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Multiamine-Grafted magnetic nanocatchers for enhanced removal of chlortetracycline from aqueous solution
IF 15.1 1区 工程技术 Q1 ENGINEERING, CHEMICAL Pub Date : 2025-01-28 DOI: 10.1016/j.cej.2025.160051
Bingbing Li, Xixi Liu, Mengdi Wu, Yanxin Ye, Yanyan Chen, Junhong Liu, Jie Sun, Shuangcheng Zhi
Human health and ecosystems have been seriously threatened by the increasing contamination of antibiotics in water resources. Therefore, it is crucial to develop effective adsorbents for the efficient removal of antibiotics from aquatic environments. Herein, a magnetic and multitentacle nanodevice is designed and synthesized, which consists of an Fe3O4 core and a multiamine shell (M@LMa). Notably, multitentacled grippers of aminated lignin on the surface of multifunctional nanocatchers with enhanced capturing ability are covalently anchored onto magnetic cores through 3-amino-propyltriethoxysilane, which significantly improves the stability of the nanostructure. In the presence of chlortetracycline (CTC), the proposed nanocatchers exhibit excellent capability for the effective elimination of CTC from aqueous solutions. In addition, M@LMa demonstrates both specific CTC capture via noncovalent interactions, such as π-π stacking, hydrogen bonding interactions, and electrostatic interactions, and efficient magnetic separation for the elimination of antibiotics from aqueous solutions. This study paves the way for the development of multifunctional lignin-based magnetic nanodevices and their applications in the removal of antibiotics from wastewater.
{"title":"Multiamine-Grafted magnetic nanocatchers for enhanced removal of chlortetracycline from aqueous solution","authors":"Bingbing Li, Xixi Liu, Mengdi Wu, Yanxin Ye, Yanyan Chen, Junhong Liu, Jie Sun, Shuangcheng Zhi","doi":"10.1016/j.cej.2025.160051","DOIUrl":"https://doi.org/10.1016/j.cej.2025.160051","url":null,"abstract":"Human health and ecosystems have been seriously threatened by the increasing contamination of antibiotics in water resources. Therefore, it is crucial to develop effective adsorbents for the efficient removal of antibiotics from aquatic environments. Herein, a magnetic and multitentacle nanodevice is designed and synthesized, which consists of an Fe<sub>3</sub>O<sub>4</sub> core and a multiamine shell (M@LMa). Notably, multitentacled grippers of aminated lignin on the surface of multifunctional nanocatchers with enhanced capturing ability are covalently anchored onto magnetic cores through 3-amino-propyltriethoxysilane, which significantly improves the stability of the nanostructure. In the presence of chlortetracycline (CTC), the proposed nanocatchers exhibit excellent capability for the effective elimination of CTC from aqueous solutions. In addition, M@LMa demonstrates both specific CTC capture <em>via</em> noncovalent interactions, such as π-π stacking, hydrogen bonding interactions, and electrostatic interactions, and efficient magnetic separation for the elimination of antibiotics from aqueous solutions. This study paves the way for the development of multifunctional lignin-based magnetic nanodevices and their applications in the removal of antibiotics from wastewater.","PeriodicalId":270,"journal":{"name":"Chemical Engineering Journal","volume":"27 1","pages":""},"PeriodicalIF":15.1,"publicationDate":"2025-01-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143055431","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
Pyroligneous acid amendments alleviated antibiotic resistance genes pollution in agricultural soil via inhibiting horizontal gene transformation
IF 15.1 1区 工程技术 Q1 ENGINEERING, CHEMICAL Pub Date : 2025-01-28 DOI: 10.1016/j.cej.2025.160070
Mengying Shao, Xiaohan Ma, Min Zhang, Yuxin Li, Liuqingqing Liu, Jiamin Wang, Wei Meng, Cuizhu Sun, Hao Zheng, Xianxiang Luo, Fengmin Li
Pyroligneous acids (PAs) amendments could reduce soil antibiotic resistance genes (ARGs) pollution, but their impacts on horizontal transformation of extracellular ARGs (eARGs) remain unclear. Here, a wood residues derived PA was selected to investigate its effect on ARG dissemination via transformation using a soil microcosm experiment and an in vitro transformation system. The PA application effectively decreased the abundances of representative ARGs and mobile genetic elements, demonstrating that the weakened horizontal gene transfer alleviated ARG pollution in the soil. PA showed an amount-dependent inhibition on the transformation as well as the three distilled fractions and chemical components, proving that their important roles in inhibiting eARG transformation. The relatively low-amount (1 μL mL−1) of PA suppressed the transformation mainly by destroying the plasmid pBR322 structure, while the high-amount (10–100 μL mL−1) of PA inhibited the transformation due to the inactivation of recipient Escherichia coli DH5α by inducing oxidative stress and destroying cell membrane, and damages of plasmid by reducing eARGs abundance and broking the base deoxyribose, and phosphate skeletons. These findings expand the understanding of PA amendments mitigating ARG pollution in agricultural soils via inhibiting horizontal gene transformation, and also provide a practical strategy to remediate soil ARG pollution.
{"title":"Pyroligneous acid amendments alleviated antibiotic resistance genes pollution in agricultural soil via inhibiting horizontal gene transformation","authors":"Mengying Shao, Xiaohan Ma, Min Zhang, Yuxin Li, Liuqingqing Liu, Jiamin Wang, Wei Meng, Cuizhu Sun, Hao Zheng, Xianxiang Luo, Fengmin Li","doi":"10.1016/j.cej.2025.160070","DOIUrl":"https://doi.org/10.1016/j.cej.2025.160070","url":null,"abstract":"Pyroligneous acids (PAs) amendments could reduce soil antibiotic resistance genes (ARGs) pollution, but their impacts on horizontal transformation of extracellular ARGs (eARGs) remain unclear. Here, a wood residues derived PA was selected to investigate its effect on ARG dissemination via transformation using a soil microcosm experiment and an <em>in vitro</em> transformation system. The PA application effectively decreased the abundances of representative ARGs and mobile genetic elements, demonstrating that the weakened horizontal gene transfer alleviated ARG pollution in the soil. PA showed an amount-dependent inhibition on the transformation as well as the three distilled fractions and chemical components, proving that their important roles in inhibiting eARG transformation. The relatively low-amount (1 μL mL<sup>−1</sup>) of PA suppressed the transformation mainly by destroying the plasmid pBR322 structure, while the high-amount (10–100 μL mL<sup>−1</sup>) of PA inhibited the transformation due to the inactivation of recipient <em>Escherichia coli</em> DH5α by inducing oxidative stress and destroying cell membrane, and damages of plasmid by reducing eARGs abundance and broking the base deoxyribose, and phosphate skeletons. These findings expand the understanding of PA amendments mitigating ARG pollution in agricultural soils via inhibiting horizontal gene transformation, and also provide a practical strategy to remediate soil ARG pollution.","PeriodicalId":270,"journal":{"name":"Chemical Engineering Journal","volume":"7 1","pages":""},"PeriodicalIF":15.1,"publicationDate":"2025-01-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143055208","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
Improving electrocatalytic activity through multi-element doping to A-site of Fe-based perovskite cathode for solid oxide fuel cells
IF 15.1 1区 工程技术 Q1 ENGINEERING, CHEMICAL Pub Date : 2025-01-28 DOI: 10.1016/j.cej.2025.160067
Dongli Shang, Binze Zhang, Lijie Zhang, Jin Li, Yongtao Zhao, Yuhu Huang, Kaibin Tang, Changrong Xia
Perovskite oxide La0.5Sr0.5FeO3-δ (LSF) is a potential Co-free electrocatalyst for oxygen reduction reaction (ORR) in solid oxide fuel cells (SOFCs). To improve its catalytic activity, this work performs multi-element doping to the A-site elements La and Sr, forming a high-entropy oxide Ba0.2Sr0.2La0.2Pr0.2Sm0.2FeO3-δ (H-LSF) and a medium-entropy material Ba0.35Sr0.35La0.1Pr0.1Sm0.1FeO3-δ (M−LSF). The multi-element doping effects are investigated on various physicochemical properties including crystalline structure, chemical compatibility with electrolyte, valence state of B-site Fe, amount of adsorbed oxygen species, oxygen nonstoichiometric value, sinterability, thermal expansion coefficient, electrical conductivity, chemical oxygen surface exchange coefficient (kchem), and electrochemical performance. While the multi-element doping does not change the phase structure and compatibility, it decreases the electronic conductivity, increases the oxygen vacancy concentration and kchem. Consequently, it improves ORR activity such as reduces interfacial polarization resistance and elevates peak power density. The best performance is observed with the medium-entropy perovskite rather than the high-entropy material. M−LSF shows kchem of 21.5 × 105 cm s−1 at 750 °C, 32 % higher than H-LSF and 4 times as high as LSF. In addition, M−LSF electrode exhibits interfacial polarization resistance of 0.090 2 at 750 °C, about 1/2 of H-LSF and 1/5 of LSF. Furthermore, single cell with M−LSF cathode demonstrates peak power density of 1.72 W cm−2 at 800 °C, 25 % higher than H-LSF and more than twice as LSF. Therefore, multi-element doping to the A-site of ferrite-based cobalt-free perovskite could be an effective method to improve the cathode performance.
{"title":"Improving electrocatalytic activity through multi-element doping to A-site of Fe-based perovskite cathode for solid oxide fuel cells","authors":"Dongli Shang, Binze Zhang, Lijie Zhang, Jin Li, Yongtao Zhao, Yuhu Huang, Kaibin Tang, Changrong Xia","doi":"10.1016/j.cej.2025.160067","DOIUrl":"https://doi.org/10.1016/j.cej.2025.160067","url":null,"abstract":"Perovskite oxide La<sub>0.5</sub>Sr<sub>0.5</sub>FeO<sub>3-δ</sub> (LSF) is a potential Co-free electrocatalyst for oxygen reduction reaction (ORR) in solid oxide fuel cells (SOFCs). To improve its catalytic activity, this work performs multi-element doping to the A-site elements La and Sr, forming a high-entropy oxide Ba<sub>0.2</sub>Sr<sub>0.2</sub>La<sub>0.2</sub>Pr<sub>0.2</sub>Sm<sub>0.2</sub>FeO<sub>3-δ</sub> (H-LSF) and a medium-entropy material Ba<sub>0.35</sub>Sr<sub>0.35</sub>La<sub>0.1</sub>Pr<sub>0.1</sub>Sm<sub>0.1</sub>FeO<sub>3-δ</sub> (M−LSF). The multi-element doping effects are investigated on various physicochemical properties including crystalline structure, chemical compatibility with electrolyte, valence state of B-site Fe, amount of adsorbed oxygen species, oxygen nonstoichiometric value, sinterability, thermal expansion coefficient, electrical conductivity, chemical oxygen surface exchange coefficient (<em>k</em><sub>chem</sub>), and electrochemical performance. While the multi-element doping does not change the phase structure and compatibility, it decreases the electronic conductivity, increases the oxygen vacancy concentration and <em>k</em><sub>chem</sub>. Consequently, it improves ORR activity such as reduces interfacial polarization resistance and elevates peak power density. The best performance is observed with the medium-entropy perovskite rather than the high-entropy material. M−LSF shows <em>k</em><sub>chem</sub> of 21.5 × 10<strong><sup>−</sup></strong><sup>5</sup> cm s<sup>−1</sup> at 750 °C, 32 % higher than H-LSF and 4 times as high as LSF. In addition, M−LSF electrode exhibits interfacial polarization resistance of 0.090 <sup>2</sup> at 750 °C, about 1/2 of H-LSF and 1/5 of LSF. Furthermore, single cell with M−LSF cathode demonstrates peak power density of 1.72 W cm<sup>−2</sup> at 800 °C, 25 % higher than H-LSF and more than twice as LSF. Therefore, multi-element doping to the A-site of ferrite-based cobalt-free perovskite could be an effective method to improve the cathode performance.","PeriodicalId":270,"journal":{"name":"Chemical Engineering Journal","volume":"71 1","pages":""},"PeriodicalIF":15.1,"publicationDate":"2025-01-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143055211","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
Solar interfacial evaporation hydrogel with distributed packaging of phase change materials for continuous desalination
IF 15.1 1区 工程技术 Q1 ENGINEERING, CHEMICAL Pub Date : 2025-01-28 DOI: 10.1016/j.cej.2025.160061
Qian Chen, He Zhang, Lie Zou, Rui Yang, Guangyong Zeng, Pengcheng Lin, Liu Yang, Mingming Zheng, Xiaoke Li
Solar-driven interfacial evaporation (SDIE) is now widely recognized as a promising solution to the global freshwater crisis. This recognition stems from its low energy consumption and environmentally friendly characteristics. However, the performance is hampered by variations in solar intensity due to daily cycles and weather changes, significantly affecting evaporation rates and freshwater yield. One of the most effective strategies for addressing this issue is to integrate solar energy storage materials with SDIE. In this study, we integrated a phase change energy storage material (Na2SO4·10H2O) into a solar evaporator encapsulated within a dual-network hydrogel composed of sodium alginate and polyacrylamide. Additionally, Chinese ink was utilized as a light absorber to improve the efficiency of photo-thermal conversion. This hydrogel-based evaporator effectively stores surplus solar energy and releases latent heat, enabling continuous and efficient seawater desalination even under low-light conditions. Experimental findings indicate that the evaporation rate was highly 2.72 kg·m−2·h−1 under 1 sun, and the evaporation efficiency was 92.8 %. Notably, the phase change material exhibits significant heat storage capacity, with a phase change latent heat of 181.42 J·g−1. Consequently, In the absence of solar radiation, the evaporation rate remains sustained at 1.25 kg·m−2·h−1, representing a 16.8 % increase in freshwater production compared to hydrogels lacking phase change materials. Moreover, the hydrogel-based evaporator demonstrates robust performance in purifying total dissolved solids (TDS) and major salt ions from seawater, showcasing exceptional durability under high acid-base and salinity conditions. This study underscores a promising pathway towards sustainable and efficient desalination processes utilizing intermittent renewable solar energy.
{"title":"Solar interfacial evaporation hydrogel with distributed packaging of phase change materials for continuous desalination","authors":"Qian Chen, He Zhang, Lie Zou, Rui Yang, Guangyong Zeng, Pengcheng Lin, Liu Yang, Mingming Zheng, Xiaoke Li","doi":"10.1016/j.cej.2025.160061","DOIUrl":"https://doi.org/10.1016/j.cej.2025.160061","url":null,"abstract":"Solar-driven interfacial evaporation (SDIE) is now widely recognized as a promising solution to the global freshwater crisis. This recognition stems from its low energy consumption and environmentally friendly characteristics. However, the performance is hampered by variations in solar intensity due to daily cycles and weather changes, significantly affecting evaporation rates and freshwater yield. One of the most effective strategies for addressing this issue is to integrate solar energy storage materials with SDIE. In this study, we integrated a phase change energy storage material (Na<sub>2</sub>SO<sub>4</sub>·10H<sub>2</sub>O) into a solar evaporator encapsulated within a dual-network hydrogel composed of sodium alginate and polyacrylamide. Additionally, Chinese ink was utilized as a light absorber to improve the efficiency of photo-thermal conversion. This hydrogel-based evaporator effectively stores surplus solar energy and releases latent heat, enabling continuous and efficient seawater desalination even under low-light conditions. Experimental findings indicate that the evaporation rate was highly 2.72 kg·m<sup>−2</sup>·h<sup>−1</sup> under 1 sun, and the evaporation efficiency was 92.8 %. Notably, the phase change material exhibits significant heat storage capacity, with a phase change latent heat of 181.42 J·g<sup>−1</sup>. Consequently, In the absence of solar radiation, the evaporation rate remains sustained at 1.25 kg·m<sup>−2</sup>·h<sup>−1</sup>, representing a 16.8 % increase in freshwater production compared to hydrogels lacking phase change materials. Moreover, the hydrogel-based evaporator demonstrates robust performance in purifying total dissolved solids (TDS) and major salt ions from seawater, showcasing exceptional durability under high acid-base and salinity conditions. This study underscores a promising pathway towards sustainable and efficient desalination processes utilizing intermittent renewable solar energy.","PeriodicalId":270,"journal":{"name":"Chemical Engineering Journal","volume":"85 1 1","pages":""},"PeriodicalIF":15.1,"publicationDate":"2025-01-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143055395","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
Pig urine-induced ternary buffering complex and microbial community for mitigating acid inhibition in high-solid anaerobic digestion of rice straw
IF 15.1 1区 工程技术 Q1 ENGINEERING, CHEMICAL Pub Date : 2025-01-28 DOI: 10.1016/j.cej.2025.160027
Wenjian Dong, Zihao Jiang, Lin Luo, Jiachao Zhang, Wenyan Zhao, Akhmadzhan A. Makhsumkhanov, Chao Liu, Binghua Yan
Acid inhibition is frequently recognized as the primary challenge in high-solid anaerobic digestion, often leading to severe process inhibition or even system failure. Maintaining microbial pH homeostasis is becoming increasingly critical. In this study, a pH ternary buffering complex was developed in the straw digestion system by integrating carbonate and ammonium derived from pig urine with volatile fatty acids present in the reactor. Results showed that the pH ternary buffering complex alleviated acid inhibition and promoted methane production significantly. The methane production of 342.66 mL·gVSremoval−1 was achieved in the reactor with ternary buffering complex, which corresponding to 29-fold of that without buffering. Abundances of key enzyme genes in hydrolytic and acidogenic stages was improved by the ternary buffer complex. Besides, the buffering complex optimized acidogenic metabolic pathway and NADH/NAD+ balance during methane production. To alleviate acid inhibition, the ternary buffering complex was supposed to work with extracellular excess H+ in a timely manner and promoted proton pump that transferred intracellular H+ out of the cell to prevent cytoplasmic acidification. Simultaneously, NH4+ was transported into the cell to replenish the significant loss of intracellular cations (H+) and maintained cellular osmotic pressure. Thus this study opens a door for alleviation of acid inhibition and maintenance of microbial cellular homeostasis.
{"title":"Pig urine-induced ternary buffering complex and microbial community for mitigating acid inhibition in high-solid anaerobic digestion of rice straw","authors":"Wenjian Dong, Zihao Jiang, Lin Luo, Jiachao Zhang, Wenyan Zhao, Akhmadzhan A. Makhsumkhanov, Chao Liu, Binghua Yan","doi":"10.1016/j.cej.2025.160027","DOIUrl":"https://doi.org/10.1016/j.cej.2025.160027","url":null,"abstract":"Acid inhibition is frequently recognized as the primary challenge in high-solid anaerobic digestion, often leading to severe process inhibition or even system failure. Maintaining microbial pH homeostasis is becoming increasingly critical. In this study, a pH ternary buffering complex was developed in the straw digestion system by integrating carbonate and ammonium derived from pig urine with volatile fatty acids present in the reactor. Results showed that the pH ternary buffering complex alleviated acid inhibition and promoted methane production significantly. The methane production of 342.66 mL·gVS<sub>removal</sub><sup>−1</sup> was achieved in the reactor with ternary buffering complex, which corresponding to 29-fold of that without buffering. Abundances of key enzyme genes in hydrolytic and acidogenic stages was improved by the ternary buffer complex. Besides, the buffering complex optimized acidogenic metabolic pathway and NADH/NAD<sup>+</sup> balance during methane production. To alleviate acid inhibition, the ternary buffering complex was supposed to work with extracellular excess H<sup>+</sup> in a timely manner and promoted proton pump that transferred intracellular H<sup>+</sup> out of the cell to prevent cytoplasmic acidification. Simultaneously, NH<sub>4</sub><sup>+</sup> was transported into the cell to replenish the significant loss of intracellular cations (H<sup>+</sup>) and maintained cellular osmotic pressure. Thus this study opens a door for alleviation of acid inhibition and maintenance of microbial cellular homeostasis.","PeriodicalId":270,"journal":{"name":"Chemical Engineering Journal","volume":"40 1","pages":""},"PeriodicalIF":15.1,"publicationDate":"2025-01-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143055399","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
Spin-state regulation of heteronuclear Cu-Co dual-atomic sites via tuning electronic asymmetry for enhanced oxygen reduction
IF 15.1 1区 工程技术 Q1 ENGINEERING, CHEMICAL Pub Date : 2025-01-28 DOI: 10.1016/j.cej.2025.160020
Heng Wang, Xinzhi Zhou, Jiaxin Su, Zixian Liu, Bingbing Xiao, Long Yang, Jun Wang, Yuanli Li, Xunyu Lu, Xiaofeng Zhu
Modulating electronic asymmetry of transition metal (TM) sites attributes to switching their spin state and regulating bonding to oxygen-containing intermediates, thereby facilitating their performance for oxygen reduction reaction (ORR). Herein, we engineer the local coordination structure of the Cu-Co dual-atomic site by integrating phosphorous. The constructed CuCoNPC therefore possesses asymmetric active sites (CoN3-CuN3P), leading to a high spin-state of reactive Co sites. The accordingly tuned dyz orbital occupation consequently triggers the rate-determining step of ORR switching from first (*O2→*OOH) to the last protonation (*OH → H2O). As a result, the CuCoNPC exhibits exceptional ORR activity, with jk of 54 mA cm−2 at 0.75 VRHE and half-wave potential (E1/2) of 0.86 VRHE, overwhelming that of Pt in alkaline electrolyte. Meanwhile, it also displays a Pt-comparable onset (0.82 VRHE) and E1/2 (0.72 VRHE) in acidic media. Finally, the CuCoNPC catalyst superior performance in liquid-form (Pmax = 194 mW cm−2) and all-solid-state flexible (OCP = 1.51 V) zinc-air batteries. This work provides valuable guidance in developing active TM-based ORR catalysts via tuning electronic asymmetry.
{"title":"Spin-state regulation of heteronuclear Cu-Co dual-atomic sites via tuning electronic asymmetry for enhanced oxygen reduction","authors":"Heng Wang, Xinzhi Zhou, Jiaxin Su, Zixian Liu, Bingbing Xiao, Long Yang, Jun Wang, Yuanli Li, Xunyu Lu, Xiaofeng Zhu","doi":"10.1016/j.cej.2025.160020","DOIUrl":"https://doi.org/10.1016/j.cej.2025.160020","url":null,"abstract":"Modulating electronic asymmetry of transition metal (TM) sites attributes to switching their spin state and regulating bonding to oxygen-containing intermediates, thereby facilitating their performance for oxygen reduction reaction (ORR). Herein, we engineer the local coordination structure of the Cu-Co dual-atomic site by integrating phosphorous. The constructed CuCoNPC therefore possesses asymmetric active sites (CoN<sub>3</sub>-CuN<sub>3</sub>P), leading to a high spin-state of reactive Co sites. The accordingly tuned <em>d<sub>yz</sub></em> orbital occupation consequently triggers the rate-determining step of ORR switching from first (*O<sub>2</sub>→*OOH) to the last protonation (*OH → H<sub>2</sub>O). As a result, the CuCoNPC exhibits exceptional ORR activity, with <em>j</em><sub>k</sub> of 54 mA cm<sup>−2</sup> at 0.75 V<sub>RHE</sub> and half-wave potential (<em>E</em><sub>1/2</sub>) of 0.86 V<sub>RHE</sub>, overwhelming that of Pt in alkaline electrolyte. Meanwhile, it also displays a Pt-comparable onset (0.82 V<sub>RHE</sub>) and <em>E</em><sub>1/2</sub> (0.72 V<sub>RHE</sub>) in acidic media. Finally, the CuCoNPC catalyst superior performance in liquid-form (<em>P</em><sub>max</sub> = 194 mW cm<sup>−2</sup>) and all-solid-state flexible (OCP = 1.51 V) zinc-air batteries. This work provides valuable guidance in developing active TM-based ORR catalysts <em>via</em> tuning electronic asymmetry.","PeriodicalId":270,"journal":{"name":"Chemical Engineering Journal","volume":"17 1","pages":""},"PeriodicalIF":15.1,"publicationDate":"2025-01-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143055435","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
Functionalities and properties of conductive hydrogel with nanocellulose integration 集成纳米纤维素的导电水凝胶的功能和特性
IF 15.1 1区 工程技术 Q1 ENGINEERING, CHEMICAL Pub Date : 2025-01-28 DOI: 10.1016/j.cej.2025.159872
Meng Zhang, Ting Chen, Ting Xu, Han Zhang, Xuan Wang, Junjie Qi, Qiang Dong, Liyu Zhu, Zhanhui Yuan, Chuanling Si
In the realm of sustainable materials, nanocellulose has emerged as a particularly noteworthy contender, garnering considerable attention with exceptional mechanical properties, biocompatibility, and renewability. Within the domain of conductive hydrogels, nanocellulose distinctive characteristics position it as a preeminent reinforcing and dispersing agent, thereby markedly augmenting the overall performance of hydrogels. This article reviews the progress of nanocellulose applications in conductive hydrogels and discusses its mechanism of action as reinforcing and dispersing agents in detail, as well as the preparation methods with different conductive fillers (carbon materials, conductive polymers, metal nanoparticles and metal ions). Additionally, the extant research findings on the mechanical, self-healing, self-adhesion and freeze resistance properties of the conductive hydrogels are comprehensively introduced. In conclusion, the article provides a comprehensive outlook on the ongoing issues of nanocellulose-based conductive hydrogels and their possible future directions.
{"title":"Functionalities and properties of conductive hydrogel with nanocellulose integration","authors":"Meng Zhang, Ting Chen, Ting Xu, Han Zhang, Xuan Wang, Junjie Qi, Qiang Dong, Liyu Zhu, Zhanhui Yuan, Chuanling Si","doi":"10.1016/j.cej.2025.159872","DOIUrl":"https://doi.org/10.1016/j.cej.2025.159872","url":null,"abstract":"In the realm of sustainable materials, nanocellulose has emerged as a particularly noteworthy contender, garnering considerable attention with exceptional mechanical properties, biocompatibility, and renewability. Within the domain of conductive hydrogels, nanocellulose distinctive characteristics position it as a preeminent reinforcing and dispersing agent, thereby markedly augmenting the overall performance of hydrogels. This article reviews the progress of nanocellulose applications in conductive hydrogels and discusses its mechanism of action as reinforcing and dispersing agents in detail, as well as the preparation methods with different conductive fillers (carbon materials, conductive polymers, metal nanoparticles and metal ions). Additionally, the extant research findings on the mechanical, self-healing, self-adhesion and freeze resistance properties of the conductive hydrogels are comprehensively introduced. In conclusion, the article provides a comprehensive outlook on the ongoing issues of nanocellulose-based conductive hydrogels and their possible future directions.","PeriodicalId":270,"journal":{"name":"Chemical Engineering Journal","volume":"38 1","pages":""},"PeriodicalIF":15.1,"publicationDate":"2025-01-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143050750","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
High efficiency selective recovery of Al from high-alumina fly ash by multistage activation and carbonation on-site application scale
IF 15.1 1区 工程技术 Q1 ENGINEERING, CHEMICAL Pub Date : 2025-01-28 DOI: 10.1016/j.cej.2025.160003
Shanshan Zhang, Lijie Yu, Yi Lv, Tianyu Zeng, Haobo Hou, Jirong Lan
A method of calcination activation-chemical separation-carbonization precipitation was developed for selective recovery of Al from high-alumina fly ash (HAFA). Specifically, calcium carbide slag, CaF2 and HAFA were used for mechanical mixing and calcination, and then, Al was leached with sodium carbonate solution, followed by the use of CaO to separation and removal of Si, the next step of filtration to remove the residue to obtain, and finally, the precipitation recovery of Al was realized by the passage of CO2 into the solution. Consequently, the formation of soluble calcium aluminate (C12A7) and insoluble dicalcium silicate (C2S) is promoted, effectively achieving the separation of silicon and aluminum during the calcination process. Desiliconization and carbonation of the leaching solution yielded aluminum hydroxide with a conversion rate of 96.67 % and a purity of 98.40 %. Pilot-scale experiments achieve an overall aluminum extraction rate of over 80 % and an aluminum purity of 98 %. In addition, the process absorbs 0.564 tons of CO2 per ton of Al(OH)3 produced. This study highlights the feasibility of large-scale collaborative carbon sequestration and efficient HAFA resource treatment.
{"title":"High efficiency selective recovery of Al from high-alumina fly ash by multistage activation and carbonation on-site application scale","authors":"Shanshan Zhang, Lijie Yu, Yi Lv, Tianyu Zeng, Haobo Hou, Jirong Lan","doi":"10.1016/j.cej.2025.160003","DOIUrl":"https://doi.org/10.1016/j.cej.2025.160003","url":null,"abstract":"A method of calcination activation-chemical separation-carbonization precipitation was developed for selective recovery of Al from high-alumina fly ash (HAFA). Specifically, calcium carbide slag, CaF<sub>2</sub> and HAFA were used for mechanical mixing and calcination, and then, Al was leached with sodium carbonate solution, followed by the use of CaO to separation and removal of Si, the next step of filtration to remove the residue to obtain, and finally, the precipitation recovery of Al was realized by the passage of CO<sub>2</sub> into the solution. Consequently, the formation of soluble calcium aluminate (C<sub>12</sub>A<sub>7</sub>) and insoluble dicalcium silicate (C<sub>2</sub>S) is promoted, effectively achieving the separation of silicon and aluminum during the calcination process. Desiliconization and carbonation of the leaching solution yielded aluminum hydroxide with a conversion rate of 96.67 % and a purity of 98.40 %. Pilot-scale experiments achieve an overall aluminum extraction rate of over 80 % and an aluminum purity of 98 %. In addition, the process absorbs 0.564 tons of CO<sub>2</sub> per ton of Al(OH)<sub>3</sub> produced. This study highlights the feasibility of large-scale collaborative carbon sequestration and efficient HAFA resource treatment.","PeriodicalId":270,"journal":{"name":"Chemical Engineering Journal","volume":"23 1","pages":""},"PeriodicalIF":15.1,"publicationDate":"2025-01-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143050582","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
Advanced low-temperature self-healable bio-polyurethanes with double-alkane-tailed ringing units for applications in self-powered flexible control panels
IF 15.1 1区 工程技术 Q1 ENGINEERING, CHEMICAL Pub Date : 2025-01-28 DOI: 10.1016/j.cej.2025.160019
Hong Wang, Mingjie Gao, Linman Zhang, Ziyue Su, Chaoyu Chen, Weijun Yang, Pengwu Xu, Deyu Niu, Pibo Ma, Piming Ma
Elastomers with dynamic covalent bonds are typically used to develop self-healing flexible control panels, however, their self-healing efficiency is low at low temperatures which hampers the stable operation and durability of the control panels. This work used a new strategy to achieve low-temperature self-healing in bio-based polyurethane elastomers (PDLBE) by designing a dynamic van der Waals force network. The elastomers are synthesized by using biobased monomers containing a double-alkane-tailed ringing unit and show self-healing efficiencies close to 90 % even under low temperature (−20 °C), supercooled brine (30 % NaCl @ −20 °C), and alkali (pH = 14) conditions. In addition, the PDLBE exhibits rapid self-healing capability, superior elongation rate (12,000 %), and reprocessability. Both experimental and molecular simulation results indicate that the low-temperature self-healing properties are mainly attributed to the abundant vdW forces and self-plasticization generated by the double-alkane-tailed ringing unit. Subsequently, low-temperature triboelectric nanogenerator (LT-TENG) and LT-TENG-based flexible control panels are successfully made from the elastomers, showing a recovery of 97 % at − 20 ℃ and a stable output (∼13 mW/m2) at − 30 ℃ after damage and even after 1200 cycles. This study presents a novel route for the preparation of low-temperature self-healable bio-elastomers and may expand their application in TENGs and flexible control panels in harsh environments.
{"title":"Advanced low-temperature self-healable bio-polyurethanes with double-alkane-tailed ringing units for applications in self-powered flexible control panels","authors":"Hong Wang, Mingjie Gao, Linman Zhang, Ziyue Su, Chaoyu Chen, Weijun Yang, Pengwu Xu, Deyu Niu, Pibo Ma, Piming Ma","doi":"10.1016/j.cej.2025.160019","DOIUrl":"https://doi.org/10.1016/j.cej.2025.160019","url":null,"abstract":"Elastomers with dynamic covalent bonds are typically used to develop self-healing flexible control panels, however, their self-healing efficiency is low at low temperatures which hampers the stable operation and durability of the control panels. This work used a new strategy to achieve low-temperature self-healing in bio-based polyurethane elastomers (PDLBE) by designing a dynamic van der Waals force network. The elastomers are synthesized by using biobased monomers containing a double-alkane-tailed ringing unit and show self-healing efficiencies close to 90 % even under low temperature (−20 °C), supercooled brine (30 % NaCl @ −20 °C), and alkali (pH = 14) conditions. In addition, the PDLBE exhibits rapid self-healing capability, superior elongation rate (12,000 %), and reprocessability. Both experimental and molecular simulation results indicate that the low-temperature self-healing properties are mainly attributed to the abundant vdW forces and self-plasticization generated by the double-alkane-tailed ringing unit. Subsequently, low-temperature triboelectric nanogenerator (LT-TENG) and LT-TENG-based flexible control panels are successfully made from the elastomers, showing a recovery of 97 % at − 20 ℃ and a stable output (∼13 mW/m<sup>2</sup>) at − 30 ℃ after damage and even after 1200 cycles. This study presents a novel route for the preparation of low-temperature self-healable bio-elastomers and may expand their application in TENGs and flexible control panels in harsh environments.","PeriodicalId":270,"journal":{"name":"Chemical Engineering Journal","volume":"40 1","pages":""},"PeriodicalIF":15.1,"publicationDate":"2025-01-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143050753","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
Bioinspired 1D structures for water harvesting: Theory, design and application
IF 15.1 1区 工程技术 Q1 ENGINEERING, CHEMICAL Pub Date : 2025-01-28 DOI: 10.1016/j.cej.2025.159917
Xikui Wang, Hong Luo, Ningkang Luo, Han Wei, Xueqiu Zhou, Bingli Qin, Yi Mei, Moyuan Cao, Youfa Zhang
The scarcity of water represents a significant challenge confronting the global community. One of the viable strategies to mitigate the water crisis involves the extraction of moisture from the atmosphere via bionics techniques. Within this domain, the emulation of one-dimensional (1D) biological structures, such as fibers inspired by the principles of spider silk or other organisms, emerges as a pivotal approach within the field of bionics. This paper provides a comprehensive review of the water harvesting mechanisms inherent to bioinspired 1D structures, examining the factors that influence droplet capture, dropwise condensation, droplet transport, and removal. Furthermore, it summarizes the primary water harvesting processes of bionic 1D structures and delineates methods to enhance the efficiency of water collection. Subsequent sections of this paper explore the water collection performance and structural optimization of various artificial 1D structures. In conclusion, the paper encapsulates the applications of bioinspired 1D structures, proposing directions for improvement and future developmental prospects.
{"title":"Bioinspired 1D structures for water harvesting: Theory, design and application","authors":"Xikui Wang, Hong Luo, Ningkang Luo, Han Wei, Xueqiu Zhou, Bingli Qin, Yi Mei, Moyuan Cao, Youfa Zhang","doi":"10.1016/j.cej.2025.159917","DOIUrl":"https://doi.org/10.1016/j.cej.2025.159917","url":null,"abstract":"The scarcity of water represents a significant challenge confronting the global community. One of the viable strategies to mitigate the water crisis involves the extraction of moisture from the atmosphere via bionics techniques. Within this domain, the emulation of one-dimensional (1D) biological structures, such as fibers inspired by the principles of spider silk or other organisms, emerges as a pivotal approach within the field of bionics. This paper provides a comprehensive review of the water harvesting mechanisms inherent to bioinspired 1D structures, examining the factors that influence droplet capture, dropwise condensation, droplet transport, and removal. Furthermore, it summarizes the primary water harvesting processes of bionic 1D structures and delineates methods to enhance the efficiency of water collection. Subsequent sections of this paper explore the water collection performance and structural optimization of various artificial 1D structures. In conclusion, the paper encapsulates the applications of bioinspired 1D structures, proposing directions for improvement and future developmental prospects.","PeriodicalId":270,"journal":{"name":"Chemical Engineering Journal","volume":"23 1","pages":""},"PeriodicalIF":15.1,"publicationDate":"2025-01-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143050754","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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