ChemSusChem最新文献_第5页

Tri-Anion Solvation Structure Electrolyte Improves the Electrochemical Performance of Li||LiNi_0.8Co_0.1Mn_0.1O₂ Batteries. 三阴离子溶解结构电解质改善了锂镍0.8钴0.1锰0.1O2电池的电化学性能。

IF 7.5 2区化学

ChemSusChem Pub Date : 2025-01-14 Epub Date: 2024-09-18 DOI: 10.1002/cssc.202401029

Miaolan Sun, Yuxiang Xie, Huayu Huang, Yixin Huang, Hui Chen, Shishi Liu, Peng Dai, Rui Huang, Ling Huang, Shigang Sun

{"title":"Tri-Anion Solvation Structure Electrolyte Improves the Electrochemical Performance of Li||LiNi0.8Co0.1Mn0.1O2 Batteries.","authors":"Miaolan Sun, Yuxiang Xie, Huayu Huang, Yixin Huang, Hui Chen, Shishi Liu, Peng Dai, Rui Huang, Ling Huang, Shigang Sun","doi":"10.1002/cssc.202401029","DOIUrl":"10.1002/cssc.202401029","url":null,"abstract":"Li||LiNi0.8Co0.1Mn0.1O2 batteries, which consist of lithium metal anode (LMA) matched with NCM811 cathode, have an energy density more than twice that of lithium ion battery (LIB). However, the unstable electrode/electrolyte interface still hinders its practical application. Ether electrolytes show promise in improving the stability of LMA and NCM811 cathodes. However, a robust and stable electrode/electrolyte interface in Li||NCM811 batteries cannot be easily and efficiently achieved with most of the ether electrolytes reported in present studies. Herein, we present a straightforward and efficient tri-anion synergistic strategy to overcome this bottleneck. The addition of ClO4 - and NO3 - anions to LiFSI-based ether electrolytes forms a unique solvation structure with tri-anion (FSI-/ClO4 -/NO3 -) participation (LB511). This structure not only enhances the electrochemical window of the ether electrolytes but also achieves a stable Li||NCM811 batteries interface. The interaction between electrode and electrolyte is suppressed and an inorganic-rich (LiF/Li3N/LiCl) SEI/CEI layer is formed. Meanwhile, the coordination structure in the LB511 electrolyte increases the overpotential for Li deposition, resulting in a uniform and dense layer of Li deposition. Therefore, the Li||Cu cells using the LB511 electrolyte have an average CE of 99.6 %. The Li||NCM811 batteries was cycled stably for 250 cycles with a capacity retention of 81 % in the LB511 electrolyte (N/P=2.5, 0.5 C).","PeriodicalId":149,"journal":{"name":"ChemSusChem","volume":" ","pages":"e202401029"},"PeriodicalIF":7.5,"publicationDate":"2025-01-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141791468","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

Low-Temperature and High-Rate Rechargeable Aluminum Batteries Enabled by Ternary Eutectic Electrolytes. 采用三元共晶电解质的低温高倍率可充电铝电池。

IF 7.5 2区化学

ChemSusChem Pub Date : 2025-01-14 Epub Date: 2024-09-23 DOI: 10.1002/cssc.202400983

Raju Vadthya, Christopher Fetrow, Olumide Oladoyin, James Wu, Sergei Ivanov, You Wang, Dongchang Chen, Xiao-Dong Zhou, Shuya Wei

{"title":"Low-Temperature and High-Rate Rechargeable Aluminum Batteries Enabled by Ternary Eutectic Electrolytes.","authors":"Raju Vadthya, Christopher Fetrow, Olumide Oladoyin, James Wu, Sergei Ivanov, You Wang, Dongchang Chen, Xiao-Dong Zhou, Shuya Wei","doi":"10.1002/cssc.202400983","DOIUrl":"10.1002/cssc.202400983","url":null,"abstract":"Rechargeable aluminum batteries (RABs) have garnered extensive scientific attention as a promising alternative chemistry due to the inherent advantages associated with aluminum (Al) metal anodes, including their high theoretical capacities, cost-effectiveness, environmental friendliness, and inherent non-flammable properties. Nonetheless, the practical energy density of RABs is constrained by the electrolytes that support lower operational voltage windows. Herein, we report a ternary eutectic electrolyte composed of 1-ethyl-3-methylimidazolium chloride ([C2C1im]Cl):1-butyl-3-methylimidazolium chloride ([C4C1im]Cl):aluminum chloride (AlCl3) for the application of RABs. The electrolyte exhibits a high operational potential window (~3 V vs. Al/Al3+ on SS 316) and high ionic conductivity (~8.3 mS cm-1) while exhibiting only a low temperature glass transition at -65 °C suitable for all-climate conditions. Al||graphene nanoplatelets cell delivers a high capacity of ~117 mAh/g, and ~43 mAh/g at a very high current densities of 1 A/g and 5 A/g, respectively. The cells render a reversible capacity of 20 mAh/g at -20 °C and 17 mAh/g at -40 °C, indicating their suitability for operation under extreme environmental conditions. We comprehensively evaluated the design and optimization of carbon paper-based battery systems. The ternary eutectic electrolyte demonstrates exceptional electrochemical performance, thus signifying its substantial potential for utilization in high-performance energy storage systems in all climates.","PeriodicalId":149,"journal":{"name":"ChemSusChem","volume":" ","pages":"e202400983"},"PeriodicalIF":7.5,"publicationDate":"2025-01-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141791466","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

Surface State Modulation via Electrochemical Heterogeneous Redox Reactions for Full-Color Emission Carbon Dots. 通过电化学异质氧化还原反应调控表面状态，实现全彩发光碳点。

IF 7.5 2区化学

ChemSusChem Pub Date : 2025-01-14 Epub Date: 2024-09-23 DOI: 10.1002/cssc.202401313

Jinli Li, Chengxiang Sun, Qiang Li, Xiran Xu, Baolin Li, Yijia Tian, Dianyuan Zheng, Rongbin Yao, Kang Yuan, Ziyang Guo

{"title":"Surface State Modulation via Electrochemical Heterogeneous Redox Reactions for Full-Color Emission Carbon Dots.","authors":"Jinli Li, Chengxiang Sun, Qiang Li, Xiran Xu, Baolin Li, Yijia Tian, Dianyuan Zheng, Rongbin Yao, Kang Yuan, Ziyang Guo","doi":"10.1002/cssc.202401313","DOIUrl":"10.1002/cssc.202401313","url":null,"abstract":"Carbon dots (CDs) still suffer from unclear surface state fluorescence mechanism for fine modulation. Here, redox reactions for cathode and anode within electrochemical method are firstly employed to construct differentiated strategy for surface-state modulation, so as to obtain CDs with controllable emission in separated electrodes simultaneously. The fluorescence peaks of CDs from blue to red centered at 425 nm (mCDs-), 530 nm (mCDs+), 580 nm (oCDs-) and 665 nm (oCDs+) are mainly originated from the different bombardment effects of the ions and reaction tendencies of modifier during the electrolysis process. The phenylenediamine (as modifier) tends to introduce the amino groups on the surface of CDs- while introduced nitrogen atoms into the carbon nucleus skeleton around the anode, thus leading to much larger size and the formation of the graphite N for CDs+. It is the different surface states formed by phenylenediamine and the absorption redshift triggered by graphite N that ensures the tunable emission. The improved electrochemical method is of great significance for finely spectra modulation and efficient synthesis.","PeriodicalId":149,"journal":{"name":"ChemSusChem","volume":" ","pages":"e202401313"},"PeriodicalIF":7.5,"publicationDate":"2025-01-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141858445","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

Immobilization and Catalytic Conversion of Polysulfide by In-Situ Generated Nickel in Hollow Carbon Fibers for High-Rate Lithium-Sulfur Batteries. 用于高倍率锂硫电池的中空碳纤维中原位生成的镍对多硫化物的固定和催化转化。

IF 7.5 2区化学

ChemSusChem Pub Date : 2025-01-14 Epub Date: 2024-09-24 DOI: 10.1002/cssc.202401178

Ying Liu, Mingxu Li, Rong Yang, Qinglong Meng, Dong-Ho Baek, Hyung-Tae Lim, Jae-Kwang Kim, Jou-Hyeon Ahn

{"title":"Immobilization and Catalytic Conversion of Polysulfide by In-Situ Generated Nickel in Hollow Carbon Fibers for High-Rate Lithium-Sulfur Batteries.","authors":"Ying Liu, Mingxu Li, Rong Yang, Qinglong Meng, Dong-Ho Baek, Hyung-Tae Lim, Jae-Kwang Kim, Jou-Hyeon Ahn","doi":"10.1002/cssc.202401178","DOIUrl":"10.1002/cssc.202401178","url":null,"abstract":"Lithium-sulfur (Li-S) batteries are considered promising energy-storage systems because of their high theoretical energy density, low cost, and eco-friendliness. However, problems such as the shuttle effect can result in the loss of active materials, poor cyclability, and rapid capacity degradation. The utilization of a structural configuration that enhances electrochemical performance via dual adsorption-catalysis strategies can overcome the limitations of Li-S batteries. In this study, an integrated interlayer structure, in which hollow carbon fibers (HCFs) were modified with in-situ-generated Ni nanoparticles, was prepared by scalable one-step carbonization. Highly hierarchically porous HCFs act as the carbon skeleton and provide a continuous three-dimensional conductive network that enhances ion/electron diffusion. Ni nanoparticles with superior anchoring and catalytic abilities can prevent the shuttle effect and increase the conversion rate, thereby promoting the electrochemical performance. This synergistic effect resulted in a high capacity retention of 582 mAh g-1 at 1 C after 100 cycles, providing an excellent rate capability of up to 3 C. The novel structure, wherein Ni nanoparticles are embedded in cotton-tissue-derived HCFs, provides a new avenue for enhancing electrochemical performance at high C rates. This results in a low-cost, sustainable, and high-performance hybrid material for the development of practical Li-S batteries.","PeriodicalId":149,"journal":{"name":"ChemSusChem","volume":" ","pages":"e202401178"},"PeriodicalIF":7.5,"publicationDate":"2025-01-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141896237","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

Copper-Catalyzed Oxidation of 5-Hydroxymethylfurfural to 2,5-Diformylfuran Assisted by TEMPOL in Liquid Sunlight Methanol. 铜催化的 5-羟甲基呋喃醛在 TEMPOL 辅助下在液态日光甲醇中氧化成 2,5-二甲酰呋喃。

IF 7.5 2区化学

ChemSusChem Pub Date : 2025-01-14 Epub Date: 2024-10-25 DOI: 10.1002/cssc.202401527

Xing-Long Li, Shao-Jun Qing, Xun Sun, Zhen Yu, Hua-Jian Xu, Yao Fu

{"title":"Copper-Catalyzed Oxidation of 5-Hydroxymethylfurfural to 2,5-Diformylfuran Assisted by TEMPOL in Liquid Sunlight Methanol.","authors":"Xing-Long Li, Shao-Jun Qing, Xun Sun, Zhen Yu, Hua-Jian Xu, Yao Fu","doi":"10.1002/cssc.202401527","DOIUrl":"10.1002/cssc.202401527","url":null,"abstract":"2,5-diformylfuran (DFF) is a significant biomass-derived compound with diverse applications in novel furan-based materials, fragrances, fuel additives, and drug synthesis. A pivotal challenge in DFF synthesis was developing a method to produce DFF under mild conditions using sustainable feedstocks. In this study, an affordable 4-hydroxy-2,2,6,6-tetramethylpiperidine (TEMPOL)- assisted Cu(OAc)2 catalytic system for aerobic oxidation reaction of HMF to DFF in liquid sunlight methanol solvent was developed. The effects of parameters such as metal species, catalyst amount, solvent species, base structure, and reaction temperature were systematically investigated. The evolution of product distribution in the reaction solution at various times was monitored and analyzed using 1H-NMR spectroscopy. FT-IR and ESI-MS characterizations were employed to integrate experimental findings and elucidate the reaction mechanism. The highest DFF yield of 96 % and complete conversion of HMF were obtained. Furthermore, a total DFF yield of 68.6 % was achieved from fructose using a two-steps method, demonstrating the potential for scalable production. The establishment of this catalytic system presents a novel approach for the selective preparation of DFF from sustainable feedstock.","PeriodicalId":149,"journal":{"name":"ChemSusChem","volume":" ","pages":"e202401527"},"PeriodicalIF":7.5,"publicationDate":"2025-01-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142015766","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

Enhancing Benzylamine Electro-Oxidation and Hydrogen Evolution Through in-situ Electrochemical Activation of CoC₂O₄ Nanoarrays. 通过 CoC2O4 纳米阵列的原位电化学活化提高苄胺的电氧化和氢气进化。

IF 7.5 2区化学

ChemSusChem Pub Date : 2025-01-14 Epub Date: 2024-10-23 DOI: 10.1002/cssc.202401446

Guanqiao Zhang, Jialai Hu, Wanling Zhang, Kun Yu, Wenbiao Zhang, Qingsheng Gao

{"title":"Enhancing Benzylamine Electro-Oxidation and Hydrogen Evolution Through in-situ Electrochemical Activation of CoC2O4 Nanoarrays.","authors":"Guanqiao Zhang, Jialai Hu, Wanling Zhang, Kun Yu, Wenbiao Zhang, Qingsheng Gao","doi":"10.1002/cssc.202401446","DOIUrl":"10.1002/cssc.202401446","url":null,"abstract":"The sluggish anodic oxygen evolution reaction (OER) seriously restricts the overall efficiency of water splitting. Here, we present an environmentally friendly and efficient aniline oxidation (BOR) to replace the sluggish OER, accomplishing the co-production of H2 and high value-added benzonitrile (BN) at low voltages. Cobalt oxalates grown on cobalt foam (CoC2O4 ⋅ 2H2O/CF) are adopted as the pre-catalysts, which further evolve into working electrocatalysts active for BOR and HER via appropriate electrochemical activation. Thereinto, cyclic voltammetry activation at positive potentials is performed to reconstruct cobalt oxalate via extensive oxidation, resulting in enriched Co(III) species and nanoporous structures beneficial for BOR, while chronoamperometry at negative potentials is introduced for the cathodic activation toward efficient HER with obvious improvement. The two activated electrodes can be combined into a two-electrode system, which achieves a high current density of 75 mA cm-2 at the voltage of 1.95 V, with the high Faraday efficiencies of both BOR (90.0 %) and HER (90.0 %) and the satisfactory yield of BN (76.8 %).","PeriodicalId":149,"journal":{"name":"ChemSusChem","volume":" ","pages":"e202401446"},"PeriodicalIF":7.5,"publicationDate":"2025-01-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142003132","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

Strong Covalent Metal-Ligand Interaction Enables a Fast Kinetic and Structurally Stable Na-Ion Layered Cathode. 强共价金属配体相互作用实现了快速动力学和结构稳定的 Na 离子层状阴极。

IF 7.5 2区化学

ChemSusChem Pub Date : 2025-01-14 Epub Date: 2024-10-25 DOI: 10.1002/cssc.202401538

Jing-Chang Li, Sheng Xu, Jiaming Tian, Bo Peng, Yu Sun, Jiayi Tang, Zhaoguo Liu, Yuankai Liu, Daxian Zuo, Chengrong Xu, Yuan Rao, Yu Deng, Haoshen Zhou, Shaohua Guo

{"title":"Strong Covalent Metal-Ligand Interaction Enables a Fast Kinetic and Structurally Stable Na-Ion Layered Cathode.","authors":"Jing-Chang Li, Sheng Xu, Jiaming Tian, Bo Peng, Yu Sun, Jiayi Tang, Zhaoguo Liu, Yuankai Liu, Daxian Zuo, Chengrong Xu, Yuan Rao, Yu Deng, Haoshen Zhou, Shaohua Guo","doi":"10.1002/cssc.202401538","DOIUrl":"10.1002/cssc.202401538","url":null,"abstract":"Anionic redox chemistry has attracted increasing attention for the improvement in the reversible capacity and energy density of cathode materials in Li/Na-ion batteries. However, adverse electrochemical behaviors, such as voltage hysteresis and sluggish kinetics resulting from weak metal-ligand interactions, commonly occur with anionic redox reactions. Currently, the mechanistic investigation driving these issues still remains foggy. Here, we chemically designed Na0.8Fe0.4Ti0.6S2 and Na0.8Fe0.4Ti0.6O2 as model cathodes to explore the covalency effects on metal-ligand interactions during anionic redox process. Na0.8Fe0.4Ti0.6S2 with strengthened covalent interaction of metal-ligand bonds exhibits smaller voltage hysteresis and faster kinetics than Na0.8Fe0.4Ti0.6O2 during (de)sodiation process. Theoretical calculations suggest that Fe is the dominant redox-active center in Na0.8Fe0.4Ti0.6S2, whereas the redox-active center moves from Fe to O with the removal of Na+ in Na0.8Fe0.4Ti0.6O2. We attribute the above different redox behaviors between Na0.8Fe0.4Ti0.6S2 and Na0.8Fe0.4Ti0.6O2 to the charge transfer kinetics from ligand to metal. Moreover, the structural stability of Na0.8Fe0.4Ti0.6S2 is enhanced by increasing the cation migration barriers through strong metal-ligand bonds during desodiation. These insights into the originality of metal-ligand interactions provide guidance for the design of high-capacity and structurally stable cathode materials for Li/Na-ion batteries.","PeriodicalId":149,"journal":{"name":"ChemSusChem","volume":" ","pages":"e202401538"},"PeriodicalIF":7.5,"publicationDate":"2025-01-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142071546","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

Carbon Nanotube Supported Fluorine Substituted Iron Phthalocyanine Enabling Boosted Polysulfide Redox Conversion Kinetics and Cyclic Stability. 碳纳米管支撑的氟取代铁酞菁可促进多硫化物氧化还原转化动力学和循环稳定性。

IF 7.5 2区化学

ChemSusChem Pub Date : 2025-01-14 Epub Date: 2024-10-22 DOI: 10.1002/cssc.202400451

Jiaqi Zhao, Zhanwei Xu, Yujiao Zhang, Qingzhu Jin, Longhua Guo, Siyu Chen, Xuetao Shen, Jiayin Li, Zhi Li

{"title":"Carbon Nanotube Supported Fluorine Substituted Iron Phthalocyanine Enabling Boosted Polysulfide Redox Conversion Kinetics and Cyclic Stability.","authors":"Jiaqi Zhao, Zhanwei Xu, Yujiao Zhang, Qingzhu Jin, Longhua Guo, Siyu Chen, Xuetao Shen, Jiayin Li, Zhi Li","doi":"10.1002/cssc.202400451","DOIUrl":"10.1002/cssc.202400451","url":null,"abstract":"The sluggish transition and shuttle of polysulfides (LiPS) significantly hinder the application and commercialization of Li-S batteries. Herein, carbon nanotubes (CNTs) supported 10 nm sized iron Hexadecafluorophthalocyanine (FePcF16/CNTs) are prepared using a solid synthesis approach. The well-exposed FePcF16 molecular improve the LiPS capture efficiency and redox kinetics by its central Fe-N4 units and F functional groups. The strong electron withdraw F groups significantly promote the conjugate effect and decrease the steric hindrance during mass migration procedure. Distribution of relaxation time (DRT) analysis shows that the Fe-N4 units exhibit strong affinity towards LiPS and the F groups further improve the Li+ diffusion rate in Li2S nucleation and oxidation procedure, accomplishing a porous surface on cathode. As a result, the FePcF16/CNTs separator exhibits a high initial capacity of 1136.2 mAh g-1 at 0.2 C, outstanding rate capacity of 624.9 mAh g-1 at 5 C and superior long-term stability at 2 C surviving 300 cycles with a low capacity decay of 0.43 ‰ per cycle.","PeriodicalId":149,"journal":{"name":"ChemSusChem","volume":" ","pages":"e202400451"},"PeriodicalIF":7.5,"publicationDate":"2025-01-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142015765","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

Potassium Carbonate as a Low-Cost and Highly Active Solid Base Catalyst for Low-Temperature Methanolysis of Polycarbonate. 碳酸钾作为低成本、高活性的固体碱催化剂用于聚碳酸酯的低温甲醇分解。

IF 7.5 2区化学

ChemSusChem Pub Date : 2025-01-14 Epub Date: 2024-10-30 DOI: 10.1002/cssc.202401676

Tzu-Ming Lin, Philip Anggo Krisbiantoro, Miyu Sato, Yu-Chia Chang, Eduardo C Atayde, Weisheng Liao, Yuichi Kamiya, Ryoichi Otomo, Kevin C-W Wu

{"title":"Potassium Carbonate as a Low-Cost and Highly Active Solid Base Catalyst for Low-Temperature Methanolysis of Polycarbonate.","authors":"Tzu-Ming Lin, Philip Anggo Krisbiantoro, Miyu Sato, Yu-Chia Chang, Eduardo C Atayde, Weisheng Liao, Yuichi Kamiya, Ryoichi Otomo, Kevin C-W Wu","doi":"10.1002/cssc.202401676","DOIUrl":"10.1002/cssc.202401676","url":null,"abstract":"As the demand for polycarbonate (PC) plastic increases over the years, the development of a chemical recycling system to produce virgin-like-quality monomers is indispensable not only to attain completely sustainable cycles but also to contribute to the decrease in global plastic pollution. Herein, potassium carbonate (K2CO3) was used as a low-cost, readily available, and highly active solid base catalyst for low-temperature PC methanolysis in the presence of THF as a solvent, producing highly pure and crystalline bisphenol A (BPA) and with a catalytic performance higher than group IIA metal oxides (MgO, CaO, and SrO) and some group IA metal carbonates (NaHCO3, KHCO3, and Na2CO3). THF was the best solvent in aiding the reaction owing to it having a similar polar parameter (δp) to that of PC according to Hansen solubility parameters. By the reaction over the catalyst, 100% PC conversion, 97% BPA yield, and 86% dimethyl carbonate yield were achieved within just 20 min at 60 °C. The catalyst possessed an apparent activation energy (Ea) of 52.3 kJ mol-1, which is the lowest value so far for heterogeneous catalysts, while the mechanistic study revealed that the reaction proceeded via the methoxide pathway. The reusability test demonstrated that the catalyst was reusable at least four times. Furthermore, this catalytic system was successfully applied to actual post-consumer PC wastes and polyesters, including polyethylene terephthalate (PET) and polylactic acid (PLA).","PeriodicalId":149,"journal":{"name":"ChemSusChem","volume":" ","pages":"e202401676"},"PeriodicalIF":7.5,"publicationDate":"2025-01-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142102595","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

The Stability Challenge of Furanic Platform Chemicals in Acidic and Basic Conditions. 呋喃平台化学品在酸性和碱性条件下的稳定性挑战。

IF 7.5 2区化学

ChemSusChem Pub Date : 2025-01-14 Epub Date: 2024-11-15 DOI: 10.1002/cssc.202401849

Denis A Kolykhalov, Anastasia N Golysheva, Kirill S Erokhin, Bogdan Ya Karlinskii, Valentine P Ananikov

{"title":"The Stability Challenge of Furanic Platform Chemicals in Acidic and Basic Conditions.","authors":"Denis A Kolykhalov, Anastasia N Golysheva, Kirill S Erokhin, Bogdan Ya Karlinskii, Valentine P Ananikov","doi":"10.1002/cssc.202401849","DOIUrl":"10.1002/cssc.202401849","url":null,"abstract":"The transition toward renewable resources is pivotal for the sustainability of the chemical industry, making the exploration of biobased furanic platform chemicals derived from plant biomass of paramount importance. These compounds, promising alternatives to petroleum-derived aromatics, face challenges in terms of stability under synthetic conditions, limiting their practical application in the fuel, chemical, and pharmaceutical sectors. Our study presents a comprehensive evaluation of the stability of furan derivatives in various solvents and under different conditions, addressing the significant challenge of their instability. Through systematic experiments involving GC-MS, NMR, FT-IR and SEM analyses, we identified key degradation pathways and conditions that either promote stability or lead to undesirable degradation products. These findings demonstrate the strong stabilizing effect of polar aprotic solvents, especially DMF, and reveal the dependence of furan stability on solvent and additive type. This research opens new avenues in the utilization of renewable furans by providing critical insights into their behavior under synthetic conditions, significantly impacting the development of sustainable materials and processes. The broad appeal of this study lies in its potential to guide the selection of conditions for the efficient and sustainable synthesis of furan-based chemicals, marking a significant advance in green chemistry and materials science.","PeriodicalId":149,"journal":{"name":"ChemSusChem","volume":" ","pages":"e202401849"},"PeriodicalIF":7.5,"publicationDate":"2025-01-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142491610","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