Silicon (Si) has been widely accepted as a promising anode material owing to its high theoretical capacity (3590 mAh g–1) and abundance. Nevertheless, its practical application in next-generation batteries has long been hindered by several inherent challenges, including an unstable solid-electrolyte interphase (SEI), large volume changes, and low electrical conductivity. Herein, a facile and effective chemical route is proposed to construct a functional organic molecule that could constrain the framework and tune the interfacial properties of Si/C electrodes. Superior electrochemical performance with high anode material loading (∼8.0 mg cm–2) and high areal capacity (above 3.0 mAh cm–2) is achieved for the Si/C anode in terms of excellent cycling stability. A unique interfacial anchoring mechanism is found that plays a major role in effectively alleviating the huge volume expansion and maintaining the integrity of the Si/C electrode. Moreover, an investigation of the surface chemistry confirms that the constructed molecule can improve the stability of the SEI by promoting the formation of a LiF-rich interphase. Our findings provide deep insights into the design of high-performance Si/C anodes for practical applications in next-generation batteries.
硅(Si)由于其高理论容量(3590 mAh g-1)和丰度而被广泛认为是一种有前途的阳极材料。然而,它在下一代电池中的实际应用一直受到一些固有挑战的阻碍,包括不稳定的固体电解质界面(SEI)、大体积变化和低导电性。本文提出了一种简单有效的化学途径来构建一个功能有机分子,该有机分子可以约束Si/C电极的框架并调节其界面性质。优异的电化学性能,高负极材料负载(~ 8.0 mg cm-2)和高面积容量(大于3.0 mAh cm-2),为Si/C阳极实现了优异的循环稳定性。发现了一种独特的界面锚定机制,对有效缓解Si/C电极的巨大体积膨胀和保持其完整性起着重要作用。此外,对表面化学的研究证实,构建的分子可以通过促进富liff间相的形成来提高SEI的稳定性。我们的研究结果为下一代电池中实际应用的高性能Si/C阳极的设计提供了深刻的见解。
{"title":"Interfacial Anchoring Effect Enables a Stable and High-Areal-Capacity Silicon/Carbon Composite Anode","authors":"Yipeng Sun, Jinjin Ma, Xiaoting Lin, Haoqi Ren, Weihan Li, Changhong Wang, Tsun-Kong Sham, Xueliang Sun","doi":"10.1021/acssuschemeng.5c13091","DOIUrl":"https://doi.org/10.1021/acssuschemeng.5c13091","url":null,"abstract":"Silicon (Si) has been widely accepted as a promising anode material owing to its high theoretical capacity (3590 mAh g<sup>–1</sup>) and abundance. Nevertheless, its practical application in next-generation batteries has long been hindered by several inherent challenges, including an unstable solid-electrolyte interphase (SEI), large volume changes, and low electrical conductivity. Herein, a facile and effective chemical route is proposed to construct a functional organic molecule that could constrain the framework and tune the interfacial properties of Si/C electrodes. Superior electrochemical performance with high anode material loading (∼8.0 mg cm<sup>–2</sup>) and high areal capacity (above 3.0 mAh cm<sup>–2</sup>) is achieved for the Si/C anode in terms of excellent cycling stability. A unique interfacial anchoring mechanism is found that plays a major role in effectively alleviating the huge volume expansion and maintaining the integrity of the Si/C electrode. Moreover, an investigation of the surface chemistry confirms that the constructed molecule can improve the stability of the SEI by promoting the formation of a LiF-rich interphase. Our findings provide deep insights into the design of high-performance Si/C anodes for practical applications in next-generation batteries.","PeriodicalId":25,"journal":{"name":"ACS Sustainable Chemistry & Engineering","volume":"23 1","pages":""},"PeriodicalIF":8.4,"publicationDate":"2026-02-04","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146115822","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2026-02-04DOI: 10.1021/acssuschemeng.5c13600
Dumitru Moraru, Giacomo Trapasso, Davide Dalla Torre, Thomas Griesser, Fabio Aricò, Marco Sangermano
The present work reports for the first time thiol–yne photoresins prepared from novel alkyne derivatives of isosorbide and its epimers, isomannide and isoidide. Isosorbide was selected as a key biobased monomer for this study in consideration of its unique rigid V-shaped structure and peculiar reactivity, as well as for the growing interest in this cyclic sugar due to its numerous industrial applications in polymer science. Dialkyl carbonate chemistry was used for the preparation of dipropargyl derivatives of isosorbide and its epimers via alkoxycarbonylation reaction conducted under mild conditions using catalytic amounts of 1,5,7-triazabicyclo[4.4.0]dec-5-ene (TBD). Dialkyne monomers were then employed to produce biobased thiol–yne photoresins, formulated using trimethylolpropane tris(3-mercaptopropionate) as a trifunctional thiol. The photopolymerization behavior was investigated by real-time Fourier-transform infrared spectroscopy and differential scanning calorimetry (DSC) to assess conversion efficiency and reaction kinetics. The resulting networks were characterized by DSC and dynamic mechanical thermal analysis. Furthermore, residual thiol groups enabled surface modification with poly(ethylene glycol) methacrylate (PEGMA) to enhance hydrophilicity, as confirmed by contact angle measurements. Finally, the optimized isosorbide-based network formulation was successfully printed by digital light processing, achieving accurate 3D-printed structures.
{"title":"Thiol–Yne Photocurable Isosorbide-Derived Networks: Formulation and 3D Printing","authors":"Dumitru Moraru, Giacomo Trapasso, Davide Dalla Torre, Thomas Griesser, Fabio Aricò, Marco Sangermano","doi":"10.1021/acssuschemeng.5c13600","DOIUrl":"https://doi.org/10.1021/acssuschemeng.5c13600","url":null,"abstract":"The present work reports for the first time thiol–yne photoresins prepared from novel alkyne derivatives of isosorbide and its epimers, isomannide and isoidide. Isosorbide was selected as a key biobased monomer for this study in consideration of its unique rigid V-shaped structure and peculiar reactivity, as well as for the growing interest in this cyclic sugar due to its numerous industrial applications in polymer science. Dialkyl carbonate chemistry was used for the preparation of dipropargyl derivatives of isosorbide and its epimers via alkoxycarbonylation reaction conducted under mild conditions using catalytic amounts of 1,5,7-triazabicyclo[4.4.0]dec-5-ene (TBD). Dialkyne monomers were then employed to produce biobased thiol–yne photoresins, formulated using trimethylolpropane tris(3-mercaptopropionate) as a trifunctional thiol. The photopolymerization behavior was investigated by real-time Fourier-transform infrared spectroscopy and differential scanning calorimetry (DSC) to assess conversion efficiency and reaction kinetics. The resulting networks were characterized by DSC and dynamic mechanical thermal analysis. Furthermore, residual thiol groups enabled surface modification with poly(ethylene glycol) methacrylate (PEGMA) to enhance hydrophilicity, as confirmed by contact angle measurements. Finally, the optimized isosorbide-based network formulation was successfully printed by digital light processing, achieving accurate 3D-printed structures.","PeriodicalId":25,"journal":{"name":"ACS Sustainable Chemistry & Engineering","volume":"34 1","pages":""},"PeriodicalIF":8.4,"publicationDate":"2026-02-04","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146115823","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2026-02-04DOI: 10.1021/acssuschemeng.5c12258
Bo Jiang, Chengyang Du, Chuchu Chen, Xinyu Guo, Wenjuan Wu, Chaofeng Zhang, Sehrish Manan, Yongcan Jin, Zhiqiang Liang
Visible-light-driven TiO2 photocatalysts are attractive for energy and environment applications, yet the currently developed TiO2 photocatalysts generally feature a wide band gap, activation solely to UV wavelength, and rapid charge carrier recombination. Herein, inspired by the light absorption strategy of the plant structure, a vertically aligned multiscale photocatalyst based on 3D printing is developed, where the carbonized lignin/TiO2 pillars, TiO2 nanorods, and Pd nanoparticles serve as tree trunks, branches, and leaves, respectively. The hierarchical photocatalyst composed of Pd/C and anatase/rutile-type TiO2 heterojunction not only exhibits a high specific surface area (592.23 m2·g–1) for multiple light scattering but also expands the UV activation region into the visible light spectrum, with the visible light absorption over 80% and the work function as low as 2.81 eV, which can highly promote the mass transfer for surface/interface reaction under visible light. As a proof of concept, the photocatalyst demonstrates an outstanding photocatalytic nitro-hydrogenation performance to industrial concentrated 4-nitrophenol (2.0 g·L–1), with the turnover frequency up to ∼16.0 mol4-NP·mol–1·min–1, and no obvious deterioration is observed even after 10 cycles. This study provides a facile and scalable 3D printing strategy to promote the light-harvesting capacity of TiO2 for efficient solar energy utilization and sustainable environment engineering.
{"title":"Vertically Aligned Multiscale Heterojunction Arrays via 3D Printing for Efficient Photocatalytic Nitro-Hydrogenation","authors":"Bo Jiang, Chengyang Du, Chuchu Chen, Xinyu Guo, Wenjuan Wu, Chaofeng Zhang, Sehrish Manan, Yongcan Jin, Zhiqiang Liang","doi":"10.1021/acssuschemeng.5c12258","DOIUrl":"https://doi.org/10.1021/acssuschemeng.5c12258","url":null,"abstract":"Visible-light-driven TiO<sub>2</sub> photocatalysts are attractive for energy and environment applications, yet the currently developed TiO<sub>2</sub> photocatalysts generally feature a wide band gap, activation solely to UV wavelength, and rapid charge carrier recombination. Herein, inspired by the light absorption strategy of the plant structure, a vertically aligned multiscale photocatalyst based on 3D printing is developed, where the carbonized lignin/TiO<sub>2</sub> pillars, TiO<sub>2</sub> nanorods, and Pd nanoparticles serve as tree trunks, branches, and leaves, respectively. The hierarchical photocatalyst composed of Pd/C and anatase/rutile-type TiO<sub>2</sub> heterojunction not only exhibits a high specific surface area (592.23 m<sup>2</sup>·g<sup>–1</sup>) for multiple light scattering but also expands the UV activation region into the visible light spectrum, with the visible light absorption over 80% and the work function as low as 2.81 eV, which can highly promote the mass transfer for surface/interface reaction under visible light. As a proof of concept, the photocatalyst demonstrates an outstanding photocatalytic nitro-hydrogenation performance to industrial concentrated 4-nitrophenol (2.0 g·L<sup>–1</sup>), with the turnover frequency up to ∼16.0 mol<sub>4-NP</sub>·mol<sup>–1</sup>·min<sup>–1</sup>, and no obvious deterioration is observed even after 10 cycles. This study provides a facile and scalable 3D printing strategy to promote the light-harvesting capacity of TiO<sub>2</sub> for efficient solar energy utilization and sustainable environment engineering.","PeriodicalId":25,"journal":{"name":"ACS Sustainable Chemistry & Engineering","volume":"46 1","pages":""},"PeriodicalIF":8.4,"publicationDate":"2026-02-04","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146116271","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Methane oxidative coupling (OCM) based on the chemical-looping (CL) concept represents a promising pathway for the high-value upgrading of methane; however, commercialization is hindered by low olefin yields and deactivation of the oxygen carrier. In this study, we demonstrate that CO2 assistance significantly improves the performance of Li2CO3-promoted perovskite oxygen carriers in CL-OCM. The methane conversion increases from 22.7% to 30% and C2 selectivity increases from 50% to 89.6% when 10% of CO2 was introduced, while maintaining stable performance over 50 consecutive cycles. The presence of CO2 stabilizes the crystalline phase of the oxygen carrier. By maintaining the lattice oxygen concentration via a synergistic oxygen replenishment mechanism, the oxygen carrier achieves enhanced and durable catalytic activity. 13C isotopic labeling experiments elucidate the conversion pathways of CH4 and CO2, and 18O isotope tracing further confirms a surface lattice-oxygen exchange mechanism between CO2 and the oxygen carrier. These findings provide a viable strategy for advancing the commercialization of OCM and enabling the efficient synergistic utilization of CH4 and CO2.
{"title":"Enhanced Oxidative Coupling of CH4 to Olefins via CO2 Assistance over Alkali Metal-Supported Perovskite","authors":"Chenkai Sun, Yuxuan Xu, Junming Liang, Anqing Zheng, Zengli Zhao, Fang He, Kun Zhao","doi":"10.1021/acssuschemeng.5c11616","DOIUrl":"https://doi.org/10.1021/acssuschemeng.5c11616","url":null,"abstract":"Methane oxidative coupling (OCM) based on the chemical-looping (CL) concept represents a promising pathway for the high-value upgrading of methane; however, commercialization is hindered by low olefin yields and deactivation of the oxygen carrier. In this study, we demonstrate that CO<sub>2</sub> assistance significantly improves the performance of Li<sub>2</sub>CO<sub>3</sub>-promoted perovskite oxygen carriers in CL-OCM. The methane conversion increases from 22.7% to 30% and C<sub>2</sub> selectivity increases from 50% to 89.6% when 10% of CO<sub>2</sub> was introduced, while maintaining stable performance over 50 consecutive cycles. The presence of CO<sub>2</sub> stabilizes the crystalline phase of the oxygen carrier. By maintaining the lattice oxygen concentration via a synergistic oxygen replenishment mechanism, the oxygen carrier achieves enhanced and durable catalytic activity. <sup>13</sup>C isotopic labeling experiments elucidate the conversion pathways of CH<sub>4</sub> and CO<sub>2</sub>, and <sup>18</sup>O isotope tracing further confirms a surface lattice-oxygen exchange mechanism between CO<sub>2</sub> and the oxygen carrier. These findings provide a viable strategy for advancing the commercialization of OCM and enabling the efficient synergistic utilization of CH<sub>4</sub> and CO<sub>2</sub>.","PeriodicalId":25,"journal":{"name":"ACS Sustainable Chemistry & Engineering","volume":"5 1","pages":""},"PeriodicalIF":8.4,"publicationDate":"2026-02-03","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146101990","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2026-02-03DOI: 10.1021/acssuschemeng.5c08192
Aqsa Arooj, Bi-Long Chen, Yi-Ting Hu, Ting-Ting Zhang, Md Sohrab Ali, Zhiqiang Zhao, Yu-Ming Zheng, Jia-Cheng E. Yang
Converting organic wastes into clean energy is vital to the development of sustainable urban and zero/low-carbon communities but is challenging to achieve because of inefficient electron flux between acidogens and methanogens. Inspired by the unique electron configuration of Fe–S clusters in ferredoxin and their electron–proton transfer function in methanogenesis, we designed biologically adaptive micro/nanostructured multivalent iron carbon ensembles (mNICE) as cell synthesis accelerators, in which the high-spin Fe(III) sites would serve as biomimetic biological centers to directionally activate the key enzymes of methanogenesis. Upon successfully constructing mNICE-oriented real syntrophic microbial consortia, mNICE were found to dynamically buffer the acidogenic electrons and establish a directional electron transport chain between acidogens and methanogens. These roles subsequently synchronized proton flux via accelerating the regeneration of F420H2 and CoM–SH/CoB–SH via activating the critical F420 hydrogenase and heterodisulfide reductase. Such biotic-abiotic interfacial interactions between mNICE and syntrophic multicellular communities sustained organic-loading rates via improving the degradation of volatile fatty acids and retarding their toxicity to methanogens. As a result, mNICE elevated the methane yield by 134.20%. This work highlights the importance of steering the activity of key enzymes across the cell-material interface in the development of sustainable waste-to-energy conversion systems.
{"title":"Micro/Nanostructured Multivalent Iron Carbonaceous Ensembles Amplified the Methanogenesis of Syntrophic Microbial Cells","authors":"Aqsa Arooj, Bi-Long Chen, Yi-Ting Hu, Ting-Ting Zhang, Md Sohrab Ali, Zhiqiang Zhao, Yu-Ming Zheng, Jia-Cheng E. Yang","doi":"10.1021/acssuschemeng.5c08192","DOIUrl":"https://doi.org/10.1021/acssuschemeng.5c08192","url":null,"abstract":"Converting organic wastes into clean energy is vital to the development of sustainable urban and zero/low-carbon communities but is challenging to achieve because of inefficient electron flux between acidogens and methanogens. Inspired by the unique electron configuration of Fe–S clusters in ferredoxin and their electron–proton transfer function in methanogenesis, we designed biologically adaptive micro/nanostructured multivalent iron carbon ensembles (mNICE) as cell synthesis accelerators, in which the high-spin Fe(III) sites would serve as biomimetic biological centers to directionally activate the key enzymes of methanogenesis. Upon successfully constructing mNICE-oriented real syntrophic microbial consortia, mNICE were found to dynamically buffer the acidogenic electrons and establish a directional electron transport chain between acidogens and methanogens. These roles subsequently synchronized proton flux via accelerating the regeneration of F<sub>420</sub>H<sub>2</sub> and CoM–SH/CoB–SH via activating the critical F<sub>420</sub> hydrogenase and heterodisulfide reductase. Such biotic-abiotic interfacial interactions between mNICE and syntrophic multicellular communities sustained organic-loading rates via improving the degradation of volatile fatty acids and retarding their toxicity to methanogens. As a result, mNICE elevated the methane yield by 134.20%. This work highlights the importance of steering the activity of key enzymes across the cell-material interface in the development of sustainable waste-to-energy conversion systems.","PeriodicalId":25,"journal":{"name":"ACS Sustainable Chemistry & Engineering","volume":"58 1","pages":""},"PeriodicalIF":8.4,"publicationDate":"2026-02-03","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146101985","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2026-02-03DOI: 10.1021/acssuschemeng.5c09262
Runtian Miao, Xingyu Fan, Ning Zhang, Minjuan Gao, Yaling Mao, Yueqin Li
Hydrogel-based zinc–ion batteries (ZIBs) stand out as promising flexible energy storage devices, benefiting from their synergistic advantages of high theoretical specific capacity, reliable safety performance, and cost-effectiveness. However, conventional hydrogel-based ZIBs are plagued by inadequate ionic conductivity and structural instability at subzero temperatures, which consequently lead to sluggish Zn-ion migration kinetics and severe capacity decay. Herein, we introduced zwitterionic proline (PL) as an antifreezing additive into cross-linked polyacrylamide/carboxymethyl chitosan (PAM/CMCS) to address the above-mentioned challenges. PL can reduce hydrogen bonds between free water, thus endowing the hydrogel electrolyte (HE) with good antifreezing and antidrying performance, interfacial adhesive, high ionic conductivity (30.20 ± 0.47 mS/cm), and enhanced interfacial adhesion. Notably, the PL additive facilitates more uniform zinc deposition in the PAM/CMCS/PL electrolyte relative to the bare PAM/CMCS electrolyte and the ZnSO4 aqueous electrolyte. Accordingly, the PAM/CMCS/PL HE confers outstanding long-term cycling stability on the Zn//Zn symmetric cell. The asymmetrical Zn//MXene@PANI flexible ZIBs can deliver a specific capacity of 154.8 mAh/g at 0.5 A/g and maintain 84.9% capacity with an excellent Coulombic efficiency above 99% after 500 cycles. This flexible ZIB can withstand severe deformations and operate normally at low temperatures (75.2 mAh/g at 1.0 A/g, even at −30 °C). High-performance flexible ZIBs with outstanding low-temperature tolerance are successfully fabricated in this work, providing insightful references for advancing multifunctional flexible energy storage systems and wearable electronics.
由于具有理论比容量高、安全性能可靠、成本效益高等协同优势,水凝胶型锌离子电池(zbs)作为一种有前景的柔性储能设备脱颖而出。然而,传统的水凝胶基ZIBs在零下温度下受到离子电导率不足和结构不稳定的困扰,从而导致zn离子迁移动力学缓慢和严重的容量衰减。本文将两性离子脯氨酸(PL)作为抗冻添加剂引入交联聚丙烯酰胺/羧甲基壳聚糖(PAM/CMCS)中,以解决上述问题。PL可以减少游离水之间的氢键,从而使水凝胶电解质(HE)具有良好的抗冻抗干性能、界面粘连性、高离子电导率(30.20±0.47 mS/cm)、增强界面粘连性。值得注意的是,相对于裸PAM/CMCS电解质和ZnSO4水溶液电解质,PL添加剂有助于在PAM/CMCS/PL电解质中更均匀地沉积锌。因此,PAM/CMCS/PL HE在Zn//Zn对称电池上具有出色的长期循环稳定性。不对称Zn//MXene@PANI柔性ZIBs在0.5 a /g时可提供154.8 mAh/g的比容量,并在500次循环后保持84.9%的容量,库仑效率超过99%。这种灵活的ZIB可以承受严重的变形,并在低温下正常工作(1.0 A/g时75.2 mAh/g,即使在- 30°C)。成功制备了耐低温性能优异的高性能柔性ZIBs,为推进多功能柔性储能系统和可穿戴电子产品的发展提供了有意义的参考。
{"title":"Fabrication of Antifreezing and Adhesive Hydrogel Electrolytes Based on Zwitterionic Proline for Flexible Zinc Ion Batteries with Low-Temperature Tolerance","authors":"Runtian Miao, Xingyu Fan, Ning Zhang, Minjuan Gao, Yaling Mao, Yueqin Li","doi":"10.1021/acssuschemeng.5c09262","DOIUrl":"https://doi.org/10.1021/acssuschemeng.5c09262","url":null,"abstract":"Hydrogel-based zinc–ion batteries (ZIBs) stand out as promising flexible energy storage devices, benefiting from their synergistic advantages of high theoretical specific capacity, reliable safety performance, and cost-effectiveness. However, conventional hydrogel-based ZIBs are plagued by inadequate ionic conductivity and structural instability at subzero temperatures, which consequently lead to sluggish Zn-ion migration kinetics and severe capacity decay. Herein, we introduced zwitterionic proline (PL) as an antifreezing additive into cross-linked polyacrylamide/carboxymethyl chitosan (PAM/CMCS) to address the above-mentioned challenges. PL can reduce hydrogen bonds between free water, thus endowing the hydrogel electrolyte (HE) with good antifreezing and antidrying performance, interfacial adhesive, high ionic conductivity (30.20 ± 0.47 mS/cm), and enhanced interfacial adhesion. Notably, the PL additive facilitates more uniform zinc deposition in the PAM/CMCS/PL electrolyte relative to the bare PAM/CMCS electrolyte and the ZnSO<sub>4</sub> aqueous electrolyte. Accordingly, the PAM/CMCS/PL HE confers outstanding long-term cycling stability on the Zn//Zn symmetric cell. The asymmetrical Zn//MXene@PANI flexible ZIBs can deliver a specific capacity of 154.8 mAh/g at 0.5 A/g and maintain 84.9% capacity with an excellent Coulombic efficiency above 99% after 500 cycles. This flexible ZIB can withstand severe deformations and operate normally at low temperatures (75.2 mAh/g at 1.0 A/g, even at −30 °C). High-performance flexible ZIBs with outstanding low-temperature tolerance are successfully fabricated in this work, providing insightful references for advancing multifunctional flexible energy storage systems and wearable electronics.","PeriodicalId":25,"journal":{"name":"ACS Sustainable Chemistry & Engineering","volume":"87 1","pages":""},"PeriodicalIF":8.4,"publicationDate":"2026-02-03","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146101986","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2026-02-03DOI: 10.1021/acssuschemeng.5c10606
Yan Hou, Hao Zhao, Lei Yan, Yi Wang, Shuguang Xiang, Xiaoyan Sun, Lili Wang, Li Xia, Shaohui Tao
As global energy and environmental pressures increase, the recovery of industrial low-temperature waste heat (LTWH) has become increasingly important. This study develops four novel cogeneration systems based on chemical heat pumps to simultaneously provide thermal energy and electricity from LTWH. Through system optimization, the internal cogeneration system (NORC-IAH) identified the optimized NORC-IAH (NORC-IAH1), which effectively converts LTWH, generating electricity and high-temperature heat. Exergy, economic, and environmental assessments were conducted for NORC-IAH1. Exergy analysis shows the highest exergy loss in the distillation column T1, at 599.85 kW, and the lowest exergy efficiencies for pumps P1 and T1, at 37.25% and 41.94%, respectively. Economic analysis reveals a total annual cost of $712,641.65/year, with T1 and heat exchanger H1 contributing the most, indicating potential improvements in heat transfer efficiency. Life cycle assessment highlights the carcinogenic risk from sulfidic tailings during the stainless steel construction stage. This study provides a foundation for industrial heat recovery and environmental sustainability.
{"title":"Exergy, Economic, and Life Cycle Assessment of Novel Cogeneration Systems Based on Chemical Heat Pumps","authors":"Yan Hou, Hao Zhao, Lei Yan, Yi Wang, Shuguang Xiang, Xiaoyan Sun, Lili Wang, Li Xia, Shaohui Tao","doi":"10.1021/acssuschemeng.5c10606","DOIUrl":"https://doi.org/10.1021/acssuschemeng.5c10606","url":null,"abstract":"As global energy and environmental pressures increase, the recovery of industrial low-temperature waste heat (LTWH) has become increasingly important. This study develops four novel cogeneration systems based on chemical heat pumps to simultaneously provide thermal energy and electricity from LTWH. Through system optimization, the internal cogeneration system (NORC-IAH) identified the optimized NORC-IAH (NORC-IAH1), which effectively converts LTWH, generating electricity and high-temperature heat. Exergy, economic, and environmental assessments were conducted for NORC-IAH1. Exergy analysis shows the highest exergy loss in the distillation column T1, at 599.85 kW, and the lowest exergy efficiencies for pumps P1 and T1, at 37.25% and 41.94%, respectively. Economic analysis reveals a total annual cost of $712,641.65/year, with T1 and heat exchanger H1 contributing the most, indicating potential improvements in heat transfer efficiency. Life cycle assessment highlights the carcinogenic risk from sulfidic tailings during the stainless steel construction stage. This study provides a foundation for industrial heat recovery and environmental sustainability.","PeriodicalId":25,"journal":{"name":"ACS Sustainable Chemistry & Engineering","volume":"44 1","pages":""},"PeriodicalIF":8.4,"publicationDate":"2026-02-03","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146101987","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2026-02-03DOI: 10.1021/acssuschemeng.5c11490
Hyeokjun Cho, Jae Wang Ko, Seung Geol Lee
Dope dyeing offers an eco–efficient alternative to conventional textile coloration by incorporating pigments directly into the polymer melt, minimizing water and chemical use. This study presents a sustainable data–driven framework that reduces repetitive dyeing trials and resource consumption during color matching of dope–dyed recycled PET/PCT microfiber fabrics. A two–stage hybrid machine learning model─combining k–nearest neighbors (kNN), feature expansion, and residual modeling─was developed to predict subtle color variations within the narrow CIELAB output range inherent to dope–dyed systems. The model achieved R2 values above 0.83 for L*, a*, and b*, and external validation with untrained dyeing recipes yielded a mean ΔE of 0.65 with visually negligible deviation. By accurately pre–estimating color outcomes, this approach minimizes iterative experiments, energy use, and wastewater generation, contributing to sustainable textile manufacturing. The proposed framework demonstrates that data–driven color prediction can enhance process efficiency and environmental performance in dope–dyed fabric production, supporting circular and low–impact coloration technologies.
{"title":"Sustainable Machine-Learning Framework for Efficient Color Prediction in Dope-Dyed Recycled PET/PCT","authors":"Hyeokjun Cho, Jae Wang Ko, Seung Geol Lee","doi":"10.1021/acssuschemeng.5c11490","DOIUrl":"https://doi.org/10.1021/acssuschemeng.5c11490","url":null,"abstract":"Dope dyeing offers an eco–efficient alternative to conventional textile coloration by incorporating pigments directly into the polymer melt, minimizing water and chemical use. This study presents a sustainable data–driven framework that reduces repetitive dyeing trials and resource consumption during color matching of dope–dyed recycled PET/PCT microfiber fabrics. A two–stage hybrid machine learning model─combining k–nearest neighbors (kNN), feature expansion, and residual modeling─was developed to predict subtle color variations within the narrow CIELAB output range inherent to dope–dyed systems. The model achieved <i>R</i><sup>2</sup> values above 0.83 for <i>L</i>*, <i>a</i>*, and <i>b</i>*, and external validation with untrained dyeing recipes yielded a mean Δ<i>E</i> of 0.65 with visually negligible deviation. By accurately pre–estimating color outcomes, this approach minimizes iterative experiments, energy use, and wastewater generation, contributing to sustainable textile manufacturing. The proposed framework demonstrates that data–driven color prediction can enhance process efficiency and environmental performance in dope–dyed fabric production, supporting circular and low–impact coloration technologies.","PeriodicalId":25,"journal":{"name":"ACS Sustainable Chemistry & Engineering","volume":"29 1","pages":""},"PeriodicalIF":8.4,"publicationDate":"2026-02-03","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146101988","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
In this study, we propose a novel, environmentally, economically, and energetically sustainable approach for the valorization of vegetable-tanned leather waste, aiming at producing biobased adhesives with antibacterial properties and promising water resistance. The treatment of leather scraps was carried out using various Natural Deep Eutectic Solvents (NADES) in mild conditions (1 h, 60 °C), i.e., lactic acid:urea in a molar ratio of 2:1, choline chloride:lactic acid in a molar ratio of 1:1, and choline chloride dehydrated oxalic acid in a molar ratio of 1:1. The resulting bioadhesives exhibited excellent binding performances, in particular, on wood substrates. Structural modifications and its thermal behavior of collagen after the treatment were investigated using Fourier Transform Infrared Spectroscopy with Attenuated Total Reflectance (ATR-FTIR), Thermogravimetric Analysis (TGA and TGA/FTIR), Evolved Gas Analysis–Mass Spectrometry (EGA-MS), Pyrolysis–Gas Chromatography–Mass Spectrometry (Py-GC-MS), and proteomic techniques. Overall, this approach highlights a circular and green strategy for upcycling leather industry byproducts into high-performance materials, aligning with current goals in waste minimization and resource efficiency.
{"title":"From Waste to Function: Valorization of Collagen-Based Wastes with Natural Deep Eutectic Solvents for Bioadhesive Applications","authors":"Chiara Pelosi, Eleonora Micheli, Elena Pulidori, Giulia Caroti, Brunella Cipolletta, Beatrice Campanella, Iacopo Corsi, Silvia Pizzimenti, Leila Birolo, Ilaria Bonaduce, Celia Duce, Emilia Bramanti","doi":"10.1021/acssuschemeng.5c11526","DOIUrl":"https://doi.org/10.1021/acssuschemeng.5c11526","url":null,"abstract":"In this study, we propose a novel, environmentally, economically, and energetically sustainable approach for the valorization of vegetable-tanned leather waste, aiming at producing biobased adhesives with antibacterial properties and promising water resistance. The treatment of leather scraps was carried out using various Natural Deep Eutectic Solvents (NADES) in mild conditions (1 h, 60 °C), i.e., lactic acid:urea in a molar ratio of 2:1, choline chloride:lactic acid in a molar ratio of 1:1, and choline chloride dehydrated oxalic acid in a molar ratio of 1:1. The resulting bioadhesives exhibited excellent binding performances, in particular, on wood substrates. Structural modifications and its thermal behavior of collagen after the treatment were investigated using Fourier Transform Infrared Spectroscopy with Attenuated Total Reflectance (ATR-FTIR), Thermogravimetric Analysis (TGA and TGA/FTIR), Evolved Gas Analysis–Mass Spectrometry (EGA-MS), Pyrolysis–Gas Chromatography–Mass Spectrometry (Py-GC-MS), and proteomic techniques. Overall, this approach highlights a circular and green strategy for upcycling leather industry byproducts into high-performance materials, aligning with current goals in waste minimization and resource efficiency.","PeriodicalId":25,"journal":{"name":"ACS Sustainable Chemistry & Engineering","volume":"62 1","pages":""},"PeriodicalIF":8.4,"publicationDate":"2026-02-03","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146101989","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2026-02-03DOI: 10.1021/acssuschemeng.5c13113
Yifan Liu, Xiangyue Wei, Shun Zhang, Xuan Zhao, Wenhao Xu, Lei Yan, Zijun Feng, Xuehui Liu, Yu-Zhong Wang, Shimei Xu
Polyester/cotton blends, which represent over 60% of the textile market, present a significant challenge for chemical recycling. Conventional solution acid hydrolysis suffers from high acid consumption and low solid/liquid ratios and results in severe equipment corrosion due to the acid-resistant nature of polyester. To address the limitation, we developed an in situ catalyst-loaded semidry acidic hydrolysis method for depolymerization of polyester/cotton blends. By leveraging hydrogen bonding between cotton and a phosphomolybdic acid (PMA) catalyst, the acidic catalyst is anchored onto the fabric, forming localized acid microreactors that facilitate the hydrolysis of polyester without requiring an additional aid solution. The semidry hydrolysis process cuts acid usage to 1/100 of conventional processes, increases the solid–liquid ratio by 3 times, and accelerates the reaction rate by 25 times, while achieving a TPA yield exceeding 94%. The corrosion is markedly suppressed. Both the impregnation solution and the used catalyst are recyclable, contributing to a more sustainable catalytic process. The study offers a sustainable and efficient strategy for recycling blended fabrics with a broad applicability.
{"title":"Semidry Acid Hydrolysis of Polyester/Cotton Blends through In Situ Catalyst Loading","authors":"Yifan Liu, Xiangyue Wei, Shun Zhang, Xuan Zhao, Wenhao Xu, Lei Yan, Zijun Feng, Xuehui Liu, Yu-Zhong Wang, Shimei Xu","doi":"10.1021/acssuschemeng.5c13113","DOIUrl":"https://doi.org/10.1021/acssuschemeng.5c13113","url":null,"abstract":"Polyester/cotton blends, which represent over 60% of the textile market, present a significant challenge for chemical recycling. Conventional solution acid hydrolysis suffers from high acid consumption and low solid/liquid ratios and results in severe equipment corrosion due to the acid-resistant nature of polyester. To address the limitation, we developed an in situ catalyst-loaded semidry acidic hydrolysis method for depolymerization of polyester/cotton blends. By leveraging hydrogen bonding between cotton and a phosphomolybdic acid (PMA) catalyst, the acidic catalyst is anchored onto the fabric, forming localized acid microreactors that facilitate the hydrolysis of polyester without requiring an additional aid solution. The semidry hydrolysis process cuts acid usage to 1/100 of conventional processes, increases the solid–liquid ratio by 3 times, and accelerates the reaction rate by 25 times, while achieving a TPA yield exceeding 94%. The corrosion is markedly suppressed. Both the impregnation solution and the used catalyst are recyclable, contributing to a more sustainable catalytic process. The study offers a sustainable and efficient strategy for recycling blended fabrics with a broad applicability.","PeriodicalId":25,"journal":{"name":"ACS Sustainable Chemistry & Engineering","volume":"189 1","pages":""},"PeriodicalIF":8.4,"publicationDate":"2026-02-03","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146101991","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}