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.2026.173896
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.
{"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.2026.173954
Fuchang Duan, Jinglei Si, Xiaoge Peng, Xiaosa Wang, Yang Ding, Wei Guo, Pan Hu, Yanan Deng, Haibo Lin, Haoqiang Cao, Yunyi Cao, Xing Zhong, Jianguo Wang
Efficient and selective electrocatalytic generation of O3 and NaClO is crucial for advanced water treatment, but remains challenging due to low oxidant selectivity and poor electrode stability. The bilayer Nd-NATO/CNT-ATO-PED and Nd-Ru-NATO/CNT-ATO-PED electrocatalysts, fabricated via pulsed electrodeposition (PED) and interlayer engineering, outperformed a monolayer electrocatalyst prepared by direct current electrodeposition (ED). These nanostructures featured abundant oxygen vacancies, tuned lattice spacing, and modulated electronic states, achieving high Faradaic efficiencies of 35.3% for electrochemical ozone production (EOP) and 96.7% for chlorine evolution reaction (CER). In situ experiments and density functional theory (DFT) calculations reveal that Nd doping promoted the lattice oxygen mechanism (LOM) pathway, reduced energy barriers, enhanced electron transfer, and facilitated a *O3 five-membered intermediate formation. Furthermore, the introduction of Nd optimized the electronic structure, synergistically lowered the overpotential, and improved the efficiency of Cl2/NaClO generation. The system was integrated into a custom flow-through reactor, achieving 97.0% degradation efficiency for 50 ppm ciprofloxacin within 2 min over 20 cycles in simulated tap water. These results establish a scalable platform for dual oxidant electrosynthesis and efficient pollutant removal, demonstrating that PED combined with interlayer engineering provides an effective design strategy for high-performance SnO2-based electrocatalysts in environmental remediation.
{"title":"Pulse electrodeposition of Nd-doped SnO2-based electrocatalysts for enhanced electrochemical production of ozone and active chlorine","authors":"Fuchang Duan, Jinglei Si, Xiaoge Peng, Xiaosa Wang, Yang Ding, Wei Guo, Pan Hu, Yanan Deng, Haibo Lin, Haoqiang Cao, Yunyi Cao, Xing Zhong, Jianguo Wang","doi":"10.1016/j.cej.2026.173954","DOIUrl":"https://doi.org/10.1016/j.cej.2026.173954","url":null,"abstract":"Efficient and selective electrocatalytic generation of O<sub>3</sub> and NaClO is crucial for advanced water treatment, but remains challenging due to low oxidant selectivity and poor electrode stability. The bilayer Nd-NATO/CNT-ATO-PED and Nd-Ru-NATO/CNT-ATO-PED electrocatalysts, fabricated via pulsed electrodeposition (PED) and interlayer engineering, outperformed a monolayer electrocatalyst prepared by direct current electrodeposition (ED). These nanostructures featured abundant oxygen vacancies, tuned lattice spacing, and modulated electronic states, achieving high Faradaic efficiencies of 35.3% for electrochemical ozone production (EOP) and 96.7% for chlorine evolution reaction (CER). In situ experiments and density functional theory (DFT) calculations reveal that Nd doping promoted the lattice oxygen mechanism (LOM) pathway, reduced energy barriers, enhanced electron transfer, and facilitated a *O<sub>3</sub> five-membered intermediate formation. Furthermore, the introduction of Nd optimized the electronic structure, synergistically lowered the overpotential, and improved the efficiency of Cl<sub>2</sub>/NaClO generation. The system was integrated into a custom flow-through reactor, achieving 97.0% degradation efficiency for 50 ppm ciprofloxacin within 2 min over 20 cycles in simulated tap water. These results establish a scalable platform for dual oxidant electrosynthesis and efficient pollutant removal, demonstrating that PED combined with interlayer engineering provides an effective design strategy for high-performance SnO<sub>2</sub>-based electrocatalysts in environmental remediation.","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":"146138347","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.2026.173953
Jinshan Liu, Yingying Chen, Miao Zhou, Zhifeng Liu
Plagued by the critical issues of ion leaching and a scarcity of active sites, nickel ferrite (NiFe2O4) catalysts exhibit significantly compromised catalytic performance for the Urea Oxidation Reaction (UOR), consequently curtailing their prospects for practical implementation. In this study, a designed Vo-NiFe1.93Al0.07O4 catalyst system was synthesized for UOR. It features both Al-driven FeO bond strengthening (to alleviate Fe3+ leaching) and oxygen vacancy (Vo) mediation. The synergistic effect arising from these modifications not only substantially strengthens the structural stability of catalyst but also remarkably accelerates the electrochemical reaction kinetics of UOR. Benefiting from this synergistic enhancement, the Vo-NiFe1.93Al0.07O4 catalyst thus delivers exceptional UOR performance, requiring only 158 mV to achieve 100 mA cm−2, a substantial improvement over the 494 mV needed for NiFe2O4. Furthermore, density functional theory (DFT) calculations reveal that the successful incorporation of Al significantly enhances the hybridization between the d-orbitals of Fe and p-orbitals of O, which notably improves the electronic delocalization between metal active sites and oxygen species, and accelerates the charge transfer process in the catalytic reaction. The prominent performances endow Vo-NiFe1.93Al0.07O4 with great promise for applications in UOR-based clean energy conversion.
{"title":"Synergistic Al-induced stabilization of FeO bonds to mitigate Fe3+ leaching and oxygen vacancy for enhanced urea oxidation catalysis","authors":"Jinshan Liu, Yingying Chen, Miao Zhou, Zhifeng Liu","doi":"10.1016/j.cej.2026.173953","DOIUrl":"https://doi.org/10.1016/j.cej.2026.173953","url":null,"abstract":"Plagued by the critical issues of ion leaching and a scarcity of active sites, nickel ferrite (NiFe<sub>2</sub>O<sub>4</sub>) catalysts exhibit significantly compromised catalytic performance for the Urea Oxidation Reaction (UOR), consequently curtailing their prospects for practical implementation. In this study, a designed V<sub>o</sub>-NiFe<sub>1.93</sub>Al<sub>0.07</sub>O<sub>4</sub> catalyst system was synthesized for UOR. It features both Al-driven Fe<img alt=\"single bond\" src=\"https://sdfestaticassets-us-east-1.sciencedirectassets.com/shared-assets/55/entities/sbnd.gif\" style=\"vertical-align:middle\"/>O bond strengthening (to alleviate Fe<sup>3+</sup> leaching) and oxygen vacancy (V<sub>o</sub>) mediation. The synergistic effect arising from these modifications not only substantially strengthens the structural stability of catalyst but also remarkably accelerates the electrochemical reaction kinetics of UOR. Benefiting from this synergistic enhancement, the V<sub>o</sub>-NiFe<sub>1.93</sub>Al<sub>0.07</sub>O<sub>4</sub> catalyst thus delivers exceptional UOR performance, requiring only 158 mV to achieve 100 mA cm<sup>−2</sup>, a substantial improvement over the 494 mV needed for NiFe<sub>2</sub>O<sub>4</sub>. Furthermore, density functional theory (DFT) calculations reveal that the successful incorporation of Al significantly enhances the hybridization between the d-orbitals of Fe and p-orbitals of O, which notably improves the electronic delocalization between metal active sites and oxygen species, and accelerates the charge transfer process in the catalytic reaction. The prominent performances endow V<sub>o</sub>-NiFe<sub>1.93</sub>Al<sub>0.07</sub>O<sub>4</sub> with great promise for applications in UOR-based clean energy conversion.","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":"146138316","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}
Strong enamel adhesion remains a challenging task in dental restoration, as light-curable methacrylate-based adhesives forms bonding interfaces through micro-mechanical interlocking by penetrating into the enamel rod gaps. The lack of sufficiently strong chemical bonding renders the adhesive interface vulnerable to integrity failure induced by polymerization stress, bacterial infiltration and material degradation. Herein, a methacrylate monomer grafted with alkoxysilane groups is developed. The sol-gel reaction of the silane moieties enables chemical bonding with hydroxyapatite in enamel, while simultaneously improving the hydrophobicity of the adhesive to enhance bonding performance. The silane-grafted monomer (Sil-BisGMA) is synthesized by reacting the two hydroxyl groups of bisphenol A glycidyl methacrylate (BisGMA) with (3-isocyanatopropyl) trimethoxysilane (IPTMS), and is subsequently used to partially or completely replace BisGMA in composite adhesive formulations. The results demonstrate that the Sil-BisGMA-formulated adhesives exhibit significantly improved performance compared with conventional BisGMA-based counterpart in terms of mechanical properties, water contact angle, surface hardness, and solvent resistance. Moreover, the incorporation of Sil-BisGMA effectively enhances the instant shear bonding strengths to enamel for various dental restorative substrates, including orthodontic metal brackets, composite resins, and glass-ceramics, by 1.62, 2.07 and 1.50 times, respectively. In addition, the good biocompatibility of the Sil-BisGMA-based adhesives is confirmed through both in vitro and in vivo evaluations. Taken together, these results indicate that the Sil-BisGMA monomer, featuring dual reactivity (light-curable polymerization and chemical bonding capability), can serve as a novel functional monomer for the development of enamel adhesives with improved bonding performance and extended restoration durability, demonstrating strong potential for clinical application.
{"title":"Silane-grafted BisGMA enables dual-bonding strategy for enhanced enamel adhesive bonding strength","authors":"Daixing Zhang, Yanyun Pang, Xinyi Huang, Yingjie Yu, Xiaoping Yang, Qing Cai","doi":"10.1016/j.cej.2026.173936","DOIUrl":"https://doi.org/10.1016/j.cej.2026.173936","url":null,"abstract":"Strong enamel adhesion remains a challenging task in dental restoration, as light-curable methacrylate-based adhesives forms bonding interfaces through micro-mechanical interlocking by penetrating into the enamel rod gaps. The lack of sufficiently strong chemical bonding renders the adhesive interface vulnerable to integrity failure induced by polymerization stress, bacterial infiltration and material degradation. Herein, a methacrylate monomer grafted with alkoxysilane groups is developed. The sol-gel reaction of the silane moieties enables chemical bonding with hydroxyapatite in enamel, while simultaneously improving the hydrophobicity of the adhesive to enhance bonding performance. The silane-grafted monomer (Sil-BisGMA) is synthesized by reacting the two hydroxyl groups of bisphenol A glycidyl methacrylate (BisGMA) with (3-isocyanatopropyl) trimethoxysilane (IPTMS), and is subsequently used to partially or completely replace BisGMA in composite adhesive formulations. The results demonstrate that the Sil-BisGMA-formulated adhesives exhibit significantly improved performance compared with conventional BisGMA-based counterpart in terms of mechanical properties, water contact angle, surface hardness, and solvent resistance. Moreover, the incorporation of Sil-BisGMA effectively enhances the instant shear bonding strengths to enamel for various dental restorative substrates, including orthodontic metal brackets, composite resins, and glass-ceramics, by 1.62, 2.07 and 1.50 times, respectively. In addition, the good biocompatibility of the Sil-BisGMA-based adhesives is confirmed through both <em>in vitro</em> and <em>in vivo</em> evaluations. Taken together, these results indicate that the Sil-BisGMA monomer, featuring dual reactivity (light-curable polymerization and chemical bonding capability), can serve as a novel functional monomer for the development of enamel adhesives with improved bonding performance and extended restoration durability, demonstrating strong potential for clinical application.","PeriodicalId":270,"journal":{"name":"Chemical Engineering Journal","volume":"182 1","pages":""},"PeriodicalIF":15.1,"publicationDate":"2026-02-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146138315","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}
The practical application of wood-based materials in sustainable triboelectric nanogenerators (TENGs) is constrained by their mechanical weakness, poor environmental tolerance, and insufficient electrical output. Incorporating functional polymers offers potential for enhancing wood-based substrates, yet weak interfacial bonding often undermines structural stability. Herein, we develop an optimized wood-based substrate (WS) featuring superior mechanical toughness, water resistance, and transparency by constructing the biomimetic hierarchical structures. The filler matrix, engineered with reactive isocyanate groups, enables the formation of stable covalent bonds at hierarchical interfaces, thereby achieving exceptional mechanical toughness (3.38 MJ/m3), water resistance, and a high dielectric constant (5.33). Leveraging these properties, the WS serves as a sustainable substrate for a rotary TENG, enabling efficient wind and water flow energy harvesting, and achieving a significantly enhanced peak power density (300.7 mW/m2) compared with most of the reported wood-based TENGs. This work opens up new avenues for designing next-generation wood-based TENGs for efficient green energy harvesting.
{"title":"Biomimetic hierarchical structure enabled mechanical toughness, water-resistant wood-based substrate for high-performance triboelectric nanogenerator","authors":"Qianqian Jia, Yupeng Liu, Caoxing Huang, Shishuai Gao, Daihui Zhang, Jifu Wang, Chunpeng Wang, Qiang Yong, Fuxiang Chu, Chuanwei Lu","doi":"10.1016/j.cej.2026.173861","DOIUrl":"https://doi.org/10.1016/j.cej.2026.173861","url":null,"abstract":"The practical application of wood-based materials in sustainable triboelectric nanogenerators (TENGs) is constrained by their mechanical weakness, poor environmental tolerance, and insufficient electrical output. Incorporating functional polymers offers potential for enhancing wood-based substrates, yet weak interfacial bonding often undermines structural stability. Herein, we develop an optimized wood-based substrate (WS) featuring superior mechanical toughness, water resistance, and transparency by constructing the biomimetic hierarchical structures. The filler matrix, engineered with reactive isocyanate groups, enables the formation of stable covalent bonds at hierarchical interfaces, thereby achieving exceptional mechanical toughness (3.38 MJ/m<sup>3</sup>), water resistance, and a high dielectric constant (5.33). Leveraging these properties, the WS serves as a sustainable substrate for a rotary TENG, enabling efficient wind and water flow energy harvesting, and achieving a significantly enhanced peak power density (300.7 mW/m<sup>2</sup>) compared with most of the reported wood-based TENGs. This work opens up new avenues for designing next-generation wood-based TENGs for efficient green energy harvesting.","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":"146138343","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.2026.173841
Lu Song, Zhi-Kun Luo, Fu-Cheng He, Lan-Ya Huang, Liang-Bin Xiong, Yong-Jun Liu, Dong-Zhi Wei, Feng-Qing Wang
The structural properties of starting materials decisively govern industrial synthesis pathways for pharmaceutical steroids. Tigogenin, an economical and abundant byproduct from sisal fiber processing, exhibits substantial potential for steroid production. However, its industrial utility is limited by its saturated A-ring structure and environmentally detrimental application processes. To address these challenges, we developed an integrated chemoenzymatic pathway. First, tigogenin extracted from sisal residue was converted to 3β-hydroxy-5α-pregnane-16-ene-20-one (3β-HP) via H₂O₂ degradation, a green alternative to Marker degradation. This was followed by efficient biotransformation to 5α-pregnane-16-ene-3,20-dione (5α-PD, >95% yield) using Streptomyces lividans TK24-152 instead of conventional Oppenauer oxidation, thereby eliminating toxic metal catalysts (CrO₃ and aluminum tert-butoxide) in these traditional reaction processes. To selectively functionalize the A-ring of 5α-PD, 3-ketosteroid-Δ4-dehydrogenase (Kst4D) and 3-ketosteroid-Δ1-dehydrogenase (Kst1D) were screened, engineered, and incorporated into S. lividans TK24-152. This generated strains (Rj4K, ReK3, and Rj4K-MnK2A395G) capable of converting 3β-HP via 5α-PD to Δ4,16(17)-diene-progesterone (4-PG), Δ1,16(17)-diene-progesterone (1-PG), and Δ1,4,16(17)-triene-progesterone (1,4-PG), respectively. To resolve bioavailability limitations of water-insoluble 3β-HP during scale-up, an emulsification system (3β-HP: Tween 80: HPCD = 10: 1: 20, w/w) was optimized. In 5 L fermenters, strains Rj4K and Rj4K-MnK2A395G demonstrated exceptional performance, achieving molar yields of 92.4% (from 20 g/L 3β-HP) and 82.2% (from 40 g/L 3β-HP) for 4-PG, and 86.7% (from 20 g/L 3β-HP) and 68.9% (from 40 g/L 3β-HP) for 1,4-PG. The overall tigogenin-to-product yields achieved 56.8–63.9% (for 4-PG) and 47.7–60.0% (for 1,4-PG), outperforming traditional diosgenin-based routes. In summary, this study establishes a sustainable chemoenzymatic strategy for steroid synthesis, enabling waste utilization while replacing hazardous reagents, with demonstrated industrial and environmental benefits.
{"title":"Green upcycling of tigogenin from sisal waste: Chemoenzymatic cascade synthesis of progesterone derivatives as an alternative to traditional steroid production processes","authors":"Lu Song, Zhi-Kun Luo, Fu-Cheng He, Lan-Ya Huang, Liang-Bin Xiong, Yong-Jun Liu, Dong-Zhi Wei, Feng-Qing Wang","doi":"10.1016/j.cej.2026.173841","DOIUrl":"https://doi.org/10.1016/j.cej.2026.173841","url":null,"abstract":"The structural properties of starting materials decisively govern industrial synthesis pathways for pharmaceutical steroids. Tigogenin, an economical and abundant byproduct from sisal fiber processing, exhibits substantial potential for steroid production. However, its industrial utility is limited by its saturated A-ring structure and environmentally detrimental application processes. To address these challenges, we developed an integrated chemoenzymatic pathway. First, tigogenin extracted from sisal residue was converted to 3β-hydroxy-5α-pregnane-16-ene-20-one (3β-HP) via H₂O₂ degradation, a green alternative to Marker degradation. This was followed by efficient biotransformation to 5α-pregnane-16-ene-3,20-dione (5α-PD, >95% yield) using <em>Streptomyces lividans</em> TK24-152 instead of conventional Oppenauer oxidation, thereby eliminating toxic metal catalysts (CrO₃ and aluminum tert-butoxide) in these traditional reaction processes. To selectively functionalize the A-ring of 5α-PD, 3-ketosteroid-Δ<sup>4</sup>-dehydrogenase (Kst4D) and 3-ketosteroid-Δ<sup>1</sup>-dehydrogenase (Kst1D) were screened, engineered, and incorporated into <em>S. lividans</em> TK24-152. This generated strains (Rj4K, ReK3, and Rj4K-MnK2<sup>A395G</sup>) capable of converting 3β-HP via 5α-PD to Δ<sup>4,16(17)</sup>-diene-progesterone (4-PG), Δ<sup>1,16(17)</sup>-diene-progesterone (1-PG), and Δ<sup>1,4,16(17)</sup>-triene-progesterone (1,4-PG), respectively. To resolve bioavailability limitations of water-insoluble 3β-HP during scale-up, an emulsification system (3β-HP: Tween 80: HPCD = 10: 1: 20, <em>w</em>/w) was optimized. In 5 L fermenters, strains Rj4K and Rj4K-MnK2<sup>A395G</sup> demonstrated exceptional performance, achieving molar yields of 92.4% (from 20 g/L 3β-HP) and 82.2% (from 40 g/L 3β-HP) for 4-PG, and 86.7% (from 20 g/L 3β-HP) and 68.9% (from 40 g/L 3β-HP) for 1,4-PG. The overall tigogenin-to-product yields achieved 56.8–63.9% (for 4-PG) and 47.7–60.0% (for 1,4-PG), outperforming traditional diosgenin-based routes. In summary, this study establishes a sustainable chemoenzymatic strategy for steroid synthesis, enabling waste utilization while replacing hazardous reagents, with demonstrated industrial and environmental benefits.","PeriodicalId":270,"journal":{"name":"Chemical Engineering Journal","volume":"73 1","pages":""},"PeriodicalIF":15.1,"publicationDate":"2026-02-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146138344","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 : 2026-02-08DOI: 10.1016/j.cej.2026.173933
Michael Rebarchik, Manos Mavrikakis
Single-atom catalysts supported on metal oxides have been demonstrated to exhibit exceptional activity while also maintaining single-atom stability. However, alternative supports such as metal nitrides and carbides have received far less attention. Herein, we use density functional theory to systematically investigate the relative thermal stability of single-atom catalysts over a host of transition metal nitride and carbide supports. By considering the binding and dimerization energies of isolated transition metal atoms across various surface facets, we identify transition metal/support pairs that show the most promise for high-density single-atom catalysts. We find that transition metal atoms can be stabilized on both defect sites and pristine surfaces over transition metal nitrides and carbides and identify promising metal/support pairings that may be suitable for achieving both stable and high-density single-atom catalysts. These results provide valuable insights to guide synthesis efforts towards achieving stable single-atom transition metal catalysts.
{"title":"Assessing metal nitrides and metal carbides as supports for thermally stable single-atom catalysts","authors":"Michael Rebarchik, Manos Mavrikakis","doi":"10.1016/j.cej.2026.173933","DOIUrl":"https://doi.org/10.1016/j.cej.2026.173933","url":null,"abstract":"Single-atom catalysts supported on metal oxides have been demonstrated to exhibit exceptional activity while also maintaining single-atom stability. However, alternative supports such as metal nitrides and carbides have received far less attention. Herein, we use density functional theory to systematically investigate the relative thermal stability of single-atom catalysts over a host of transition metal nitride and carbide supports. By considering the binding and dimerization energies of isolated transition metal atoms across various surface facets, we identify transition metal/support pairs that show the most promise for high-density single-atom catalysts. We find that transition metal atoms can be stabilized on both defect sites and pristine surfaces over transition metal nitrides and carbides and identify promising metal/support pairings that may be suitable for achieving both stable and high-density single-atom catalysts. These results provide valuable insights to guide synthesis efforts towards achieving stable single-atom transition metal catalysts.","PeriodicalId":270,"journal":{"name":"Chemical Engineering Journal","volume":"18 1","pages":""},"PeriodicalIF":15.1,"publicationDate":"2026-02-08","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146138346","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}
The construction of an environmentally responsive bactericidal platform enables intelligent and synergistic regulation of bacterial diseases. A pH-responsive pesticide nano delivery system (ZnO@PDA-KAS) was prepared by self-polymerizing a polydopamine (PDA) coating on the surface of ZnO nanospheres synthesized via a hydrothermal method, followed by conjugation with kasugamycin (KAS) in this work. The results showed that ZnO@PDA-KAS exhibited excellent cumulative release under acidic conditions, with a pesticide loading content of 9.4%. The presence of PDA significantly enhanced the adhesion and retention of nanoparticles on rice leaves, whereas fluorescein isothiocyanate-labeled ZnO@PDA exhibited good translocation capacity in rice plants. Moreover, the PDA coating effectively improved the photostability of KAS. In vivo and in vitro antibacterial tests demonstrated that ZnO@PDA-KAS displayed superior antibacterial activity against Xanthomonas oryzae pv. Oryzicola (Xoc) due to the synergistic antibacterial effects of Zn2+ and KAS. This enhanced activity was attributed to the nanoparticles' ability to severely damage bacterial microstructures, enhance rice enzyme activity, and more effectively inhibition of bacterial biofilm formation and induced more severe DNA damage in Xoc cells. Finally, the ZnO@PDA-KAS nanoparticles showed excellent biocompatibility with rice plants and L02 cells. Therefore, the environmentally responsive bactericide ZnO@PDA-KAS provides effective agricultural guidance for efficient and precise release for the management of bacterial plant diseases.
{"title":"Fabrication of a pH-responsive nanodelivery platform based on ZnO and kasugamycin for synergistic delivery in the efficient and green management of rice bacterial leaf streak","authors":"Shaoyang Sun, Xiang Li, Ziyi Wu, Ze Lv, Yingjian Ma, Rui Zhao, Xinyu Guo, Jianguo Feng, Xuemin Wu, Yong Xu","doi":"10.1016/j.cej.2026.173899","DOIUrl":"https://doi.org/10.1016/j.cej.2026.173899","url":null,"abstract":"The construction of an environmentally responsive bactericidal platform enables intelligent and synergistic regulation of bacterial diseases. A pH-responsive pesticide nano delivery system (ZnO@PDA-KAS) was prepared by self-polymerizing a polydopamine (PDA) coating on the surface of ZnO nanospheres synthesized via a hydrothermal method, followed by conjugation with kasugamycin (KAS) in this work. The results showed that ZnO@PDA-KAS exhibited excellent cumulative release under acidic conditions, with a pesticide loading content of 9.4%. The presence of PDA significantly enhanced the adhesion and retention of nanoparticles on rice leaves, whereas fluorescein isothiocyanate-labeled ZnO@PDA exhibited good translocation capacity in rice plants. Moreover, the PDA coating effectively improved the photostability of KAS. In vivo and in vitro antibacterial tests demonstrated that ZnO@PDA-KAS displayed superior antibacterial activity against <em>Xanthomonas oryzae pv. Oryzicola</em> (<em>Xoc</em>) due to the synergistic antibacterial effects of Zn<sup>2+</sup> and KAS. This enhanced activity was attributed to the nanoparticles' ability to severely damage bacterial microstructures, enhance rice enzyme activity, and more effectively inhibition of bacterial biofilm formation and induced more severe DNA damage in <em>Xoc</em> cells. Finally, the ZnO@PDA-KAS nanoparticles showed excellent biocompatibility with rice plants and L02 cells. Therefore, the environmentally responsive bactericide ZnO@PDA-KAS provides effective agricultural guidance for efficient and precise release for the management of bacterial plant diseases.","PeriodicalId":270,"journal":{"name":"Chemical Engineering Journal","volume":"92 1","pages":""},"PeriodicalIF":15.1,"publicationDate":"2026-02-08","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146138348","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 bond strengthening (to alleviate Fe3+ leaching) and oxygen vacancy (Vo) mediation. The synergistic effect arising from these modifications not only substantially strengthens the structural stability of catalyst but also remarkably accelerates the electrochemical reaction kinetics of UOR. Benefiting from this synergistic enhancement, the Vo-NiFe1.93Al0.07O4 catalyst thus delivers exceptional UOR performance, requiring only 158 mV to achieve 100 mA cm−2, a substantial improvement over the 494 mV needed for NiFe2O4. Furthermore, density functional theory (DFT) calculations reveal that the successful incorporation of Al significantly enhances the hybridization between the d-orbitals of Fe and p-orbitals of O, which notably improves the electronic delocalization between metal active sites and oxygen species, and accelerates the charge transfer process in the catalytic reaction. The prominent performances endow Vo-NiFe1.93Al0.07O4 with great promise for applications in UOR-based clean energy conversion.
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