Single-atom catalysts are emerging as promising separator modifiers to alleviate polysulfides shuttle effect and facilitate redox kinetics in lithium‑sulfur (LiS) batteries. However, single metal atom sites fail to efficiently promote complete conversion of sulfur species in the case of high sulfur content and high sulfur loading due to multi-electron and multi-phase transformation processes involved. Herein, the atomically dispersed bimetal electrocatalysts (Fe/Ni-N4-NC) derived from multivariate metalloporphyrin-based covalent organic frameworks have been proposed for polypropylene (PP) separator modification. It has been uncovered that Fe active sites are more effective in facilitating solid-liquid catalytic conversion from sulfur to long-chain polysulfides, while Ni active sites exhibit higher catalytic activity in driving subsequent liquid-solid conversion to Li2S. The dual-regulation strategy leveraged by the separated heterometallic atom sites orchestrates consecutive conversion of sulfur species, thus significantly expediting the redox kinetics and inhibiting polysulfides shuttling. Under a high sulfur loading of 5.7 mg cm−2, the resultant cell delivers high specific capacity of 1146 mA h g−1, areal capacity of 6.53 mA h cm−2 and volumetric capacity of 1088 mA h cm−3 at 0.1C. This work provides new insights and inspirations for the development of high-energy-density and long-lifetime LiS batteries.
单原子催化剂是一种很有前途的分离器改性剂，可以缓解多硫化物的穿梭效应，促进锂硫电池的氧化还原动力学。然而，在高硫含量和高硫负荷的情况下，由于涉及多电子和多相转化过程，单金属原子位点不能有效地促进硫种的完全转化。本文提出了基于多元金属卟啉共价有机骨架的原子分散双金属电催化剂（Fe/Ni-N4-NC）用于聚丙烯（PP）分离器改性。研究发现，Fe活性位点更有效地促进了从硫到长链多硫化物的固液催化转化，而Ni活性位点在随后的液固转化为Li2S方面表现出更高的催化活性。分离的异金属原子位点利用双重调控策略协调了硫的连续转化，从而显著加快了氧化还原动力学并抑制了多硫化物的穿梭。高硫载荷作用下的5.7 mg 厘米−2,1146年合成细胞提供了较高的比容量 马 h g−1,区域容量6.53马 h 厘米−2和体积容量1088马 h 厘米−3 0.1 c。这项工作为高能量密度和长寿命锂离子电池的发展提供了新的见解和启示。
{"title":"Dual-regulation of sulfur species enabled by atomically dispersed bimetal electrocatalysts to upgrade energy density and longevity of lithium‑sulfur batteries","authors":"Xiaofei Xie, Pengyue Li, Zhibin Cheng, Bowen Chang, Jiayu Huang, Xiaoju Li, Ruihu Wang","doi":"10.1016/j.cej.2026.174005","DOIUrl":"https://doi.org/10.1016/j.cej.2026.174005","url":null,"abstract":"Single-atom catalysts are emerging as promising separator modifiers to alleviate polysulfides shuttle effect and facilitate redox kinetics in lithium‑sulfur (Li<ce:glyph name=\"sbnd\"></ce:glyph>S) batteries. However, single metal atom sites fail to efficiently promote complete conversion of sulfur species in the case of high sulfur content and high sulfur loading due to multi-electron and multi-phase transformation processes involved. Herein, the atomically dispersed bimetal electrocatalysts (Fe/Ni-N<ce:inf loc=\"post\">4</ce:inf>-NC) derived from multivariate metalloporphyrin-based covalent organic frameworks have been proposed for polypropylene (PP) separator modification. It has been uncovered that Fe active sites are more effective in facilitating solid-liquid catalytic conversion from sulfur to long-chain polysulfides, while Ni active sites exhibit higher catalytic activity in driving subsequent liquid-solid conversion to Li<ce:inf loc=\"post\">2</ce:inf>S. The dual-regulation strategy leveraged by the separated heterometallic atom sites orchestrates consecutive conversion of sulfur species, thus significantly expediting the redox kinetics and inhibiting polysulfides shuttling. Under a high sulfur loading of 5.7 mg cm<ce:sup loc=\"post\">−2</ce:sup>, the resultant cell delivers high specific capacity of 1146 mA h g<ce:sup loc=\"post\">−1</ce:sup>, areal capacity of 6.53 mA h cm<ce:sup loc=\"post\">−2</ce:sup> and volumetric capacity of 1088 mA h cm<ce:sup loc=\"post\">−3</ce:sup> at 0.1C. This work provides new insights and inspirations for the development of high-energy-density and long-lifetime Li<ce:glyph name=\"sbnd\"></ce:glyph>S batteries.","PeriodicalId":270,"journal":{"name":"Chemical Engineering Journal","volume":"35 1","pages":""},"PeriodicalIF":15.1,"publicationDate":"2026-02-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146153070","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 : 2026-02-10DOI: 10.1016/j.cej.2026.174017
Naying Li, Bo Zhong, Xin Liu, Wei-Min Wu, Xintong Mei, Ruixi Liu, Li Zhou, Honghui Lin, Shaoliang Yi, Yixin He
Freeze-thaw cycling (FTC), a predominant climatic driver in alpine environments, remains an unaddressed knowledge gap regarding its impact on microplastic (MP) aging and associated microbial carbon metabolism. Here, we used controlled laboratory incubations coupled with multi-scale molecular and functional analyses to investigate MP-mediated carbon cycling under simulated FTC conditions. FTC exposure significantly modified the surface characteristics of MPs, particularly polyethylene terephthalate (PET), by inducing surface oxidation, increased roughness, and microcrack formation. These physicochemical transformations created reactive micro-environments that favored microbial colonization and metabolic potential. Under the combined stress of FTC and MPs, the abundance of sedimentary carbon-cycling genes declined by 30.39 to 31.27%. Conversely, the PET plastisphere exhibited a substantial enrichment of carbon-cycling genes (up to 3.93 × 105), effectively establishing a localized carbon cycling habitat. A dominant functional module comprising fixation, composition, and oxidation pathways accounted for 88.9% of carbon-cycling genes within the PET plastisphere, with Brevundimonas and Comamonas emerging as the key functional taxa in here. These findings demonstrate that intensified FTC can transform inert PET MPs into metabolically active microscale cycling habitats with the potential to influence local carbon-cycling processes, and highlight the need for future in situ investigations to evaluate the environmental relevance of these effects.
{"title":"Freeze–thaw cycles restructure PET microplastics in sediments into new habitat of microbial carbon metabolism","authors":"Naying Li, Bo Zhong, Xin Liu, Wei-Min Wu, Xintong Mei, Ruixi Liu, Li Zhou, Honghui Lin, Shaoliang Yi, Yixin He","doi":"10.1016/j.cej.2026.174017","DOIUrl":"https://doi.org/10.1016/j.cej.2026.174017","url":null,"abstract":"Freeze-thaw cycling (FTC), a predominant climatic driver in alpine environments, remains an unaddressed knowledge gap regarding its impact on microplastic (MP) aging and associated microbial carbon metabolism. Here, we used controlled laboratory incubations coupled with multi-scale molecular and functional analyses to investigate MP-mediated carbon cycling under simulated FTC conditions. FTC exposure significantly modified the surface characteristics of MPs, particularly polyethylene terephthalate (PET), by inducing surface oxidation, increased roughness, and microcrack formation. These physicochemical transformations created reactive micro-environments that favored microbial colonization and metabolic potential. Under the combined stress of FTC and MPs, the abundance of sedimentary carbon-cycling genes declined by 30.39 to 31.27%. Conversely, the PET plastisphere exhibited a substantial enrichment of carbon-cycling genes (up to 3.93 × 10<ce:sup loc=\"post\">5</ce:sup>), effectively establishing a localized carbon cycling habitat. A dominant functional module comprising fixation, composition, and oxidation pathways accounted for 88.9% of carbon-cycling genes within the PET plastisphere, with <ce:italic>Brevundimonas</ce:italic> and <ce:italic>Comamonas</ce:italic> emerging as the key functional taxa in here. These findings demonstrate that intensified FTC can transform inert PET MPs into metabolically active microscale cycling habitats with the potential to influence local carbon-cycling processes, and highlight the need for future in situ investigations to evaluate the environmental relevance of these effects.","PeriodicalId":270,"journal":{"name":"Chemical Engineering Journal","volume":"99 1","pages":""},"PeriodicalIF":15.1,"publicationDate":"2026-02-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146153179","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 : 2026-02-10DOI: 10.1016/j.cej.2026.173968
Yi Zheng, Chuang Liu, Qihe Ma, Shuwen Li, Zhengping Dong
The semi‑hydrogenation of alkynes plays a vital role in the petrochemical and fine chemical industries, however, achieving a balance between high activity and selectivity remains a significant challenge. In this study, mesoporous nitrogen-doped carbon spheres (NCS) enriched with pyridinic-N sites were synthesized through the in-situ pyrolysis of 3-aminophenol-based phenolic resin, enabling the immobilization of ultrafine PdCu nanoclusters. Experimental and theoretical results demonstrate that the alloyed Cu and pyridinic-N sites synergistically modulate the electronic structure and local microenvironment of Pd atoms in the PdCu nanoclusters. This coordination results in the weakest adsorption energy (−1.05 eV) for product alkenes and a d-band center of −1.48 eV, facilitating alkene desorption. Consequently, the optimized Pd1Cu1.5/NCS600 catalyst achieves 99.9% conversion and 98.1% selectivity for phenylacetylene semi‑hydrogenation, with performance nearly unaffected by free styrene. The catalyst also exhibits long-term stability, a high turnover frequency (483.4 h−1), broad applicability, and gram-scale semi‑hydrogenation with high selectivity and stability under mild conditions (30 °C, 1 atm H2). This work highlights that tailoring the chemical microenvironment of Pd active sites offers an effective strategy to simultaneously enhance catalytic activity and selectivity, offering promising potential for industrial applications in semi‑hydrogenation processes.
{"title":"In-situ pyrolysis-generated pyridinic nitrogen-regulated PdCu clusters for catalytic semi‑hydrogenation of alkynes: Unaffected by free alkenes","authors":"Yi Zheng, Chuang Liu, Qihe Ma, Shuwen Li, Zhengping Dong","doi":"10.1016/j.cej.2026.173968","DOIUrl":"https://doi.org/10.1016/j.cej.2026.173968","url":null,"abstract":"The semi‑hydrogenation of alkynes plays a vital role in the petrochemical and fine chemical industries, however, achieving a balance between high activity and selectivity remains a significant challenge. In this study, mesoporous nitrogen-doped carbon spheres (NCS) enriched with pyridinic-N sites were synthesized through the in-situ pyrolysis of 3-aminophenol-based phenolic resin, enabling the immobilization of ultrafine PdCu nanoclusters. Experimental and theoretical results demonstrate that the alloyed Cu and pyridinic-N sites synergistically modulate the electronic structure and local microenvironment of Pd atoms in the PdCu nanoclusters. This coordination results in the weakest adsorption energy (−1.05 eV) for product alkenes and a d-band center of −1.48 eV, facilitating alkene desorption. Consequently, the optimized Pd<ce:inf loc=\"post\">1</ce:inf>Cu<ce:inf loc=\"post\">1.5</ce:inf>/NCS<ce:inf loc=\"post\">600</ce:inf> catalyst achieves 99.9% conversion and 98.1% selectivity for phenylacetylene semi‑hydrogenation, with performance nearly unaffected by free styrene. The catalyst also exhibits long-term stability, a high turnover frequency (483.4 h<ce:sup loc=\"post\">−1</ce:sup>), broad applicability, and gram-scale semi‑hydrogenation with high selectivity and stability under mild conditions (30 °C, 1 atm H<ce:inf loc=\"post\">2</ce:inf>). This work highlights that tailoring the chemical microenvironment of Pd active sites offers an effective strategy to simultaneously enhance catalytic activity and selectivity, offering promising potential for industrial applications in semi‑hydrogenation processes.","PeriodicalId":270,"journal":{"name":"Chemical Engineering Journal","volume":"51 1","pages":""},"PeriodicalIF":15.1,"publicationDate":"2026-02-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146153344","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 : 2026-02-10DOI: 10.1016/j.cej.2026.174021
Chunlin Luo, Shuai Liu, Md Emdadul Haque, Brandon Robinson, Tao Wu, Debangsu Bhattacharyya, Jianli Hu, Yuxin Wang
Polyolefin waste and CO2 are among the most pressing sustainability issues. Microwave catalysis offers a promising platform for co-converting polyolefin waste and CO2 into light olefins and syngas. Here, a 40 wt% CeO2/α-Fe2O3 catalyst enables a balanced coupling of polyolefin cracking and CO2 reforming at 400 °C under microwave irradiation, achieving 36.5 mol% CO2 conversion, ~70 wt% gas yield, and 57.7 mol% light olefin selectivity. This performance arises from microwave-stimulated oxygen dynamics, wherein CeO2 activates CO2 and mitigates carbon deposition via lattice oxygen cycling, while α-Fe2O3 promotes selective hydrocarbon cracking and serves as a microwave susceptor. Mechanistic studies and DFT calculations confirm that microwave fields enhance lattice oxygen mobility, direct product selectivity, and sustain catalyst stability. Techno-economic analysis yields a net present value of +36.74 MM USD, and life-cycle assessment reveals a GHG footprint of 0.0667 kg CO2-eq/kg product-substantially lower than conventional steam cracking routes.
聚烯烃废料和二氧化碳是最紧迫的可持续性问题之一。微波催化为聚烯烃废物和二氧化碳共转化为轻质烯烃和合成气提供了一个有前途的平台。在此，40 wt%的CeO2/α-Fe2O3催化剂在400 °C微波照射下实现了聚烯烃裂解和CO2重整的平衡耦合，实现了36.5% mol%的CO2转化率、~70 wt%的气产率和57.7 mol%的轻烯烃选择性。这种性能源于微波激发的氧动力学，其中CeO2激活CO2并通过晶格氧循环减轻碳沉积，而α-Fe2O3促进选择性烃裂解并充当微波敏感器。机理研究和DFT计算证实，微波场增强了晶格氧迁移率、直接产物选择性和维持催化剂稳定性。技术经济分析得出净现值为+36.74 MM USD，生命周期评估显示温室气体足迹为0.0667 kg co2当量/kg产品，大大低于传统的蒸汽裂解路线。
{"title":"Balancing polyolefins waste and CO2 upcycling via microwave-stimulated oxygen dynamics","authors":"Chunlin Luo, Shuai Liu, Md Emdadul Haque, Brandon Robinson, Tao Wu, Debangsu Bhattacharyya, Jianli Hu, Yuxin Wang","doi":"10.1016/j.cej.2026.174021","DOIUrl":"https://doi.org/10.1016/j.cej.2026.174021","url":null,"abstract":"Polyolefin waste and CO<ce:inf loc=\"post\">2</ce:inf> are among the most pressing sustainability issues. Microwave catalysis offers a promising platform for <ce:italic>co</ce:italic>-converting polyolefin waste and CO<ce:inf loc=\"post\">2</ce:inf> into light olefins and syngas. Here, a 40 wt% CeO<ce:inf loc=\"post\">2</ce:inf>/α-Fe<ce:inf loc=\"post\">2</ce:inf>O<ce:inf loc=\"post\">3</ce:inf> catalyst enables a balanced coupling of polyolefin cracking and CO<ce:inf loc=\"post\">2</ce:inf> reforming at 400 °C under microwave irradiation, achieving 36.5 mol% CO<ce:inf loc=\"post\">2</ce:inf> conversion, ~70 wt% gas yield, and 57.7 mol% light olefin selectivity. This performance arises from microwave-stimulated oxygen dynamics, wherein CeO<ce:inf loc=\"post\">2</ce:inf> activates CO<ce:inf loc=\"post\">2</ce:inf> and mitigates carbon deposition via lattice oxygen cycling, while α-Fe<ce:inf loc=\"post\">2</ce:inf>O<ce:inf loc=\"post\">3</ce:inf> promotes selective hydrocarbon cracking and serves as a microwave susceptor. Mechanistic studies and DFT calculations confirm that microwave fields enhance lattice oxygen mobility, direct product selectivity, and sustain catalyst stability. Techno-economic analysis yields a net present value of +36.74 MM USD, and life-cycle assessment reveals a GHG footprint of 0.0667 kg CO<ce:inf loc=\"post\">2</ce:inf>-eq/kg product-substantially lower than conventional steam cracking routes.","PeriodicalId":270,"journal":{"name":"Chemical Engineering Journal","volume":"30 1","pages":""},"PeriodicalIF":15.1,"publicationDate":"2026-02-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146153348","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.2026.173938
Sinan Ateş, Ayşe Elif Ateş
Hybrid treatment systems that simultaneously enable industrial wastewater purification and on-site energy recovery have gained increasing attention as sustainable solutions for complex industrial effluents. This study reports the development and application of a reagent-free, solar-driven electro-Fenton-like membrane (SDEFM) system for the simultaneous detoxification of real pharmaceutical industry wastewater and green hydrogen recovery. Unlike studies relying on synthetic matrices, the system was evaluated using real industrial effluent, enabling a realistic assessment of treatment performance under complex wastewater conditions. The membrane-assisted configuration integrates a sacrificial iron anode and a graphite cathode operated under solar-powered UV-C irradiation (not direct solar photolysis), allowing in situ generation of reactive oxygen species (ROS) without external chemical addition. Under optimized conditions, the SDEFM system achieved up to 88% chemical oxygen demand (COD) removal, near-complete color elimination, substantial UV254 reduction, and acute toxicity abatement, as confirmed by Daphnia magna bioassays. Hydrogen production efficiencies of 40-60% relative to theoretical yields were achieved. When evaluated on a total energy basis, the process exhibited energy efficiencies of up to ~8% and exergy efficiencies approaching ~1%, confirming the feasibility of integrating wastewater treatment with renewable energy recovery. Chamber-resolved analysis revealed that deep oxidation was dominated by the anodic compartment through interfacial oxidation, while the cathodic compartment provided complementary bulk electro-Fenton activity. The results demonstrate that the SDEFM system provides a robust and scalable platform for integrated pharmaceutical wastewater detoxification and hydrogen co-production. By combining reagent-free operation, solar-powered enhancement, kinetic validation, and risk-based evaluation, this study advances circular and sustainable electrochemical treatment technologies for industrial wastewater applications.
{"title":"From decarbonization to wastewater detoxification: A solar-driven electro-Fenton like membrane system for real pharmaceutical industry wastewater","authors":"Sinan Ateş, Ayşe Elif Ateş","doi":"10.1016/j.cej.2026.173938","DOIUrl":"https://doi.org/10.1016/j.cej.2026.173938","url":null,"abstract":"Hybrid treatment systems that simultaneously enable industrial wastewater purification and on-site energy recovery have gained increasing attention as sustainable solutions for complex industrial effluents. This study reports the development and application of a reagent-free, solar-driven electro-Fenton-like membrane (SDEFM) system for the simultaneous detoxification of real pharmaceutical industry wastewater and green hydrogen recovery. Unlike studies relying on synthetic matrices, the system was evaluated using real industrial effluent, enabling a realistic assessment of treatment performance under complex wastewater conditions. The membrane-assisted configuration integrates a sacrificial iron anode and a graphite cathode operated under solar-powered UV-C irradiation (not direct solar photolysis), allowing in situ generation of reactive oxygen species (ROS) without external chemical addition. Under optimized conditions, the SDEFM system achieved up to 88% chemical oxygen demand (COD) removal, near-complete color elimination, substantial UV<ce:inf loc=\"post\">254</ce:inf> reduction, and acute toxicity abatement, as confirmed by <ce:italic>Daphnia magna</ce:italic> bioassays. Hydrogen production efficiencies of 40-60% relative to theoretical yields were achieved. When evaluated on a total energy basis, the process exhibited energy efficiencies of up to ~8% and exergy efficiencies approaching ~1%, confirming the feasibility of integrating wastewater treatment with renewable energy recovery. Chamber-resolved analysis revealed that deep oxidation was dominated by the anodic compartment through interfacial oxidation, while the cathodic compartment provided complementary bulk electro-Fenton activity. The results demonstrate that the SDEFM system provides a robust and scalable platform for integrated pharmaceutical wastewater detoxification and hydrogen co-production. By combining reagent-free operation, solar-powered enhancement, kinetic validation, and risk-based evaluation, this study advances circular and sustainable electrochemical treatment technologies for industrial wastewater applications.","PeriodicalId":270,"journal":{"name":"Chemical Engineering Journal","volume":"34 1","pages":""},"PeriodicalIF":15.1,"publicationDate":"2026-02-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146146764","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.2026.173929
Yunpeng Zhou, Shibo An, Yongzhihan He, Huilin Wei, Jun Yang, Minjie Shi, Lintong Hu, Edison Huixiang Ang
Aqueous rechargeable batteries, notable for their inherent safety, low cost, and environmental friendliness, hold great promise for large-scale energy storage. Their widespread application, however, has been limited by the instability of anode materials, which often leads to short cycle life and poor tolerance to both acidic and alkaline conditions. Herein, we report a phenothiazine-based poly(thionine-cyclohexanedione) (PTC) as a robust anode compatible with both acidic and alkaline aqueous batteries. The high molecular weight of PTC suppresses solubility, while the incorporation of rigid phenyl units imparts exceptional mechanical strength. Furthermore, polymerization enhances π-conjugation, promoting efficient electron transport. PTC delivers high capacity and excellent cycling stability in both H2SO4 and KOH electrolytes, attributed to its highly reversible redox behavior, structural robustness, and resistance to dissolution. Full cells constructed with PTC anodes paired with MnO2 and Ni(OH)2 cathodes for acidic and alkaline systems, respectively, exhibit high energy densities and prolonged cycling lifetimes. This work provides a new strategy for designing polymer-based electrode materials capable of stable operation in both acidic and alkaline aqueous batteries.
{"title":"Phenothiazine-based polymer anode enabling long-cycle aqueous rechargeable batteries under acidic and alkaline conditions","authors":"Yunpeng Zhou, Shibo An, Yongzhihan He, Huilin Wei, Jun Yang, Minjie Shi, Lintong Hu, Edison Huixiang Ang","doi":"10.1016/j.cej.2026.173929","DOIUrl":"https://doi.org/10.1016/j.cej.2026.173929","url":null,"abstract":"Aqueous rechargeable batteries, notable for their inherent safety, low cost, and environmental friendliness, hold great promise for large-scale energy storage. Their widespread application, however, has been limited by the instability of anode materials, which often leads to short cycle life and poor tolerance to both acidic and alkaline conditions. Herein, we report a phenothiazine-based poly(thionine-cyclohexanedione) (PTC) as a robust anode compatible with both acidic and alkaline aqueous batteries. The high molecular weight of PTC suppresses solubility, while the incorporation of rigid phenyl units imparts exceptional mechanical strength. Furthermore, polymerization enhances π-conjugation, promoting efficient electron transport. PTC delivers high capacity and excellent cycling stability in both H<ce:inf loc=\"post\">2</ce:inf>SO<ce:inf loc=\"post\">4</ce:inf> and KOH electrolytes, attributed to its highly reversible redox behavior, structural robustness, and resistance to dissolution. Full cells constructed with PTC anodes paired with MnO<ce:inf loc=\"post\">2</ce:inf> and Ni(OH)<ce:inf loc=\"post\">2</ce:inf> cathodes for acidic and alkaline systems, respectively, exhibit high energy densities and prolonged cycling lifetimes. This work provides a new strategy for designing polymer-based electrode materials capable of stable operation in both acidic and alkaline aqueous batteries.","PeriodicalId":270,"journal":{"name":"Chemical Engineering Journal","volume":"42 1","pages":""},"PeriodicalIF":15.1,"publicationDate":"2026-02-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146146766","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.2026.173931
Birgitte K. Ahring, Fuad Ale Enriquez, Muhammad Usman Khan, Peter Valdez, Francesca Pierobon, Timothy E. Seiple, Richard Garrison
Conventional anaerobic digestion (AD) of sewage sludge in wastewater treatment facilities suffers from low carbon conversion efficiency (CCE ≤ 40%) and requires costly CO2 removal for injection of the produced CH4 into the natural gas grid. To address these limitations, we developed the Advanced Pretreatment and Anaerobic Digestion (APAD) process. This integrates Advanced Wet Oxidation & Steam Explosion (AWOEx) pretreatment of residual sludge after conventional AD, followed by biogas upgradation using a novel methanogenic strain, Methanothermobacter wolfeii BSEL, converting CO2 with H2 into CH4 or RNG (renewable natural gas). Pilot-scale results demonstrated that AWOEx pretreatment achieved a CCE of 62% for the residual sludge, 68% higher than the conventional AD process. The CH4 production was further increased by 79%. Subsequent biogas upgrading in a trickling bed reactor with H2 further enhanced total methane output by 100% and resulted in a final CO2 concentration of ≤3%. The integrated APAD process achieved a remarkable overall CCE of 83%, resulting in a 200% increase in RNG output when compared to conventional AD. Techno-economic analysis revealed that AWOEx pretreatment alone reduced sludge treatment costs from $494 to $253 per ton of dry solids. The complete APAD process incurred a higher cost of treatment of $530 per ton, driven by prices of bottled H2. The process did, however, show gains in energy recovery and decarbonization. Renewable H2, which may reduce in price in the near future, can positively improve the economics of biogas upgrading for the APAD process.
{"title":"Improving anaerobic digestion of sewage sludge to renewable natural gas by the Advanced Pretreatment & Anaerobic Digestion technology (APAD): Pilot testing","authors":"Birgitte K. Ahring, Fuad Ale Enriquez, Muhammad Usman Khan, Peter Valdez, Francesca Pierobon, Timothy E. Seiple, Richard Garrison","doi":"10.1016/j.cej.2026.173931","DOIUrl":"https://doi.org/10.1016/j.cej.2026.173931","url":null,"abstract":"Conventional anaerobic digestion (AD) of sewage sludge in wastewater treatment facilities suffers from low carbon conversion efficiency (CCE ≤ 40%) and requires costly CO<sub>2</sub> removal for injection of the produced CH<sub>4</sub> into the natural gas grid. To address these limitations, we developed the Advanced Pretreatment and Anaerobic Digestion (APAD) process. This integrates Advanced Wet Oxidation & Steam Explosion (AWOEx) pretreatment of residual sludge after conventional AD, followed by biogas upgradation using a novel methanogenic strain, <em>Methanothermobacter wolfeii</em> BSEL, converting CO<sub>2</sub> with H<sub>2</sub> into CH<sub>4</sub> or RNG (renewable natural gas). Pilot-scale results demonstrated that AWOEx pretreatment achieved a CCE of 62% for the residual sludge, 68% higher than the conventional AD process. The CH<sub>4</sub> production was further increased by 79%. Subsequent biogas upgrading in a trickling bed reactor with H<sub>2</sub> further enhanced total methane output by 100% and resulted in a final CO<sub>2</sub> concentration of ≤3%. The integrated APAD process achieved a remarkable overall CCE of 83%, resulting in a 200% increase in RNG output when compared to conventional AD. Techno-economic analysis revealed that AWOEx pretreatment alone reduced sludge treatment costs from $494 to $253 per ton of dry solids. The complete APAD process incurred a higher cost of treatment of $530 per ton, driven by prices of bottled H<sub>2</sub>. The process did, however, show gains in energy recovery and decarbonization. Renewable H<sub>2</sub>, which may reduce in price in the near future, can positively improve the economics of biogas upgrading for the APAD process.","PeriodicalId":270,"journal":{"name":"Chemical Engineering Journal","volume":"23 1","pages":""},"PeriodicalIF":15.1,"publicationDate":"2026-02-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146138317","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}
Effective management of bubble dynamics is critical for enhancing hydrogen production efficiency in water electrolysis. This work establishes a dual Marangoni mechanism, driven by the interplay between solutal and thermal Marangoni effects, as a principal regulator of bubble behavior. Through systematic variation of applied current and electrolyte concentration, we demonstrate how this mechanism dictates bubble growth, detachment, and the resulting electrochemical oscillations. Chronoamperometry coupled with high-speed optical imaging shows that bubble evolution produces periodic potential oscillations, with a persistent microbubble carpet underlying each detached main bubble. A characteristic V-shaped dependence of bubble growth period on applied current is identified, arising from the competition between solutal and thermal Marangoni effects, where the transition current shifts to higher values with increasing electrolyte concentration. Faraday-based quantification indicates that the majority of produced hydrogen is contained within the main bubbles. While hydrogen output rises with current, optimal efficiency demands a balance between overpotential and gas evolution. Higher electrolyte concentrations lower the overpotential but modestly reduce bubble-mediated gas output. Collectively, this study deepens the fundamental understanding of how bubble dynamics govern electrochemical performance, offering guidance for the rational design of high-efficiency hydrogen evolution systems.
{"title":"Dual Marangoni-regulated bubble dynamics and potential oscillations during electrocatalytic hydrogen evolution","authors":"Xinlong Lu, Xinying Yi, Xinshuo Zhang, Devendra Yadav, Qingfan Liu, Jiwei Li, Lijing Ma, Dengwei Jing","doi":"10.1016/j.cej.2026.173926","DOIUrl":"https://doi.org/10.1016/j.cej.2026.173926","url":null,"abstract":"Effective management of bubble dynamics is critical for enhancing hydrogen production efficiency in water electrolysis. This work establishes a dual Marangoni mechanism, driven by the interplay between solutal and thermal Marangoni effects, as a principal regulator of bubble behavior. Through systematic variation of applied current and electrolyte concentration, we demonstrate how this mechanism dictates bubble growth, detachment, and the resulting electrochemical oscillations. Chronoamperometry coupled with high-speed optical imaging shows that bubble evolution produces periodic potential oscillations, with a persistent microbubble carpet underlying each detached main bubble. A characteristic V-shaped dependence of bubble growth period on applied current is identified, arising from the competition between solutal and thermal Marangoni effects, where the transition current shifts to higher values with increasing electrolyte concentration. Faraday-based quantification indicates that the majority of produced hydrogen is contained within the main bubbles. While hydrogen output rises with current, optimal efficiency demands a balance between overpotential and gas evolution. Higher electrolyte concentrations lower the overpotential but modestly reduce bubble-mediated gas output. Collectively, this study deepens the fundamental understanding of how bubble dynamics govern electrochemical performance, offering guidance for the rational design of high-efficiency hydrogen evolution systems.","PeriodicalId":270,"journal":{"name":"Chemical Engineering Journal","volume":"90 1","pages":""},"PeriodicalIF":15.1,"publicationDate":"2026-02-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146138877","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.2026.173996
Chenhua Shu, Jun Yang, Jiayi Zhang, Helin Fan, Xingyu Dai, Dan Luo, Shuo Mi, Tonghua Sun
To solve the problem of the deep eutectic solvents synthesized with small volume hydrogen bond acceptors and hydrogen bond donors entering the cavity of pore generator and occupying their pore structure, supramolecular deep eutectic solvent (SDES) was firstly introduced to construct porous deep eutectic solvent (PDES). Thereby, a PDES was synthesized by using ZIF − 8 encapsulating peroxophosphotungstate (PPT) as pore generator and SDES composed of methyl-β-cyclodextrin (M − β − CD) and levulinic acid (LA) as steric hindrance solvents. The characterization results indicated that PPT was encapsulated successfully within ZIF − 8 to prepare [PPT@ZIF − 8]. [PPT@ZIF − 8] and [M − β − CD/LA] remain structure stable after forming PDES and [M − β − CD/LA] do not fill the cavity of [PPT@ZIF − 8]. The PDES [PPT@ZIF − 8][M − β − CD/LA] was applied for oil desulfurization and the desulfurization rate of dibenzothiophene in model oils could reach 100% within 2.5 h using H2O2 as oxidant. The desulfurization by [PPT@ZIF − 8][M − β − CD/LA] combined the extractive desulfurization with [M − β − CD/LA] as extractant and the oxidative desulfurization with [PPT@ZIF − 8] as catalyst. Furthermore, [PPT@ZIF − 8][M − β − CD/LA] has excellent regeneration performance. This work will provide a new route to construct PDESs and will promote the industrial application of porous liquids.
{"title":"Synthesis of a porous deep eutectic solvent based on supramolecular deep eutectic solvent and its application in extractive−oxidative desulfurization","authors":"Chenhua Shu, Jun Yang, Jiayi Zhang, Helin Fan, Xingyu Dai, Dan Luo, Shuo Mi, Tonghua Sun","doi":"10.1016/j.cej.2026.173996","DOIUrl":"https://doi.org/10.1016/j.cej.2026.173996","url":null,"abstract":"To solve the problem of the deep eutectic solvents synthesized with small volume hydrogen bond acceptors and hydrogen bond donors entering the cavity of pore generator and occupying their pore structure, supramolecular deep eutectic solvent (SDES) was firstly introduced to construct porous deep eutectic solvent (PDES). Thereby, a PDES was synthesized by using ZIF − 8 encapsulating peroxophosphotungstate (PPT) as pore generator and SDES composed of methyl-β-cyclodextrin (M − β − CD) and levulinic acid (LA) as steric hindrance solvents. The characterization results indicated that PPT was encapsulated successfully within ZIF − 8 to prepare [PPT@ZIF − 8]. [PPT@ZIF − 8] and [M − β − CD/LA] remain structure stable after forming PDES and [M − β − CD/LA] do not fill the cavity of [PPT@ZIF − 8]. The PDES [PPT@ZIF − 8][M − β − CD/LA] was applied for oil desulfurization and the desulfurization rate of dibenzothiophene in model oils could reach 100% within 2.5 h using H<ce:inf loc=\"post\">2</ce:inf>O<ce:inf loc=\"post\">2</ce:inf> as oxidant. The desulfurization by [PPT@ZIF − 8][M − β − CD/LA] combined the extractive desulfurization with [M − β − CD/LA] as extractant and the oxidative desulfurization with [PPT@ZIF − 8] as catalyst. Furthermore, [PPT@ZIF − 8][M − β − CD/LA] has excellent regeneration performance. This work will provide a new route to construct PDESs and will promote the industrial application of porous liquids.","PeriodicalId":270,"journal":{"name":"Chemical Engineering Journal","volume":"4 1","pages":""},"PeriodicalIF":15.1,"publicationDate":"2026-02-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146146734","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.2026.173983
He Chen, Ning Sun, Xue Li, Qian Xu, Weiwei Pang, Bin Xu
Coal-based carbons, characterized by abundant availability and low cost, are considered as highly promising anode materials for sodium-ion batteries. However, the limited capacity and unsatisfied initial coulombic efficiency (ICE) caused by ordered microcrystalline structure and abundant surface defects significantly restricted the application of coal-based carbon. Herein, a novel crosslinked synergistic coating strategy is proposed to improve the electrochemical Na-storage performance of coal-based carbon. The crosslinking reaction between sucrose and lignite coal facilitates the formation of microcrystalline structure dominated by pseudo-graphitic phase. Meanwhile, the dehydration reaction of sucrose generates a coating layer featuring highly disordered microcrystalline structures on the surface of lignite coal, which not only repairs surface defects but also facilitate rapid ion transfer. Consequently, the optimal SCLC-1200 demonstrates a high reversible sodium storage capacity of 313.4 mAh g−1 with a superior ICE of 85.9%. Furthermore, it exhibits a remarkable capacity retention of 99.3% after 2000 cycles at 2C. Notably, the Na-ion full cell fabricated based on SCLC-1200 anode realizes a high energy density of 251.1 Wh kg−1, highlighting its promising prospect for practical applications. This work achieves a synergistic enhancement through coating construction, microcrystalline regulation and defect repairment, offering valuable insights for the structural design of advanced coal-based energy storage materials.
煤基碳具有可获得性高、成本低等特点，是极具发展前景的钠离子电池负极材料。然而，有序的微晶结构和大量的表面缺陷导致的容量有限和初始库仑效率（ICE）不理想，严重制约了煤基碳的应用。本文提出了一种新型的交联协同涂层策略，以提高煤基碳的电化学储钠性能。蔗糖与褐煤的交联反应有利于形成以伪石墨相为主的微晶结构。同时，蔗糖的脱水反应会在褐煤表面形成一层微晶结构高度无序的涂层，不仅可以修复表面缺陷，还可以促进离子的快速转移。因此，最佳SCLC-1200具有313.4 mAh g−1的高可逆钠存储容量和85.9%的优越ICE。此外，在2C温度下，经过2000次 循环后，其容量保持率达到99.3%。值得注意的是，基于SCLC-1200阳极制备的钠离子全电池实现了251.1 Wh kg−1的高能量密度，具有广阔的实际应用前景。本工作通过涂层构建、微晶调控和缺陷修复实现了协同增强，为先进煤基储能材料的结构设计提供了有价值的见解。
{"title":"Synergistic crosslinking-coating engineering of coal-based hard carbon for high-performance sodium-ion batteries","authors":"He Chen, Ning Sun, Xue Li, Qian Xu, Weiwei Pang, Bin Xu","doi":"10.1016/j.cej.2026.173983","DOIUrl":"https://doi.org/10.1016/j.cej.2026.173983","url":null,"abstract":"Coal-based carbons, characterized by abundant availability and low cost, are considered as highly promising anode materials for sodium-ion batteries. However, the limited capacity and unsatisfied initial coulombic efficiency (ICE) caused by ordered microcrystalline structure and abundant surface defects significantly restricted the application of coal-based carbon. Herein, a novel crosslinked synergistic coating strategy is proposed to improve the electrochemical Na-storage performance of coal-based carbon. The crosslinking reaction between sucrose and lignite coal facilitates the formation of microcrystalline structure dominated by pseudo-graphitic phase. Meanwhile, the dehydration reaction of sucrose generates a coating layer featuring highly disordered microcrystalline structures on the surface of lignite coal, which not only repairs surface defects but also facilitate rapid ion transfer. Consequently, the optimal SCLC-1200 demonstrates a high reversible sodium storage capacity of 313.4 mAh g<ce:sup loc=\"post\">−1</ce:sup> with a superior ICE of 85.9%. Furthermore, it exhibits a remarkable capacity retention of 99.3% after 2000 cycles at 2C. Notably, the Na-ion full cell fabricated based on SCLC-1200 anode realizes a high energy density of 251.1 Wh kg<ce:sup loc=\"post\">−1</ce:sup>, highlighting its promising prospect for practical applications. This work achieves a synergistic enhancement through coating construction, microcrystalline regulation and defect repairment, offering valuable insights for the structural design of advanced coal-based energy storage materials.","PeriodicalId":270,"journal":{"name":"Chemical Engineering Journal","volume":"9 1","pages":""},"PeriodicalIF":15.1,"publicationDate":"2026-02-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146146735","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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