including hydrogels, sponges, films, microspheres and microneedles. Additionally, this review describes the biofunctionalization of active molecules on SF and provides a detailed introduction to the role of SF in skin beauty, including skin whitening, firming and lifting, anti-aging, wrinkle reduction, moisturizing, and nourishing. Finally, we summarize the content and forecast future research regarding SF.
{"title":"Silk fibroin for cosmetic dermatology","authors":"Songjie Li, Han Chen, Xin Dan, Yikun Ju, Tong Li, Bo Liu, Yang Li, Lanjie Lei, Xing Fan","doi":"10.1016/j.cej.2025.159986","DOIUrl":"https://doi.org/10.1016/j.cej.2025.159986","url":null,"abstract":"People are increasingly focusing on skin health and maintenance because of improvements in living standards. Skin damage and defects caused by various factors and skin aging, spots, and pigmentation due to the passage of time and improper maintenance can be improved and restored via the beautification of the skin. A plethora of additives are used in cosmetic dermatology applications including silk fibroin (SF), which is increasingly being used due to its significant role in enhancing skin luster and elasticity, reducing pigmentation, combating skin aging, and promoting scalp care owing to its unique moisturizing, anti-inflammatory, and antioxidant properties. Additionally, SF is a low-cost, easy-to-use biomaterial that displays high biocompatibility, controllable biodegradability, and adjustable mechanical properties, which facilitate its application in the field of cosmetic dermatology. SF may offer superior solutions to skin problems. This review describes the compositional structure of SF and introduces its relevant properties in the context of cosmetic dermatology. The sources and cross-linked forms of SF, along with several extraction methods are summarized, and several SF application strategies are listed, including hydrogels, sponges, films, microspheres and microneedles. Additionally, this review describes the biofunctionalization of active molecules on SF and provides a detailed introduction to the role of SF in skin beauty, including skin whitening, firming and lifting, anti-aging, wrinkle reduction, moisturizing, and nourishing. Finally, we summarize the content and forecast future research regarding SF.","PeriodicalId":270,"journal":{"name":"Chemical Engineering Journal","volume":"119 1","pages":""},"PeriodicalIF":15.1,"publicationDate":"2025-01-27","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143050781","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}
引用次数: 0
Maintaining cardiac homeostasis by translational selenium nanoparticles with rapid selenoproteins regulation to achieve radiation-induced heart prevention
IF 15.1 1区 工程技术 Q1 ENGINEERING, CHEMICAL Pub Date : 2025-01-27 DOI: 10.1016/j.cej.2025.160005
Kewei Jin, Sujiang Shi, Dina Huang, Hongwei Huang, Binhua Zou, Wei Huang, Tianfeng Chen
Radiation-induced heart disease (RIHD) typically manifests as severe oxidative stress and immune dysregulation, which are serious sequela affecting cancer patients. Therefore, developing radioprotector that capable of inhibiting oxidative stress and regulating the immune microenvironment simultaneously is urgently desired. Selenium (Se), as the active center of antioxidant selenoproteins, is widely recognized as a promising therapeutic element in antioxidative stress therapy. Therefore, translational elemental Se nanoparticles decorated by lentinan (Se@LET) was developed and its preventive efficacy and mechanism in RIHD were systematically analyzed by comparing with four types of organic Se. In vitro experiments revealed because its rapid biotransformation to antioxidant selenoproteins, Se@LET alleviated the overproduction of ROS caused by X-Ray and further prevented G2/M phase arrest and DNA damage in cells, thus achieving superior heart prevention than other organic selenides. Meanwhile, Se@LET effectively regulated macrophage polarization and inhibit radiation-induced inflammation. Consequently, the administration of Se@LET before and after radiation showed outstanding protective effects on RIHD in vivo by regulating myocardial immunosuppressive microenvironment, but also suppressed the side effects of X-Ray. Collectively, this study demonstrates a valuable strategy for irradiation prevention by using translational element Se nanospecies and provides an attractive clinical alternative for heart protection to prevent RIHD.
{"title":"Maintaining cardiac homeostasis by translational selenium nanoparticles with rapid selenoproteins regulation to achieve radiation-induced heart prevention","authors":"Kewei Jin, Sujiang Shi, Dina Huang, Hongwei Huang, Binhua Zou, Wei Huang, Tianfeng Chen","doi":"10.1016/j.cej.2025.160005","DOIUrl":"https://doi.org/10.1016/j.cej.2025.160005","url":null,"abstract":"Radiation-induced heart disease (RIHD) typically manifests as severe oxidative stress and immune dysregulation, which are serious sequela affecting cancer patients. Therefore, developing radioprotector that capable of inhibiting oxidative stress and regulating the immune microenvironment simultaneously is urgently desired. Selenium (Se), as the active center of antioxidant selenoproteins, is widely recognized as a promising therapeutic element in antioxidative stress therapy. Therefore, translational elemental Se nanoparticles decorated by lentinan (Se@LET) was developed and its preventive efficacy and mechanism in RIHD were systematically analyzed by comparing with four types of organic Se. <em>In vitro</em> experiments revealed because its rapid biotransformation to antioxidant selenoproteins, Se@LET alleviated the overproduction of ROS caused by X-Ray and further prevented G2/M phase arrest and DNA damage in cells, thus achieving superior heart prevention than other organic selenides. Meanwhile, Se@LET effectively regulated macrophage polarization and inhibit radiation-induced inflammation. Consequently, the administration of Se@LET before and after radiation showed outstanding protective effects on RIHD <em>in vivo</em> by regulating myocardial immunosuppressive microenvironment, but also suppressed the side effects of X-Ray. Collectively, this study demonstrates a valuable strategy for irradiation prevention by using translational element Se nanospecies and provides an attractive clinical alternative for heart protection to prevent RIHD.","PeriodicalId":270,"journal":{"name":"Chemical Engineering Journal","volume":"59 1","pages":""},"PeriodicalIF":15.1,"publicationDate":"2025-01-27","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143050784","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}
引用次数: 0
Elastomer foam templated three dimensional hybrid hydrogels for heterogeneously integrated stretchable electronics
IF 15.1 1区 工程技术 Q1 ENGINEERING, CHEMICAL Pub Date : 2025-01-27 DOI: 10.1016/j.cej.2025.159937
Changqing Qin, Qian Wang, Ting Fang, Lin Wang, Cheng Yang, Yong Lin, Chong Bai, Wenqiang He, Likang Ding, Jinheng Zhang, Dongchan Li, Desheng Kong
Hydrogels are soft, tissue-like solids with promising potential in biomedical engineering and stretchable electronics. These applications require hydrogels to be shaped into intricate structures and combined with other polymers. This study introduces hybrid hydrogels that use elastomer foams as templates for controlled synthesis. Essentially, TPU foams can be easily structured into diverse 2D or 3D shapes using laser ablation. After hydrophilic modification, these foams absorb hydrogel precursors and crosslink into delicate features of up to 1 mm resolution. The resulting hydrogel/elastomer hybrid exhibits excellent stretchability, capable of withstanding tensile strains exceeding 300 %. Additionally, the hybrid hydrogels can easily bind to conductive CNT nanocomposites, creating bilayer electrodes for wearable applications. Tissue adhesive polydopamine–polyacrylamide hydrogels are used to achieve conformal attachment to the skin, achieving lower contact impedance than commercial Ag/AgCl gel electrodes. These electrodes are integrated with stretchable circuits to create multifunctional patches for electrical stimulation and biopotential recording. An integrated epidermal sensing armband captures multichannel biopotential signals from the forearm, recognizing hand gestures through machine learning to act as a human–machine interface. The foam-templated synthesis introduced in this study offers convenient access to structured hydrogels and hydrogel/polymer hybrids for various cutting-edge applications.
{"title":"Elastomer foam templated three dimensional hybrid hydrogels for heterogeneously integrated stretchable electronics","authors":"Changqing Qin, Qian Wang, Ting Fang, Lin Wang, Cheng Yang, Yong Lin, Chong Bai, Wenqiang He, Likang Ding, Jinheng Zhang, Dongchan Li, Desheng Kong","doi":"10.1016/j.cej.2025.159937","DOIUrl":"https://doi.org/10.1016/j.cej.2025.159937","url":null,"abstract":"Hydrogels are soft, tissue-like solids with promising potential in biomedical engineering and stretchable electronics. These applications require hydrogels to be shaped into intricate structures and combined with other polymers. This study introduces hybrid hydrogels that use elastomer foams as templates for controlled synthesis. Essentially, TPU foams can be easily structured into diverse 2D or 3D shapes using laser ablation. After hydrophilic modification, these foams absorb hydrogel precursors and crosslink into delicate features of up to 1 mm resolution. The resulting hydrogel/elastomer hybrid exhibits excellent stretchability, capable of withstanding tensile strains exceeding 300 %. Additionally, the hybrid hydrogels can easily bind to conductive CNT nanocomposites, creating bilayer electrodes for wearable applications. Tissue adhesive polydopamine–polyacrylamide hydrogels are used to achieve conformal attachment to the skin, achieving lower contact impedance than commercial Ag/AgCl gel electrodes. These electrodes are integrated with stretchable circuits to create multifunctional patches for electrical stimulation and biopotential recording. An integrated epidermal sensing armband captures multichannel biopotential signals from the forearm, recognizing hand gestures through machine learning to act as a human–machine interface. The foam-templated synthesis introduced in this study offers convenient access to structured hydrogels and hydrogel/polymer hybrids for various cutting-edge applications.","PeriodicalId":270,"journal":{"name":"Chemical Engineering Journal","volume":"63 1","pages":""},"PeriodicalIF":15.1,"publicationDate":"2025-01-27","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143044220","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}
引用次数: 0
Ultrathin heterogeneous nanolayer structure of FeCoNiCu multi-principal element alloy for robust water electrolysis
IF 15.1 1区 工程技术 Q1 ENGINEERING, CHEMICAL Pub Date : 2025-01-27 DOI: 10.1016/j.cej.2025.160016
Zhiyi Ding, Ziyang Chen, Xinyang Liu, Junjie Liu, Tong Wang, Aiying Chen, Bin Gan, Yong Zhang
Developing efficient, cost-effective alloy catalysts for the hydrogen evolution reaction (HER) is a promising strategy to convert electrical energy to chemical fuels efficiently, however, it remains challenge. Herein, a designed non-equimolar FeCoNiCu multi-principal element alloys (MPEAs) catalyst, fabricated via a simple physical metallurgy and chemical dealloying, exhibits HER performance comparable to commercial noble metal counterpart. The optimal (FeCoNi)70Cu30 (at.%) catalysts display a remarkable minimum overpotential of 34 mV (@10 mA cm−2) and a Tafel slope of 48 mV dec-1. Meanwhile, the electrocatalyst exhibits excellent 24 h long-term durability stability at a high current density of −500 mA cm−2. This is attributed to the multi-scale substructure of distinctive, self-supporting Colosseum-inspired skeletal structure, coupled with nanoscale porous architecture attached to ultra-thin serrated amorphous nanolayer structure, significantly enhancing the specific surface and active sites. This study provides a novel strategy for designing high-performance non-precious metal catalysts with heterogeneous substructures based on multicomponent combinations.
{"title":"Ultrathin heterogeneous nanolayer structure of FeCoNiCu multi-principal element alloy for robust water electrolysis","authors":"Zhiyi Ding, Ziyang Chen, Xinyang Liu, Junjie Liu, Tong Wang, Aiying Chen, Bin Gan, Yong Zhang","doi":"10.1016/j.cej.2025.160016","DOIUrl":"https://doi.org/10.1016/j.cej.2025.160016","url":null,"abstract":"Developing efficient, cost-effective alloy catalysts for the hydrogen evolution reaction (HER) is a promising strategy to convert electrical energy to chemical fuels efficiently, however, it remains challenge. Herein, a designed non-equimolar FeCoNiCu multi-principal element alloys (MPEAs) catalyst, fabricated via a simple physical metallurgy and chemical dealloying, exhibits HER performance comparable to commercial noble metal counterpart. The optimal (FeCoNi)<sub>70</sub>Cu<sub>30</sub> (at.%) catalysts display a remarkable minimum overpotential of 34 mV (@10 mA cm<sup>−2</sup>) and a Tafel slope of 48 mV dec<sup>-1</sup>. Meanwhile, the electrocatalyst exhibits excellent 24 h long-term durability stability at a high current density of −500 mA cm<sup>−2</sup><sub>.</sub> This is attributed to the multi-scale substructure of distinctive, self-supporting Colosseum-inspired skeletal structure, coupled with nanoscale porous architecture attached to ultra-thin serrated amorphous nanolayer structure, significantly enhancing the specific surface and active sites. This study provides a novel strategy for designing high-performance non-precious metal catalysts with heterogeneous substructures based on multicomponent combinations.","PeriodicalId":270,"journal":{"name":"Chemical Engineering Journal","volume":"67 1","pages":""},"PeriodicalIF":15.1,"publicationDate":"2025-01-27","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143050564","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}
引用次数: 0
Efficient production of 1,6-hexanediol from adipic acid by engineering of carboxylate reductase coupled with genetically modified Escherichia coli
IF 15.1 1区 工程技术 Q1 ENGINEERING, CHEMICAL Pub Date : 2025-01-27 DOI: 10.1016/j.cej.2025.160034
Chen Ma, Na Jiang, Feiyi Zhuang, Xin Wang, Kequan Chen
1,6-hexanediol (1,6-HDO) is an important C6 material for synthesis of polyesters and polyurethanes. The development of a green, and cost-effective synthesis process for 1,6-HDO production is highly desirable. Recent work has demonstrated the biological synthesis of 1,6-HDO from adipic acid (AA) or cyclohexane. However, the 1,6-HDO yields have remained extremely low. In this study, we developed an efficient whole-cell catalytic system for 1,6-HDO production from adipic acid, utilizing carboxylate reductases (CAR) and aldehyde-keto reductase (AKR) in Escherichia coli. Enzyme screening, followed by structure-guided semi-rational engineering was first performed to address the rate-limiting enzyme of CAR. A variant, MabCARW283K/L306K, was obtained with a 4-fold increase in specific activity (2.03 U mg−1), and a 2.87-fold enhancement in catalytic efficiency (156.75 s−1· mM−1). Then, the NADPH supply in E. coli was also improved by overexpressing icd and deleting pgi for a further improvement on 1,6-HDO titer. Finally, three genes of eutG, ygiQ, and yiaY involved in 1,6-HDO degradation were identified by comprehensive screening of 52 single gene knockout strains encoding the putative alcohol dehydrogenase in E. coli. Combined deletions of these three genes significantly increased the 1,6-HDO titer by 35.4 %. Under the optimized conditions, the engineered strain was capable of producing 14.5 g/L 1,6-HDO from AA, achieving a yield of 89.6 %, the highest titer reported to date. This work successfully provided an efficient and feasible biosynthetic method for the biotransformation of AA into 1,6-HDO.
{"title":"Efficient production of 1,6-hexanediol from adipic acid by engineering of carboxylate reductase coupled with genetically modified Escherichia coli","authors":"Chen Ma, Na Jiang, Feiyi Zhuang, Xin Wang, Kequan Chen","doi":"10.1016/j.cej.2025.160034","DOIUrl":"https://doi.org/10.1016/j.cej.2025.160034","url":null,"abstract":"1,6-hexanediol (1,6-HDO) is an important C6 material for synthesis of polyesters and polyurethanes. The development of a green, and cost-effective synthesis process for 1,6-HDO production is highly desirable. Recent work has demonstrated the biological synthesis of 1,6-HDO from adipic acid (AA) or cyclohexane. However, the 1,6-HDO yields have remained extremely low. In this study, we developed an efficient whole-cell catalytic system for 1,6-HDO production from adipic acid, utilizing carboxylate reductases (CAR) and aldehyde-keto reductase (AKR) in <em>Escherichia coli</em>. Enzyme screening, followed by structure-guided semi-rational engineering was first performed to address the rate-limiting enzyme of CAR. A variant, MabCAR<sup>W283K/L306K</sup>, was obtained with a 4-fold increase in specific activity (2.03 U mg<sup>−1</sup>), and a 2.87-fold enhancement in catalytic efficiency (156.75 s<sup>−1</sup>· mM<sup>−1</sup>). Then, the NADPH supply in <em>E. coli</em> was also improved by overexpressing <em>icd</em> and deleting <em>pgi</em> for a further improvement on 1,6-HDO titer. Finally, three genes of <em>eutG</em>, <em>ygiQ</em>, and <em>yiaY</em> involved in 1,6-HDO degradation were identified by comprehensive screening of 52 single gene knockout strains encoding the putative alcohol dehydrogenase in <em>E. coli</em>. Combined deletions of these three genes significantly increased the 1,6-HDO titer by 35.4 %. Under the optimized conditions, the engineered strain was capable of producing 14.5 g/L 1,6-HDO from AA, achieving a yield of 89.6 %, the highest titer reported to date. This work successfully provided an efficient and feasible biosynthetic method for the biotransformation of AA into 1,6-HDO.","PeriodicalId":270,"journal":{"name":"Chemical Engineering Journal","volume":"29 1","pages":""},"PeriodicalIF":15.1,"publicationDate":"2025-01-27","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143050563","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}
引用次数: 0
Intelligent electric energy driven ultrathin Graphene-Based Janus Films: Pioneering design for dynamic Electrochromism and superior microwave absorption
IF 15.1 1区 工程技术 Q1 ENGINEERING, CHEMICAL Pub Date : 2025-01-27 DOI: 10.1016/j.cej.2025.160008
Tian Li, Jiatong Li, Zhengkang Xu, Jinzhe Li, Tinghao Liao, Jiani Du, Shanshan Wang, Qing Qi, Li Ma, Fanbin Meng
Given the rapid evolution of radar detection technologies, there is a growing demand for stimuli-responsive, intelligent microwave absorption (MA) materials. These materials can offer dynamic and adaptive control of their MA performance in intricate radar signal settings. Concurrently, electrical signals are commonly preferred as triggers for these responsive materials, given their consistent and rapid response speed. In this study, intelligent PDA/rGO composite films are fabricated into Janus structure using a simple scratching technique, followed by UV-induced topological polymerization. Upon activation at 35 V, the film thickness increases from 39 to 82.3 μm, with an accompanying color transition from blue to red. Following this activation, the PDA/rGO composite film exhibits significantly enhanced MA performance. The optimal reflection loss (RL) increases by 723.3 %, shifting from − 3 dB to − 21.7 dB at 18 GHz relative to its initial state, with the corresponding effective absorption band (EAB) extending to 4 GHz. This is attributed to the transformation of the agglomerated rGO multilayers into the porous structure upon electrical stimulation, thereby improving the impedance matching and electromagnetic wave dissipation capability. Thus, this study presents a feasible approach to developing ultra-thin, electro-responsive composite film for efficient MA performance, paving the way for designing intelligent MA materials.
{"title":"Intelligent electric energy driven ultrathin Graphene-Based Janus Films: Pioneering design for dynamic Electrochromism and superior microwave absorption","authors":"Tian Li, Jiatong Li, Zhengkang Xu, Jinzhe Li, Tinghao Liao, Jiani Du, Shanshan Wang, Qing Qi, Li Ma, Fanbin Meng","doi":"10.1016/j.cej.2025.160008","DOIUrl":"https://doi.org/10.1016/j.cej.2025.160008","url":null,"abstract":"Given the rapid evolution of radar detection technologies, there is a growing demand for stimuli-responsive, intelligent microwave absorption (MA) materials. These materials can offer dynamic and adaptive control of their MA performance in intricate radar signal settings. Concurrently, electrical signals are commonly preferred as triggers for these responsive materials, given their consistent and rapid response speed. In this study, intelligent PDA/rGO composite films are fabricated into Janus structure using a simple scratching technique, followed by UV-induced topological polymerization. Upon activation at 35 V, the film thickness increases from 39 to 82.3 μm, with an accompanying color transition from blue to red. Following this activation, the PDA/rGO composite film exhibits significantly enhanced MA performance. The optimal reflection loss (RL) increases by 723.3 %, shifting from − 3 dB to − 21.7 dB at 18 GHz relative to its initial state, with the corresponding effective absorption band (EAB) extending to 4 GHz. This is attributed to the transformation of the agglomerated rGO multilayers into the porous structure upon electrical stimulation, thereby improving the impedance matching and electromagnetic wave dissipation capability. Thus, this study presents a feasible approach to developing ultra-thin, electro-responsive composite film for efficient MA performance, paving the way for designing intelligent MA materials.","PeriodicalId":270,"journal":{"name":"Chemical Engineering Journal","volume":"119 1","pages":""},"PeriodicalIF":15.1,"publicationDate":"2025-01-27","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143050566","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}
引用次数: 0
Z-scheme Ti3C2@Bi2O3 based MXene with multifaceted (0 0 1) and (1 0 1) TiO2 and Ti3+/oxygen vacancies: Photocatalytic degradation of dichlorophen via peroxymonosulfate activation, energy utilization and antibacterial activities
IF 15.1 1区 工程技术 Q1 ENGINEERING, CHEMICAL Pub Date : 2025-01-27 DOI: 10.1016/j.cej.2025.159992
Ikhtiar Gul, Murtaza Sayed, Faiza Rehman, Wang Jinlong, Pingfeng Fu, Yuliang Zhang, Mallikarjuna N. Nadagouda
In this study, highly porous Z-scheme Ti3C2@ 15 % Bi2O3 based Mxene with multifaceted (0 0 1) and (1 0 1) TiO2 (MTB15) was synthesized via solvothermal route. The characterization analysis indicated that the synthesized photocatalyst was featured with beneficial Ti3+ centers and oxygen vacancies (OVs). The integration of peroxymonosulfate (PMS, 0.15 mM) to the synthesized photocatalyst has significantly boosted the degradation of dichlorophen (DCP, 6.0 mg L−1) from 66.83 % (no PMS) to 98.69 % at 50 min of reaction time. The antibacterial properties of MTB15 have proven a significant reduction (1.13-log reduction) in Escherichia coli (E.coli) which is comparable to the 1.49-log reduction of the positive control. At a current density of 1 A/g, the synthesized MTB15 when applied as symmetrical supercapacitor cell (SSC) also showed unique electrochemical performance, having specific capacitance of 556.37F/g, energy density of 5.86W h kg−1, and power density of 137.00W kg−1. The H2 generation rate of MTB15 was 4.86 mmol/h g−1, which surpassed MTB0 by almost 5.85 times. Overall, the findings of this study explored the multifunctional behavior of MTB15 in terms of environmental remediation, energy storage, and generation and thus solving the real-world issues sustainably.
{"title":"Z-scheme Ti3C2@Bi2O3 based MXene with multifaceted (0 0 1) and (1 0 1) TiO2 and Ti3+/oxygen vacancies: Photocatalytic degradation of dichlorophen via peroxymonosulfate activation, energy utilization and antibacterial activities","authors":"Ikhtiar Gul, Murtaza Sayed, Faiza Rehman, Wang Jinlong, Pingfeng Fu, Yuliang Zhang, Mallikarjuna N. Nadagouda","doi":"10.1016/j.cej.2025.159992","DOIUrl":"https://doi.org/10.1016/j.cej.2025.159992","url":null,"abstract":"In this study, highly porous Z-scheme Ti<sub>3</sub>C<sub>2</sub>@ 15 % Bi<sub>2</sub>O<sub>3</sub> based Mxene with multifaceted (0<!-- --> <!-- -->0<!-- --> <!-- -->1) and (1<!-- --> <!-- -->0<!-- --> <!-- -->1) TiO<sub>2</sub> (MTB15) was synthesized via solvothermal route. The characterization analysis indicated that the synthesized photocatalyst was featured with beneficial Ti<sup>3+</sup> centers and oxygen vacancies (OVs). The integration of peroxymonosulfate (PMS, 0.15 mM) to the synthesized photocatalyst has significantly boosted the degradation of dichlorophen (DCP, 6.0 mg L<sup>−1</sup>) from 66.83 % (no PMS) to 98.69 % at 50 min of reaction time. The antibacterial properties of MTB15 have proven a significant reduction (1.13-log reduction) in <em>Escherichia coli (E.coli)</em> which is comparable to the 1.49-log reduction of the positive control. At a current density of 1 A/g, the synthesized MTB15 when applied as symmetrical supercapacitor cell (SSC) also showed unique electrochemical performance, having specific capacitance of 556.37F/g, energy density of 5.86W h kg<sup>−1</sup>, and power density of 137.00W kg<sup>−1</sup>. The H<sub>2</sub> generation rate of MTB15 was 4.86 mmol/h g<sup>−1</sup>, which surpassed MTB0 by almost 5.85 times. Overall, the findings of this study explored the multifunctional behavior of MTB15 in terms of environmental remediation, energy storage, and generation and thus solving the real-world issues sustainably.","PeriodicalId":270,"journal":{"name":"Chemical Engineering Journal","volume":"49 1","pages":""},"PeriodicalIF":15.1,"publicationDate":"2025-01-27","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143050572","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}
引用次数: 0
Unlocking long-term stability: Electrolyte additives for suppressing zinc dendrite growth in aqueous zinc metal batteries
IF 15.1 1区 工程技术 Q1 ENGINEERING, CHEMICAL Pub Date : 2025-01-27 DOI: 10.1016/j.cej.2025.160017
Hee Jae Kim, Sun Kim, Jun Ho Yu, Jae-Hong Lim, Hitoshi Yashiro, Seung-Taek Myung
Aqueous zinc-ion batteries (AZIBs) have attracted great attention for energy storage because of the safety of zinc metal in ambient air. However, the growth of zinc dendrites during repeated electrochemical cycles have hindered their practical use. To address this issue, we introduced ZnBr2 as an additive in an aqueous 1 M ZnSO4 electrolyte, effectively suppressing the dendritic growth on the surface of the zinc-metal anode. Significant improvement in Zn||Zn symmetric cell tests using 10 wt% ZnBr2-added electrolyte was observed, with a lifespan of 12,500 cycles achieved even at a high current density of 50 mA cm−2 with an areal capacity of 1 mAh cm−2. Raman spectroscopy reveals formation of HBr in the electrolyte after 12 h deposition of zinc. The presence of HBr in the electrolyte effectively suppresses the dendritic growth of zinc, as visualized by an operando beaker-cell test and synchrotron tomography. We further demonstrated the compatibility and excellent rate performance of the additive-based electrolyte in Zn || NaV3O8 full cells. Our findings provide a simple and cost-effective method to suppress dendritic growth of zinc in zinc-metal batteries
{"title":"Unlocking long-term stability: Electrolyte additives for suppressing zinc dendrite growth in aqueous zinc metal batteries","authors":"Hee Jae Kim, Sun Kim, Jun Ho Yu, Jae-Hong Lim, Hitoshi Yashiro, Seung-Taek Myung","doi":"10.1016/j.cej.2025.160017","DOIUrl":"https://doi.org/10.1016/j.cej.2025.160017","url":null,"abstract":"Aqueous zinc-ion batteries (AZIBs) have attracted great attention for energy storage because of the safety of zinc metal in ambient air. However, the growth of zinc dendrites during repeated electrochemical cycles have hindered their practical use. To address this issue, we introduced ZnBr<sub>2</sub> as an additive in an aqueous 1 M ZnSO<sub>4</sub> electrolyte, effectively suppressing the dendritic growth on the surface of the zinc-metal anode. Significant improvement in Zn||Zn symmetric cell tests using 10 wt% ZnBr<sub>2</sub>-added electrolyte was observed, with a lifespan of 12,500 cycles achieved even at a high current density of 50 mA cm<sup>−2</sup> with an areal capacity of 1 mAh cm<sup>−2</sup>. Raman spectroscopy reveals formation of HBr in the electrolyte after 12 h deposition of zinc. The presence of HBr in the electrolyte effectively suppresses the dendritic growth of zinc, as visualized by an <em>operando</em> beaker-cell test and synchrotron tomography. We further demonstrated the compatibility and excellent rate performance of the additive-based electrolyte in Zn || NaV<sub>3</sub>O<sub>8</sub> full cells. Our findings provide a simple and cost-effective method to suppress dendritic growth of zinc in zinc-metal batteries","PeriodicalId":270,"journal":{"name":"Chemical Engineering Journal","volume":"2018 1","pages":""},"PeriodicalIF":15.1,"publicationDate":"2025-01-27","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143050607","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}
引用次数: 0
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Chemical Engineering Journal
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