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.2026.173938
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.2026.173975
Abhishek Naskar, Ananya Aishwarya, Matthieu Gresil, Terence W. Turney, Arup R. Bhattacharyya
Emerging contaminants, including pharmaceutical residues, industrial dyes, and endocrine disruptors, are recognized as environmental threats due to their persistence, bioaccumulation, and resistance to conventional water treatment methods. Pharmaceuticals remain undegraded, leading to their presence in aquatic ecosystems, where even trace concentrations affect biological systems. To address this challenge, we developed a multi-functional nanocomposite integrating mono‑lithium adipate (Li-AA) exfoliated molybdenum disulphide (MoS2) and barium titanate (BaTiO3) within a PVDF matrix through melt-mixing followed by solution-casting. Li-AA acted as an anchoring and coupling agent between MoS2 and BaTiO3, served as an exfoliating agent for MoS2 sheets, and enhanced the electroactive β-phase content of PVDF. The hybrid nanofiller concentration of 1 wt% promoted strong interfacial coupling, yielding a β-phase fraction of ~95% and a piezoelectric coefficient of ~62.4 pm/V in PVDF hybrid nanocomposite. The piezopotential generated under ultra-sonic excitation enhanced electron transfer and induces reactive oxygen species, achieving over 90% degradation of industrial dyes and more than 80% removal of pharmaceutical contaminants, specifically diclofenac sodium. Diclofenac sodium is a persistent pharmaceutical pollutant known to cause hepatotoxicity, renal dysfunction, and endocrine disruption in aquatic organisms. Its accumulation in water bodies has been linked to a serious threat to ecological balance. Spectroscopic and ecotoxicological analyses confirmed structural evolution and the benign nature of the end-products, correlating microstructure, charge transport, and catalytic activity. The study elucidated the processing-structure-property-remediation relationship, while quantum chemistry-based Fukui analysis revealed the degradation pathways and reactive sites of pharmaceutical pollutants, enabling sustainable and highly efficient piezocatalytic film-based water remediation.
{"title":"Piezocatalytic hybrid nanocomposite film for ecotoxicity-assessed environmental contaminant remediation","authors":"Abhishek Naskar, Ananya Aishwarya, Matthieu Gresil, Terence W. Turney, Arup R. Bhattacharyya","doi":"10.1016/j.cej.2026.173975","DOIUrl":"https://doi.org/10.1016/j.cej.2026.173975","url":null,"abstract":"Emerging contaminants, including pharmaceutical residues, industrial dyes, and endocrine disruptors, are recognized as environmental threats due to their persistence, bioaccumulation, and resistance to conventional water treatment methods. Pharmaceuticals remain undegraded, leading to their presence in aquatic ecosystems, where even trace concentrations affect biological systems. To address this challenge, we developed a multi-functional nanocomposite integrating mono‑lithium adipate (Li-AA) exfoliated molybdenum disulphide (MoS<sub>2</sub>) and barium titanate (BaTiO<sub>3</sub>) within a PVDF matrix through melt-mixing followed by solution-casting. Li-AA acted as an anchoring and coupling agent between MoS<sub>2</sub> and BaTiO<sub>3</sub>, served as an exfoliating agent for MoS<sub>2</sub> sheets, and enhanced the electroactive β-phase content of PVDF. The hybrid nanofiller concentration of 1 wt% promoted strong interfacial coupling, yielding a β-phase fraction of ~95% and a piezoelectric coefficient of ~62.4 pm/<em>V</em> in PVDF hybrid nanocomposite. The piezopotential generated under ultra-sonic excitation enhanced electron transfer and induces reactive oxygen species, achieving over 90% degradation of industrial dyes and more than 80% removal of pharmaceutical contaminants, specifically diclofenac sodium. Diclofenac sodium is a persistent pharmaceutical pollutant known to cause hepatotoxicity, renal dysfunction, and endocrine disruption in aquatic organisms. Its accumulation in water bodies has been linked to a serious threat to ecological balance. Spectroscopic and ecotoxicological analyses confirmed structural evolution and the benign nature of the end-products, correlating microstructure, charge transport, and catalytic activity. The study elucidated the processing-structure-property-remediation relationship, while quantum chemistry-based Fukui analysis revealed the degradation pathways and reactive sites of pharmaceutical pollutants, enabling sustainable and highly efficient piezocatalytic film-based water remediation.","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":"146145943","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.2026.173885
Jian Guo, Shuo Meng, Xiao Yan, Qiuxian Wang, Ting He, Lu Chen, Lujie Zuo, Ya Tang, Hongbin Zhao
Vanadate oxides, with their low cost and high theoretical capacity, are promising cathode materials for aqueous zinc-ion batteries (AZIBs). However, their practical application is hindered by sluggish Zn2+ diffusion, poor electronic conductivity, and structural degradation during cycling. Herein, sodium ions and polyethylene glycol are co-intercalated into ammonium vanadate (PEG-NaNVO) nanobelts, resulting in expanded interlayer spacing and the introduction of oxygen vacancies. These structural modifications redistribute charge density and weaken electrostatic interactions with Zn2+, thereby facilitating rapid ion transport. Meanwhile, the synergistic effects of NaO coordination and hydrogen bonding between PEG and the VO layer of PEG-NaNVO reinforce the lattice framework and optimize the electronic structure, accelerating redox kinetics. Benefiting from these features, the PEG-NaNVO cathode delivers a high specific capacity of 550 mAh g−1 at 0.2 A g−1, an excellent rate capability of 188 mAh g−1 at 25 A g−1, and remarkable cycling stability with 81.4% capacity retention after 5000 cycles. This work demonstrates a rational co-intercalation strategy for engineering high-performance vanadium-based cathodes and highlights the potential of PEG-NaNVO for next-generation AZIBs.
钒酸盐氧化物具有成本低、理论容量大的优点，是极有前途的水性锌离子电池正极材料。然而，它们的实际应用受到Zn2+扩散缓慢，电子导电性差以及循环过程中结构降解的阻碍。在这里，钠离子和聚乙二醇共嵌入到钒酸铵（PEG-NaNVO）纳米带中，导致层间距扩大和氧空位的引入。这些结构修饰重新分配了电荷密度，减弱了与Zn2+的静电相互作用，从而促进了离子的快速传输。同时，PEG- nanvo与VO层之间的NaO配位和氢键的协同作用强化了晶格框架，优化了电子结构，加速了氧化还原动力学。得益于这些特性，PEG-NaNVO阴极在0.2 a g−1时具有550 mAh g−1的高比容量，在25 a g−1时具有188 mAh g−1的优异倍率容量，并且在5000次 循环后具有81.4%的显着循环稳定性。这项工作展示了一种合理的共插层策略，用于工程高性能钒基阴极，并突出了PEG-NaNVO在下一代AZIBs中的潜力。
{"title":"Interlayer-engineered ammonium vanadate cathodes via Na+/PEG Co-intercalation for fast and stable Zn-ion storage","authors":"Jian Guo, Shuo Meng, Xiao Yan, Qiuxian Wang, Ting He, Lu Chen, Lujie Zuo, Ya Tang, Hongbin Zhao","doi":"10.1016/j.cej.2026.173885","DOIUrl":"https://doi.org/10.1016/j.cej.2026.173885","url":null,"abstract":"Vanadate oxides, with their low cost and high theoretical capacity, are promising cathode materials for aqueous zinc-ion batteries (AZIBs). However, their practical application is hindered by sluggish Zn<sup>2+</sup> diffusion, poor electronic conductivity, and structural degradation during cycling. Herein, sodium ions and polyethylene glycol are co-intercalated into ammonium vanadate (PEG-NaNVO) nanobelts, resulting in expanded interlayer spacing and the introduction of oxygen vacancies. These structural modifications redistribute charge density and weaken electrostatic interactions with Zn<sup>2+</sup>, thereby facilitating rapid ion transport. Meanwhile, the synergistic effects of Na<img alt=\"single bond\" src=\"https://sdfestaticassets-us-east-1.sciencedirectassets.com/shared-assets/55/entities/sbnd.gif\" style=\"vertical-align:middle\"/>O coordination and hydrogen bonding between PEG and the V<img alt=\"single bond\" src=\"https://sdfestaticassets-us-east-1.sciencedirectassets.com/shared-assets/55/entities/sbnd.gif\" style=\"vertical-align:middle\"/>O layer of PEG-NaNVO reinforce the lattice framework and optimize the electronic structure, accelerating redox kinetics. Benefiting from these features, the PEG-NaNVO cathode delivers a high specific capacity of 550 mAh g<sup>−1</sup> at 0.2 A g<sup>−1</sup>, an excellent rate capability of 188 mAh g<sup>−1</sup> at 25 A g<sup>−1</sup>, and remarkable cycling stability with 81.4% capacity retention after 5000 cycles. This work demonstrates a rational co-intercalation strategy for engineering high-performance vanadium-based cathodes and highlights the potential of PEG-NaNVO for next-generation AZIBs.","PeriodicalId":270,"journal":{"name":"Chemical Engineering Journal","volume":"20 1","pages":""},"PeriodicalIF":15.1,"publicationDate":"2026-02-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146145947","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.2026.173928
Yifan Li, Yao Lu, Xinglan Li, Wanling Zhong, Kun Liu
Tetracycline hydrochloride (TC) contamination poses significant risks to aquatic environments and human health, due to its persistence and ability to induce antibiotic resistance. Conventional sulfate radical-based advanced oxidation processes (SR-AOPs) face industrial barriers from costly catalyst synthesis and poor cycling performance. This study develops an economical composite catalyst from pyrite-containing iron tailings. After “anoxic calcination-magnetic separation” pretreatment to concentrate FeS, a dual-heterostructure FeS@Cu catalyst (FeS@CuFe2S3/CuFe2S3@talc) was made via co-precipitation and secondary anoxic calcination. FeS@CuFe2S3 acts as the peroxymonosulfate (PMS) activation interface, while CuFe2S3@talc uses talc to inhibit active component aggregation, solving low active site utilization in conventional catalysts. Optimized FeS@4Cu in the PMS system removes 90.93% tetracycline within 30 min. After 6 cycles, degradation efficiency remains 77.03%, with Cu/Fe leaching (1.0/0.4 mg/L) well below GB 3838–2002 (Cu ≤ 1 mg/L) and EU (Fe ≤ 2 mg/L) limits. Mechanistically, SO4- is the main reactive oxygen species, driven by Fe(II)/Fe(III) and Cu(I)/Cu(II) bimetallic redox cycles, aided by reductive S species for metal valence recycling. FeS@CuFe2S3 tunes Fe/Cu d-band center, enhances PMS orbital hybridization, reduces OO bond cleavage barrier, and enables directional electron transfer (0.7369 e). For practical use, 7 g of granular FeS@4Cu (0.5 cm diameter, orange peel pore-forming agent / Na2SiO3 binder) maintains >72.90% TC removal after treating 34 L wastewater in fixed-bed, while retaining mechanical strength and intact pore structures. This work enables sustainable iron tailings valorization and provides an effective SR-AOPs catalyst for continuous organic wastewater treatment.
{"title":"Iron tailings-derived FeS@Cu with FeS@CuFe2S3/CuFe2S3@talc dual heterostructures: Bimetallic synergy for peroxymonosulfate activation and tetracycline hydrochloride degradation","authors":"Yifan Li, Yao Lu, Xinglan Li, Wanling Zhong, Kun Liu","doi":"10.1016/j.cej.2026.173928","DOIUrl":"https://doi.org/10.1016/j.cej.2026.173928","url":null,"abstract":"Tetracycline hydrochloride (TC) contamination poses significant risks to aquatic environments and human health, due to its persistence and ability to induce antibiotic resistance. Conventional sulfate radical-based advanced oxidation processes (SR-AOPs) face industrial barriers from costly catalyst synthesis and poor cycling performance. This study develops an economical composite catalyst from pyrite-containing iron tailings. After “anoxic calcination-magnetic separation” pretreatment to concentrate FeS, a dual-heterostructure FeS@Cu catalyst (FeS@CuFe<sub>2</sub>S<sub>3</sub>/CuFe<sub>2</sub>S<sub>3</sub>@talc) was made via co-precipitation and secondary anoxic calcination. FeS@CuFe<sub>2</sub>S<sub>3</sub> acts as the peroxymonosulfate (PMS) activation interface, while CuFe<sub>2</sub>S<sub>3</sub>@talc uses talc to inhibit active component aggregation, solving low active site utilization in conventional catalysts. Optimized FeS@4Cu in the PMS system removes 90.93% tetracycline within 30 min. After 6 cycles, degradation efficiency remains 77.03%, with Cu/Fe leaching (1.0/0.4 mg/L) well below GB 3838–2002 (Cu ≤ 1 mg/L) and EU (Fe ≤ 2 mg/L) limits. Mechanistically, SO<sub>4</sub><img alt=\"radical dot\" src=\"https://sdfestaticassets-us-east-1.sciencedirectassets.com/shared-assets/55/entities/rad.gif\" style=\"vertical-align:middle\"/><sup>-</sup> is the main reactive oxygen species, driven by Fe(II)/Fe(III) and Cu(I)/Cu(II) bimetallic redox cycles, aided by reductive S species for metal valence recycling. FeS@CuFe<sub>2</sub>S<sub>3</sub> tunes Fe/Cu d-band center, enhances PMS orbital hybridization, reduces O<img alt=\"single bond\" src=\"https://sdfestaticassets-us-east-1.sciencedirectassets.com/shared-assets/55/entities/sbnd.gif\" style=\"vertical-align:middle\"/>O bond cleavage barrier, and enables directional electron transfer (0.7369 e). For practical use, 7 g of granular FeS@4Cu (0.5 cm diameter, orange peel pore-forming agent / Na<sub>2</sub>SiO<sub>3</sub> binder) maintains >72.90% TC removal after treating 34 L wastewater in fixed-bed, while retaining mechanical strength and intact pore structures. This work enables sustainable iron tailings valorization and provides an effective SR-AOPs catalyst for continuous organic wastewater treatment.","PeriodicalId":270,"journal":{"name":"Chemical Engineering Journal","volume":"15 1","pages":""},"PeriodicalIF":15.1,"publicationDate":"2026-02-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146145948","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.2026.173896
D. Narsimulu, Ko Eun-byeol, Park Jung-jae, Kwang-Sun Ryu
All-solid-state batteries (ASSBs) have emerged as a promising alternative to conventional lithium batteries owing to their potential to maximize energy density and safety improvement. Developing suitable solid electrolytes (SE) with high ionic conductivity, improved air stability, and enhanced electrolyte/anode interfacial stability remains a significant challenge in the field of ASSBs. Overcoming these obstacles is crucial for advancing the performance and reliability of solid-state batteries. In this work, we have developed Li3-3xP1-xZrxS4−4xCl4x (0 ≤ x ≤ 0.05) and utilized it as a solid electrolyte for ASSBs. The x = 0.03 amount of Zr and Cl doping (i.e., Li2.91P0.97Zr0.03S3.88Cl0.12) exhibit highest ionic conductivity (1.6 × 10−3 S cm−1), which is 3.55 times higher than the pristine β–Li3PS4 (LPS). The measured air stability values for the Li2.91P0.97Zr0.03S3.88Cl0.12 (LPZrSCl) and β-Li3PS4 SEs is 0.045 cm3 g−1 and 0.118 cm3·g−1, respectively. After doping with Zr and Cl, the generation of H2S gas was significantly reduced, showing a reduction that is 2.62 times lower compared to the LPS. The Li-In/LPZrSCl/Li-In symmetric cell exhibits excellent stability over 400 h. The NCM811/LPZrSCl/Li-In ASSB cell shows an initial discharge capacity of 143.3 mA h g−1 and restored a high discharge capacity of 136 mA h g−1 after 250 cycles with a capacity retention of 89.3%. In contrast, the discharge capacity of β-Li3PS4 was limited to 50.1 mA h g−1 (after 250 cycles). These findings reveal that Zr and Cl co-doping play a major role in improving ionic conductivity, air stability, and electrochemical performance of β-Li3PS4. This work suggests a new idea to improve the conductivity of Li2S-P2S5 binary systems and other sulfide electrolytes to design high-capacity and energy-density solid-state batteries.
全固态电池（assb）已成为传统锂电池的一个有前途的替代品，因为它们具有最大的能量密度和安全性改进的潜力。开发具有高离子电导率、改善空气稳定性和增强电解质/阳极界面稳定性的合适固体电解质（SE）仍然是assb领域的重大挑战。克服这些障碍对于提高固态电池的性能和可靠性至关重要。在这项工作中，我们开发了Li3-3xP1-xZrxS4−4xCl4x(0 ≤ x ≤ 0.05)，并将其用作assb的固体电解质。Zr和Cl掺杂量为x = 0.03（即Li2.91P0.97Zr0.03S3.88Cl0.12）时，离子电导率最高（1.6 × 10−3 S cm−1），是原始β-Li3PS4 （LPS）的3.55倍。Li2.91P0.97Zr0.03S3.88Cl0.12 （LPZrSCl）和β-Li3PS4 SEs的空气稳定性测量值分别为0.045 cm3 g−1和0.118 cm3·g−1。掺入Zr和Cl后，H2S气体的生成明显减少，比LPS减少了2.62倍。Li-In/LPZrSCl/Li-In对称电池在400 h以上具有优异的稳定性。NCM811/LPZrSCl/Li-In ASSB电池的初始放电容量为143.3 mA h g−1，经过250 次循环后恢复到136 mA h g−1的高放电容量，容量保持率为89.3%。相比之下，β-Li3PS4的放电容量限制在50.1 mA h g−1（经过250 次循环）。这些结果表明，Zr和Cl共掺杂对改善β-Li3PS4的离子电导率、空气稳定性和电化学性能起着重要作用。这项工作为提高Li2S-P2S5二元体系和其他硫化物电解质的导电性，设计高容量和能量密度的固态电池提供了新的思路。
{"title":"High-ionic conductivity and electrochemical performances of Zr and cl co-doped β-Li3PS4 solid-electrolyte for all-solid-state Li–ion batteries","authors":"D. Narsimulu, Ko Eun-byeol, Park Jung-jae, Kwang-Sun Ryu","doi":"10.1016/j.cej.2026.173896","DOIUrl":"https://doi.org/10.1016/j.cej.2026.173896","url":null,"abstract":"All-solid-state batteries (ASSBs) have emerged as a promising alternative to conventional lithium batteries owing to their potential to maximize energy density and safety improvement. Developing suitable solid electrolytes (SE) with high ionic conductivity, improved air stability, and enhanced electrolyte/anode interfacial stability remains a significant challenge in the field of ASSBs. Overcoming these obstacles is crucial for advancing the performance and reliability of solid-state batteries. In this work, we have developed Li<sub>3-3<em>x</em></sub>P<sub>1-<em>x</em></sub>Zr<sub><em>x</em></sub>S<sub>4−4x</sub>Cl<sub>4<em>x</em></sub> (0 ≤ x ≤ 0.05) and utilized it as a solid electrolyte for ASSBs. The <em>x</em> = 0.03 amount of Zr and Cl doping (i.e., Li<sub>2.91</sub>P<sub>0.97</sub>Zr<sub>0.03</sub>S<sub>3.88</sub>Cl<sub>0.12</sub>) exhibit highest ionic conductivity (1.6 × 10<sup>−3</sup> S cm<sup>−1</sup>), which is 3.55 times higher than the pristine β–Li<sub>3</sub>PS<sub>4</sub> (LPS). The measured air stability values for the Li<sub>2.91</sub>P<sub>0.97</sub>Zr<sub>0.03</sub>S<sub>3.88</sub>Cl<sub>0.12</sub> (LPZrSCl) and β-Li<sub>3</sub>PS<sub>4</sub> SEs is 0.045 cm<sup>3</sup> g<sup>−1</sup> and 0.118 cm<sup>3</sup>·g<sup>−1</sup>, respectively. After doping with Zr and Cl, the generation of H<sub>2</sub>S gas was significantly reduced, showing a reduction that is 2.62 times lower compared to the LPS. The Li-In/LPZrSCl/Li-In symmetric cell exhibits excellent stability over 400 h. The NCM811/LPZrSCl/Li-In ASSB cell shows an initial discharge capacity of 143.3 mA h g<sup>−1</sup> and restored a high discharge capacity of 136 mA h g<sup>−1</sup> after 250 cycles with a capacity retention of 89.3%. In contrast, the discharge capacity of β-Li<sub>3</sub>PS<sub>4</sub> was limited to 50.1 mA h g<sup>−1</sup> (after 250 cycles). These findings reveal that Zr and Cl co-doping play a major role in improving ionic conductivity, air stability, and electrochemical performance of β-Li<sub>3</sub>PS<sub>4.</sub> This work suggests a new idea to improve the conductivity of Li<sub>2</sub>S-P<sub>2</sub>S<sub>5</sub> binary systems and other sulfide electrolytes to design high-capacity and energy-density solid-state batteries.","PeriodicalId":270,"journal":{"name":"Chemical Engineering Journal","volume":"44 1","pages":""},"PeriodicalIF":15.1,"publicationDate":"2026-02-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146138318","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}
O coordination and hydrogen bonding between PEG and the V
- is the main reactive oxygen species, driven by Fe(II)/Fe(III) and Cu(I)/Cu(II) bimetallic redox cycles, aided by reductive S species for metal valence recycling. FeS@CuFe2S3 tunes Fe/Cu d-band center, enhances PMS orbital hybridization, reduces O
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