ChemSusChemPub Date : 2025-09-04DOI: 10.1002/cssc.202402709
Guillaume Navallon, Federico Monaco, Katharina Märker, Peter Cloetens, Jakub Drnec, Duncan Atkins, Lionel Picard, Sandrine Lyonnard
{"title":"Ionic Conductivity of Composite Polymer Electrolyte: Clarifying the Role of the Interface with Nonconductive Particles.","authors":"Guillaume Navallon, Federico Monaco, Katharina Märker, Peter Cloetens, Jakub Drnec, Duncan Atkins, Lionel Picard, Sandrine Lyonnard","doi":"10.1002/cssc.202402709","DOIUrl":"https://doi.org/10.1002/cssc.202402709","url":null,"abstract":"<p><p>Solid-state electrolytes are considered as an enabler for batteries with extended energy density. Polymers are promising materials but show insufficient ion transport properties, a limitation that can be lifted by the fabrication of composite polymer electrolytes. Nevertheless, the role of the inorganic particles in tuning the conduction properties is often unclear, especially when inert fillers are added. Herein, poly(trimethylene carbonate) and alumina particles: α-Al<sub>2</sub>O<sub>3</sub>, γ-AlOOH and γ-Al<sub>2</sub>O<sub>3</sub> are mixed by two dispersion methods to prepare a series of composites. The correlations between microstructure, surface chemistry, and transport properties are studied, which are evaluated by combining synchrotron nanotomography, solid-state nuclear magnetic resonance, and electrochemical impedance spectroscopy, respectively. An increase of the conductivity by a factor of 1.9 ± 0.6 (1.4 ± 0.4) is observed for α-Al<sub>2</sub>O<sub>3</sub> (γ-AlOOH) while no beneficial effect of dispersion is seen for γ-Al<sub>2</sub>O<sub>3</sub>. It is found that dispersion of the particles is crucial, with an interfacial area between polymer matrix and inorganic fillers increased by a factor of 1.3-3 when the particles are dispersed. Moreover, the density of surface groups is estimated at the interface and correlations are found to the changes in conductivity, showing that interactions at the interface of the particles are one key parameter driving the composite performance.</p>","PeriodicalId":149,"journal":{"name":"ChemSusChem","volume":" ","pages":"e2402709"},"PeriodicalIF":6.6,"publicationDate":"2025-09-04","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144990962","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}
{"title":"A Small-Molecule Organic Cathode with Two Electron-Withdrawing Cyano Bonds for Li-Ion Batteries.","authors":"Jiahui Hu, Lingxiao Li, Wu Tang, Xuesong He, Lichuan He, Wentao Lv, Jiahao Zhang, Cong Fan","doi":"10.1002/cssc.202501151","DOIUrl":"https://doi.org/10.1002/cssc.202501151","url":null,"abstract":"<p><p>Perylene-3,4,9,10-tetracarboxylic dianhydride [PTCDA, theoretical specific capacity (C<sub>T</sub>) = 130 mAh g<sup>-1</sup>] is an efficient n-type organic cathode in Li-ion batteries with the median potential of ≈2.5 V (vs. Li). In order to improve its working potential, a new insoluble small-molecule organic cathode named 1,7-dicyano-perylene-tetracarboxylic dianhydride (PTCDA-2CN) is designed and synthesized with two electron-withdrawing groups cyano bonds (-CN). As expected, PTCDA-2CN can exhibit the high working potential ≈2.8 V (vs. Li) with its decreased lowest unoccupied molecular orbital energy, which is ≈0.3 V higher than PTCDA. And the introduction of two -CN groups can maintain the basis C<sub>T</sub> value of 121 mAh g<sup>-1</sup> for PTCDA-2CN. Consequently, PTCDA-2CN exhibits the good cathode performances in Li-ion half/full cells. In half cells, PTCDA-2CN can show the discharge capacities of 117-107 mAh g<sup>-1</sup> with the stable cycling retention of 91% during 100 cycles. Meanwhile, using the reduced state (LiC<sub>6</sub>) of graphite (C) as the anode, the LiC<sub>6</sub>//PTCDA-2CN full cells can also exhibit good performances of 116-98 at 50 mA g<sup>-1</sup> with the high median voltage of 2.7 V. PTCDA-2CN is one of the highest potentials ever reported for the n-type organic cathodes in Li-ion batteries.</p>","PeriodicalId":149,"journal":{"name":"ChemSusChem","volume":" ","pages":"e2501151"},"PeriodicalIF":6.6,"publicationDate":"2025-09-04","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144990883","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}
ChemSusChemPub Date : 2025-09-04DOI: 10.1002/cssc.202501270
Shasha Chen, Xiaoying Long, Faysal Md, Kailong Hu, Kaikai Li
{"title":"Probing MnO<sub>2</sub> Cycling Stability in Aqueous Zinc-Ion Batteries using Chemical Strain Analysis.","authors":"Shasha Chen, Xiaoying Long, Faysal Md, Kailong Hu, Kaikai Li","doi":"10.1002/cssc.202501270","DOIUrl":"https://doi.org/10.1002/cssc.202501270","url":null,"abstract":"<p><p>The mechanical degradation of cathodes during charge-discharge cycling poses a critical limitation to the cycle life of aqueous zinc-ion batteries (AZIBs). Although the degradation of MnO<sub>2</sub> cathodes has been extensively investigated, the underlying reaction mechanisms have long remained a subject of debate, and the associated mechanical evolution during cycling is still poorly understood. In this work, a comprehensive investigation of electrochemical phase transitions and chemical strain evolution in δ-MnO<sub>2</sub> cathode is presented using a custom-built in situ strain testing system based on digital image correlation. The results reveal that the discharge-charge mechanism of δ-MnO<sub>2</sub> proceeds through initial cointercalation of H<sup>+</sup> and Zn<sup>2+</sup> causing elastic deformation, followed by phase transformation to ZnMn<sub>2</sub>O<sub>4</sub>. During charging, this phase transformation coupled with ZnMn<sub>3</sub>O<sub>7</sub> formation induces irreversible plastic deformation, generating substantial residual strain and cathode volume expansion. Increasing current density can effectively reduce residual strain by suppressing phase transformation, thereby enhancing electrode cycling stability.</p>","PeriodicalId":149,"journal":{"name":"ChemSusChem","volume":" ","pages":"e202501270"},"PeriodicalIF":6.6,"publicationDate":"2025-09-04","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144990906","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}
ChemSusChemPub Date : 2025-09-03DOI: 10.1002/cssc.202501165
Yebin Choi, Seohyeon Kim, Yulan Li, Byeong Jun Cha, Hyun Ook Seo, Young Dok Kim
{"title":"Photocatalytic Activation of Dealuminated Zeolite through In Situ Formation of Defective Graphene.","authors":"Yebin Choi, Seohyeon Kim, Yulan Li, Byeong Jun Cha, Hyun Ook Seo, Young Dok Kim","doi":"10.1002/cssc.202501165","DOIUrl":"https://doi.org/10.1002/cssc.202501165","url":null,"abstract":"<p><p>Adsorbents such as zeolite are widely used for volatile organic compounds (VOCs) removal, but a practical challenge is the decrease in VOCs removal efficiency under humid environment by competitive adsorption between water vapor and VOCs, which requires frequent regeneration using external energy. A combination of zeolites with photocatalytic materials can address this issue by oxidizing adsorbed VOCs from the zeolite surface to CO<sub>2</sub> gas under light irradiation. Herein, the in situ formation of photocatalytic active defect-rich graphene is presented on a commercial zeolite surface (ZSM-5) when properly dealuminated ZSM-5 is exposed to an acetaldehyde/humid air mixture under visible light. This in situ photocatalytic activation occurs when a critical amount of local surface coverage of acetaldehyde and water molecules is achieved on a dealuminated zeolite surface under visible light. The findings not only provide a deeper understanding of VOCs removal by zeolite but also suggest a new and simple approach to enhancing the performance of zeolite for VOCs removal through the combination with a photocatalytic material.</p>","PeriodicalId":149,"journal":{"name":"ChemSusChem","volume":" ","pages":"e2501165"},"PeriodicalIF":6.6,"publicationDate":"2025-09-03","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144990910","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}
ChemSusChemPub Date : 2025-09-03DOI: 10.1002/cssc.202501318
Daqi Song, Mutian Ma, Zhangyi Zheng, Shiwei Mei, Zhihe Wei, Wenjun Yang, Jun Zhong, Zhao Deng, Yang Peng
{"title":"Stabilizing Reticular Frameworks and Modulating Interfacial Water via Conductive Polymer Encapsulation in Metal-Organic Frameworks Electrocatalysts for Efficient Methane Production.","authors":"Daqi Song, Mutian Ma, Zhangyi Zheng, Shiwei Mei, Zhihe Wei, Wenjun Yang, Jun Zhong, Zhao Deng, Yang Peng","doi":"10.1002/cssc.202501318","DOIUrl":"10.1002/cssc.202501318","url":null,"abstract":"<p><p>The electrochemical reduction of CO<sub>2</sub> to CH<sub>4</sub> offers a promising pathway for renewable energy storage, yet remains limited by sluggish kinetics, poor catalyst stability, and competing hydrogen evolution reactions (HER). Herein, a host-guest strategy is reported for engineering metal-organic frameworks (MOFs) through the encapsulation of conductive polymers to stabilize reticular skeletons and regulate interfacial water for efficient CO<sub>2</sub>-to-CH<sub>4</sub> conversion. Specifically, polypyrrole (PPy) and polyaniline (PANI) are confined within Cu-anchored UiO-67 frameworks, resulting in hybrid catalysts-PPy@Cu-UiO-67 and PANI@Cu-UiO-67-with preserved crystallinity and enhanced electronic conductivity. Among them, PANI@Cu-UiO-67 exhibits superior CH<sub>4</sub> Faradaic efficiency (FE<sub>CH4</sub> up to 71.1%), outperforming PPy@Cu-UiO-67 and unmodified Cu-UiO-67. Spectroscopic analysis reveals that the polymers reinforce structural integrity and induce distinct perturbations in the interfacial water network. In situ Raman and attenuated total reflection surface-enhanced infrared absorption spectroscopy measurements identify the dominance of weakly hydrogen-bonded water (2-HB·H<sub>2</sub>O) at the PANI-modified interface, which supports rapid proton transfer while suppressing HER. This study offers a rational design strategy for MOF electrocatalysts by integrating conductive polymers to modulate both the electronic and interfacial environments for high-efficiency methane production.</p>","PeriodicalId":149,"journal":{"name":"ChemSusChem","volume":" ","pages":"e202501318"},"PeriodicalIF":6.6,"publicationDate":"2025-09-03","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144937345","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}
ChemSusChemPub Date : 2025-09-03DOI: 10.1002/cssc.202501352
Lulu Deng, Hailong He, Zhonghao Chen, Yao Meng, Lei Wang
{"title":"Efficient Recovery and Fast Hydrolysis of Polyethylene Terephthalate by Dihydrolevoglucosenone (Cyrene).","authors":"Lulu Deng, Hailong He, Zhonghao Chen, Yao Meng, Lei Wang","doi":"10.1002/cssc.202501352","DOIUrl":"10.1002/cssc.202501352","url":null,"abstract":"<p><p>Polyethylene terephthalate (PET) is a versatile, relatively low-cost thermoplastic polymer, but its nonbiodegradability and extensive use lead to significant accumulation and environmental risks. The main roadblocks of current plastic recycling technologies include low-quality recycled plastics and inefficient degradation under harsh conditions, which highlights the urgent need to develop efficient and sustainable recycling processes. Herein, for the first time, a strategy is developed using bio-based solvent dihydrolevoglucosenone (Cyrene) for efficient recycling of waste PET-to-polymer or monomer. In this study, Cyrene effectively dissolves PET at 165 °C within 20 min. Furthermore, PET dissolved in Cyrene and regenerated by ethanol as an antisolvent, exhibiting excellent chemical and thermal stability with minimal degradation. Cyrene also functions as a cosolvent for the alkaline hydrolysis of PET, resulting in ≈100% PET degradation to terephthalic acid (TPA) with a yield of 98.2% within 18 min at 80 °C. The presence of Cyrene enhances the interface compatibility between PET and solvent, while the hydroxyl groups in EG form hydrogen bonds with Cyrene, facilitating the interaction between PET and NaOH. Overall, this study contributes to the advancement of solvent-based recycling strategies for the cost-effective recovery of PET waste.</p>","PeriodicalId":149,"journal":{"name":"ChemSusChem","volume":" ","pages":"e202501352"},"PeriodicalIF":6.6,"publicationDate":"2025-09-03","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144937214","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}
ChemSusChemPub Date : 2025-09-02DOI: 10.1002/cssc.70082
Zhe Wan, Liping Yang, Zhen Liang, Shuxia Li, Li Chen, Xin Liu, Peng Li, Yangjun Xia, Ning Kang, Chenglong Wang
{"title":"Front Cover: Improving Moisture Proof and Heat Dissipation of Perovskite Solar Cells with Metal Oleate Passivation Layer (ChemSusChem 17/2025)","authors":"Zhe Wan, Liping Yang, Zhen Liang, Shuxia Li, Li Chen, Xin Liu, Peng Li, Yangjun Xia, Ning Kang, Chenglong Wang","doi":"10.1002/cssc.70082","DOIUrl":"10.1002/cssc.70082","url":null,"abstract":"<p><b>The Front Cover</b> highlights a multifunctional passivation strategy for perovskite solar cells that uses europium oleate (Eu(OA)<sub>3</sub>) coated on both top and side surfaces of the perovskite film. This layer effectively passivates the surface defects of the perovskite film, and improves the moisture resistance and heat dissipation of the film, thereby improving the photovoltaic performance and working stability of perovskite solar cells. More information can be found in the Research Article by Y. Xia, N. Kang, C. Wang and co-workers (DOI: 10.1002/cssc.202500196).\u0000 <figure>\u0000 <div><picture>\u0000 <source></source></picture><p></p>\u0000 </div>\u0000 </figure></p>","PeriodicalId":149,"journal":{"name":"ChemSusChem","volume":"18 17","pages":""},"PeriodicalIF":6.6,"publicationDate":"2025-09-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://chemistry-europe.onlinelibrary.wiley.com/doi/epdf/10.1002/cssc.70082","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144927669","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}
ChemSusChemPub Date : 2025-09-02DOI: 10.1002/cssc.202500656
Ao Yu, Qi Huang, Wenhao Yang, Ping Peng, Fang-Fang Li
{"title":"Fullerene: A Potential Platform for Hydrogen Evolution Reaction.","authors":"Ao Yu, Qi Huang, Wenhao Yang, Ping Peng, Fang-Fang Li","doi":"10.1002/cssc.202500656","DOIUrl":"https://doi.org/10.1002/cssc.202500656","url":null,"abstract":"<p><p>Hydrogen energy is widely regarded as a promising clean energy alternative to fossil fuels due to its high energy density and excellent environmental compatibility. Electrochemical water splitting has emerged as one of the most viable technologies for large-scale hydrogen production, driving the requirements to develop efficient hydrogen evolution reaction (HER) catalysts. Fullerenes, with their unique molecular architecture and electronic properties, are emerging as a highly promising class of electrocatalysts for the HER, offering exceptional catalytic activity and stability. This concept summarizes the recent advancements in fullerene-based electrocatalysts, highlighting the dual functionality of fullerenes as both a template for synthesizing atomically dispersed, subnanometer metal clusters and a modulator of electronic interactions at catalytically active interfaces. These developments have not only enhanced HER efficiency but also unlocked innovative possibilities for deploying fullerene-based electrocatalysts across a wider spectrum of catalytic transformations.</p>","PeriodicalId":149,"journal":{"name":"ChemSusChem","volume":" ","pages":"e202500656"},"PeriodicalIF":6.6,"publicationDate":"2025-09-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144937259","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}
ChemSusChemPub Date : 2025-09-02DOI: 10.1002/cssc.202501601
Xiaohui Zhang, Yuantao Miao, Shan Tang
{"title":"High-Density Polyethylenes with Dual Degradability Enabled by In-Chain Photolyzable and Mechanoresponsive Units.","authors":"Xiaohui Zhang, Yuantao Miao, Shan Tang","doi":"10.1002/cssc.202501601","DOIUrl":"https://doi.org/10.1002/cssc.202501601","url":null,"abstract":"<p><p>Polyethylenes are the most widely produced plastics but are also major pollutants due to their exceptional chemical stability. Developing environmentally friendly alternatives that can simultaneously respond to multiple degradation triggers to replace conventional polyolefins is desirable. Herein, a novel class of high-density polyethylene materials that degrade upon exposure to light irradiation and mechanical force is reported. This dual degradability is achieved by incorporating in-chain photolyzable carbonyl and mechanoresponsive cyclobutane units via catalytic terpolymerization of ethylene, CO, and cyclobutene derivatives. Incorporating low densities of carbonyl and mechanoresponsive units has minimal impact on the thermomechanical properties of the polyethylene. Mechanical activation through ball-milling triggers hydrolytic degradation via force-induced cycloreversion of the cyclobutane units. This dual degradability can potentially reduce their environmental persistence in the environment.</p>","PeriodicalId":149,"journal":{"name":"ChemSusChem","volume":" ","pages":"e2501601"},"PeriodicalIF":6.6,"publicationDate":"2025-09-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144937202","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}
ChemSusChemPub Date : 2025-09-02DOI: 10.1002/cssc.202501351
Tianhua Chen, Yongzheng Zhang, Simeng Wang, Jin Li, Hongzhen Lin, Dusan Losic, Shimou Chen, Jian Wang
{"title":"Interfacial Li<sup>+</sup> Diffusion Booster Accelerated by Enhanced Metal-Organic Framework Sieving and Wettability for High-Voltage Solid-State Lithium Metal Batteries.","authors":"Tianhua Chen, Yongzheng Zhang, Simeng Wang, Jin Li, Hongzhen Lin, Dusan Losic, Shimou Chen, Jian Wang","doi":"10.1002/cssc.202501351","DOIUrl":"10.1002/cssc.202501351","url":null,"abstract":"<p><p>Solid-state lithium metal batteries (SSLMBs) are promising for realizing higher energy density. However, the poor interfacial Li<sup>+</sup> transport kinetics and Li dendrite growth inhibit SSLMBs, leading to sluggish interfacial ion diffusion and depressive lifespan, which is attributed to high barriers blocked by anions or interface space in solid-state electrolytes. Herein, a flexible solid-state polymer skeleton employed with ionic liquid and metal-organic frameworks (PIM) electrolyte is proposed to strengthen interfacial Li ion exchange by improving the Li<sup>+</sup> sieving effect and interfacial wettability. Thanks to the immobilization effect of TFSI<sup>-</sup> anions affected by positive metal atom centers and pore morphology, the PIM electrolyte exhibits exceptional properties, i.e., a high ionic conductivity up to 3.1 mS cm<sup>-1</sup> at 60 °C and an improved Li<sup>+</sup> transference number of 0.65, enabling symmetric cells of Li metal to run steadily for over 1000 h with lower voltage hysteresis (25 mV). Meanwhile, matching with high-voltage electrodes, the solid-state PIM electrolyte exhibits good compatibility and stability toward LiNi<sub>0.6</sub>Co<sub>0.2</sub>Mn<sub>0.2</sub>O<sub>2</sub> and LiFePO<sub>4</sub> electrodes, showing the capacity retentions of 85.5% and 96.5% after 120 and 400 cycles, respectively. This work suggests low interfacial diffusion resistances and high compatibility for make it a promising candidate for future solid-state battery.</p>","PeriodicalId":149,"journal":{"name":"ChemSusChem","volume":" ","pages":"e202501351"},"PeriodicalIF":6.6,"publicationDate":"2025-09-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144937200","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}