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Tandem Catalysis as a Platform for the Mild Synthesis of Renewable Aliphatic Polyanhydrides 串联催化作为温和合成可再生脂肪族聚酸酐的平台。
IF 5.9 2区 化学
ChemSusChem Pub Date : 2026-11-05 DOI: 10.1002/cssc.71206
Lucie Fournier, Jakhongir Bekmirzaev, Malaury Simon, Fanny Betermier, Carine Robert, Robert T. Mathers, Régis M. Gauvin, Christophe M. Thomas
{"title":"Tandem Catalysis as a Platform for the Mild Synthesis of Renewable Aliphatic Polyanhydrides","authors":"Lucie Fournier,&nbsp;Jakhongir Bekmirzaev,&nbsp;Malaury Simon,&nbsp;Fanny Betermier,&nbsp;Carine Robert,&nbsp;Robert T. Mathers,&nbsp;Régis M. Gauvin,&nbsp;Christophe M. Thomas","doi":"10.1002/cssc.71206","DOIUrl":"10.1002/cssc.71206","url":null,"abstract":"<p>The development of one-pot catalytic strategies that transform renewable feedstocks into functional polymers remains an important challenge in sustainable polymer chemistry. Here, we report a tandem-catalyzed strategy for the mild step-growth polymerization of a fatty acid-derived monomer into high-molar-mass aliphatic polyanhydrides. Selective ruthenium-catalyzed self-metathesis of 10-undecenoic acid affords eicos-10-enedioic acid with high conversion and minimal olefin positional isomerization within the substrate. The resulting diacid is subsequently converted into a polyanhydride through magnesium-catalyzed dehydrative polycondensation using dimethyl dicarbonate as a stoichiometric dehydrating reagent. The two catalytic transformations are operationally compatible and can be performed as a sequential one-pot process without isolation of the diacid intermediate. The orthogonal Ru/Mg sequence affords polyanhydrides with weight-average molar masses above 30 kg/mol, while the independently optimized magnesium-catalyzed polymerization reaches weight-average molar masses above 80 kg/mol. A ruthenium species derived from the metathesis catalyst can also promote the dehydrative coupling step, providing an auto-tandem pathway, although with lower molar-mass control. The resulting polyanhydride films exhibit water contact angles of 95°–100°, within the range reported for polyethylene and polypropylene surfaces. This work establishes a mild and step-efficient route from a renewable unsaturated fatty acid to hydrophobic aliphatic polyanhydrides.</p>","PeriodicalId":149,"journal":{"name":"ChemSusChem","volume":"19 21","pages":""},"PeriodicalIF":5.9,"publicationDate":"2026-11-05","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://onlinelibrary.wiley.com/doi/epdf/10.1002/cssc.71206","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149331841","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Mo─O─S-Bridged MoS2@MoO2 Heterostructures Enable Accelerated Zn2+ Storage Kinetics in Aqueous Zinc-Ion Batteries Mo─O─s桥接MoS2@MoO2异质结构加速锌离子电池中Zn2+的储存动力学。
IF 5.9 2区 化学
ChemSusChem Pub Date : 2026-11-05 DOI: 10.1002/cssc.71198
Sifan Qiao, Xinyan Zhou, Chao Li, Zhou Jiang, Fuxi Liu, Aofei Wei, Jingjuan Li, Wei Zhang
{"title":"Mo─O─S-Bridged MoS2@MoO2 Heterostructures Enable Accelerated Zn2+ Storage Kinetics in Aqueous Zinc-Ion Batteries","authors":"Sifan Qiao,&nbsp;Xinyan Zhou,&nbsp;Chao Li,&nbsp;Zhou Jiang,&nbsp;Fuxi Liu,&nbsp;Aofei Wei,&nbsp;Jingjuan Li,&nbsp;Wei Zhang","doi":"10.1002/cssc.71198","DOIUrl":"10.1002/cssc.71198","url":null,"abstract":"<p>Layered transition metal dichalcogenides (e.g., MoS<sub>2</sub>, VS<sub>2</sub>) possess intrinsic two-dimensional diffusion channels for Zn<sup>2+</sup>, rendering them promising cathode candidates for aqueous zinc-ion batteries (AZIBs). However, for MoS<sub>2</sub> cathode, it is still challenging to unlock the limited electrochemically active sites for ideal performance. Herein, based on MoS<sub>2</sub>@MoO<sub>2</sub> heterostructure fabricated via a one-step hydrothermal method, their engineered heterointerface lowers the desolvation energy via modifying the Helmholtz layer. In particular, the generation of Mo─O─S bridge bonds and abundant coordinatively unsaturated sites accelerate hydrated Zn<sup>2+</sup> migration. Consequently, the optimized MoS<sub>2</sub>@MoO<sub>2</sub> delivers an outstanding discharge specific capacity of 325.74 mAh g<sup>−1</sup> at 0.1 A g<sup>−1</sup> and an excellent capacity retention of 95.6% after 6000 cycles at 10 A g<sup>−1</sup>.</p>","PeriodicalId":149,"journal":{"name":"ChemSusChem","volume":"19 21","pages":""},"PeriodicalIF":5.9,"publicationDate":"2026-11-05","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149331839","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Structure–Performance Relationships in Metal–Organic Framework Mg2(olz) Catalysts for CO2 Adsorption and Hydrogenation to Methanol 金属-有机骨架Mg2(olz)催化剂对CO2吸附和加氢制甲醇的结构-性能关系
IF 5.9 2区 化学
ChemSusChem Pub Date : 2026-11-05 DOI: 10.1002/cssc.71202
Anna Liutkova, Fabio André Peixoto Esteves, Anastasia Molokova, Marianela López Romero, Davide Salusso, Andrea Testino, Emiliya Poghosyan, Marco Ranocchiari
{"title":"Structure–Performance Relationships in Metal–Organic Framework Mg2(olz) Catalysts for CO2 Adsorption and Hydrogenation to Methanol","authors":"Anna Liutkova,&nbsp;Fabio André Peixoto Esteves,&nbsp;Anastasia Molokova,&nbsp;Marianela López Romero,&nbsp;Davide Salusso,&nbsp;Andrea Testino,&nbsp;Emiliya Poghosyan,&nbsp;Marco Ranocchiari","doi":"10.1002/cssc.71202","DOIUrl":"10.1002/cssc.71202","url":null,"abstract":"<p>We investigated a Cu–Zn-modified Mg<sub>2</sub>(olz) catalyst for carbon dioxide (CO<sub>2</sub>) hydrogenation to methanol under low CO<sub>2</sub> partial pressures, relevant to dilute CO<sub>2</sub> streams in industrial gas treatment and carbon capture. The catalyst was prepared via wet impregnation of presynthesized Cu–Zn species into the metal-organic framework (MOF). Batch tests under mild temperatures and low CO<sub>2</sub> concentration showed that the MOF-based system achieved higher methanol yields than a commercial catalyst at 150 °C. Step-response experiments in a plug-flow reactor revealed that the MOF retained a significant amount of CO<sub>2</sub> under high-pressure and dynamic conditions. In situ diffuse reflectance infrared Fourier transform spectroscopy identified methanol-related surface intermediates, while ex situ postreaction <sup>1</sup>H nuclear magnetic resonance spectroscopy supported the formation and retention of methanol and oxygenated species in the MOF-based catalyst. X-ray absorption spectroscopy showed partial reduction of oxygenated Cu species during reaction, while in situ X-ray diffraction demonstrated structural stability of the Mg<sub>2</sub>(olz) MOF framework. These results indicate that Mg<sub>2</sub>(olz)-based materials combine CO<sub>2</sub> adsorption capacity with catalytic functionality. Adsorption and catalytic functions coexist rather than being directly coupled. The material exhibits methanol productivity at low temperature in the presence of a solvent phase and remains structurally stable under the investigated catalytic conditions.</p>","PeriodicalId":149,"journal":{"name":"ChemSusChem","volume":"19 21","pages":""},"PeriodicalIF":5.9,"publicationDate":"2026-11-05","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://onlinelibrary.wiley.com/doi/epdf/10.1002/cssc.71202","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149331840","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Atomic Layer-Deposited LSO Coating Stabilizes the Interface and Enhances the Electrochemical Performance of High-Nickel NCM811 Cathode Material 原子层沉积LSO涂层稳定了高镍NCM811正极材料的界面,提高了材料的电化学性能。
IF 5.9 2区 化学
ChemSusChem Pub Date : 2026-11-04 DOI: 10.1002/cssc.71193
Yao Yao, Zhongyuan Luo, Jianguo Duan, Jiyue Hou, Yongshun Liang, Chunman Yang, Xiaoyuan Zeng, Jie Xiao, Yiyong Zhang, Kaomin Zhang, Peng Dong, Yingjie Zhang, Yannan Zhang
{"title":"Atomic Layer-Deposited LSO Coating Stabilizes the Interface and Enhances the Electrochemical Performance of High-Nickel NCM811 Cathode Material","authors":"Yao Yao,&nbsp;Zhongyuan Luo,&nbsp;Jianguo Duan,&nbsp;Jiyue Hou,&nbsp;Yongshun Liang,&nbsp;Chunman Yang,&nbsp;Xiaoyuan Zeng,&nbsp;Jie Xiao,&nbsp;Yiyong Zhang,&nbsp;Kaomin Zhang,&nbsp;Peng Dong,&nbsp;Yingjie Zhang,&nbsp;Yannan Zhang","doi":"10.1002/cssc.71193","DOIUrl":"10.1002/cssc.71193","url":null,"abstract":"<p>LiNi<sub>0.8</sub>Co<sub>0.1</sub>Mn<sub>0.1</sub>O<sub>2</sub> (NCM811) cathode material has attracted considerable attention because of its potential to achieve substantially higher energy densities, but the practical deployment of NCM811 remains hindered by severe interfacial and structural degradation during repeated cycling. Atomic layer deposition (ALD) was employed in this study to construct an amorphous Li─Si─O (LSO) coating layer with different thicknesses on the surface of NCM811 cathode materials, and their effects on the structural characteristics, interfacial properties, and electrochemical performance were systematically investigated. Among all the samples, 50 LSO@NCM811 exhibits the best electrochemical performance, retaining a discharge capacity of 115.96 mAh g<sup>−1</sup> after 500 cycles at 1 C under a cutoff voltage of 4.3 V. By constructing a stable and ionically conductive interfacial protective layer, the LSO coating achieves the synergistic optimization of interfacial stability, structural stability, and electrochemical kinetics, thereby markedly enhancing the electrochemical performance of NCM811 cathode materials. This work provides important insights into interfacial engineering design for high-nickel layered cathode materials of lithium-ion batteries.</p>","PeriodicalId":149,"journal":{"name":"ChemSusChem","volume":"19 21","pages":""},"PeriodicalIF":5.9,"publicationDate":"2026-11-04","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149316453","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Electron Catalysis for Enhanced Per- and Polyfluoroalkyl Substances Degradation in Nonthermal Plasma 非热等离子体中增强全氟烷基和多氟烷基物质降解的电子催化
IF 5.9 2区 化学
ChemSusChem Pub Date : 2026-11-03 DOI: 10.1002/cssc.71169
Kimberley M. Christopher, Radha Krishna Murthy Bulusu, Mark Shteyman, Bruce R. Locke, Igor V. Alabugin
{"title":"Electron Catalysis for Enhanced Per- and Polyfluoroalkyl Substances Degradation in Nonthermal Plasma","authors":"Kimberley M. Christopher,&nbsp;Radha Krishna Murthy Bulusu,&nbsp;Mark Shteyman,&nbsp;Bruce R. Locke,&nbsp;Igor V. Alabugin","doi":"10.1002/cssc.71169","DOIUrl":"https://doi.org/10.1002/cssc.71169","url":null,"abstract":"<p>Per- and polyfluoroalkyl substances (PFAS) are persistent environmental pollutants resistant to degradation due to strong C─F bonds. Efficient, energy-saving methods for PFAS remediation remain a critical challenge. Here, we develop a computational framework revealing that radical anions of perfluorosulfonic acids serve as key intermediates where electron attachment weakens C─F and C─S bonds by up to 80 kcal/mol, enabling degradation pathways inaccessible to neutral or deprotonated species. Electrons and hydrogen atoms emerge as the dominant agents of defluorination, while hydroxyl radicals play a secondary role. Coupled with experimental validation in a nonthermal plasma reactor, we demonstrate that electron upconversion facilitates catalytic defluorination cycles through radical–anion cross-reactions, enhancing fluoride release up to four-fold. These findings unify plasma, photoredox, and electrochemical approaches under an electron-catalytic mechanism, suggesting broadly applicable, greener strategies for destroying persistent fluorinated pollutants.</p>","PeriodicalId":149,"journal":{"name":"ChemSusChem","volume":"19 21","pages":""},"PeriodicalIF":5.9,"publicationDate":"2026-11-03","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149310950","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Tracking and Tuning the C1/C2 Pathway: In Situ Spectroscopy and Mechanistic Insights Into Ethylene Glycol Oxidation on Metal-Based Catalysts 跟踪和调整C1/C2途径:在金属基催化剂上乙二醇氧化的原位光谱和机理见解
IF 5.9 2区 化学
ChemSusChem Pub Date : 2026-11-03 DOI: 10.1002/cssc.71186
Chaoqun Chang, Lu Zhao, Qi An
{"title":"Tracking and Tuning the C1/C2 Pathway: In Situ Spectroscopy and Mechanistic Insights Into Ethylene Glycol Oxidation on Metal-Based Catalysts","authors":"Chaoqun Chang,&nbsp;Lu Zhao,&nbsp;Qi An","doi":"10.1002/cssc.71186","DOIUrl":"https://doi.org/10.1002/cssc.71186","url":null,"abstract":"<p>The electrocatalytic ethylene glycol oxidation reaction (EGOR), using ethylene glycol (EG) obtained from hydrolyzed polyethylene terephthalate (PET) waste, offers a route for converting this plastic into valuable chemicals. However, steering selectivity between the C<sub>1</sub> and C<sub>2</sub> pathways remains challenging. This Review focuses on in situ spectroscopy for tracking interfacial reaction dynamics under operating conditions. We summarize how in situ Raman and Fourier transform infrared spectroscopy enable real-time identification of adsorbed intermediates and active species, providing mechanistic insights inaccessible to ex situ methods. We then evaluate noble-metal and non-noble-metal catalysts and discuss how their structural characteristics regulate EG adsorption, OH<sup>−</sup> activation, and intermediate conversion. Particular attention is given to tuning C<sub>1</sub>/C<sub>2</sub> branching to improve activity, selectivity, and poisoning resistance. We further survey EGOR applications in electrolysis systems, including pairing with hydrogen evolution for coproduction of value-added chemicals and hydrogen and coupling with CO<sub>2</sub> reduction or organic synthesis to construct energy-efficient electrochemical cells. Ultimately, such mechanistic understanding offers guidance for rational catalyst design and sustainable PET upcycling.</p>","PeriodicalId":149,"journal":{"name":"ChemSusChem","volume":"19 21","pages":""},"PeriodicalIF":5.9,"publicationDate":"2026-11-03","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149310874","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Functional Group-Driven Dissolution and Interfacial Instability in Naphthalene-Derived Organic Anodes for Li-Ion Storage 功能基驱动的萘衍生锂离子有机阳极溶解和界面不稳定性
IF 5.9 2区 化学
ChemSusChem Pub Date : 2026-11-03 DOI: 10.1002/cssc.71197
Michael Silvano, Nguyet N. T. Pham, Duc-Anh Le, Yu-Sheng Su
{"title":"Functional Group-Driven Dissolution and Interfacial Instability in Naphthalene-Derived Organic Anodes for Li-Ion Storage","authors":"Michael Silvano,&nbsp;Nguyet N. T. Pham,&nbsp;Duc-Anh Le,&nbsp;Yu-Sheng Su","doi":"10.1002/cssc.71197","DOIUrl":"https://doi.org/10.1002/cssc.71197","url":null,"abstract":"<p>The practical viability of small-molecule organic anodes is often limited by active material dissolution and the accompanying interfacial instability in liquid electrolytes. Herein, we investigate how functional group chemistry influences Li/Li<sup>+</sup> interactions, dissolution behavior, interfacial evolution, and electrochemical accessibility in naphthalene-derived organic anodes. Using naphthalene as a model framework, we systematically compare hydroxylated and carboxylated derivatives through combined computational, electrochemical, spectroscopic, and morphological analyses. Density functional theory (DFT) calculations reveal stronger localized Li<sup>+</sup> interactions at the vicinal dihydroxyl groups of 2,3-dihydroxynaphthalene (DHN) and the carboxyl group of 2-naphthoic acid (NPA) than in Naph and the monohydroxylated derivatives. However, this enhanced local affinity does not translate into improved electrochemical reversibility. Naphthalene and the monohydroxylated derivatives exhibit limited dissolution, relatively stable interfacial behavior, and sustained cycling performance over 1000 cycles. In contrast, DHN and NPA exhibit greater active material dissolution and more extensive interfacial reconstruction, resulting in reduced electrochemical accessibility and inferior reversibility. This work highlights the importance of balancing favorable Li/Li<sup>+</sup> interactions with resistance to dissolution and interfacial reconstruction to preserve electrochemically accessible active material in small-molecule organic anodes.</p>","PeriodicalId":149,"journal":{"name":"ChemSusChem","volume":"19 21","pages":""},"PeriodicalIF":5.9,"publicationDate":"2026-11-03","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://onlinelibrary.wiley.com/doi/epdf/10.1002/cssc.71197","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149310872","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Integrating Intrinsic Solid–Solid Phase Change and Flame Retardancy Into Closed-Loop Recyclable Polyimine Aerogels via Dynamic Covalent Networks 通过动态共价网络将固有固固相变和阻燃性集成到闭环可回收聚酰亚胺气凝胶中
IF 5.9 2区 化学
ChemSusChem Pub Date : 2026-11-03 DOI: 10.1002/cssc.71207
Yufei Cao, Shuo Yang, Siqi Lu, Zihe Lu, Muyang Li, Tao Yang, Wenwen Wu, Dongli Fan, Peng Zhu, Haiyan Ma, Jie Liu, Yufeng Cao, Tao Qian
{"title":"Integrating Intrinsic Solid–Solid Phase Change and Flame Retardancy Into Closed-Loop Recyclable Polyimine Aerogels via Dynamic Covalent Networks","authors":"Yufei Cao,&nbsp;Shuo Yang,&nbsp;Siqi Lu,&nbsp;Zihe Lu,&nbsp;Muyang Li,&nbsp;Tao Yang,&nbsp;Wenwen Wu,&nbsp;Dongli Fan,&nbsp;Peng Zhu,&nbsp;Haiyan Ma,&nbsp;Jie Liu,&nbsp;Yufeng Cao,&nbsp;Tao Qian","doi":"10.1002/cssc.71207","DOIUrl":"https://doi.org/10.1002/cssc.71207","url":null,"abstract":"<p>Organic aerogels are promising scaffolds for phase change materials (PCMs) in thermal management, but their inherent flammability and PCM leakage limit practical applications. In this work, we report a molecular design strategy for fully recyclable, bio-based polyimine aerogels (DPI-P<sub><i>x</i></sub>-OA<sub><i>y</i></sub>) that synergistically integrate intrinsic phase-change functionality, flame retardancy, and closed-loop recyclability within a single dynamic covalent network. A vanillin-derived organophosphate node (TFMP) was incorporated as a flame-retardant cross-linker, while octadecylamine (OA) served as a phase-change unit, achieving leakage-free thermal regulation with a melting enthalpy up to ~17.81 J/g. The resulting aerogels exhibited excellent processability, high load-bearing capacity, and self-extinguishing behavior with reduced heat release. Moreover, the OA side chains further improved thermal insulation through increased phonon scattering and latent heat absorption, collectively contributing to excellent infrared stealth and thermal protection. In addition, the aerogels also acted as high-capacity scaffolds for solid–liquid PCMs. Upon encapsulation of polyethylene glycol (PEG10K), the melting enthalpy further increased to ~147.4 J/g. Furthermore, the dynamic imine bonds enabled closed-loop monomer recycling under mild acidic conditions, further enhancing the material's sustainability. This work offers a unified platform for sustainable multifunctional aerogels that reconciles thermal storage, fire safety, and closed-loop recyclability.</p>","PeriodicalId":149,"journal":{"name":"ChemSusChem","volume":"19 21","pages":""},"PeriodicalIF":5.9,"publicationDate":"2026-11-03","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149310949","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Iodide-Mediated Charge Storage in Deep Eutectic Solvent Electrolytes for Nontoxic Printed Supercapacitors 用于无毒印刷超级电容器的深共晶溶剂电解质中碘化物介导的电荷存储
IF 5.9 2区 化学
ChemSusChem Pub Date : 2026-11-03 DOI: 10.1002/cssc.71194
Chirag Mevada, Aapo Kattainen, Jari Keskinen, Matti Mäntysalo
{"title":"Iodide-Mediated Charge Storage in Deep Eutectic Solvent Electrolytes for Nontoxic Printed Supercapacitors","authors":"Chirag Mevada,&nbsp;Aapo Kattainen,&nbsp;Jari Keskinen,&nbsp;Matti Mäntysalo","doi":"10.1002/cssc.71194","DOIUrl":"https://doi.org/10.1002/cssc.71194","url":null,"abstract":"<p>Deep eutectic solvents (DESs) are promising sustainable electrolytes for printed energy storage devices owing to their low toxicity, low cost, and tunable physicochemical properties. Herein, a redox-active DES electrolyte based on choline chloride–urea was developed for nontoxic printed symmetric supercapacitors (SCs) by incorporating potassium iodide (KI) as a charge-storage enhancer. The influence of KI concentration on electrolyte stability, rheological behavior, and electrochemical performance was systematically investigated. While the addition of 1 wt% water effectively suppressed DES crystallization during storage, KI introduced reversible iodide/triiodide redox reactions that enhanced charge storage beyond conventional electric double-layer capacitance (EDLC). The DES-1H<sub>2</sub>O-2.5KI electrolyte provided a balanced performance, with a specific capacitance of 55 F g<sup>−1</sup>@ 0.1 A g<sup>−1</sup>, an energy density of 24.8 W h kg<sup>−1</sup>, and capacitance retention of 98% after 10,000 cycles. Trasatti analysis revealed a balanced charge storage mechanism with contributions from both EDLC (47%) and pseudocapacitance (53%). In contrast, higher KI concentrations increased electrolyte viscosity and diffusion limitations, resulting in reduced electrochemical efficiency. The results demonstrate that controlled incorporation of iodide redox species provides an effective strategy for improving the performance of DES electrolytes while maintaining electrolyte stability and sustainability. These findings highlight the potential of redox-active DES electrolytes for sustainable printed SCs.</p>","PeriodicalId":149,"journal":{"name":"ChemSusChem","volume":"19 21","pages":""},"PeriodicalIF":5.9,"publicationDate":"2026-11-03","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://onlinelibrary.wiley.com/doi/epdf/10.1002/cssc.71194","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149310948","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Dual-Particle Aqueous Fe/Ni Semi-solid Flow Batteries With High Energy Density and Halved Energy Cost Enabled by Electrolyte Modulation 电解质调制可实现高能量密度、能量成本减半的双颗粒水Fe/Ni半固态液流电池。
IF 5.9 2区 化学
ChemSusChem Pub Date : 2026-10-30 DOI: 10.1002/cssc.71196
Xin Liu, Jiao Zheng, Daiqi Zhou, Qi Zhao, Changsheng Ding, Haitao Feng, Zhang Chen, Yuanyuan Cui, Yanfeng Gao
{"title":"Dual-Particle Aqueous Fe/Ni Semi-solid Flow Batteries With High Energy Density and Halved Energy Cost Enabled by Electrolyte Modulation","authors":"Xin Liu,&nbsp;Jiao Zheng,&nbsp;Daiqi Zhou,&nbsp;Qi Zhao,&nbsp;Changsheng Ding,&nbsp;Haitao Feng,&nbsp;Zhang Chen,&nbsp;Yuanyuan Cui,&nbsp;Yanfeng Gao","doi":"10.1002/cssc.71196","DOIUrl":"10.1002/cssc.71196","url":null,"abstract":"<p>Semi-solid flow batteries (SSFBs) break traditional solubility limits, yet sluggish electrochemical kinetics, parasitic hydrogen evolution, and high slurry viscosity severely restrict their practical energy density and cycling life. Herein, a dual-particle aqueous Fe/Ni SSFB is present that utilizes low-cost Fe<sub>2</sub>O<sub>3</sub> and Ni(OH)<sub>2</sub> particles as anode and cathode active materials, respectively. Through systematic electrolyte engineering, the bottlenecks of electrochemical performance and electrolyte viscosity are simultaneously addressed. Specifically, redox targeting is introduced to boost cathode kinetics, with trace additives concurrently suppressing anodic hydrogen evolution, enabling a 10 wt% Fe/Ni achieves an energy density boost from 3 to 21 Wh L<sup>−1</sup>, along with stable operation for 100 cycles. To break the viscosity-loading trade-off, functional dispersants are employed to halve the electrolyte viscosity. This breakthrough enables stable operation at 30 wt% solid loading, yielding an energy densities of 58 Wh L<sup>−1</sup> at 10 mA cm<sup>−2</sup> (6.7-fold higher than dispersant-free), which outperform the reported aqueous metal-based SSFBs in literature. Benefiting from the use of low-cost active materials and trace additives, the energy cost is merely 24 US$ kWh<sup>−1</sup> (vs ≥48 US$ kWh<sup>−1</sup> for reported SSFBs). This study provides a paradigm shift toward economically viable and high-performance SSFBs.</p>","PeriodicalId":149,"journal":{"name":"ChemSusChem","volume":"19 21","pages":""},"PeriodicalIF":5.9,"publicationDate":"2026-10-30","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149293469","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
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