ChemSusChem最新文献_第3页

Rate-Dependent Capacity Evolution and Time-Controlled Degradation of MnO2 Cathodes in Aqueous Zinc-Ion Batteries 锌离子电池中MnO2阴极的速率依赖容量演化和时间控制降解

IF 5.9 2区化学

ChemSusChem Pub Date : 2026-10-10 DOI: 10.1002/cssc.71142

Di Zhu, Yangyang Wang, Yuqi Pan, Jiacheng Wu, Justin Prabowo, Mingyao Gu, Li Wei, Yuan Chen

{"title":"Rate-Dependent Capacity Evolution and Time-Controlled Degradation of MnO2 Cathodes in Aqueous Zinc-Ion Batteries","authors":"Di Zhu, Yangyang Wang, Yuqi Pan, Jiacheng Wu, Justin Prabowo, Mingyao Gu, Li Wei, Yuan Chen","doi":"10.1002/cssc.71142","DOIUrl":"https://doi.org/10.1002/cssc.71142","url":null,"abstract":"The excellent cycling stability of MnO2 cathodes in aqueous zinc-ion batteries (AZIBs) at high current densities often deteriorates at lower current densities, yet the origin of this rate-dependent behavior remains unclear. Here, we uncover the interplay between current density and cumulative cycling time by tracking the electrochemical and structural evolution of α-MnO2 cathodes in Mn2+-containing electrolytes. Low current densities promote more extensive Mn2+-mediated dissolution–deposition, leading to greater accumulation of a porous, metastable Zn–Mn–O intermediate and pronounced capacity enhancement. Notably, while the magnitude of the capacity enhancement strongly depends on current density, the capacity maximum occurs within a relatively narrow cumulative cycling time of ~350–450 h across the tested current densities in 2 M ZnSO4 + 0.2 M MnSO4 electrolyte. Upon prolonged cycling, the metastable Zn–Mn–O intermediate gradually diminishes, accompanied by the emergence of crystalline ZnMn2O4, increased electrode polarization, and rapid capacity fading. These findings reveal that current density affects the extent of capacity enhancement, whereas cumulative cycling time provides a more consistent measure of the subsequent capacity evolution than cycle number. This time-domain understanding explains the contrasting cycling behavior of MnO2 cathodes at different current densities and provides mechanistic guidance for evaluating and improving their long-term durability in AZIBs.","PeriodicalId":149,"journal":{"name":"ChemSusChem","volume":"19 19","pages":""},"PeriodicalIF":5.9,"publicationDate":"2026-10-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://onlinelibrary.wiley.com/doi/epdf/10.1002/cssc.71142","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149146121","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

θ-Metallacarboranes as Sustainable Photoredox Oxidation Catalysts of Unsaturated Fatty Acids From Oil and Pork Lard θ-金属碳硼烷作为油和猪油中不饱和脂肪酸的可持续光氧化还原催化剂。

IF 5.9 2区化学

ChemSusChem Pub Date : 2026-10-10 DOI: 10.1002/cssc.71113

Isabel Guerrero, Clara Viñas, Isabel Romero, Rosario Núñez, Francesc Teixidor

{"title":"θ-Metallacarboranes as Sustainable Photoredox Oxidation Catalysts of Unsaturated Fatty Acids From Oil and Pork Lard","authors":"Isabel Guerrero, Clara Viñas, Isabel Romero, Rosario Núñez, Francesc Teixidor","doi":"10.1002/cssc.71113","DOIUrl":"10.1002/cssc.71113","url":null,"abstract":"The sustainable management and valorization of unsaturated fatty acid-rich lipid streams is a key challenge within circular economy strategies. Herein, we present a proof of concept for the photoredox oxidation of unsaturated fatty acids using θ-metallacarborane complexes Na[Co(1,2-C2B9H11)2] ([Na]1) and Na[Fe(1,2-C2B9H11)2] ([Na]2) as water-soluble, earth-abundant photoredox catalysts. Commercial sunflower oil and pork lard served as convenient model systems mimicking waste lipid streams, while targeting future application to postconsumer used cooking oils. Under UVA irradiation in aqueous media, these complexes convert oleic- and linoleic-acid derivatives into epoxides, vicinal diols and shorter-chain oxygenated acids, with reaction selectivity finely tuned by pH, irradiation time and oxidant. Notably, [Na]1 exhibits superior oxidative power and acts as a “molecular scissor,” promoting C─C bond cleavage of vicinal diols and enabling the formation of mono- and dicarboxylic acids such as pelargonic and azelaic acids, valuable nonpetroleum-based building blocks. Sodium persulfate affords high conversions with controlled over-oxidation, while O2 enhances diol selectivity. θ-Metallacarboranes thus emerge as a sustainable platform for upgrading waste lipid streams into value-added chemicals in water, advancing circular economy goals without competing with food supply chains.","PeriodicalId":149,"journal":{"name":"ChemSusChem","volume":"19 19","pages":""},"PeriodicalIF":5.9,"publicationDate":"2026-10-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149163501","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

Toward Integrated Upcycling of Lithium-Ion Battery: Advances and Outlooks 锂离子电池集成升级回收：进展与展望

IF 5.9 2区化学

ChemSusChem Pub Date : 2026-10-10 DOI: 10.1002/cssc.71122

Jingkun Wu, Zixiang Meng, Yuyang Yi, Jingyu Sun

引用次数: 0

Confined Phase Transition Infiltration Coupled With In Situ Pore Sealing: Constructing Hard Carbon Rich in Closed Pore for Plateau-Capacity-Dominated Sodium Storage 封闭相变入渗与原位封孔耦合：在封闭孔中构建富硬碳用于高原容量为主的钠储存

IF 5.9 2区化学

ChemSusChem Pub Date : 2026-10-10 DOI: 10.1002/cssc.71134

Wenbo Hou, Xiaoxian Xu, Lili Ma, Wancheng Li, Hui Peng, Guofu Ma, Lei Zhu, Yuxi Xu

{"title":"Confined Phase Transition Infiltration Coupled With In Situ Pore Sealing: Constructing Hard Carbon Rich in Closed Pore for Plateau-Capacity-Dominated Sodium Storage","authors":"Wenbo Hou, Xiaoxian Xu, Lili Ma, Wancheng Li, Hui Peng, Guofu Ma, Lei Zhu, Yuxi Xu","doi":"10.1002/cssc.71134","DOIUrl":"https://doi.org/10.1002/cssc.71134","url":null,"abstract":"Biomass-derived hard carbon (HC) is a promising candidate for anode materials in sodium-ion batteries (SIBs). However, abundant open pores generated during activation process often lead to severe proliferation of the solid electrolyte interphase (SEI) and irreversible Na+ consumption, severely compromising the initial Coulombic efficiency (ICE) and low-voltage plateau capacity. This work proposes a synergistic strategy of confined phase transition infiltration and in situ pore sealing, using waste green tea as a precursor to construct a HC anode dominated by plateau capacity. Low dose of ZnCl2 induces controllable hydrolysis and aromatization of cellulose and generate nanoscale open pores. These pores act as confined microreactors, inducing an in situ chemical vapor deposition like carbon growth that effectively “stitching” the open voids into solvent sieving closed pores. Consequently, it delivers a remarkable ICE of 79.1%, a high reversible capacity of 342.3 mAh g−1 at 0.1 A g−1, and robust cycling stability (86.2% retention after 1000 cycles at 1.0 A g−1). In-/ex situ analysis reveals that its reversible sodium storage mechanism encompasses a triple synergy of defect adsorption, interlayer intercalation, and closed pore filling with quasi metallic sodium clusters. The confined pore sealing engineering strategy provides a robust paradigm for designing high-performance HC anodes.","PeriodicalId":149,"journal":{"name":"ChemSusChem","volume":"19 19","pages":""},"PeriodicalIF":5.9,"publicationDate":"2026-10-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149146119","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

Hydrolysis of 1,4-Butanediol-Derived Polyesters Into Tetrahydrofuran and Dicarboxylic Acids Over Lewis Acidic Ionic Liquids 1,4-丁二醇衍生聚酯在路易斯酸性离子液体上水解成四氢呋喃和二羧酸

IF 5.9 2区化学

ChemSusChem Pub Date : 2026-10-10 DOI: 10.1002/cssc.71121

Ying Wang, Wei Zeng, Yusi Wang, Hui Zhang, Rongxiang Li, Fengtao Zhang, Xiaoqian Chang, Yanfei Zhao, Zhimin Liu

{"title":"Hydrolysis of 1,4-Butanediol-Derived Polyesters Into Tetrahydrofuran and Dicarboxylic Acids Over Lewis Acidic Ionic Liquids","authors":"Ying Wang, Wei Zeng, Yusi Wang, Hui Zhang, Rongxiang Li, Fengtao Zhang, Xiaoqian Chang, Yanfei Zhao, Zhimin Liu","doi":"10.1002/cssc.71121","DOIUrl":"https://doi.org/10.1002/cssc.71121","url":null,"abstract":"Chemical transformation of discarded polyesters into high-value chemicals is of great significance for advancing circular economy and sustainable development. Herein, we report a facile and efficient strategy for one-pot conversion of 1,4-butanediol-based polyesters (BDPs) via equivalent water hydrolysis. The reaction is achieved over 1-butyl-3-methyl-imidazolium chloride-ZnCl2-based ionic liquids ([BMIm][ZnnCl2n + 1]) under mild conditions (e.g., 120 °C), producing tetrahydrofuran (THF) and corresponding dicarboxylic acids. Among the designed ionic liquids, [BMIm][Zn4Cl9] showed the optimal catalytic performance, affording dicarboxylic acids and THF in excellent yields. Moreover, the catalyst possesses excellent recyclability and can be reused for five consecutive runs without obvious activity attenuation. Mechanism investigation endorses that BDPs are first hydrolyzed to generate acyloxyl alcohol intermediates, which are further converted into THF and dicarboxylic acids through ring-closing C─OH/C─O metathesis under the cooperation of cation-anion pairs in the ionic liquid catalyst. This work establishes a simple, green, and novel protocol for the selective degradation and valorization of BDPs, holding great potential for practical industrial applications.","PeriodicalId":149,"journal":{"name":"ChemSusChem","volume":"19 19","pages":""},"PeriodicalIF":5.9,"publicationDate":"2026-10-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149146117","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

Highly Active Pd Clusters Enabled With Controllable Oxygen Vacancy for the Synergistic Decarbonylation of Furfural to Furan 具有可控氧空位的高活性Pd簇用于糠醛协同脱羰制呋喃。

IF 5.9 2区化学

ChemSusChem Pub Date : 2026-10-08 DOI: 10.1002/cssc.71093

Xinru Zhao, Haijun Deng, Longyang Wang, Ouyang Liu, Dandan Han, Armin Rezayan, Dan Wu, Zongwu Zhang, Qianli Ma, Xinqing Chen, Jianshe Wang, Yongsheng Zhang, Chunbao Xu

{"title":"Highly Active Pd Clusters Enabled With Controllable Oxygen Vacancy for the Synergistic Decarbonylation of Furfural to Furan","authors":"Xinru Zhao, Haijun Deng, Longyang Wang, Ouyang Liu, Dandan Han, Armin Rezayan, Dan Wu, Zongwu Zhang, Qianli Ma, Xinqing Chen, Jianshe Wang, Yongsheng Zhang, Chunbao Xu","doi":"10.1002/cssc.71093","DOIUrl":"10.1002/cssc.71093","url":null,"abstract":"Precisely regulated metal clusters are crucial for maximizing the utilization efficiency of active metal atoms. In this study, we controllably introduced oxygen vacancy (Ov) into TiO2 via H2 reduction to regulate the assembly of Pd atoms for furfural decarbonylation. The optimized Pd/TiO2 catalyst with smaller Pd clusters and a suitable oxygen vacancy concentration achieved a 99.9% furfural conversion and a 92.4% furan selectivity at 200 °C and 0.3 MPa N2 pressure, showing high catalytic performance under relatively mild conditions. Structural characterizations revealed that oxygen vacancies acted as anchoring sites for Pd species, and an appropriate vacancy concentration favored the formation of highly dispersed Pd clusters rather than larger Pd nanoparticles. Comprehensive structural and electronic analyses revealed strong interactions between Pd species and oxygen-vacant TiO2, leading to the formation of Pd2+-Ov-Ti interfacial sites. These interfacial sites promote carbonyl activation and CO elimination, while adjacent Pd0 sites facilitated H transfer to produce furan. This work not only develops a highly efficient and tunable Pd-based catalyst for the furfural decarbonylation, but also provides a versatile strategy for optimizing catalytic interface via oxygen vacancies.","PeriodicalId":149,"journal":{"name":"ChemSusChem","volume":"19 19","pages":""},"PeriodicalIF":5.9,"publicationDate":"2026-10-08","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149134527","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

Photobiocatalytic Linear Deracemization of β-Hydroxynitriles β-羟基腈的光生物催化线性脱羧。

IF 5.9 2区化学

ChemSusChem Pub Date : 2026-10-06 DOI: 10.1002/cssc.71108

Sara Filgueira, Fernando López-Gallego, Vicente Gotor-Fernández

引用次数: 0

Dual Porphyrin Sensitized Photocatalytic System for Visible-Light-Driven CO2 Reduction 可见光驱动CO2还原的双卟啉敏化光催化系统。

IF 5.9 2区化学

ChemSusChem Pub Date : 2026-10-06 DOI: 10.1002/cssc.71128

Anna Katsari, Emmanouil Nikoloudakis, Georgios Charalambidis, Antonios Iliakis, Fabrice Odobel, Emmanuel Stratakis

{"title":"Dual Porphyrin Sensitized Photocatalytic System for Visible-Light-Driven CO2 Reduction","authors":"Anna Katsari, Emmanouil Nikoloudakis, Georgios Charalambidis, Antonios Iliakis, Fabrice Odobel, Emmanuel Stratakis","doi":"10.1002/cssc.71128","DOIUrl":"10.1002/cssc.71128","url":null,"abstract":"Dye-sensitized photocatalysis offers a powerful strategy for combining the molecular selectivity of transition-metal catalysts with the robustness and charge-separation capabilities of semiconductor materials. Herein, we report a dual porphyrin–sensitized TiO2 platform for visible-light-driven CO2 reduction, integrating a Zn-porphyrin photosensitizer with newly designed Fe-porphyrin catalysts bearing urea-based secondary-sphere functionalities. These hydrogen-bonding motifs promote CO2 preorganization and stabilization of key reduced intermediates at the metal center. Systematic comparison of homogeneous and heterogeneous systems reveals a pronounced enhancement in activity and durability upon immobilization onto TiO2 nanoparticles. Optimization studies demonstrate that catalytic activity is strongly governed by both sacrificial electron donor (SED) availability and proton concentration. Under anhydrous conditions, increased SED concentration boosts turnover numbers, while the introduction of controlled amounts of water enhances proton-coupled electron transfer but ultimately compromises catalyst stability at higher concentrations. Under optimized conditions, the best-performing assembly achieves turnover numbers (TONs) exceeding 15,000 after 96 h of irradiation, representing, to the best of our knowledge, the highest reported TON for Fe-porphyrin-based dye-sensitized photocatalytic systems (DSPs). These findings highlight the delicate balance between electron and proton management in dye-sensitized architectures and provide key design principles for developing durable and efficient molecular–semiconductor hybrids for solar-driven CO2 conversion.","PeriodicalId":149,"journal":{"name":"ChemSusChem","volume":"19 19","pages":""},"PeriodicalIF":5.9,"publicationDate":"2026-10-06","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.ncbi.nlm.nih.gov/pmc/articles/PMC13641692/pdf/","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149101895","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

Emerging Applications of CO2-Based Polyurethanes: Bridging Material Sustainability and High-Performance Engineering 二氧化碳基聚氨酯的新兴应用：桥梁材料的可持续性和高性能工程。

IF 5.9 2区化学

ChemSusChem Pub Date : 2026-10-04 DOI: 10.1002/cssc.71132

Kihyuk Sung, Hye-Young Jang

{"title":"Emerging Applications of CO2-Based Polyurethanes: Bridging Material Sustainability and High-Performance Engineering","authors":"Kihyuk Sung, Hye-Young Jang","doi":"10.1002/cssc.71132","DOIUrl":"10.1002/cssc.71132","url":null,"abstract":"Carbon dioxide-derived polyols (CO2-polyols), synthesized via the copolymerization of CO2 with epoxides, have emerged as a compelling sustainable alternative to petroleum-based polyols for polyurethane (PU) manufacturing, offering the dual benefit of sequestering waste CO2 and reducing reliance on fossil feedstocks. However, the carbonate linkages embedded within the CO2-polyol backbone impart a chain rigidity that alters intermolecular interactions and physico-mechanical behavior relative to conventional polyols, creating uncertainty over how CO2 incorporation translates into end-use performance and slowing industrial adoption despite clear environmental incentives. This review maps the diverse application frontiers of CO2-polyol-derived PUs. Specifically, we highlight their critical roles in adhesives, coatings, thermal stimuli- responsive shape-memory materials, waterborne PUs with enhanced hydrolytic and oxidative resistance, lithium-ion battery binders, and polyurethane foams. Across these systems, we describe how tuning the carbonate unit content and polyol functionality allows the rigidity, crosslink density, and thermal transitions of the resulting PUs to be precisely engineered, often matching or exceeding the performance of conventional counterparts while retaining a favorable sustainability profile. Collectively, this review provides a practical design framework to accelerate the transition of CO2-polyol-based PUs from laboratory-scale demonstrations to industrially viable, sustainable materials.","PeriodicalId":149,"journal":{"name":"ChemSusChem","volume":"19 19","pages":""},"PeriodicalIF":5.9,"publicationDate":"2026-10-04","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.ncbi.nlm.nih.gov/pmc/articles/PMC13635276/pdf/","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149101853","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

Insights Into the Oxygen Evolution Reaction on an Mn-Bearing Hematite Electrocatalyst in an Acidic Electrolyte 含锰赤铁矿电催化剂在酸性电解液中的析氧反应研究。

IF 5.9 2区化学

ChemSusChem Pub Date : 2026-10-04 DOI: 10.1002/cssc.71101

Moritz Karl Rosenthal, Kim Eklund, Eeva-Leena Rautama, Lilian Moumaneix, Polina Kalachikova, Nastaran Farrahi, Xiangze Kong, Antti J. Karttunen, Tanja Kallio

{"title":"Insights Into the Oxygen Evolution Reaction on an Mn-Bearing Hematite Electrocatalyst in an Acidic Electrolyte","authors":"Moritz Karl Rosenthal, Kim Eklund, Eeva-Leena Rautama, Lilian Moumaneix, Polina Kalachikova, Nastaran Farrahi, Xiangze Kong, Antti J. Karttunen, Tanja Kallio","doi":"10.1002/cssc.71101","DOIUrl":"10.1002/cssc.71101","url":null,"abstract":"Platinum group metal-free catalysts have attracted significant attention due to the high cost and scarcity of iridium for the oxygen evolution reaction (OER) in acidic media. However, the fundamental understanding of catalyst formation and active species under acidic conditions remains limited. In this work, iron–manganese oxide catalysts based on <math></math> were synthesized via a hydrothermal approach followed by calcination. The as-prepared materials consist of poorly crystalline Fe2O3/FeOOH and MnO2 phases that transform into a disordered mixed-metal oxide upon thermal treatment. Raman spectroscopy supported by quantum-chemical calculations indicates the formation of a solid solution in which Mn induces lattice distortion and partial disruption of Fe─O─Fe bonding within the hematite structure. The highest OER activity and stability are obtained after calcination at 350 °C, corresponding to an optimum degree of structural disorder for adsorption processes. Operando Raman spectroscopy reveals potential-dependent spectral changes, including the emergence of a band at ≈450 cm−1 and enhanced intensity at ≈610 cm−1, indicating the formation of high-valent surface species during OER operation. These findings suggest cooperative Fe–Mn interactions and a possible role for substitution-induced structural disorder in promoting OER activity.","PeriodicalId":149,"journal":{"name":"ChemSusChem","volume":"19 19","pages":""},"PeriodicalIF":5.9,"publicationDate":"2026-10-04","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.ncbi.nlm.nih.gov/pmc/articles/PMC13635278/pdf/","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149101824","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