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Arginine as a Multifunctional Additive for High Performance S-Cathode. 精氨酸作为高性能s阴极的多功能添加剂。
IF 7.5 2区 化学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2025-01-03 DOI: 10.1002/cssc.202402284
Lulu Ren, Ying Guo, Chunhua Ying, Justin Tangxin Zhong, Jin Liu, Wei-Hong Katie Zhong

Advancement of sulfur (S) cathode of lithium-sulfur (Li-S) batteries is hindered by issues such as insulating nature of sulfur, sluggish redox kinetics, polysulfide dissolution and shuttling. To address these issues, we initiate a study on applying an important amino acid of protein, arginine (Arg), as a functional additive into S cathode. Based on our simulation study, the positively charged Arg facilitates strong interactions with polysulfides. The experimental results indicate that the interaction enable capability of trapping polysulfides within the S cathode, responsible for reducing shuttle effects. Furthermore, the positively charged Arg also promotes efficient ion diffusion and polysulfides conversion. The new findings include that, with addition of only 1 wt % Arg, the resultant cathode demonstrates effectively enhanced electrolyte wettability, polysulfide adsorption and redox kinetics, leading to enhanced rate performance and long-term cycling stability. This study highlights the great potential of amino acids being able to act as effective functional bio-additives in S cathode, paving a new way to high-performance and sustainable energy storage solutions.

硫的绝缘性、氧化还原动力学缓慢、多硫化物溶解和穿梭等问题阻碍了锂硫电池硫(S)阴极的发展。为了解决这些问题,我们开始研究将蛋白质的重要氨基酸精氨酸(Arg)作为功能添加剂应用于S阴极。基于我们的模拟研究,带正电的Arg促进了与多硫化物的强相互作用。实验结果表明,这种相互作用能够在S阴极内捕获多硫化物,从而减少穿梭效应。此外,带正电的精氨酸还能促进离子的有效扩散和多硫化物的转化。新发现包括,仅添加1wt %的Arg,生成的阴极就能有效地增强电解质润湿性、多硫化物吸附和氧化还原动力学,从而提高速率性能和长期循环稳定性。这项研究强调了氨基酸作为S阴极有效的功能性生物添加剂的巨大潜力,为高性能和可持续的储能解决方案铺平了新的道路。
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引用次数: 0
Cover Feature: Isolation of β-O-4-Rich Lignin From Birch in High Yields Enabled by Continuous-Flow Supercritical Water Treatment (ChemSusChem 1/2025)
IF 7.5 2区 化学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2025-01-03 DOI: 10.1002/cssc.202580102
Davide Rigo, Tijana Fechter, Ewellyn Capanema, Daryna Diment, Marie Alopaeus, Dmitry Tarasov, Danilo Cantero, Mikhail Balakshin

The Cover Feature shows how continuous-flow supercritical water treatment of birch followed by alkali extraction of lignin allowed the isolation of lignin and lignin carbohydrate complexes (LCCs) in 13–19 wt % yield with respect to the initial woody biomass with a high number of β-O-4 moieties up to 57/100 Ar. Such an approach may be extended to other biomass feedstocks, enabling the isolation of non-degraded lignins/LCCs with tunable structure and properties. More information can be found in the Research Article by D. Rigo, E. Capanema and co-workers. Cover design: Eric Gabriel.

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引用次数: 0
Cover Feature: Efficient Hydrodeoxygenation of Lignin-Derived Phenolic Compounds Over Ru-Based Catalyst with Biochar and Al2O3 as Composite Support (ChemSusChem 1/2025)
IF 7.5 2区 化学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2025-01-03 DOI: 10.1002/cssc.202580103
Tao Yin, Yichao Ye, Hao Jiang, Chengyin Lin, Riyang Shu, Zhipeng Tian, Chao Wang, Ning Shi

The Cover Feature shows a novel and stable Ru-based catalyst with biochar and Al2O3 as composite support (Ru/C-Al2O3) that was employed in the hydrodeoxygenation of lignin-derived phenolic compounds. H2 was efficiently activated to form active H species that participate in the hydrogenation of guaiacol. Moreover, under catalysis of the Al2O3 acid site, deoxygenation then occurs to form cyclohexane. The composite support has a large surface area, thus improving Ru metal dispersion and enhancing its catalytic activity. More information can be found in the Research Article by R. Shu, N. Shi and co-workers (DOI: 10.1002/cssc.202401870).

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引用次数: 0
Front Cover: Upcycling of Chitin to Cross-Coupling Catalysts: Tailored Supports and Opportunities in Mechanochemistry (ChemSusChem 1/2025)
IF 7.5 2区 化学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2025-01-03 DOI: 10.1002/cssc.202580101
Oscar Trentin, Daniel Ballesteros-Plata, Enrique Rodríguez-Castellón, Leonardo Puppulin, Maurizio Selva, Alvise Perosa, Daily Rodríguez-Padrón

The Front Cover shows the solvent-free mechanochemical synthesis of chitin-derived, palladium-based catalytic systems by extrusion. In their Research Article, A. Perosa, D. RodrÍguez-Padrón and co-workers explore the impact of nanoparticle size, N-doping in the support, and their synergistic effects in Heck–Mizoroki and Suzuki–Miyaura cross-coupling reactions. The authors also uncover how these factors drive more sustainable and efficient catalytic processes.

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引用次数: 0
Cover Feature: Aromatic Poly(dithioacetal)s: Spanning Degradability, Thermostability, and High Refractive Index Towards Eco-friendly Optics (ChemSusChem 1/2025)
IF 7.5 2区 化学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2025-01-03 DOI: 10.1002/cssc.202580104
Seigo Watanabe, Tomoya Yano, Zexin An, Kenichi Oyaizu

The Cover Feature shows aromatic poly(dithioacetal)s, which are multifunctional materials for eco-friendly optics with a high refractive index (>1.7), visible transparency, thermal stability, on-demand degradability, and recyclability. Cyclic low-molecular-weight products from zinc-catalyzed polymer degradation lead to acid-catalyzed repolymerization to the raw polymer, representing a closed-loop recycling process without any deterioration in the optical properties. More information can be found in the Research Article by K. Oyaizu and co-workers.

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引用次数: 0
Complete Aqueous Defluorination of GenX (Hexafluoropropylene Oxide Dimer Acid Anion) by Pulsed Electrolysis with Polarity Reversal. 极性反转脉冲电解对GenX(六氟环氧丙烷二聚体酸性阴离子)的完全水除氟。
IF 7.5 2区 化学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2025-01-03 DOI: 10.1002/cssc.202402093
Ziyi Meng, Madeleine K Wilsey, Astrid M Müller

Per- and polyfluoroalkyl substances (PFAS) are extremely stable chemicals that are essential for modern life and decarbonization technologies. Yet PFAS are persistent pollutants that are harmful to human health. Hexafluoropropylene oxide dimer acid (GenX), a replacement for the PFAS chemical perfluorooctanoic acid, continues to pollute waterways. In this study, we report the complete defluorination of GenX through electrocatalysis in aqueous LiOH electrolytes, utilizing high surface area anodes consisting of pulsed laser in liquid synthesized [NiFe]-(OH)₂ nanocatalysts on hydrophilic carbon fiber paper. Additional experiments with industrial nickel-iron alloy demonstrated exceptional stability for >100 hours. Including a brief interval of reversed polarity in pulsed electrolysis and optimizing the pulse train sequence enabled the complete defluorination of GenX. Our facile approach employs only nonprecious materials, does not require bisulfate or other auxiliary chemical agents that are consumed, and thus provides a promising strategy for alleviating the environmental impact of PFAS pollutants.

全氟烷基和多氟烷基物质(PFAS)是非常稳定的化学物质,对现代生活和脱碳技术至关重要。然而,PFAS是对人类健康有害的持久性污染物。六氟环氧丙烷二聚酸(GenX)是PFAS化学品全氟辛酸的替代品,它继续污染水道。在这项研究中,我们报道了通过电催化在LiOH水溶液中完全脱氟,利用由脉冲激光组成的高表面积阳极在亲水性碳纤维纸上合成[NiFe]-(OH) 2纳米催化剂。工业镍铁合金的附加实验证明了bbb100小时的优异稳定性。在脉冲电解中加入极性反转的短暂间隔,并优化脉冲序列序列,使GenX完全去氟化。我们简单的方法只使用非贵重材料,不需要消耗硫酸氢盐或其他辅助化学剂,因此为减轻PFAS污染物对环境的影响提供了一个有希望的策略。
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引用次数: 0
"ZnO-In-Carbon-Cage" Decorated Carbon Fibers as a Stable Lithium Host with Enhanced Kinetics for Lithium Metal Batteries. “ZnO-in-Carbon-Cage”装饰碳纤维作为锂金属电池的稳定锂宿主,具有增强的动力学。
IF 7.5 2区 化学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2025-01-02 DOI: 10.1002/cssc.202402472
Shuling Fan, Zhongcheng Sun, Can Liu, Fangmin Ye, Meinan Liu

Lithium (Li) metal anodes (LMAs), which show a great potential in constructing high-specific-energy-density Li metal batteries (LMBs), have abstracted wide research interest. However, the generation of Li dendrites and the repeated change of volume upon Li plating/stripping severely block the practical commercialization of LMBs. Herein, the functional carbon fibers (CFs) decorated with ZnO embedded carbon cage (ZnO@C-d-CFs) were fabricated successfully by a two-step route including the in-situ growth of Zn-based metal organic frameworks (MOFs) and subsequent carbonization process, which enriched the lithiophilic sites of CFs host and improved Li+ kinetics of Li+ plating/stripping. Markedly, our designed ZnO@C-d-CFs possessed an obvious surface stability for Li+ plating/stripping (e. g., 1000 cycles with a CE of ~100 % for ZnO@C-d-CFs||Li cell, 1200 h for Li-ZnO@C-d-CFs|| Li-ZnO@C-d-CFs cell), and demonstrated a great potential in practical LMBs (e. g., a low-capacity decay of 0.067 mAh g-1 per cycle within the monitored 900 cycles in Li-ZnO@C-d-CFs||LiFePO4 (LFP) cell). The impressive results verified an effectiveness of surface modification on Li host to boost the stable LMAs.

锂金属阳极(LMAs)在构建高比能量密度锂金属电池(lmb)方面显示出巨大的潜力,引起了广泛的研究兴趣。然而,锂枝晶的产生和锂镀/剥离过程中体积的反复变化严重阻碍了lmb的实际商业化。本文通过原位生长锌基金属有机骨架(mof)和随后的碳化两步工艺,成功制备了ZnO包埋碳笼(ZnO@C-d-CFs)修饰的功能碳纤维(CFs),丰富了CFs主体的亲锂位点,提高了Li+电镀/剥离的动力学。值得注意的是,我们设计的ZnO@C-d-CFs对于Li+电镀/剥落具有明显的表面稳定性(例如,ZnO@C-d-CFs||锂电池1000次循环,CE为~100%,Li-ZnO@C-d-CFs||Li-ZnO@C-d-CFs电池1200 h),并且在实际的lmb中展示了巨大的潜力(例如,在监测的Li-ZnO@C-d-CFs||LiFePO₄(LFP)电池900次循环中,每循环0.067 mAh g-1的低容量衰减)。这些令人印象深刻的结果验证了对Li宿主进行表面改性以提高稳定lma的有效性。
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引用次数: 0
Effect of Carbon Nanotubes Conductors on Electrolyte Wettability and Electrochemical Performance of Lithium-Ion Battery Electrodes. 碳纳米管导体对锂离子电池电极电解质润湿性和电化学性能的影响
IF 7.5 2区 化学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2025-01-02 DOI: 10.1002/cssc.202402517
Shaohai Dong, Yuhang Lyu, Zhan-Sheng Guo

Electrolyte wettability significantly effects the electrochemical performance of lithium-ion batteries (LIBs). In this study, buoyancy testing is employed to accurately measure the force-time curve of electrolyte penetration into the electrodes and thereby calculate the wettability rate. Electrochemical performance is comprehensively evaluated through CR2025 coin half-cell testing, four-point probe analysis, and C-rate cycling experiments. The effects of conductive agent content, morphology, and size on wettability, conductivity and electrochemical performance are investigated. The results show that carbon nanotube (CNT) conductive agent have strong effect on electrolyte wettability, conductivity, and electrochemical performance. Specifically, electrodes with 3 % CNT content show a 48.9 % increase in wettability, a 95.7 % reduction in electrode resistance, and a 10 % increase in cycle life compared to 1 % CNT. The results show that wettability and conductivity have an equally important effect on electrochemical properties. Larger CNT sizes improve wettability but increase electrode resistance, negatively impacting LIB performance. CNT conductive agents facilitate electrolyte movement along the nanotubes, reducing tortuosity and enhancing wettability. Optical observation of the wetting process on the surface and cross-section of the pure conductive agent electrode strongly supports this conclusion. These results provide valuable insight into optimizing LIB performance by manipulating CNT properties and incorporating them as conductive agents.

电解质的润湿性对锂离子电池的电化学性能有重要影响。在本研究中,浮力测试可以精确测量电解质渗透到电极中的力-时间曲线,从而计算润湿性。通过CR2025硬币半电池测试、四点探针分析和c倍率循环实验,综合评价电化学性能。研究了导电剂的含量、形貌和粒径对润湿性、电导率和电化学性能的影响。结果表明,碳纳米管(CNT)导电剂对电解质的润湿性、电导率和电化学性能有较强的影响。与1%碳纳米管相比,3%碳纳米管含量的电极的润湿性增加了48.9%,电极电阻降低了95.7%,循环寿命增加了10%。润湿性和导电性对电化学性能有同样重要的影响。更大的碳纳米管尺寸提高了润湿性,但增加了电极电阻,对LIB性能产生了负面影响。碳纳米管导电剂促进电解质沿着纳米管运动,减少扭曲和提高润湿性。对纯导电剂电极表面和截面的润湿过程的光学观察有力地支持了这一结论。这些结果为通过操纵碳纳米管特性并将其作为导电剂来优化LIB性能提供了有价值的见解。
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引用次数: 0
Advanced Alkali Metal Batteries Based on MOFs and Their Composites. 基于MOFs及其复合材料的新型碱金属电池。
IF 7.5 2区 化学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2025-01-02 DOI: 10.1002/cssc.202402289
Wenting Li, Chengze Li, Jin Guo, Tianhao Jiang, Wei Kang, Huan Pang

The integration of metal-organic frameworks (MOFs) with functional materials has established a versatile platform for a wide range of energy storage applications. Due to their large specific surface area, high porosity, and tunable structural properties, MOFs hold significant promise as components in energy storage systems, including electrodes, electrolytes, and separators for alkali metal-ion batteries (AIBs). Although lithium-ion batteries (LIBs) are widely used, their commercial graphite anode materials are nearing their theoretical capacity limits, and the scarcity of lithium and cobalt resources increases costs. Although zinc-ion batteries (ZIBs) suffer from limited cycling stability, they are attractive for their low cost, high capacity, and excellent safety. Meanwhile, potassium-ion (PIBs) and sodium-ion batteries (SIBs) show promise due to their affordability and abundant resources, but they encounter issues such as short cycle life and low energy density. This review outlines the applications of MOF composites in LIBs, SIBs, and ZIBs, introduces common synthesis methods, and forecasts future development directions and challenges in energy storage applications. We emphasize how the understanding can lay the foundation for developing MOF composites with enhanced functionalities.

金属有机框架(MOFs)与功能材料的集成为广泛的储能应用建立了一个多功能平台。由于mof具有较大的比表面积、高孔隙率和可调的结构特性,它作为储能系统的组件,包括电极、电解质和碱金属离子电池(aib)的分离器,具有重要的前景。虽然锂离子电池(LIBs)被广泛使用,但其商用石墨负极材料已接近其理论容量极限,而且锂和钴资源的稀缺性增加了成本。尽管锌离子电池的循环稳定性有限,但其成本低、容量大、安全性好等优点具有很大的吸引力。与此同时,钾离子电池(PIBs)和钠离子电池(SIBs)因价格合理、资源丰富而具有广阔的应用前景,但也存在循环寿命短、能量密度低等问题。综述了MOF复合材料在lib、SIBs和ZIBs中的应用,介绍了常用的合成方法,并预测了未来在储能应用中的发展方向和挑战。我们强调这种理解如何为开发具有增强功能的MOF复合材料奠定基础。
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引用次数: 0
Lignin Tandem Catalytic Transformation to Phenolic Aryl Acrylic Esters as Plant Growth Regulators. 植物生长调节剂木质素串联催化转化酚醛芳基丙烯酸酯。
IF 7.5 2区 化学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2025-01-02 DOI: 10.1002/cssc.202402540
Bingbing Luo, Chaofeng Zhang, Huijun Zhang, Kaiyi Su, Bo Jiang, Jinlan Cheng, Yongcan Jin

Based on the concept "Derived from Agroforestry, belong to (Servicing) Agroforestry", we herein achieved the tandem catalytic transformation of lignin to phenolic aryl acrylic esters, which can work as plant growth regulators. The transformation involves the first catalytic oxidative fractionation (COF) of lignin into aromatic aldehydes, which can further undergo Knoevenagel condensation with acids/esters with active Cα-H to generate the phenolic aryl acrylic esters. For the first lignin transformation, the Cu salt (CuSO4) in a 7.5 wt % NaOH aqueous solution could achieve the selective cleavage of lignin C-C bonds to provide a 25.0 wt % yield of aromatic aldehydes. Subsequently, the unique basic sites of the self-assembled hybrid system of CeO2 and 2-cyanopyridine could overcome the limitations of traditional homogeneous/heterogeneous bases and facilitate the condensation between phenolic-containing aromatic aldehydes and malonic ester to aryl acrylic esters. Furthermore, the lignin-based phenolic aryl acrylic esters showed different plant growth regulation activity based on the various structural groups for peppermint seed cultivation. The above results can expand the high-value utilization of lignin in the agroforestry field.

基于“源于农林业,属于(服务)农林业”的理念,我们实现了木质素的串联催化转化为酚醛芳丙烯酸酯,可以作为植物生长调节剂。木质素首先催化氧化分馏(COF)生成芳香醛,然后与具有活性c - α- h的酸/酯发生Knoevenagel缩合,生成酚醛芳基丙烯酸酯。对于第一次木质素转化,在7.5% NaOH水溶液中,Cu盐(CuSO4)可以实现木质素C-C键的选择性裂解,从而提供25.0 wt%的芳醛产率。随后,CeO2与2-氰吡啶自组装杂化体系的独特碱基可以克服传统均/非均相碱的限制,促进含酚芳醛和丙二酸酯之间缩合成芳丙烯酸酯。此外,木质素基酚芳基丙烯酸酯在薄荷种子栽培中表现出不同结构基团的植物生长调节活性。上述结果可拓展木质素在农林业领域的高价值利用。
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引用次数: 0
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