ACS Sustainable Chemistry & Engineering最新文献

{"title":"Interfacial Si–O–Zn Coordination in Chitosan Hydrogel Electrolytes Regulating (002)-Oriented Zn Deposition for Flexible Energy Storage and Sensing","authors":"Shuting Liu,&nbsp;Mingde Tong,&nbsp;Qingkun Tang,&nbsp;Xinyan Lv,&nbsp;Zuyun Chen,&nbsp;Songshan Zeng,&nbsp;Xiaoyuan Yu","doi":"10.1021/acssuschemeng.6c07104","DOIUrl":"10.1021/acssuschemeng.6c07104","url":null,"abstract":"<p>Sustainable wearable electronics demand flexible energy-storage and sensing devices made by greener, low-impact routes. Aqueous zinc-based hydrogel electrolytes are attractive here, but their use is limited by uncontrolled zinc dendrite growth and by the difficulty of combining fast Zn²⁺ transport with controlled interfacial deposition. Most hydrogels resist dendrites only through passive physical confinement, without actively governing interfacial zinc deposition. Herein, using chitosan, a renewable polysaccharide obtained from chitin-rich seafood waste, we construct an interfacial Si–O–Zn coordination motif within a hydrogel electrolyte through a mild, all-aqueous, one-step in situ polymerization that requires no separate activation step. Chitosan and acrylamide form the matrix, zinc trifluoromethanesulfonate (Zn(OTf)₂) is the zinc source, and nanosilicon acts as a functional filler. Chitosan bridges the organic and inorganic domains through its -NH₂/-OH groups, while free Zn²⁺ ions coordinate with surface silanols to form interfacial Si–O–Zn coordination interactions. The optimized CAA-6-Si_(3:1) electrolyte delivers a high ionic conductivity (36.04 ± 1.71 mS cm^–1), a wide electrochemical stability window (2.56 V), and a Zn²⁺ transference number of 0.583. Spectroscopic and structural analyses reveal that the interfacial Si–O–Zn sites actively steer Zn²⁺ toward the low-energy (002) plane, suppressing dendrites rather than merely blocking them; accordingly, Zn || Zn symmetric cells cycle stably for 1820 h at 2 mA cm^–2 and 535 h at 5 mA cm^–2. The same electrolyte integrates readily into multiple flexible devices: zinc-ion hybrid capacitors retain 90.4% capacity after 50,000 cycles at 10 A g^–1, with stable performance under bending, and strain sensors (gauge factor = 1.54) reliably monitor physiological signals. By coupling interfacial coordination chemistry to zinc deposition, this chitosan hydrogel electrolyte combines fast Zn²⁺ transport with (002)-oriented, dendrite-suppressed plating. Made from a renewable feedstock through a mild, low-impact process, it offers a sustainable route to flexible energy-storage and sensing devices.</p>","PeriodicalId":25,"journal":{"name":"ACS Sustainable Chemistry & Engineering","volume":"14 41","pages":"18637–18651"},"PeriodicalIF":7.6,"publicationDate":"2026-10-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149091188","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}

{"title":"Simultaneous Interlayer Expansion and Defect Engineering in Hydrated V2O5 Cathodes for Fast-Charging Aqueous Zinc Batteries","authors":"Huihua Li,&nbsp;Dong Wang,&nbsp;Hao Xu,&nbsp;Yidong Miao,&nbsp;Weihao Li,&nbsp;Alexey Y. Ganin,&nbsp;Jian Wang,&nbsp;Huang Zhang","doi":"10.1021/acssuschemeng.6c06903","DOIUrl":"10.1021/acssuschemeng.6c06903","url":null,"abstract":"<p>Aqueous zinc-ion batteries (AZIBs) offer a safe, scalable path to grid storage, but their progress is limited by cathode materials that exhibit sluggish Zn²⁺ diffusion. Commercial vanadium pentoxide (V₂O₅), though possessing a high theoretical capacity, inherently suffers from this kinetic limitation. Here, a water-assisted mechanochemical strategy is developed to introduce interlayer hydration and V⁴⁺-rich oxygen defects into commercial V₂O₅, improving both ion transport and electron transfer. Hydration expands the interlayer spacing for Zn²⁺ migration, while V⁴⁺ states enhance charge transfer, forming a coupled ion–electron pathway. The treatment also expands the (001) spacing, creates oxygen vacancies, and exfoliates bulk particles into porous nanosheets. The optimally modified V₂O₅ cathode delivers exceptional Zn²⁺ storage performance with a high reversible capacity of 563.7 mAh g^–1 at 0.2 A g^–1, outstanding cycling stability with 237 mAh g^–1 retained after 5000 cycles at 10 A g^–1, and a near-unity Coulombic efficiency. Comprehensive kinetic analyses confirm that the modified V₂O₅ exhibits a dominant pseudocapacitive mechanism, significantly reduced charge-transfer resistance, and an order-of-magnitude enhancement in the apparent Zn²⁺ diffusion coefficient. This work demonstrates that the coordinated regulation of interlayer water and oxygen vacancies is a highly effective strategy to activate commercial V₂O₅, and the mechanochemical route provides a potentially scalable strategy for activating commercial oxide cathode materials.</p>","PeriodicalId":25,"journal":{"name":"ACS Sustainable Chemistry & Engineering","volume":"14 41","pages":"18624–18636"},"PeriodicalIF":7.6,"publicationDate":"2026-10-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149091275","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}

{"title":"Integrated Valorization of Plastic Waste into Synthetic Fuels and Electricity via Multi-Stage Upgrading: Process Modeling and Techno-Economic Analysis","authors":"Leonardo Colelli,&nbsp;Gholamreza Masoudi Rad,&nbsp;Kamran Alam,&nbsp;Giorgio Vilardi,&nbsp;Nicola Verdone","doi":"10.1021/acssuschemeng.6c04701","DOIUrl":"10.1021/acssuschemeng.6c04701","url":null,"abstract":"<p>An integrated process for the valorization of 1000 kg/h of heterogeneous plastic waste (Plasmix) into hydrogen, purified CO₂, light and heavy liquid fuels, and electricity was developed and simulated using Aspen Plus. The process combines non-catalytic pyrolysis with sequential syngas upgrading, tar catalytic conversion, and extensive heat integration to maximize product recovery and economic performance. In the pyrolysis stage (600 °C, 12 bar), Plasmix is efficiently converted into gas, tar, char, and wastewater, with the gaseous fraction representing the largest product share (42.1%), followed by tar (23.0%), char (20.6%), and water (14.3%). The syngas stream is upgraded via reforming, water–gas shift, CO₂ separation, and pressure swing adsorption to produce hydrogen (59 kg/h) and purified CO₂ (533 kg/h), while the tar fraction is converted into liquid fuels, yielding 228 kg/h of light fuel and 23 kg/h of heavy fuel. Process integration enables substantial energy recovery, resulting in a net electricity export of approximately 18.2 MW. Economic evaluation shows a fixed capital investment of 12.21 M$, with annual revenues of 15.50 M$/year and operating expenditures of 5.33 M$/year, confirming strong baseline profitability. Sensitivity analysis identifies hydrogen and electricity selling prices as the dominant economic drivers, whereas the plastic waste fee provides a secondary contribution to profitability enhancement. Monte Carlo analysis further confirms robust financial performance under uncertainty, with predominantly positive net present values ranging from –33.6 to 129.9 M$, indicating limited downside risk and strong overall economic resilience. The internal rate of return varies between 0 and 52%, while discounted payback periods range from 0.7 to 10 years depending on market conditions. These results demonstrate that the proposed process achieves high mass valorization efficiency and economically resilient performance, providing a promising pathway for sustainable plastic waste-to-energy and waste-to-fuels integration within a circular carbon framework.</p>","PeriodicalId":25,"journal":{"name":"ACS Sustainable Chemistry & Engineering","volume":"14 41","pages":"18503–18517"},"PeriodicalIF":7.6,"publicationDate":"2026-10-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149091278","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}

{"title":"Reproducibility of Colloidal Lignin Particle Preparation: An Interlaboratory Evaluation","authors":"Ioanna Sapouna,&nbsp;Daniel Barker-Rothschild,&nbsp;Emilia Ikävalko,&nbsp;Selena de la Caridad Díaz Rodríguez,&nbsp;Gerard Lligadas,&nbsp;Peyman Gholami,&nbsp;Paula Nousiainen,&nbsp;Hai Liu,&nbsp;Muhammad Farooq,&nbsp;Umberto Danelon,&nbsp;Michele Back,&nbsp;Matteo Gigli,&nbsp;Massimo Sgarzi,&nbsp;Kirsi S. Mikkonen,&nbsp;Orlando J. Rojas,&nbsp;Lin Dai,&nbsp;Monika Österberg,&nbsp;Claudia Crestini,&nbsp;Adrian Moreno,&nbsp;Mika H. Sipponen","doi":"10.1021/acssuschemeng.6c05879","DOIUrl":"10.1021/acssuschemeng.6c05879","url":null,"abstract":"<p>The reproducibility of the preparation of colloidal lignin particles (CLPs) was evaluated through a coordinated interlaboratory study involving seven independent research groups from around the world. The objective was to assess the robustness of the anti-solvent precipitation method and identify parameters requiring further standardization, while also setting a unified terminology. Laboratories prepared CLPs following a common procedure and characterized key physicochemical properties, including the pH and concentration of both lignin solution and CLP dispersion, as well as the mass yield of the dispersion. The particle hydrodynamic diameter (reported based on number, intensity, and volume) and PDI were compared to the diameter and particle-diameter dispersity (<em>Ð</em>_d) obtained from SEM image analysis. Additionally, four shape descriptors derived from the same analysis were used for the morphological characterization of the CLPs. This study represents the first systematic interlaboratory quantification of CLP preparation reproducibility and provides a direct comparison of characterization approaches, including dynamic light scattering (DLS) and SEM-based analysis. Statistical evaluation of the data included z-score assessment, outlier testing, and estimation of repeatability and reproducibility using mixed-effects modeling. The results demonstrate that the overall preparation route is largely reproducible across laboratories. Increased variability was observed for dispersity-related parameters and morphology metrics, primarily reflecting methodological differences in data evaluation and reporting. These findings identify critical sources of variability and establish practical guidelines for standardizing CLP preparation and characterization across laboratories, supporting reliable comparison and continued development of lignin-based colloidal materials.</p>","PeriodicalId":25,"journal":{"name":"ACS Sustainable Chemistry & Engineering","volume":"14 41","pages":"18570–18581"},"PeriodicalIF":7.6,"publicationDate":"2026-10-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149091348","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}

{"title":"Economic and Environmental Evaluation of Sequential vs Single-Reactor Tandem Catalytic Routes for Furan-Derived Amine Production","authors":"Catherine Yezeguelian,&nbsp;Marc Pera-Titus","doi":"10.1021/acssuschemeng.6c04070","DOIUrl":"10.1021/acssuschemeng.6c04070","url":null,"abstract":"<p>The development of intensified catalytic processes for biomass valorization is a key strategy to improve the sustainability of chemical manufacturing. In this work, we compare a conventional two-reactor and a single-reactor tandem process for the production of the furfural-derived amine 1-(furan-2-yl)-4-methylpentan-2-amine (F-ALD-1-NH₂), combining technoeconomic analysis (TEA) and cradle-to-gate life cycle assessment (LCA). Both routes involve aldol condensation of furfural with methyl isobutyl ketone followed by reductive amination but differ in process configuration, yields, and catalyst requirements. Under base-case conditions, the two-reactor process outperforms the single-reactor configuration, exhibiting 16–20% lower full manufacturing cost (€5250/ton vs €6313/ton) and systematically reduced environmental impacts across all midpoint categories (e.g., 21% lower global warming potential). These differences are primarily driven by the higher overall yield (91% vs 74%) and lower catalyst loading of the two-reactor process. However, sensitivity analysis reveals that process intensification becomes advantageous under optimized conditions. By improving yield, reducing catalyst loading, and optimizing solvent ratios, the single-reactor process could achieve up to 10% lower manufacturing cost and 5–20% lower environmental impacts relative to the two-reactor configuration. Across both routes, key drivers of cost and environmental performance include furfural and solvent consumption, catalyst loading and regeneration, and energy demand for separations. Uncertainty analysis confirms the statistical robustness of these trends for selected impact categories. This study demonstrates that while process intensification does not inherently guarantee improved sustainability, it can deliver significant economic and environmental benefits when reaction performance and process parameters are carefully optimized. These findings highlight the importance of integrating early-stage TEA and LCA to guide the design and development of intensified catalytic processes for renewable chemical production.</p>","PeriodicalId":25,"journal":{"name":"ACS Sustainable Chemistry & Engineering","volume":"14 41","pages":"18481–18502"},"PeriodicalIF":7.6,"publicationDate":"2026-10-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149091344","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}

{"title":"Low-Temperature Phase-Separating Hydro-alcoholytic Depolymerization of Polyurethanes","authors":"Anjana S. Sarala,&nbsp;Gabriele Rossignolo,&nbsp;Thomas Andersen,&nbsp;Jakob Gammelgaard Brøgger,&nbsp;Alessandra Lorenzetti,&nbsp;Bjarke S. Donslund,&nbsp;Troels Skrydstrup","doi":"10.1021/acssuschemeng.6c07117","DOIUrl":"10.1021/acssuschemeng.6c07117","url":null,"abstract":"<p>Polyurethane (PU) is a non-biodegradable thermoset plastic and a persistent waste burden with an annual production of around 26 million tonnes. Conventional disposal routes squander valuable resources and generate greenhouse gas emissions. Though chemical recycling offers a sustainable reuse route by depolymerizing PU into monomers, existing methods remain energy-intensive and require burdensome purification, highlighting the need for improved strategies. Here, we present a low-temperature, base-mediated hydrolysis that efficiently depolymerizes PU into high-purity polyols and oligoureas. Applied to flexible foam, the process is completed within an hour at 100 °C, producing distinct phase separation that enables easy recovery of the individual components. Other PU materials, including end-of-life mixed foam waste, are also effectively depolymerized, underscoring the potential as a practical recycling strategy. Finally, the process was scaled up to a 100 g reaction, with a polyol recovery of &gt;85%, demonstrating its feasibility for large-scale implementation. The recycled polyol matched the virgin polyol in hydroxyl number, and the oligourea fraction was hydrolyzed into the corresponding anilines displaying the potential for full monomer recovery. This low-temperature hydrolysis approach not only enables efficient release of monomers under mild conditions but also simplifies downstream separation, positioning it as an attractive alternative to existing chemical recycling methods.</p>","PeriodicalId":25,"journal":{"name":"ACS Sustainable Chemistry & Engineering","volume":"14 41","pages":"18669–18681"},"PeriodicalIF":7.6,"publicationDate":"2026-10-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149091345","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}

{"title":"Fully Biobased Shellac/Latex Composites Reinforced with Modified Posidonia Oceanica Fibers: Mechanical and Acoustic Performance with Micromechanical Modeling","authors":"Pelin Altay,&nbsp;Emine Dilara Kocak,&nbsp;Mete Kayihan","doi":"10.1021/acssuschemeng.5c12563","DOIUrl":"10.1021/acssuschemeng.5c12563","url":null,"abstract":"<p>Fully biobased composites combining renewable matrices and marine biomass-derived reinforcements offer a sustainable route toward multifunctional materials with tailored mechanical and acoustic properties. In this study, fully biobased composites were fabricated using a shellac/natural rubber latex matrix reinforced with marine biomass-derived <em>Posidonia oceanica</em> (PO) waste fibers. To improve interfacial compatibility, fibers were modified with succinic acid, a bio-based platform chemical, under ultrasonic treatment, providing a green and efficient surface functionalization strategy for fully biobased composites. Tensile testing showed that at 0.5% fiber content, elastic modulus (4.64 MPa), tensile strength (0.55 MPa), and elongation at break (255%) all improved compared with the neat matrix (3.59 MPa, 0.48 MPa, 196%). At 1%, stiffness further increased (4.72 MPa), but strength and ductility decreased due to fiber agglomeration, while 2% yielded maximum elongation (286%) despite reduced stiffness. Acoustic characterization revealed superior absorption at intermediate loadings, with coefficients of 0.41–0.44 at 6300 Hz, and a maximum of 0.52 at 2%. Micromechanical modeling performed via finite element analysis supported these findings, confirming stress concentration transitions from the matrix to the fiber-matrix interface with increasing fiber content and validating the experimental tensile results with less than 7% deviation. Among the investigated compositions, composites containing 0.5–1 wt % PO fibers exhibited the most balanced combination of stiffness, ductility, and acoustic absorption, demonstrating the potential of ultrasonically succinic acid-modified marine-derived fibers for developing fully biobased lightweight materials with multifunctional performance.</p>","PeriodicalId":25,"journal":{"name":"ACS Sustainable Chemistry & Engineering","volume":"14 41","pages":"18436–18446"},"PeriodicalIF":7.6,"publicationDate":"2026-10-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149091351","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}

{"title":"Hydrogen Production from Zero-Valent Iron in Anaerobic Bicarbonate-Rich Media: The Role of Low-Dose Scrap Aluminum","authors":"Antigoni Kisouri,Nicolas P. L. Magnard,Marie-Lou Levé,Ioannis Vyrides","doi":"10.1021/acssuschemeng.6c06503","DOIUrl":"https://doi.org/10.1021/acssuschemeng.6c06503","url":null,"abstract":"Abstract Hydrogen (H2) production from zero-valent iron (ZVI) in bicarbonate-rich media is a promising low-temperature route, although progressive surface passivation remains a limitation. The influence of ZVI concentration (10–50 g/L), scrap aluminum (Al) addition, temperature (4–80 °C), sodium bicarbonate concentration (0–70 g/L NaHCO3), multi-cycle operation, and manual grinding was evaluated under anaerobic conditions. Temperature strongly affected kinetics, with an apparent activation energy of ∼30.8 kJ/mol for the ZVI–Al–bicarbonate system. The highest overall H2 yield approached 50% in the ZVI–Al system at 80 °C, substantially exceeding the yields obtained at lower temperature and in the absence of Al. Bicarbonate, especially above 30 g/L NaHCO3, played a critical role by sustaining proton availability through the bicarbonate/carbonate equilibrium and thereby promoting Fe corrosion and H2 evolution. The resulting progressive increase in pH created alkaline conditions that, in the presence of Al, further enhanced H2 generation. In multi-cycle experiments, manual grinding further improved performance by partially restoring reactivity, resulting in H2 yields approaching 50%. XRD analysis showed that siderite (FeCO3) remained the dominant Fe-bearing corrosion product, while Fe–Al layered double hydroxide, minor chukanovite, and aluminum hydroxide (Al(OH)3) were detected only in the presence of Al.","PeriodicalId":25,"journal":{"name":"ACS Sustainable Chemistry & Engineering","volume":"38 1","pages":""},"PeriodicalIF":8.4,"publicationDate":"2026-10-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149209489","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}

{"title":"Tunnel/P2 Interlocking Structure Coupled with TiO2 Interface Modification for Synergistically Enhanced Structural Stability of Sodium-Ion Battery Cathodes","authors":"Yu Duan,Jia-xuan He,Shuo Bao,Tong Li,Ying-ying Huang,Yi Zhang,Yan-sheng Yin,Jin-lin Lu","doi":"10.1021/acssuschemeng.6c07871","DOIUrl":"https://doi.org/10.1021/acssuschemeng.6c07871","url":null,"abstract":"Abstract Layered Mn-based oxides are promising cathode materials for sodium-ion batteries, which are prone to an irreversible P2-O2 phase transition during cycling and thus exhibit poor cyclic stability. Although tunnel-type Mn-based oxides feature a stable structure, they deliver a low sodium storage capacity. In this work, tunnel/P2 interlocked cathode materials are synthesized by adjusting sodium content and further modified via Ti/Cu co-doping and 1 wt % TiO2 surface coating for synergistic optimization. The results show that Ti/Cu co-doping lowers the proportion of Mn3+ to 42.83% and efficiently restrains Jahn–Teller distortion. The optimized Na0.66Mn0.8Ti0.1Cu0.1O2 achieves an initial discharge specific capacity of 153.7 mAh·g–1 and an average sodium-ion diffusion coefficient of 3.9 × 10–11 cm2·s–1, showing outstanding kinetic performance. The TiO2-coated sample still retains a stable dual-phase structure consisting of a 64.3% P2 phase and a 35.7% tunnel phase, with the average sodium-ion diffusion coefficient increasing to 5.06 × 10–11 cm2·s–1. It maintains a high capacity retention of 91.85% after 50 cycles at 20 mA·g–1 and 67.5% after 200 cycles at 200 mA·g–1. In situ XRD tests confirm that the (002) diffraction peak of the P2 phase shifts reversibly by 0.12° during charge and discharge. The diffraction peaks of the tunnel phase weaken temporarily at high voltage and recover completely after discharge, demonstrating excellent structural reversibility. This study greatly boosts the electrochemical properties of Mn-based cathodes through combined modification strategies, offering solid experimental data and practical references for the development of high-performance cathode materials for sodium-ion batteries.","PeriodicalId":25,"journal":{"name":"ACS Sustainable Chemistry & Engineering","volume":"15 1","pages":""},"PeriodicalIF":8.4,"publicationDate":"2026-10-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149209779","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}

{"title":"High-Entropy Strategy Engineered Superparaelectric Critical States Enabling Superior Capacitive Energy Storage in Lead-Free Sustainable Ceramics","authors":"Jiangping Huang,&nbsp;Yu Zhang,&nbsp;Lin Xia,&nbsp;Yue Pan,&nbsp;Haiyao Zhang,&nbsp;Xiuli Chen,&nbsp;Xu Li,&nbsp;Huanfu Zhou","doi":"10.1021/acssuschemeng.6c04808","DOIUrl":"10.1021/acssuschemeng.6c04808","url":null,"abstract":"<p>Dielectric ceramic capacitors with superior energy storage performance serve as core components for next-generation advanced pulsed power systems and miniaturized electronic devices. However, the performance optimization of bulk dielectric ceramics is constrained by the inherent difficulty of simultaneously achieving high polarization and high efficiency. To address this issue, we propose a high-entropy strategy to construct the superparaelectric critical state—a crossover region from superparaelectric to relaxor state—for tuning the polarization configuration. Through rational compositional design, we incorporate Sr_0.7Sm_0.2(Zr_0.5Ta_0.4)O₃ linear dielectric into a tetragonal Bi_0.375Na_0.375Ba_0.25TiO₃ matrix with high dielectric permittivity and large polarization, successfully shifting the maximum dielectric constant to near room temperature, enhancing rapid domain switching, and reducing hysteresis. Multiscale structural characterization reveals that the high-entropy design introduces strong local disorder to construct dynamic polar nanodomains, enabling the concurrent achievement of both high polarization and high efficiency. Consequently, the optimized ceramic delivers superior energy storage performance, including a recoverable energy density of 8.52 J/cm³ with an ultrahigh 93.86% efficiency and decent thermal stability (25–150 °C). This work provides a viable paradigm for designing high-performance dielectric ceramics for advanced capacitive energy storage applications.</p>","PeriodicalId":25,"journal":{"name":"ACS Sustainable Chemistry & Engineering","volume":"14 41","pages":"18518–18529"},"PeriodicalIF":7.6,"publicationDate":"2026-10-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149091271","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}