Pub Date : 2025-04-22DOI: 10.1016/j.cej.2025.162963
Emre Turan, Robert Dieckmann, Michael Geske, Raoul Naumann d’Alnoncourt, Michael Bender, Johannes Bode, Benjamin Frank, Dina Zakgeym, Grigorios Kolios, Frank Rosowski
Direct resistive heating is an effective and sustainable method for supplying heat to endothermic reactions. Ethanol dehydration, a sustainable route for producing ethylene, was chosen as the test reaction. A physical mixture of graphitic carbon particles serving as conductors and γ-Al2O3 as catalyst particles was prepared to create an electrically conductive fixed bed. A minimum of 33.4 vol% of conductive material ensured sufficient bed resistivity. Successful direct resistive heating was demonstrated, with near complete ethanol-to-ethylene conversion achieved at a bed temperature of 325 °C and a WHSVEtOH of 3.2 h−1. In contrast to the industrial process, which requires superheating to 470 °C with steam as the heat carrier gas, direct resistive heating operated at a lower temperature with 10 times higher productivity, without the need for a heat carrier gas. Upscaling in a 500 ml ceramic tubular reactor confirmed scalability, showcasing a sustainable method for ethylene production using green energy and renewable bio-ethanol.
{"title":"Direct resistive heating of a catalytic fixed-bed reactor for ethanol dehydration","authors":"Emre Turan, Robert Dieckmann, Michael Geske, Raoul Naumann d’Alnoncourt, Michael Bender, Johannes Bode, Benjamin Frank, Dina Zakgeym, Grigorios Kolios, Frank Rosowski","doi":"10.1016/j.cej.2025.162963","DOIUrl":"https://doi.org/10.1016/j.cej.2025.162963","url":null,"abstract":"Direct resistive heating is an effective and sustainable method for supplying heat to endothermic reactions. Ethanol dehydration, a sustainable route for producing ethylene, was chosen as the test reaction. A physical mixture of graphitic carbon particles serving as conductors and γ-Al<sub>2</sub>O<sub>3</sub> as catalyst particles was prepared to create an electrically conductive fixed bed. A minimum of 33.4 vol% of conductive material ensured sufficient bed resistivity. Successful direct resistive heating was demonstrated, with near complete ethanol-to-ethylene conversion achieved at a bed temperature of 325 °C and a WHSV<sub>EtOH</sub> of 3.2 h<sup>−1</sup>. In contrast to the industrial process, which requires superheating to 470 °C with steam as the heat carrier gas, direct resistive heating operated at a lower temperature with 10 times higher productivity, without the need for a heat carrier gas. Upscaling in a 500 ml ceramic tubular reactor confirmed scalability, showcasing a sustainable method for ethylene production using green energy and renewable bio-ethanol.","PeriodicalId":270,"journal":{"name":"Chemical Engineering Journal","volume":"17 1","pages":""},"PeriodicalIF":15.1,"publicationDate":"2025-04-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143862847","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"工程技术","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2025-04-22DOI: 10.1016/j.cej.2025.162958
Xiaoyu Liu, Lingui Huang, Xiuan Xi, Yan Yi, Giday Fisseha, Jie Gao, Yong Xi, Yuanfeng Liao, Jianwen Liu, Jiujun Zhang, Xian-Zhu Fu, Jing-Li Luo
The BaCo0.4Fe0.4Zr0.1Y0.1O3-δ (BCFZY) perovskite oxide is a highly promising cathode material for solid oxide fuel cells (SOFCs), mainly due to its exceptional three-phase conductivity at the elevated temperatures and remarkable oxygen reduction reaction (ORR) activity. Nevertheless, its limited electronic and ionic conductivities at relatively lower temperatures poses a significant challenge for its low-temperature applications. To address this issue, the Cu doping in the B-site of BCFZY is proposed. It is observed that Cu doping significantly enhances both the electronic conductivity and oxygen exchange kinetics, leading to a notable reduction in polarization resistance and a substantial improvement in ORR catalytic activity. Specifically, the Ni-YSZ anode-supported single cell equipped with BCFZYCu4 as the cathode exhibits a remarkable power density of 1.30 W cm−2 at 700 ℃, which surpasses that of the single cell with BCFZY cathode by 51.16 %. An in-depth mechanism study has revealed that the enhanced performance is closely linked to the increased orbitals hybridization induced by Cu doping. This not only enlarges the covalency of the Co-O/Cu–O bonds but also shifts the metal 3d and O 2p band center closer to the Fermi level, which significantly facilitates the oxygen adsorption, dissociation, and oxygen ion exchange processes of the BCFZYCu4 cathode.
BaCo0.4Fe0.4Zr0.1Y0.1O3-δ（BCFZY）包晶氧化物是一种非常有前途的固体氧化物燃料电池（SOFC）阴极材料，这主要是因为它在高温下具有优异的三相电导率和显著的氧还原反应（ORR）活性。然而，在相对较低的温度下，其有限的电子和离子导电性为其低温应用带来了巨大挑战。为了解决这一问题，有人提出在 BCFZY 的 B 位掺杂铜。研究发现，掺杂铜可显著提高电子传导性和氧交换动力学，从而明显降低极化电阻，大幅提高 ORR 催化活性。具体而言，以 BCFZYCu4 为阴极的 Ni-YSZ 阳极支持单电池在 700 ℃ 时的功率密度达到了 1.30 W cm-2，比以 BCFZY 为阴极的单电池高出 51.16%。深入的机理研究表明，性能的提高与铜掺杂引起的轨道杂化增加密切相关。这不仅扩大了 Co-O/Cu-O 键的共价性，还使金属 3d 和 O 2p 带中心更接近费米级，从而极大地促进了 BCFZYCu4 阴极的氧吸附、解离和氧离子交换过程。
{"title":"Regulating the d-p orbital hybridization in BaCo0.4Fe0.4Zr0.1Y0.1O3-δ via Cu doping for high-performance solid oxide fuel cells cathode","authors":"Xiaoyu Liu, Lingui Huang, Xiuan Xi, Yan Yi, Giday Fisseha, Jie Gao, Yong Xi, Yuanfeng Liao, Jianwen Liu, Jiujun Zhang, Xian-Zhu Fu, Jing-Li Luo","doi":"10.1016/j.cej.2025.162958","DOIUrl":"https://doi.org/10.1016/j.cej.2025.162958","url":null,"abstract":"The BaCo<sub>0.4</sub>Fe<sub>0.4</sub>Zr<sub>0.1</sub>Y<sub>0.1</sub>O<sub>3-δ</sub> (BCFZY) perovskite oxide is a highly promising cathode material for solid oxide fuel cells (SOFCs), mainly due to its exceptional three-phase conductivity at the elevated temperatures and remarkable oxygen reduction reaction (ORR) activity. Nevertheless, its limited electronic and ionic conductivities at relatively lower temperatures poses a significant challenge for its low-temperature applications. To address this issue, the Cu doping in the B-site of BCFZY is proposed. It is observed that Cu doping significantly enhances both the electronic conductivity and oxygen exchange kinetics, leading to a notable reduction in polarization resistance and a substantial improvement in ORR catalytic activity. Specifically, the Ni-YSZ anode-supported single cell equipped with BCFZYCu4 as the cathode exhibits a remarkable power density of 1.30 W cm<sup>−2</sup> at 700 ℃, which surpasses that of the single cell with BCFZY cathode by 51.16 %. An in-depth mechanism study has revealed that the enhanced performance is closely linked to the increased orbitals hybridization induced by Cu doping. This not only enlarges the covalency of the Co-O/Cu–O bonds but also shifts the metal 3<em>d</em> and O 2<em>p</em> band center closer to the Fermi level, which significantly facilitates the oxygen adsorption, dissociation, and oxygen ion exchange processes of the BCFZYCu4 cathode.","PeriodicalId":270,"journal":{"name":"Chemical Engineering Journal","volume":"6 1","pages":""},"PeriodicalIF":15.1,"publicationDate":"2025-04-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143862807","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"工程技术","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2025-04-22DOI: 10.1016/j.cej.2025.162947
Dun Wei, Haoran Dong, Baixue Ouyang, Peng Chen, Tingzheng Zhang, Yingjie He, Lei Huang, Haiying Wang
Bismuth (Bi), possessing intrinsic faradaic properties, has garnered significant attention as a highly promising anode material for capacitive deionization (CDI) due to its superior capacity and strong Cl− affinity. However, the substantial volume expansion and pronounced pulverization of the Bi electrode during the chlorination/dechlorination conversion process significantly compromise its cycling stability. Herein, conductive porous Bi-based metal–organic framework (Bi-Fc-MOF) nanoflowers with dual redox active sites were strategically designed and fabricated as CDI anodes, leveraging the organic linker coordination effect. The organic linker strategically disperses Bi centers at the molecular level within the framework, effectively preventing the agglomeration and fragmentation of Bi particles and thus ensuring long-term cycling performance. The synergistic mechanism involving Bi node conversion reactions and the Fe2+/Fe3+ redox couple charge compensation effect from the ferrocene center enhances the Cl− capture. Owing to these unique and advantageous features, Bi-Fc-MOF exhibits exceptional dechlorination capacity (107.21 mg g−1), high charge efficiency (0.93), and outstanding long-term cycling stability (92.26 % after 50 cycles). Impressively, the systematic ex-situ characterization revealed the synergistic Cl− storage mechanism of the conversion reaction-coupled charge compensation effect in Bi-Fc-MOF. This study offers innovative insights into the design and development of advanced high-performance CDI anode materials
{"title":"Conductive bismuth-based metal-organic frameworks with dual redox sites for efficient capacitive deionization","authors":"Dun Wei, Haoran Dong, Baixue Ouyang, Peng Chen, Tingzheng Zhang, Yingjie He, Lei Huang, Haiying Wang","doi":"10.1016/j.cej.2025.162947","DOIUrl":"https://doi.org/10.1016/j.cej.2025.162947","url":null,"abstract":"Bismuth (Bi), possessing intrinsic faradaic properties, has garnered significant attention as a highly promising anode material for capacitive deionization (CDI) due to its superior capacity and strong Cl<sup>−</sup> affinity. However, the substantial volume expansion and pronounced pulverization of the Bi electrode during the chlorination/dechlorination conversion process significantly compromise its cycling stability. Herein, conductive porous Bi-based metal–organic framework (Bi-Fc-MOF) nanoflowers with dual redox active sites were strategically designed and fabricated as CDI anodes, leveraging the organic linker coordination effect. The organic linker strategically disperses Bi centers at the molecular level within the framework, effectively preventing the agglomeration and fragmentation of Bi particles and thus ensuring long-term cycling performance. The synergistic mechanism involving Bi node conversion reactions and the Fe<sup>2+</sup>/Fe<sup>3+</sup> redox couple charge compensation effect from the ferrocene center enhances the Cl<sup>−</sup> capture. Owing to these unique and advantageous features, Bi-Fc-MOF exhibits exceptional dechlorination capacity (107.21 mg g<sup>−1</sup>), high charge efficiency (0.93), and outstanding long-term cycling stability (92.26 % after 50 cycles). Impressively, the systematic ex-situ characterization revealed the synergistic Cl<sup>−</sup> storage mechanism of the conversion reaction-coupled charge compensation effect in Bi-Fc-MOF. This study offers innovative insights into the design and development of advanced high-performance CDI anode materials","PeriodicalId":270,"journal":{"name":"Chemical Engineering Journal","volume":"2 1","pages":""},"PeriodicalIF":15.1,"publicationDate":"2025-04-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143857885","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"工程技术","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2025-04-22DOI: 10.1016/j.cej.2025.162927
Yadong Guo, Janak Lal Pathak, Yinyin Huang, Jingru Han, Junyan Zeng, Ling Chen, Yongshan Li, Wenbo Du, Liping Wang, Lan Yang
Effective repair of severe bone defects is a significant challenge in clinical practice. Recent research has highlighted the potential of apoptotic vesicles derived from mesenchymal stem cells (MSC-ApoEVs) for tissue repair. This study specifically explored the use of ApoEVs derived from periodontal ligament stem cells (PDLSCs-ApoEVs) and their ability to treat localized bone defects. In a mouse model with cranial defects, PDLSCs-ApoEVs were found to stimulate bone regeneration effectively. However, in vitro studies showed that these vesicles had limited ability to promote osteogenic differentiation in bone marrow stromal cells (BMSCs). Further investigation revealed that PDLSCs-ApoEVs enhanced angiogenesis and osteogenesis by coupling these two processes. The mechanism involved is MAPK1/3 within PDLSCs-ApoEVs, which increased the expression of STC1 in endothelial cells through the MAPK1/3-FOS pathway. STC1, a secretory protein, promoted both angiogenesis and osteogenic differentiation, forming H-type blood vessels in the bone-forming environment. This combined effect of angiogenesis and osteogenesis significantly improved bone repair in the mouse model. Overall, this study sheds light on the role and mechanisms of PDLSCs-ApoEVs in bone formation, offering new perspectives on their potential for tissue regeneration therapy.
{"title":"PDLSCs-ApoEVs enhance bone regeneration through MAPK1/3-induced STC1 upregulation in endothelial cells via the FOS pathway","authors":"Yadong Guo, Janak Lal Pathak, Yinyin Huang, Jingru Han, Junyan Zeng, Ling Chen, Yongshan Li, Wenbo Du, Liping Wang, Lan Yang","doi":"10.1016/j.cej.2025.162927","DOIUrl":"https://doi.org/10.1016/j.cej.2025.162927","url":null,"abstract":"Effective repair of severe bone defects is a significant challenge in clinical practice. Recent research has highlighted the potential of apoptotic vesicles derived from mesenchymal stem cells (MSC-ApoEVs) for tissue repair. This study specifically explored the use of ApoEVs derived from periodontal ligament stem cells (PDLSCs-ApoEVs) and their ability to treat localized bone defects. In a mouse model with cranial defects, PDLSCs-ApoEVs were found to stimulate bone regeneration effectively. However, in vitro studies showed that these vesicles had limited ability to promote osteogenic differentiation in bone marrow stromal cells (BMSCs). Further investigation revealed that PDLSCs-ApoEVs enhanced angiogenesis and osteogenesis by coupling these two processes. The mechanism involved is MAPK1/3 within PDLSCs-ApoEVs, which increased the expression of STC1 in endothelial cells through the MAPK1/3-FOS pathway. STC1, a secretory protein, promoted both angiogenesis and osteogenic differentiation, forming H-type blood vessels in the bone-forming environment. This combined effect of angiogenesis and osteogenesis significantly improved bone repair in the mouse model. Overall, this study sheds light on the role and mechanisms of PDLSCs-ApoEVs in bone formation, offering new perspectives on their potential for tissue regeneration therapy.","PeriodicalId":270,"journal":{"name":"Chemical Engineering Journal","volume":"24 1","pages":""},"PeriodicalIF":15.1,"publicationDate":"2025-04-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143862834","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}
Aqueous zinc-ion batteries (AZIBs) are identified as a serious contender for flexible energy storage devices on account of their safety and low cost. Nevertheless, the rapid capacity decay attributed to the structural deterioration and by-product formation of active materials has hindered their further development, which is more evident at low current density. Herein, we prepared a flexible self-supported hybrid cathode material VGS-811, composed of V2O5·1.6H2O (VOH), graphene oxide (GO), and single-walled carbon nanotubes (SWCNTs), which delivers extremely high specific capacity of 443.6 mAh g−1 at 0.1 A g−1 and exhibits remarkable cycle stability with a capacity retention of 86.7 % after 5000 cycles at 0.5 A g−1. In this cathode, GO matrix prevents direct VOH-electrolyte contact, effectively mitigating its dissolution. Simultaneously, SWCNTs facilitate by-product decomposition and enhance electrochemical kinetics through their superior conductivity. For the active material VOH, Zn2+ is embedded into the interlayers to form Zn-O bonds through in-situ electrochemical reaction in the first cycle, which act as pillars between adjacent [VO] layers to maintain structural stability. In addition, due to the high conductivity and flexibility of VGS-811, the assembled flexible soft-packaged AZIBs display stable electrochemical performances at different deformation states. This work provides insights on the combination of active materials with carbon materials and in-situ electrochemical conversion.
{"title":"Freestanding vanadium oxides/carbon hybrid cathode with long-term cyclability at low current density for flexible aqueous zinc ion batteries","authors":"Zhouyang Qin, Gaoxu Han, Yilin Yang, Shengle Hao, Lingxiao Yu, Yuxiao Lin, Yunsong Li, Ruitao Lv, Wanci Shen, Feiyu Kang, Zheng-Hong Huang","doi":"10.1016/j.cej.2025.162952","DOIUrl":"https://doi.org/10.1016/j.cej.2025.162952","url":null,"abstract":"Aqueous zinc-ion batteries (AZIBs) are identified as a serious contender for flexible energy storage devices on account of their safety and low cost. Nevertheless, the rapid capacity decay attributed to the structural deterioration and by-product formation of active materials has hindered their further development, which is more evident at low current density. Herein, we prepared a flexible self-supported hybrid cathode material VGS-811, composed of V<sub>2</sub>O<sub>5</sub>·1.6H<sub>2</sub>O (VOH), graphene oxide (GO), and single-walled carbon nanotubes (SWCNTs), which delivers extremely high specific capacity of 443.6 mAh g<sup>−1</sup> at 0.1 A g<sup>−1</sup> and exhibits remarkable cycle stability with a capacity retention of 86.7 % after 5000 cycles at 0.5 A g<sup>−1</sup>. In this cathode, GO matrix prevents direct VOH-electrolyte contact, effectively mitigating its dissolution. Simultaneously, SWCNTs facilitate by-product decomposition and enhance electrochemical kinetics through their superior conductivity. For the active material VOH, Zn<sup>2+</sup> is embedded into the interlayers to form Zn-O bonds through in-situ electrochemical reaction in the first cycle, which act as pillars between adjacent [VO] layers to maintain structural stability. In addition, due to the high conductivity and flexibility of VGS-811, the assembled flexible soft-packaged AZIBs display stable electrochemical performances at different deformation states. This work provides insights on the combination of active materials with carbon materials and in-situ electrochemical conversion.","PeriodicalId":270,"journal":{"name":"Chemical Engineering Journal","volume":"4 1","pages":""},"PeriodicalIF":15.1,"publicationDate":"2025-04-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143862835","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"工程技术","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2025-04-22DOI: 10.1016/j.cej.2025.162980
Luxuan Zhang, Qinting Zhu, Yuting Zhou, Bo Xu, Man Zhou, Ping Wang, Qiang Wang, Yuanyuan Yu
Radiative cooling textiles are increasingly recognized as an effective strategy for energy-efficient thermal regulation. In this study, we present a novel radiative cooling textile, PTFE/SiO2@Cotton, fabricated through in-situ synthesis of silica particles on cotton fabric followed by a polytetrafluoroethylene (PTFE) coating. The in-situ growth of SiO2 nanoparticles significantly improved the durability of the fabric, ensuring long-term stability under various environmental conditions. The designed two-ply structure, which utilized the difference in refractive indices between PTFE (n = 1.29) and SiO2 (n = 1.47), enhanced the backscattering of sunlight, resulting in a remarkable solar reflectance of 80.2 % in the visible light range (0.2–2.5 µm). The PTFE/ SiO2@Cotton fabric exhibited high emissivity in both the first (8 ∼ 13 µm) and second (16 ∼ 25 µm) atmospheric windows, with an average emissivity of 97.8 % in the 4 ∼ 25 µm range. This dual-window emission provides effective radiative cooling in both dry and humid climates, making it adaptable to a variety of environmental conditions. Under simulated sunlight, the PTFE/ SiO2@Cotton fabric demonstrated a temperature reduction of up to 11 °C compared to unmodified cotton fabric. Outdoor experiments further validated the cooling performance of the fabric, showing a temperature reduction of approximately 5 °C under peak solar irradiance (∼900 W/m2). In addition, the fabric had excellent UV resistance (UPF 186.8), self-cleaning properties, and washability, making it a practical solution for personal and architectural radiant cooling applications. This work provides a scalable and cost-effective approach to radiative cooling textiles, with significant potential for real-world implementation in diverse climatic conditions.
{"title":"Dual-window emissive radiative cooling textiles with a PTFE/SiO2 bilayer coating for enhanced thermal management","authors":"Luxuan Zhang, Qinting Zhu, Yuting Zhou, Bo Xu, Man Zhou, Ping Wang, Qiang Wang, Yuanyuan Yu","doi":"10.1016/j.cej.2025.162980","DOIUrl":"https://doi.org/10.1016/j.cej.2025.162980","url":null,"abstract":"Radiative cooling textiles are increasingly recognized as an effective strategy for energy-efficient thermal regulation. In this study, we present a novel radiative cooling textile, PTFE/SiO<sub>2</sub>@Cotton, fabricated through in-situ synthesis of silica particles on cotton fabric followed by a polytetrafluoroethylene (PTFE) coating. The in-situ growth of SiO<sub>2</sub> nanoparticles significantly improved the durability of the fabric, ensuring long-term stability under various environmental conditions. The designed two-ply structure, which utilized the difference in refractive indices between PTFE (n = 1.29) and SiO<sub>2</sub> (n = 1.47), enhanced the backscattering of sunlight, resulting in a remarkable solar reflectance of 80.2 % in the visible light range (0.2–2.5 µm). The PTFE/ SiO<sub>2</sub>@Cotton fabric exhibited high emissivity in both the first (8 ∼ 13 µm) and second (16 ∼ 25 µm) atmospheric windows, with an average emissivity of 97.8 % in the 4 ∼ 25 µm range. This dual-window emission provides effective radiative cooling in both dry and humid climates, making it adaptable to a variety of environmental conditions. Under simulated sunlight, the PTFE/ SiO<sub>2</sub>@Cotton fabric demonstrated a temperature reduction of up to 11 °C compared to unmodified cotton fabric. Outdoor experiments further validated the cooling performance of the fabric, showing a temperature reduction of approximately 5 °C under peak solar irradiance (∼900 W/m<sup>2</sup>). In addition, the fabric had excellent UV resistance (UPF 186.8), self-cleaning properties, and washability, making it a practical solution for personal and architectural radiant cooling applications. This work provides a scalable and cost-effective approach to radiative cooling textiles, with significant potential for real-world implementation in diverse climatic conditions.","PeriodicalId":270,"journal":{"name":"Chemical Engineering Journal","volume":"4 1","pages":""},"PeriodicalIF":15.1,"publicationDate":"2025-04-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143862845","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"工程技术","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2025-04-22DOI: 10.1016/j.cej.2025.162951
Yue Hou, Jiao Li, Guofeng Tian, Rui Tian, Chao Lu
Alkoxy radicals (RO•) and peroxy radicals (ROO•) are generated during thermo-oxidation of polymers under oxygen environment, leading to RO•-dominated or ROO•-dominated reaction pathways with severely deteriorated polymer chains or terminated reaction. However, it has been a long-standing challenge to in-situ distinguish RO• and ROO• radicals due to their short-lived lifetime. In principle, chemiluminescence (CL) deserves to become an efficient strategy for in-situ monitoring for various radicals. However, it fails to differentiate RO• and ROO• radicals due to their fully overlapping emission wavelengths. In this contribution, we have proposed a CL dynamic fitting strategy to distinguish RO• and ROO• radicals of in-situ production during thermal oxidation under the different oxygen-containing environment. Based on two equations, <span><span style=""><math><mrow is="true"><mi is="true">ln</mi><mi is="true">I</mi><mspace is="true" width="3.33333pt"></mspace><mo is="true" linebreak="goodbreak" linebreakstyle="after">=</mo><mspace is="true" width="3.33333pt"></mspace><mi is="true">ln</mi><mi is="true">A</mi><mo is="true">·</mo><msub is="true"><mi is="true">k</mi><mrow is="true"><mi is="true" mathvariant="italic">RO</mi></mrow></msub><mspace is="true" width="3.33333pt"></mspace><mo is="true" linebreak="badbreak" linebreakstyle="after">-</mo><mspace is="true" width="3.33333pt"></mspace><mi is="true">ln</mi><mfenced close=")" is="true" open="("><mrow is="true"><mrow is="true"><mn is="true">1</mn><mspace is="true" width="3.33333pt"></mspace><mo is="true">+</mo><mspace is="true" width="3.33333pt"></mspace><mi is="true">Y</mi><mo is="true">·</mo><msup is="true"><mi is="true">e</mi><mrow is="true"><mo is="true">-</mo><msub is="true"><mi is="true">k</mi><mrow is="true"><mi is="true" mathvariant="italic">RO</mi></mrow></msub><mi is="true">t</mi></mrow></msup></mrow></mrow></mfenced><mo is="true">,</mo><mspace is="true" width="3.33333pt"></mspace><mi is="true">a</mi><mi is="true">n</mi><mi is="true">d</mi><mspace is="true" width="3.33333pt"></mspace><mi is="true">ln</mi><mi is="true">I</mi><mspace is="true" width="3.33333pt"></mspace><mo is="true" linebreak="goodbreak" linebreakstyle="after">=</mo><mspace is="true" width="3.33333pt"></mspace><mi is="true">ln</mi><mi is="true">B</mi><mspace is="true" width="3.33333pt"></mspace><mo is="true" linebreak="badbreak" linebreakstyle="after">-</mo><mspace is="true" width="3.33333pt"></mspace><msub is="true"><mi is="true">k</mi><mrow is="true"><mi is="true" mathvariant="italic">ROO</mi></mrow></msub><mi is="true">t</mi><mspace is="true" width="3.33333pt"></mspace><mo is="true" linebreak="badbreak" linebreakstyle="after">-</mo><mspace is="true" width="3.33333pt"></mspace><mn is="true">2</mn><mi is="true">ln</mi><mfenced close=")" is="true" open="("><mrow is="true"><mrow is="true"><mn is="true">1</mn><mspace is="true" width="3.33333pt"></mspace><mo is="true">+</mo><mspace is="true" width="3.33333pt"></mspace><mi is="true">
{"title":"Unraveling thermo-oxidation degradation pathways of polymers by in-situ differentiating the alkyl-related reactive oxygen radicals","authors":"Yue Hou, Jiao Li, Guofeng Tian, Rui Tian, Chao Lu","doi":"10.1016/j.cej.2025.162951","DOIUrl":"https://doi.org/10.1016/j.cej.2025.162951","url":null,"abstract":"Alkoxy radicals (RO•) and peroxy radicals (ROO•) are generated during thermo-oxidation of polymers under oxygen environment, leading to RO•-dominated or ROO•-dominated reaction pathways with severely deteriorated polymer chains or terminated reaction. However, it has been a long-standing challenge to in-situ distinguish RO• and ROO• radicals due to their short-lived lifetime. In principle, chemiluminescence (CL) deserves to become an efficient strategy for in-situ monitoring for various radicals. However, it fails to differentiate RO• and ROO• radicals due to their fully overlapping emission wavelengths. In this contribution, we have proposed a CL dynamic fitting strategy to distinguish RO• and ROO• radicals of in-situ production during thermal oxidation under the different oxygen-containing environment. Based on two equations, <span><span style=\"\"><math><mrow is=\"true\"><mi is=\"true\">ln</mi><mi is=\"true\">I</mi><mspace is=\"true\" width=\"3.33333pt\"></mspace><mo is=\"true\" linebreak=\"goodbreak\" linebreakstyle=\"after\">=</mo><mspace is=\"true\" width=\"3.33333pt\"></mspace><mi is=\"true\">ln</mi><mi is=\"true\">A</mi><mo is=\"true\">·</mo><msub is=\"true\"><mi is=\"true\">k</mi><mrow is=\"true\"><mi is=\"true\" mathvariant=\"italic\">RO</mi></mrow></msub><mspace is=\"true\" width=\"3.33333pt\"></mspace><mo is=\"true\" linebreak=\"badbreak\" linebreakstyle=\"after\">-</mo><mspace is=\"true\" width=\"3.33333pt\"></mspace><mi is=\"true\">ln</mi><mfenced close=\")\" is=\"true\" open=\"(\"><mrow is=\"true\"><mrow is=\"true\"><mn is=\"true\">1</mn><mspace is=\"true\" width=\"3.33333pt\"></mspace><mo is=\"true\">+</mo><mspace is=\"true\" width=\"3.33333pt\"></mspace><mi is=\"true\">Y</mi><mo is=\"true\">·</mo><msup is=\"true\"><mi is=\"true\">e</mi><mrow is=\"true\"><mo is=\"true\">-</mo><msub is=\"true\"><mi is=\"true\">k</mi><mrow is=\"true\"><mi is=\"true\" mathvariant=\"italic\">RO</mi></mrow></msub><mi is=\"true\">t</mi></mrow></msup></mrow></mrow></mfenced><mo is=\"true\">,</mo><mspace is=\"true\" width=\"3.33333pt\"></mspace><mi is=\"true\">a</mi><mi is=\"true\">n</mi><mi is=\"true\">d</mi><mspace is=\"true\" width=\"3.33333pt\"></mspace><mi is=\"true\">ln</mi><mi is=\"true\">I</mi><mspace is=\"true\" width=\"3.33333pt\"></mspace><mo is=\"true\" linebreak=\"goodbreak\" linebreakstyle=\"after\">=</mo><mspace is=\"true\" width=\"3.33333pt\"></mspace><mi is=\"true\">ln</mi><mi is=\"true\">B</mi><mspace is=\"true\" width=\"3.33333pt\"></mspace><mo is=\"true\" linebreak=\"badbreak\" linebreakstyle=\"after\">-</mo><mspace is=\"true\" width=\"3.33333pt\"></mspace><msub is=\"true\"><mi is=\"true\">k</mi><mrow is=\"true\"><mi is=\"true\" mathvariant=\"italic\">ROO</mi></mrow></msub><mi is=\"true\">t</mi><mspace is=\"true\" width=\"3.33333pt\"></mspace><mo is=\"true\" linebreak=\"badbreak\" linebreakstyle=\"after\">-</mo><mspace is=\"true\" width=\"3.33333pt\"></mspace><mn is=\"true\">2</mn><mi is=\"true\">ln</mi><mfenced close=\")\" is=\"true\" open=\"(\"><mrow is=\"true\"><mrow is=\"true\"><mn is=\"true\">1</mn><mspace is=\"true\" width=\"3.33333pt\"></mspace><mo is=\"true\">+</mo><mspace is=\"true\" width=\"3.33333pt\"></mspace><mi is=\"true\">","PeriodicalId":270,"journal":{"name":"Chemical Engineering Journal","volume":"219 1","pages":""},"PeriodicalIF":15.1,"publicationDate":"2025-04-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143857884","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"工程技术","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2025-04-22DOI: 10.1016/j.cej.2025.162953
Zhiyong Ran, Yue Li, Xiankun Lin, Qiang He
Electrochemical biosensors have promising applications such as the detection of biomarkers for cancer diagnosis, but their performance is still limited by the passive diffusion of molecules. Due to the autonomous and steerable motion capabilities, magnetically-driven micromotors display the advantages of enhancing diffusion and micro-mixing. However, developing micromotor-enhanced electrochemical biosensors is still challenging. Herein, we report magnetically-driven helical PANI-Fe3O4@SP-HP5@AuNPs (PFSHA) micromotors, in which the combination of the micromotor technology and host–guest recognition strategy enables sensitive detection of p53 DNA. The micromotors are fabricated by integrating gold nanoparticle-stabilized pillar[5]arenes (HP5@AuNPs), polyaniline (PANI), and iron oxide (Fe3O4) nanoparticles onto Spirulina (SP). Under a rotating magnetic field, the micromotors exhibit steerable motility with an average speed of 21.7 µm/s. Consequently, the micromotor-functionalized electrochemical biosensors achieve high sensitivity and a detection limit of 0.66 pM towards p53 DNA, with a linear range from 1 pM to 100 µM. The advantages of the micromotors, including autonomous motion, micro-mixing, enhanced diffusion, and improved mass transfer, enable significant improvement in the performance of electrochemical biosensing. Therefore, integrating micromotor technology into sensing analysis paves a promising way to address the limitations of existing electrochemical biosensors, offering new solutions for advanced clinical diagnosis.
{"title":"Pillar[5]arene@AuNP-Functionalized, Magnetically-Propelled helical micromotors for On-The-Fly electrochemical biosensing of p53 DNA sequence","authors":"Zhiyong Ran, Yue Li, Xiankun Lin, Qiang He","doi":"10.1016/j.cej.2025.162953","DOIUrl":"https://doi.org/10.1016/j.cej.2025.162953","url":null,"abstract":"Electrochemical biosensors have promising applications such as the detection of biomarkers for cancer diagnosis, but their performance is still limited by the passive diffusion of molecules. Due to the autonomous and steerable motion capabilities, magnetically-driven micromotors display the advantages of enhancing diffusion and micro-mixing. However, developing micromotor-enhanced electrochemical biosensors is still challenging. Herein, we report magnetically-driven helical PANI-Fe<sub>3</sub>O<sub>4</sub>@SP-HP5@AuNPs (PFSHA) micromotors, in which the combination of the micromotor technology and host–guest recognition strategy enables sensitive detection of p53 DNA. The micromotors are fabricated by integrating gold nanoparticle-stabilized pillar[5]arenes (HP5@AuNPs), polyaniline (PANI), and iron oxide (Fe<sub>3</sub>O<sub>4</sub>) nanoparticles onto Spirulina (SP). Under a rotating magnetic field, the micromotors exhibit steerable motility with an average speed of 21.7 µm/s. Consequently, the micromotor-functionalized electrochemical biosensors achieve high sensitivity and a detection limit of 0.66 pM towards p53 DNA, with a linear range from 1 pM to 100 µM. The advantages of the micromotors, including autonomous motion, micro-mixing, enhanced diffusion, and improved mass transfer, enable significant improvement in the performance of electrochemical biosensing. Therefore, integrating micromotor technology into sensing analysis paves a promising way to address the limitations of existing electrochemical biosensors, offering new solutions for advanced clinical diagnosis.","PeriodicalId":270,"journal":{"name":"Chemical Engineering Journal","volume":"51 1","pages":""},"PeriodicalIF":15.1,"publicationDate":"2025-04-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143862774","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"工程技术","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2025-04-22DOI: 10.1016/j.cej.2025.162961
Jianghui Qiu, Xiafei Gao, Juan Peng
The formaldehyde oxidation reaction (FOR) with ultra-low potential is an ideal alternative to the oxygen evolution reaction (OER), significantly reducing hydrogen production energy consumption. This reaction not only generates high-value formic acid but also releases H2 at low potential, enhancing hydrogen production efficiency and economic viability. However, developing efficient and low-cost electrocatalysts remains a key challenge. In this study, a Pt single atom on Cu nanowire catalyst shows high catalytic activity for formaldehyde oxidation reaction (FOR). The catalyst achieves a current density of 100 mA cm−2 at 0.09 V vs. RHE, with formic acid yield, selectivity, and formaldehyde conversion rate all close to 100 %. A bipolar hydrogen production system (FOR-HER) based on PtSA-Cu NWs and Pt/C assembly achieves a current density of 100 mA cm−2 at a low cell voltage of 0.12 V, demonstrating a Faraday efficiency close to 100 % for H2 at both the anode and cathode, and can stable operation for 30 h. Density functional theory (DFT) studies reveal that the interaction between Pt single atoms and Cu enhances hydrogen adsorption, significantly reducing the free energy of H* coupling and thereby improving hydrogen production efficiency. This study elucidates the intrinsic mechanism behind the enhanced performance, providing valuable guidance for the development of high-performance, low-cost single-atom catalysts.
{"title":"Pt single atoms on Cu nanowires facilitate anodic hydrogen production through efficient electrochemical formaldehyde oxidation","authors":"Jianghui Qiu, Xiafei Gao, Juan Peng","doi":"10.1016/j.cej.2025.162961","DOIUrl":"https://doi.org/10.1016/j.cej.2025.162961","url":null,"abstract":"The formaldehyde oxidation reaction (FOR) with ultra-low potential is an ideal alternative to the oxygen evolution reaction (OER), significantly reducing hydrogen production energy consumption. This reaction not only generates high-value formic acid but also releases H<sub>2</sub> at low potential, enhancing hydrogen production efficiency and economic viability. However, developing efficient and low-cost electrocatalysts remains a key challenge. In this study, a Pt single atom on Cu nanowire catalyst shows high catalytic activity for formaldehyde oxidation reaction (FOR). The catalyst achieves a current density of 100 mA cm<sup>−2</sup> at 0.09 V vs. RHE, with formic acid yield, selectivity, and formaldehyde conversion rate all close to 100 %. A bipolar hydrogen production system (FOR-HER) based on Pt<sub>SA</sub>-Cu NWs and Pt/C assembly achieves a current density of 100 mA cm<sup>−2</sup> at a low cell voltage of 0.12 V, demonstrating a Faraday efficiency close to 100 % for H<sub>2</sub> at both the anode and cathode, and can stable operation for 30 h. Density functional theory (DFT) studies reveal that the interaction between Pt single atoms and Cu enhances hydrogen adsorption, significantly reducing the free energy of H* coupling and thereby improving hydrogen production efficiency. This study elucidates the intrinsic mechanism behind the enhanced performance, providing valuable guidance for the development of high-performance, low-cost single-atom catalysts.","PeriodicalId":270,"journal":{"name":"Chemical Engineering Journal","volume":"108 1","pages":""},"PeriodicalIF":15.1,"publicationDate":"2025-04-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143862831","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"工程技术","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2025-04-22DOI: 10.1016/j.cej.2025.162982
Xi Li, Xiangyi Ren, Haixia Yuan, Liying Wang, Minfeng Huo
The anthracycline doxorubicin (DOX) is an effective clinical drug for tumor chemotherapy, but its lethal cardiotoxicity limits its clinical applicability. Medical protection against DOX-induced cardiotoxicity and progressive heart failure remains challenging. Here, we present a feasible strategy in which polyvinylpyrrolidone, strontium, and ferricyanide are integrated to form self-assembled strontium Prussian blue (SrPB) to prevent DOX-induced cardiomyotoxicity effectively. The in vitro and in vivo results showed that SrPB significantly improved cardiomyocyte survival and cardiac function in the DOX-challenged murine model. Mechanistically, mitochondrial function analysis revealed that DOX-induced mitochondrial damage by increasing the amount of mitochondrial reactive oxygen species (mtROS) and decreasing the energy metabolism. SrPB administration effectively improved mitochondrial energy metabolism by scavenging mtROS and improving the intermediate products of glycolysis and glycoxidation. Together, our findings provide an intriguing paradigm for targeting mitochondrial energy metabolism to inhibit DOX-induced cardiotoxicity and demonstrate the therapeutic potential of SrPB for further clinical application.
{"title":"Strontium Prussian blue Promotes cardiac energy metabolism to alleviate Doxorubicin-Induced cardiotoxicity","authors":"Xi Li, Xiangyi Ren, Haixia Yuan, Liying Wang, Minfeng Huo","doi":"10.1016/j.cej.2025.162982","DOIUrl":"https://doi.org/10.1016/j.cej.2025.162982","url":null,"abstract":"The anthracycline doxorubicin (DOX) is an effective clinical drug for tumor chemotherapy, but its lethal cardiotoxicity limits its clinical applicability. Medical protection against DOX-induced cardiotoxicity and progressive heart failure remains challenging. Here, we present a feasible strategy in which polyvinylpyrrolidone, strontium, and ferricyanide are integrated to form self-assembled strontium Prussian blue (SrPB) to prevent DOX-induced cardiomyotoxicity effectively. The in vitro and in vivo results showed that SrPB significantly improved cardiomyocyte survival and cardiac function in the DOX-challenged murine model. Mechanistically, mitochondrial function analysis revealed that DOX-induced mitochondrial damage by increasing the amount of mitochondrial reactive oxygen species (mtROS) and decreasing the energy metabolism. SrPB administration effectively improved mitochondrial energy metabolism by scavenging mtROS and improving the intermediate products of glycolysis and glycoxidation. Together, our findings provide an intriguing paradigm for targeting mitochondrial energy metabolism to inhibit DOX-induced cardiotoxicity and demonstrate the therapeutic potential of SrPB for further clinical application.","PeriodicalId":270,"journal":{"name":"Chemical Engineering Journal","volume":"13 1","pages":""},"PeriodicalIF":15.1,"publicationDate":"2025-04-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143862778","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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