Pub Date : 2026-02-09DOI: 10.1016/j.cej.2026.173972
Maolin Qin, Lufeng Yao, Haiqing Wang, Le Zou, Jiawei He, Mengqi Jin, Xinrui Huang, Zichang Wu, Zhuoyang Song, Suhong Lu, Dong Peng, Kailiang Zhou, Jian Xiao, Ke Xu, Hongyu Zhang, Liangliang Yang, Lu Ge
Owing to the limited ability of the central nervous system to regenerate, spinal cord injury (SCI) continues to be a significant problem. Stem cell transplantation represents an attractive and promising therapeutic strategy for treating SCI; nevertheless, its clinical application remains limited by the intense inflammatory cascade and difficulties associated with achieving the stable proliferation and differentiation. To address these challenges, we propose an innovative “internal–external” synergistic strategy for stem cell transplantation for SCI repair. Adipose-derived stem cells (ADSCs) were endocytosed with apoptotic bodies (ABs) to form engineered stem cells, which were then loaded into Pueraria hydrogels (ABs@ADSCs/PUE). ABs preserved mitochondrial homeostasis and further regulated the c-Caspase 1-GSDMD-IL1β/IL-18 pathway to prevent pyroptosis. Moreover, the PUE hydrogel effectively eliminated ROS from the “outside” of ADSCs, providing favourable “soil” for stem cells to function. Mechanistically, transcriptomics sequencing and animal experiments revealed that ABs@ADSCs/PUE promoted autophagy and further inhibited ADSCs pyroptosis, subsequently restructuring the ADSCs–Microglia axis by regulating the cGAS/STING signalling pathway to prevent inflammation. In a murine model of SCI, ABs@ADSCs/PUE increased axonal and myelin regeneration, and further promoted the recovery of motor function. This research offers novel therapeutic perspectives on stem cell applications for the clinical rehabilitation of spinal cord injury.
由于中枢神经系统的再生能力有限,脊髓损伤(SCI)一直是一个重要的问题。干细胞移植是治疗脊髓损伤的一种有吸引力和前景的治疗策略;然而,它的临床应用仍然受到强烈的炎症级联反应和难以实现稳定的增殖和分化的限制。为了解决这些挑战,我们提出了一种创新的“内外”协同策略,用于干细胞移植修复脊髓损伤。脂肪源性干细胞(ADSCs)与凋亡小体(ABs)内吞形成工程化干细胞,然后将其装载到葛根水凝胶中(ABs@ADSCs/PUE)。ABs维持线粒体稳态,并进一步调节c-Caspase 1- gsdmd - il -1 β/IL-18通路,防止热亡。此外,PUE水凝胶有效地消除了来自ADSCs“外部”的ROS,为干细胞发挥功能提供了有利的“土壤”。机制上,转录组学测序和动物实验显示ABs@ADSCs/PUE促进自噬,进一步抑制ADSCs焦亡,随后通过调节cGAS/STING信号通路重组ADSCs -小胶质细胞轴,从而预防炎症。在小鼠脊髓损伤模型中,ABs@ADSCs/PUE增加轴突和髓鞘再生,进一步促进运动功能的恢复。本研究为干细胞在脊髓损伤临床康复中的应用提供了新的治疗前景。
{"title":"“Internal-external” synergistic strategy with engineered ADSCs by apoptotic bodies and antioxidant hydrogel mitigate pyroptosis and reshape the ADSCs-microglia axis for spinal cord injury recovery","authors":"Maolin Qin, Lufeng Yao, Haiqing Wang, Le Zou, Jiawei He, Mengqi Jin, Xinrui Huang, Zichang Wu, Zhuoyang Song, Suhong Lu, Dong Peng, Kailiang Zhou, Jian Xiao, Ke Xu, Hongyu Zhang, Liangliang Yang, Lu Ge","doi":"10.1016/j.cej.2026.173972","DOIUrl":"https://doi.org/10.1016/j.cej.2026.173972","url":null,"abstract":"Owing to the limited ability of the central nervous system to regenerate, spinal cord injury (SCI) continues to be a significant problem. Stem cell transplantation represents an attractive and promising therapeutic strategy for treating SCI; nevertheless, its clinical application remains limited by the intense inflammatory cascade and difficulties associated with achieving the stable proliferation and differentiation. To address these challenges, we propose an innovative “internal–external” synergistic strategy for stem cell transplantation for SCI repair. Adipose-derived stem cells (ADSCs) were endocytosed with apoptotic bodies (ABs) to form engineered stem cells, which were then loaded into Pueraria hydrogels (ABs@ADSCs/PUE). ABs preserved mitochondrial homeostasis and further regulated the c-Caspase 1-GSDMD-IL1β/IL-18 pathway to prevent pyroptosis. Moreover, the PUE hydrogel effectively eliminated ROS from the “outside” of ADSCs, providing favourable “soil” for stem cells to function. Mechanistically, transcriptomics sequencing and animal experiments revealed that ABs@ADSCs/PUE promoted autophagy and further inhibited ADSCs pyroptosis, subsequently restructuring the ADSCs–Microglia axis by regulating the cGAS/STING signalling pathway to prevent inflammation. In a murine model of SCI, ABs@ADSCs/PUE increased axonal and myelin regeneration, and further promoted the recovery of motor function. This research offers novel therapeutic perspectives on stem cell applications for the clinical rehabilitation of spinal cord injury.","PeriodicalId":270,"journal":{"name":"Chemical Engineering Journal","volume":"30 1","pages":""},"PeriodicalIF":15.1,"publicationDate":"2026-02-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146146739","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 : 2026-02-09DOI: 10.1016/j.cej.2026.173967
Xianpeng Li, Tong Zhu, Xianguo Ji, Hao Lin, Zhirong Sun
Non-radical oxidation in heterogeneous electro-Fenton systems is crucial for removing organic contaminants in complex wastewater matrices. However, the generation mechanism of singlet oxygen (1O2) remains unclear, especially the transformation among reactive oxygen species during generation. Herein, the 1O2 generation mechanism driven by FeCo-NC dual active sites was elucidated through probe testing and electron paramagnetic resonance experiments involving selective quenchers. The main pathway for 1O2 formation was identified as the reaction of superoxide radicals (O2•–) with hydroxyl radicals (•OH), with a significant synergistic effect. The electron coupling between O2•– and •OH facilitated electron transfer from O2•– to •OH, accelerating the reaction kinetics. The density functional theory calculations indicated that O2•– and •OH selectively adsorbed at the Co and Fe sites, enhancing their collisions. The charge redistribution between FeCo facilitated the coupling of O2•– and •OH, significantly enhancing the production efficiency of 1O2 in the system. Quantitative analysis revealed individual contributions of O2•– and •OH accounting for only 4.7% and 2.0% of the overall 1O2 yield, highlighting the inefficiency of single-radical for 1O2 generation. Under the coexistence of O2•– and •OH, their reaction contributed at least 78.6% of 1O2 production. Overall, the proposed mechanistic insights into radical transformations of 1O2 generation offer effective strategies for non-radical oxidation of wastewater.
{"title":"Synergistic effect of hydroxyl and superoxide radicals-driven by highly dispersed FeCo-NC dual active sites in singlet oxygen generation in heterogeneous electro-Fenton systems","authors":"Xianpeng Li, Tong Zhu, Xianguo Ji, Hao Lin, Zhirong Sun","doi":"10.1016/j.cej.2026.173967","DOIUrl":"https://doi.org/10.1016/j.cej.2026.173967","url":null,"abstract":"Non-radical oxidation in heterogeneous electro-Fenton systems is crucial for removing organic contaminants in complex wastewater matrices. However, the generation mechanism of singlet oxygen (<ce:sup loc=\"pre\">1</ce:sup>O<ce:inf loc=\"post\">2</ce:inf>) remains unclear, especially the transformation among reactive oxygen species during generation. Herein, the <ce:sup loc=\"pre\">1</ce:sup>O<ce:inf loc=\"post\">2</ce:inf> generation mechanism driven by FeCo-NC dual active sites was elucidated through probe testing and electron paramagnetic resonance experiments involving selective quenchers. The main pathway for <ce:sup loc=\"pre\">1</ce:sup>O<ce:inf loc=\"post\">2</ce:inf> formation was identified as the reaction of superoxide radicals (O<ce:inf loc=\"post\">2</ce:inf><ce:sup loc=\"post\">•–</ce:sup>) with hydroxyl radicals (•OH), with a significant synergistic effect. The electron coupling between O<ce:inf loc=\"post\">2</ce:inf><ce:sup loc=\"post\">•–</ce:sup> and •OH facilitated electron transfer from O<ce:inf loc=\"post\">2</ce:inf><ce:sup loc=\"post\">•–</ce:sup> to •OH, accelerating the reaction kinetics. The density functional theory calculations indicated that O<ce:inf loc=\"post\">2</ce:inf><ce:sup loc=\"post\">•–</ce:sup> and •OH selectively adsorbed at the Co and Fe sites, enhancing their collisions. The charge redistribution between FeCo facilitated the coupling of O<ce:inf loc=\"post\">2</ce:inf><ce:sup loc=\"post\">•–</ce:sup> and •OH, significantly enhancing the production efficiency of <ce:sup loc=\"pre\">1</ce:sup>O<ce:inf loc=\"post\">2</ce:inf> in the system. Quantitative analysis revealed individual contributions of O<ce:inf loc=\"post\">2</ce:inf><ce:sup loc=\"post\">•–</ce:sup> and •OH accounting for only 4.7% and 2.0% of the overall <ce:sup loc=\"pre\">1</ce:sup>O<ce:inf loc=\"post\">2</ce:inf> yield, highlighting the inefficiency of single-radical for <ce:sup loc=\"pre\">1</ce:sup>O<ce:inf loc=\"post\">2</ce:inf> generation. Under the coexistence of O<ce:inf loc=\"post\">2</ce:inf><ce:sup loc=\"post\">•–</ce:sup> and •OH, their reaction contributed at least 78.6% of <ce:sup loc=\"pre\">1</ce:sup>O<ce:inf loc=\"post\">2</ce:inf> production. Overall, the proposed mechanistic insights into radical transformations of <ce:sup loc=\"pre\">1</ce:sup>O<ce:inf loc=\"post\">2</ce:inf> generation offer effective strategies for non-radical oxidation of wastewater.","PeriodicalId":270,"journal":{"name":"Chemical Engineering Journal","volume":"95 1","pages":""},"PeriodicalIF":15.1,"publicationDate":"2026-02-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146146757","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 : 2026-02-09DOI: 10.1016/j.cej.2026.173915
Rui Zhou, Hongjiang Li, Shenmin Li, Yingna Cui, Xinping Wang
To address the problem of the PtZn catalysts' degradation in propane dehydrogenation (PDH) process due to Zn loss, the ZnS-1 zeolites containing high amount of framework Zn(II) were applied as catalyst supports encapsulating Pt and the third metal in this work. The high amount of framework Zn(II) allowed introduction of third metal ions, La (III), Y (III), In (III) together with Pt(II) into the zeolite channels. It is found that Y could effectively modulate the property of Pt in the PtY@ZnS-1 catalyst as the successor of Zn forming alloy with Pt when Zn lost during the PDH reaction. With the help of Y, the 0.3PtY@7Zn(L) catalyst displayed rather high activity and better regeneration stability in 3045 h' long-term reaction being conducted at 550 °C.
为解决PtZn催化剂在丙烷脱氢(PDH)过程中因Zn损失而降解的问题,采用含有大量骨架Zn(II)的ZnS-1分子筛作为包封Pt和第三金属的催化剂载体。高含量的骨架Zn(II)允许引入第三种金属离子La (III), Y (III), In (III)和Pt(II)进入沸石通道。发现当PDH反应中Zn损失时,Y作为Pt形成Zn合金的继承者,可以有效地调节PtY@ZnS-1催化剂中Pt的性质。在Y的帮助下,0.3PtY@7Zn(L)催化剂在550 °C下进行3045 h的长时反应时表现出较高的活性和较好的再生稳定性。
{"title":"Design and preparation of PtY@ZnS-1 catalyst with applicable catalytic property for propane dehydrogenation","authors":"Rui Zhou, Hongjiang Li, Shenmin Li, Yingna Cui, Xinping Wang","doi":"10.1016/j.cej.2026.173915","DOIUrl":"https://doi.org/10.1016/j.cej.2026.173915","url":null,"abstract":"To address the problem of the Pt<ce:glyph name=\"sbnd\"></ce:glyph>Zn catalysts' degradation in propane dehydrogenation (PDH) process due to Zn loss, the ZnS-1 zeolites containing high amount of framework Zn(II) were applied as catalyst supports encapsulating Pt and the third metal in this work. The high amount of framework Zn(II) allowed introduction of third metal ions, La (III), Y (III), In (III) together with Pt(II) into the zeolite channels. It is found that Y could effectively modulate the property of Pt in the PtY@ZnS-1 catalyst as the successor of Zn forming alloy with Pt when Zn lost during the PDH reaction. With the help of Y, the 0.3PtY@7Zn(L) catalyst displayed rather high activity and better regeneration stability in 3045 h' long-term reaction being conducted at 550 °C.","PeriodicalId":270,"journal":{"name":"Chemical Engineering Journal","volume":"45 1","pages":""},"PeriodicalIF":15.1,"publicationDate":"2026-02-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146146782","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 : 2026-02-09DOI: 10.1016/j.cej.2026.173973
Yonghang Yu, Xiaocheng Bao, Cui Du, Kaiwei Chen, Dedong Ji, Chen Zhou, Shengyang Yang
Solar-driven interfacial evaporation has emerged as a highly promising route, leveraging abundant solar energy for efficient desalination. However, many existing solar evaporators still face challenges such as salt accumulation and, crucially, fail to reduce heavy metal concentrations to the ultra-low levels required by drinking water standards. To address this gap, we have developed a room-temperature fabricated graphene oxide/siloxane-PVA hydrogel (GO/SPH) evaporator wherein solar-driven evaporation works in synergy with integrated chelating amino groups to achieve the thorough removal of heavy metal ions concurrent with desalination. The optimized 3.0 wt% GO/SPH composite demonstrates a remarkable evaporation rate of 2.21 kg m−2 h−1 under 1 sun irradiation, a two-fold improvement over the pristine SPH. This exceptional dual-function performance is underpinned by its synergistic architecture. For solar evaporation, GO within the matrix acts as a highly efficient photothermal agent, achieving 91.4% conversion efficiency. Concurrently, for heavy metal remediation, amino ligands derived from the APTMS crosslinker enable the selective sequestration of Cu2+, Cr3+, Cd2+, and Pb2+ ions through specific coordination chemistry. Crucially, the entire evaporator is stabilized by a hydrolytically stable SiOSi network, which ensures robust multi-cycle performance by retaining over 95% of its initial efficiency and preserving its decontamination integrity over extended operation.
太阳能驱动的界面蒸发已经成为一种非常有前途的途径,利用丰富的太阳能进行有效的海水淡化。然而,许多现有的太阳能蒸发器仍然面临着诸如盐积累等挑战,而且至关重要的是,它们无法将重金属浓度降低到饮用水标准所要求的超低水平。为了解决这一问题,我们开发了一种室温制备氧化石墨烯/硅氧烷-聚乙烯醇水凝胶(GO/SPH)蒸发器,其中太阳能驱动的蒸发与集成螯合氨基协同工作,在脱盐的同时实现重金属离子的彻底去除。优化后的3.0 wt% GO/SPH复合材料在1次太阳照射下的蒸发速率为2.21 kg m−2 h−1,比原始SPH提高了两倍。这种特殊的双重功能性能是由其协同结构支撑的。对于太阳能蒸发,基质内的氧化石墨烯作为高效光热剂,转换效率达到91.4%。同时,对于重金属的修复,APTMS交联剂衍生的氨基配体通过特定的配位化学可以选择性地隔离Cu2+、Cr3+、Cd2+和Pb2+离子。至关重要的是,整个蒸发器由水解稳定的SiOSi网络稳定,通过保持95%以上的初始效率并在长时间运行中保持其去污完整性,确保了强大的多循环性能。
{"title":"Self-catalyzed engineering of chelating sites onto a GO/PVA photothermal membrane: A strategy for synergistic solar desalination and thorough heavy metal removal","authors":"Yonghang Yu, Xiaocheng Bao, Cui Du, Kaiwei Chen, Dedong Ji, Chen Zhou, Shengyang Yang","doi":"10.1016/j.cej.2026.173973","DOIUrl":"https://doi.org/10.1016/j.cej.2026.173973","url":null,"abstract":"Solar-driven interfacial evaporation has emerged as a highly promising route, leveraging abundant solar energy for efficient desalination. However, many existing solar evaporators still face challenges such as salt accumulation and, crucially, fail to reduce heavy metal concentrations to the ultra-low levels required by drinking water standards. To address this gap, we have developed a room-temperature fabricated graphene oxide/siloxane-PVA hydrogel (GO/SPH) evaporator wherein solar-driven evaporation works in synergy with integrated chelating amino groups to achieve the thorough removal of heavy metal ions concurrent with desalination. The optimized 3.0 wt% GO/SPH composite demonstrates a remarkable evaporation rate of 2.21 kg m<ce:sup loc=\"post\">−2</ce:sup> h<ce:sup loc=\"post\">−1</ce:sup> under 1 sun irradiation, a two-fold improvement over the pristine SPH. This exceptional dual-function performance is underpinned by its synergistic architecture. For solar evaporation, GO within the matrix acts as a highly efficient photothermal agent, achieving 91.4% conversion efficiency. Concurrently, for heavy metal remediation, amino ligands derived from the APTMS crosslinker enable the selective sequestration of Cu<ce:sup loc=\"post\">2+</ce:sup>, Cr<ce:sup loc=\"post\">3+</ce:sup>, Cd<ce:sup loc=\"post\">2+</ce:sup>, and Pb<ce:sup loc=\"post\">2+</ce:sup> ions through specific coordination chemistry. Crucially, the entire evaporator is stabilized by a hydrolytically stable Si<ce:glyph name=\"sbnd\"></ce:glyph>O<ce:glyph name=\"sbnd\"></ce:glyph>Si network, which ensures robust multi-cycle performance by retaining over 95% of its initial efficiency and preserving its decontamination integrity over extended operation.","PeriodicalId":270,"journal":{"name":"Chemical Engineering Journal","volume":"95 1","pages":""},"PeriodicalIF":15.1,"publicationDate":"2026-02-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146146786","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 : 2026-02-09DOI: 10.1016/j.cej.2026.173734
Ben Liu, Chong Chen, Wenqi Zhu, Yongjun Gu, Yiwen Hu, Hongbing Lei, Duo Li, Xuran Xu, Xiuduo Song, Fengqi Zhao, Wei Jiang, Gazi Hao
In the manufacturing of modified double-base (MDB) propellants, comprising nitrocellulose and nitroglycerin, calendered intermediate products are subjected to continuous thermal processing during manufacturing, where heat accumulation may trigger pyrolysis and potential ignition. Although numerous studies have investigated the thermal behavior of final MDB propellants, the safety of calendered intermediates remains insufficiently explored, especially under representative processing conditions. To address this gap, this study systematically investigates the pyrolysis pathways and ignition mechanisms of calendered MDB intermediates by integrating microscale thermogravimetric–differential scanning calorimetry–Fourier transform infrared–mass spectrometry (TG-DSC-FTIR-MS) with macroscale programmed hot–surface heating tests. Both analyses consistently revealed a three–stage behavior: thermal softening, melting and foaming, and rapid decomposition/burning, accompanied by the release of CO₂, NO₂, NO, CH₂O, HCN, and N₂O. Kinetic analysis showed that the average activation energy in stage I (52.0 kJ/mol) is 63.4% lower than that in stage II (142.1 kJ/mol), indicating a particular susceptibility to nitroglycerin–dominated initial decomposition—a primary fire hazard during production. Notably, the macroscale mass loss at 110 °C reached 7.1%, considerably exceeding the microscale value (3.6%) and underscoring the enhanced reactivity under bulk heating conditions. Ignition occurred at approximately 226 °C, followed by the peak concentrations of N₂O (65 ppm) and NO₂ (45 ppm). Statistical analysis further identified a combustion probability threshold between 220 °C and 230 °C, verifying that temperature and gas concentration are critical predictors of ignition. These findings highlight the elevated thermal risks associated with calendered propellant intermediates and provide a theoretical basis for design of safer manufacturing processes for MDB propellants.
{"title":"Micro–macroscale pyrolysis and ignition for exploring thermal safety behaviors of modified double-base propellants","authors":"Ben Liu, Chong Chen, Wenqi Zhu, Yongjun Gu, Yiwen Hu, Hongbing Lei, Duo Li, Xuran Xu, Xiuduo Song, Fengqi Zhao, Wei Jiang, Gazi Hao","doi":"10.1016/j.cej.2026.173734","DOIUrl":"https://doi.org/10.1016/j.cej.2026.173734","url":null,"abstract":"In the manufacturing of modified double-base (MDB) propellants, comprising nitrocellulose and nitroglycerin, calendered intermediate products are subjected to continuous thermal processing during manufacturing, where heat accumulation may trigger pyrolysis and potential ignition. Although numerous studies have investigated the thermal behavior of final MDB propellants, the safety of calendered intermediates remains insufficiently explored, especially under representative processing conditions. To address this gap, this study systematically investigates the pyrolysis pathways and ignition mechanisms of calendered MDB intermediates by integrating microscale thermogravimetric–differential scanning calorimetry–Fourier transform infrared–mass spectrometry (TG-DSC-FTIR-MS) with macroscale programmed hot–surface heating tests. Both analyses consistently revealed a three–stage behavior: thermal softening, melting and foaming, and rapid decomposition/burning, accompanied by the release of CO₂, NO₂, NO, CH₂O, HCN, and N₂O. Kinetic analysis showed that the average activation energy in stage I (52.0 kJ/mol) is 63.4% lower than that in stage II (142.1 kJ/mol), indicating a particular susceptibility to nitroglycerin–dominated initial decomposition—a primary fire hazard during production. Notably, the macroscale mass loss at 110 °C reached 7.1%, considerably exceeding the microscale value (3.6%) and underscoring the enhanced reactivity under bulk heating conditions. Ignition occurred at approximately 226 °C, followed by the peak concentrations of N₂O (65 ppm) and NO₂ (45 ppm). Statistical analysis further identified a combustion probability threshold between 220 °C and 230 °C, verifying that temperature and gas concentration are critical predictors of ignition. These findings highlight the elevated thermal risks associated with calendered propellant intermediates and provide a theoretical basis for design of safer manufacturing processes for MDB propellants.","PeriodicalId":270,"journal":{"name":"Chemical Engineering Journal","volume":"6 1","pages":""},"PeriodicalIF":15.1,"publicationDate":"2026-02-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146146810","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}
Halogenated pollutants (HPs) in water pose serious risks, yet conventional dehalogenation technologies often suffer from sluggish kinetics and rapid catalyst deactivation. Here, we unveil the synergistic effects of crystal-facet on dehalogenation kinetics and poison tolerance of Pd-based electrocatalytic membranes (EMs) for ultrafast and robust dehalogenation. Preferential exposure of the (111) facet drives the electrodeposited Pd layer to evolve from a loose to a dense porous architecture due to its lower surface energy. This topological transition reduces the average pore size by ~46% and enhances the volumetric density of active sites. Concurrently, it facilitates pollutant diffusion and improves atomic hydrogen (*H) utilization, compensating for the lower *H generation capacity of (111) facet. Furthermore, we identify phenol desorption, rather than halogen desorption, as the rate-determining step and reveal a linear correlation between the energy barrier and the d-band center of Pd facets. The (111) facet, possessing a d-band center 0.10 and 0.18 eV lower than those of the (200) and (220) facets, respectively, significantly facilitates phenol desorption and thereby promotes active site renewal. Benefiting from these synergistic effects, the (111)-dominated Pd layer delivers 5–8 times faster kinetics and higher durability than (200)-dominated counterparts, eliminating >99% of 4-chlorophenol within ~8 ms. Moreover, the (111)-dominated EM enables nearly complete and durable removal of trace 4-chlorophenol from real drinking water with a low energy consumption of 0.09 kWh/m3, outperforming conventional membrane separation and electrochemical technologies. Overall, this study offers novel mechanistic insights into the fundamental role of crystal-facet in dictating dehalogenation kinetics and poison tolerance of EMs, paving the way toward rational design of high-performance EMs for advanced water purification.
{"title":"Synergistic effects of crystal-facet on dehalogenation kinetics and poison tolerance of Pd-based electrocatalytic membranes for efficient removal of halogenated pollutants","authors":"Yinkun Sun, Dongwei Lu, Xianci Pan, Rongxin Zeng, Zhiyu Sun, Xueying Chen, Yumei Wang, Qingcan Zhou, Yichao Hu, Linlin Zang, Guanjin Liu, Jun Ma","doi":"10.1016/j.cej.2026.173966","DOIUrl":"https://doi.org/10.1016/j.cej.2026.173966","url":null,"abstract":"Halogenated pollutants (HPs) in water pose serious risks, yet conventional dehalogenation technologies often suffer from sluggish kinetics and rapid catalyst deactivation. Here, we unveil the synergistic effects of crystal-facet on dehalogenation kinetics and poison tolerance of Pd-based electrocatalytic membranes (EMs) for ultrafast and robust dehalogenation. Preferential exposure of the (111) facet drives the electrodeposited Pd layer to evolve from a loose to a dense porous architecture due to its lower surface energy. This topological transition reduces the average pore size by ~46% and enhances the volumetric density of active sites. Concurrently, it facilitates pollutant diffusion and improves atomic hydrogen (*H) utilization, compensating for the lower *H generation capacity of (111) facet. Furthermore, we identify phenol desorption, rather than halogen desorption, as the rate-determining step and reveal a linear correlation between the energy barrier and the d-band center of Pd facets. The (111) facet, possessing a d-band center 0.10 and 0.18 eV lower than those of the (200) and (220) facets, respectively, significantly facilitates phenol desorption and thereby promotes active site renewal. Benefiting from these synergistic effects, the (111)-dominated Pd layer delivers 5–8 times faster kinetics and higher durability than (200)-dominated counterparts, eliminating >99% of 4-chlorophenol within ~8 ms. Moreover, the (111)-dominated EM enables nearly complete and durable removal of trace 4-chlorophenol from real drinking water with a low energy consumption of 0.09 kWh/m<ce:sup loc=\"post\">3</ce:sup>, outperforming conventional membrane separation and electrochemical technologies. Overall, this study offers novel mechanistic insights into the fundamental role of crystal-facet in dictating dehalogenation kinetics and poison tolerance of EMs, paving the way toward rational design of high-performance EMs for advanced water purification.","PeriodicalId":270,"journal":{"name":"Chemical Engineering Journal","volume":"39 1","pages":""},"PeriodicalIF":15.1,"publicationDate":"2026-02-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146146740","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 : 2026-02-09DOI: 10.1016/j.cej.2026.173956
Yuwei Song, Songlin Nie, Hui Ji, Junzhou Meng, Sen Kong
High-performance ultraviolet (UV) photoreactors are essential for efficiently treating ballast water and preventing the spread of invasive species. This study presents a novel collision-atomization UV photoreactor that enhances radiation absorption by atomizing water into fine droplets that directly interact with UV lamps. A multiphase-flow simulation framework was developed using Computational Fluid Dynamics (CFD), coupling radiation fields, fluid dynamics, and microbial trajectories with an experimentally validated polynomial inactivation kinetics model for real-time simulation of internal processes. A comparative parametric analysis was carried out to examine the impacts of lamp arrangement, lamp orientation, and dead-zone treatment on the performance of the photoreactor. This analysis resulted in the determination of a representative baseline configuration. Subsequently, based on this reference configuration, an enhanced NSGA-II multi-objective optimization approach with improved search capabilities was employed to explore the trade-off between microbial inactivation efficiency and dose distribution uniformity and to acquire Pareto-optimal design solutions. Numerical results showed a 13.0% improvement in average microbial inactivation and an 11.3% reduction in dose distribution variation for a representative Pareto-optimal configuration compared to the baseline case. Yeast inactivation experiments confirmed a log reduction exceeding 2.5 (over 99.7% microbial removal) within 30 min, demonstrating consistently improved performance relative to the baseline configuration. The developed method offers a reliable tool for guiding the design and optimization of multiphase-flow UV photoreactor designs.
{"title":"Optimization of a novel collision-atomization UV photoreactor based on microbial particle tracking and multiphase flow coupled simulation","authors":"Yuwei Song, Songlin Nie, Hui Ji, Junzhou Meng, Sen Kong","doi":"10.1016/j.cej.2026.173956","DOIUrl":"https://doi.org/10.1016/j.cej.2026.173956","url":null,"abstract":"High-performance ultraviolet (UV) photoreactors are essential for efficiently treating ballast water and preventing the spread of invasive species. This study presents a novel collision-atomization UV photoreactor that enhances radiation absorption by atomizing water into fine droplets that directly interact with UV lamps. A multiphase-flow simulation framework was developed using Computational Fluid Dynamics (CFD), coupling radiation fields, fluid dynamics, and microbial trajectories with an experimentally validated polynomial inactivation kinetics model for real-time simulation of internal processes. A comparative parametric analysis was carried out to examine the impacts of lamp arrangement, lamp orientation, and dead-zone treatment on the performance of the photoreactor. This analysis resulted in the determination of a representative baseline configuration. Subsequently, based on this reference configuration, an enhanced NSGA-II multi-objective optimization approach with improved search capabilities was employed to explore the trade-off between microbial inactivation efficiency and dose distribution uniformity and to acquire Pareto-optimal design solutions. Numerical results showed a 13.0% improvement in average microbial inactivation and an 11.3% reduction in dose distribution variation for a representative Pareto-optimal configuration compared to the baseline case. Yeast inactivation experiments confirmed a log reduction exceeding 2.5 (over 99.7% microbial removal) within 30 min, demonstrating consistently improved performance relative to the baseline configuration. The developed method offers a reliable tool for guiding the design and optimization of multiphase-flow UV photoreactor designs.","PeriodicalId":270,"journal":{"name":"Chemical Engineering Journal","volume":"7 1","pages":""},"PeriodicalIF":15.1,"publicationDate":"2026-02-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146146760","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 : 2026-02-09DOI: 10.1016/j.cej.2026.173982
Ze Li, Tianfeng Ma, Zhen Feng, Haiyan Wang, Shuling Liu, Yanyan Liu, Hucheng Zhang, Jianji Wang, Baojun Li
The development of efficient bifunctional catalysts for oxygen reduction and evolution reactions (ORR/OER) is crucial for advancing rechargeable zinc-air batteries (ZABs). Herein, we report a three-dimensional N-doped CoFe alloy embedded in hierarchical carbon (CoxFeN@3D-GC) as a high-performance catalyst. This unique architecture, synthesized via a one-pot pyrolysis process, integrates in-situ grown carbon nanotubes grafted onto reduced graphene oxide sheets, with CoFe nanoparticles uniformly dispersed within the matrix. The CoxFeN@3D-GC catalyst exhibits outstanding bifunctional activity, achieving a half-wave potential of 0.935 V for ORR and an overpotential of only 298 mV at 10 mA cm−2 for OER, rivaling the performance of noble-metal benchmarks (Pt/C and RuO2). When deployed in a practical ZAB, it delivers a peak power density of 246 mW cm−2, a specific capacity of 815 mAh g−1, and remarkable stability over 800 cycles. Combined experimental and theoretical analyses reveal that the superior performance originates from the synergistic interplay among the bimetallic CoFe heterostructure, the hierarchical conductive network, and the N-doped carbon matrix, which collectively optimize charge transfer, mass transport, and reaction kinetics.
开发高效的氧还原演化双功能催化剂(ORR/OER)是推进可充电锌空气电池(ZABs)发展的关键。在此,我们报道了一种三维n掺杂CoFe合金嵌入分层碳(CoxFeN@3D-GC)作为高性能催化剂。这种独特的结构通过一锅热解工艺合成,将原位生长的碳纳米管接枝到还原的氧化石墨烯片上,并将CoFe纳米颗粒均匀地分散在基体中。CoxFeN@3D-GC催化剂表现出出色的双功能活性,ORR的半波电位为0.935 V, OER在10 mA cm−2时的过电位仅为298 mV,与贵金属基准(Pt/C和RuO2)的性能相匹敌。当在实际ZAB中部署时,它提供246 mW cm−2的峰值功率密度,815 mAh g−1的比容量,以及超过800 周期的显着稳定性。实验与理论相结合的分析表明,这种优异的性能源于双金属CoFe异质结构、分层导电网络和n掺杂碳基体之间的协同作用,共同优化了电荷传递、质量输运和反应动力学。
{"title":"N-doped CoFe alloy coupled to hierarchical carbon as 3D catalysts for synergistic reversible oxygen electrocatalysis in Zn-air batteries","authors":"Ze Li, Tianfeng Ma, Zhen Feng, Haiyan Wang, Shuling Liu, Yanyan Liu, Hucheng Zhang, Jianji Wang, Baojun Li","doi":"10.1016/j.cej.2026.173982","DOIUrl":"https://doi.org/10.1016/j.cej.2026.173982","url":null,"abstract":"The development of efficient bifunctional catalysts for oxygen reduction and evolution reactions (ORR/OER) is crucial for advancing rechargeable zinc-air batteries (ZABs). Herein, we report a three-dimensional N-doped CoFe alloy embedded in hierarchical carbon (Co<ce:inf loc=\"post\">x</ce:inf>FeN@3D-GC) as a high-performance catalyst. This unique architecture, synthesized via a one-pot pyrolysis process, integrates in-situ grown carbon nanotubes grafted onto reduced graphene oxide sheets, with CoFe nanoparticles uniformly dispersed within the matrix. The Co<ce:inf loc=\"post\">x</ce:inf>FeN@3D-GC catalyst exhibits outstanding bifunctional activity, achieving a half-wave potential of 0.935 V for ORR and an overpotential of only 298 mV at 10 mA cm<ce:sup loc=\"post\">−2</ce:sup> for OER, rivaling the performance of noble-metal benchmarks (Pt/C and RuO<ce:inf loc=\"post\">2</ce:inf>). When deployed in a practical ZAB, it delivers a peak power density of 246 mW cm<ce:sup loc=\"post\">−2</ce:sup>, a specific capacity of 815 mAh g<ce:sup loc=\"post\">−1</ce:sup>, and remarkable stability over 800 cycles. Combined experimental and theoretical analyses reveal that the superior performance originates from the synergistic interplay among the bimetallic CoFe heterostructure, the hierarchical conductive network, and the N-doped carbon matrix, which collectively optimize charge transfer, mass transport, and reaction kinetics.","PeriodicalId":270,"journal":{"name":"Chemical Engineering Journal","volume":"31 1","pages":""},"PeriodicalIF":15.1,"publicationDate":"2026-02-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146146784","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}
Dual-atom catalysts (DACs) have emerged at the forefront of heterogeneous catalysis research due to their unique properties, effectively bridging the material gap between single-atom catalysts (SACs) and nanoclusters. Among their critical design parameters, precise manipulation of dual-atom spatial distribution significantly influences electronic structure, coordination environment, and catalytic behavior. This paper systematically reviews recent advancements in modulation strategies for fixed dual atom sites, focusing on precise synthesis methods, characterization techniques, and synergistic catalytic mechanisms at sub-level scales. It decodes the multi-dimensional impacts of site configuration on active site stability, reaction pathway selectivity, and underlying mechanisms while emphasizing the design principles behind structure-performance relationships as well as cascading pathways and modulation rules. By integrating experimental breakthroughs with theoretical modeling, this review aims to establish a comprehensive framework for rationally designing DACs and provides a roadmap for future innovations in precision catalysis.
{"title":"Decoding synergy: from the precise construction of dual-atom catalysts to synergistic engineering","authors":"Yaning Fu, Linping Shi, Dongxue Liu, Yipeng Liu, Tong Liu, Yunyin Niu, Youcai Lu, Qingchao Liu","doi":"10.1016/j.cej.2026.173784","DOIUrl":"https://doi.org/10.1016/j.cej.2026.173784","url":null,"abstract":"Dual-atom catalysts (DACs) have emerged at the forefront of heterogeneous catalysis research due to their unique properties, effectively bridging the material gap between single-atom catalysts (SACs) and nanoclusters. Among their critical design parameters, precise manipulation of dual-atom spatial distribution significantly influences electronic structure, coordination environment, and catalytic behavior. This paper systematically reviews recent advancements in modulation strategies for fixed dual atom sites, focusing on precise synthesis methods, characterization techniques, and synergistic catalytic mechanisms at sub-level scales. It decodes the multi-dimensional impacts of site configuration on active site stability, reaction pathway selectivity, and underlying mechanisms while emphasizing the design principles behind structure-performance relationships as well as cascading pathways and modulation rules. By integrating experimental breakthroughs with theoretical modeling, this review aims to establish a comprehensive framework for rationally designing DACs and provides a roadmap for future innovations in precision catalysis.","PeriodicalId":270,"journal":{"name":"Chemical Engineering Journal","volume":"92 1","pages":""},"PeriodicalIF":15.1,"publicationDate":"2026-02-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146146807","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 : 2026-02-09DOI: 10.1016/j.cej.2026.173958
Meng Gao, Hongjun Jing, Jun Dai, Shaojie Chen, Zhang Chaowei, Shan Junwei, Zhang Hengfei, Cui Yuanquan, Shixuan Lei
As demand for sustainable building materials continues to rise, coal gangue aggregate (CGA) has emerged as a promising alternative due to its high value potential. This study aims to enhance the physical and mechanical properties of CGA through solution impregnation modification. The effects of different modification treatments on CGA were systematically investigated using macroscopic performance tests in conjunction with microstructural characterization. The results indicate that among the six modification methods, M4 and M6 modified CGA exhibited superior macroscopic performance. The water absorption of M4 decreased by 43.99%, and its contact angle reached 135°. The crushing value and porosity of M6 decreased by 12.31% and 47.22%, respectively. Mercury intrusion porosimetry results revealed that the pore structure of CGA before and after modification exhibited prominent fractal characteristics, with D1 ranging from 2.214 to 2.361 and D2 ranging from 2.755 to 2.976. Microstructural analyses demonstrated that sodium silicate, nano-silica, and silane enhanced the physical and mechanical properties of CGA through physical penetration and chemical reactions. Overall, M6 has greater advantages in terms of macroscopic performance and economic cost, and shows considerable application potential in the reuse of solid waste. The findings of this study provide new insights and technical approaches for improving the performance of CGA.
{"title":"Performance enhancement evaluation of coal gangue aggregates based on chemical solution modification: mechanical properties and microstructural characteristics","authors":"Meng Gao, Hongjun Jing, Jun Dai, Shaojie Chen, Zhang Chaowei, Shan Junwei, Zhang Hengfei, Cui Yuanquan, Shixuan Lei","doi":"10.1016/j.cej.2026.173958","DOIUrl":"https://doi.org/10.1016/j.cej.2026.173958","url":null,"abstract":"As demand for sustainable building materials continues to rise, coal gangue aggregate (CGA) has emerged as a promising alternative due to its high value potential. This study aims to enhance the physical and mechanical properties of CGA through solution impregnation modification. The effects of different modification treatments on CGA were systematically investigated using macroscopic performance tests in conjunction with microstructural characterization. The results indicate that among the six modification methods, M4 and M6 modified CGA exhibited superior macroscopic performance. The water absorption of M4 decreased by 43.99%, and its contact angle reached 135°. The crushing value and porosity of M6 decreased by 12.31% and 47.22%, respectively. Mercury intrusion porosimetry results revealed that the pore structure of CGA before and after modification exhibited prominent fractal characteristics, with <em>D</em><sub>1</sub> ranging from 2.214 to 2.361 and <em>D</em><sub>2</sub> ranging from 2.755 to 2.976. Microstructural analyses demonstrated that sodium silicate, nano-silica, and silane enhanced the physical and mechanical properties of CGA through physical penetration and chemical reactions. Overall, M6 has greater advantages in terms of macroscopic performance and economic cost, and shows considerable application potential in the reuse of solid waste. The findings of this study provide new insights and technical approaches for improving the performance of CGA.","PeriodicalId":270,"journal":{"name":"Chemical Engineering Journal","volume":"27 1","pages":""},"PeriodicalIF":15.1,"publicationDate":"2026-02-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146145945","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}