ChemSusChem最新文献_第2页

Harnessing Deep Eutectic Solvents for Regioselective Polar Additions to α,βUnsaturated Ketones and Aldehydes. 利用深共晶溶剂对 α、β 不饱和酮和醛进行区域选择性极性加成。

IF 7.5 2区化学

ChemSusChem Pub Date : 2024-11-18 DOI: 10.1002/cssc.202402083

Andrew W J Platten, Iva Manasi, Mario Campana, Karen Edler, Eva Hevia

{"title":"Harnessing Deep Eutectic Solvents for Regioselective Polar Additions to α,βUnsaturated Ketones and Aldehydes.","authors":"Andrew W J Platten, Iva Manasi, Mario Campana, Karen Edler, Eva Hevia","doi":"10.1002/cssc.202402083","DOIUrl":"10.1002/cssc.202402083","url":null,"abstract":"Advancing the use of air-sensitive polar organometallic Grignard and organolithium reagents under more environmentally benign conditions, here we report the addition of these reagents to a-b unsaturated ketones and aldehydes using the deep eutetic solvent (DES) choline chloride (ChCl): glycerol (Gly) (1:2), under air. Reactions occur at room temperature within seconds with excellent regioselective control. Furthering understanding of how these C-C bond forming processes take place in these reaction media, we have explored the surface concentration of the organic substrate (chalcone) in DES using interfacial tension and neutron reflectivity measurements, finding that chalcone is concentrated at the DES-hydrocarbon interface compared to the bulk concentration, although the interfacial chalcone concentration is still relatively low in this system. The influence of aggregation of the organometallic reagent in the organic solvent employed has also been evaluated, revealing the importance of achieving a balance between activation (via de-aggregation) and stability (to avoid its decomposition in the DES). This DES approach has been successfully extended to double additions to a-b unsaturated estes and for one pot sequential 1,4 and 1,2 additions to ketones, providing a new entry point to a range of tertiary-alcohols, minimising the use of organic solvents and avoiding intermediate time-consuming purification steps.","PeriodicalId":149,"journal":{"name":"ChemSusChem","volume":" ","pages":"e202402083"},"PeriodicalIF":7.5,"publicationDate":"2024-11-18","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142646221","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

Cerium Dioxide-Induced Abundant Cu+/Cu0 Sites for Electrocatalytic Reduction of Carbon Dioxide to C2+ Products. 二氧化铈诱导丰富的 Cu+/Cu0 位点，用于电催化将二氧化碳还原为 C2+ 产物。

IF 7.5 2区化学

ChemSusChem Pub Date : 2024-11-18 DOI: 10.1002/cssc.202402097

Yuwen Wang, Jiajun Wang, Shuang Liu, Xuan Zhang, Lin Jin, Lanlan Feng, Demeng Kong, Chenxi Zhang, Yajuan Wei, Jingbo Zhang

{"title":"Cerium Dioxide-Induced Abundant Cu+/Cu0 Sites for Electrocatalytic Reduction of Carbon Dioxide to C2+ Products.","authors":"Yuwen Wang, Jiajun Wang, Shuang Liu, Xuan Zhang, Lin Jin, Lanlan Feng, Demeng Kong, Chenxi Zhang, Yajuan Wei, Jingbo Zhang","doi":"10.1002/cssc.202402097","DOIUrl":"10.1002/cssc.202402097","url":null,"abstract":"In recent years, the electrochemical reduction of carbon dioxide (CO2RR) has made many advances in C2+ production. Cu+/Cu0 site is beneficial for C-C coupling process, but the oxidation state of copper cannot be well maintained during the reaction process, resulting in a decrease in catalyst activity. Based on this consideration, in this work, transition metal oxide CeO2 with a hollow cube structure and oxygen vacancies was introduced to stabilize and increase Cu+/Cu0 active sites (Ce1Cu2). The catalyst exhibits excellent CO2RR performance, with FEC2+ achieving 73.52% and jC2+ > 280 mA/cm2 at 1.26 V (vs. RHE). Ethanol is the main C2+ product and FEethanol reaches 39% at 1.26 V. The experimental results indicate that the presence of CeO2 provides a large number of oxygen vacancies and forming Cu+-O2--Ce4+ structure by the strong interaction of CeO2 and Cu NPs. The structure of Cu+-O2--Ce4+ and abundant oxygen vacancies lay a good foundation for the CO2 adsorption. Moreover, it increases the content of Cu+/Cu0 sites, effectively inhibiting hydrogen evolution reaction, promoting the C-C coupling interaction, thereby facilitating the generation of C2+ products. The DFT theoretical calculation further demonstrates that Ce1Cu2 is more inclined towards the ethanol pathway, confirming its high selectivity for ethanol.","PeriodicalId":149,"journal":{"name":"ChemSusChem","volume":" ","pages":"e202402097"},"PeriodicalIF":7.5,"publicationDate":"2024-11-18","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142666544","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

Lignin-Assisted Photoreactions: Unveiling New Frontiers in Light-Induced Chemistry. 木质素辅助光反应：揭开光诱导化学的新前沿。

IF 7.5 2区化学

ChemSusChem Pub Date : 2024-11-17 DOI: 10.1002/cssc.202402117

Hongda Guo, Xiongfei Luo, Luyao Wang, Chenhui Yang, Shujun Li, Shouxin Liu, Jian Li, Zhijun Chen

{"title":"Lignin-Assisted Photoreactions: Unveiling New Frontiers in Light-Induced Chemistry.","authors":"Hongda Guo, Xiongfei Luo, Luyao Wang, Chenhui Yang, Shujun Li, Shouxin Liu, Jian Li, Zhijun Chen","doi":"10.1002/cssc.202402117","DOIUrl":"https://doi.org/10.1002/cssc.202402117","url":null,"abstract":"Lignin, the most abundant aromatic biopolymer, is emerging as a mainstay of the upcoming revolution in sustainable materials processing. Despite the inherent challenges associated with the heterogeneous structure of lignin, significant progress has recently been made in developing innovative strategies to valorize this fascinating aromatic biopolymer to deliver industry-demanded products via photoreactions. The purpose of this review is to unravel insights into these creative approaches in lignin-assisted photoreactions, focusing on photopolymerization to construct functional polymeric materials and photoreduction to provide valuable chemicals, wherein lignin serves as a macromolecular photoinitiator and a reductive photocatalyst, respectively. The existing strategies for improving the photochemical quantum yield of lignin in photopolymerization and harnessing lignin macromolecules as photoresponsive polymers to facilitate electron transfer in photocatalytic reactions are also summarized. In the future, such photochemical lignin valorization concepts could potentially provide new possibilities for achieving a profitable value chain for integrated biorefinery processes.","PeriodicalId":149,"journal":{"name":"ChemSusChem","volume":" ","pages":"e202402117"},"PeriodicalIF":7.5,"publicationDate":"2024-11-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142646224","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

Photocatalytic Upcycling of Plastic Waste into Syngas by ZnS/Ga2O3 Z-scheme Heterojunction. 利用 ZnS/Ga2O3 Z 型异质结进行光催化，将塑料垃圾转化为合成气。

IF 7.5 2区化学

ChemSusChem Pub Date : 2024-11-16 DOI: 10.1002/cssc.202402310

Tong Xu, Tao Shan, Yuting Jiang, Lian-Hua Xu, Huiyan Zhang, Sheng Chu

引用次数: 0

Crystallization of Cathode Active Material Precursors from Tartaric Acid Solution. 酒石酸溶液中阴极活性材料前驱体的结晶。

IF 7.5 2区化学

ChemSusChem Pub Date : 2024-11-16 DOI: 10.1002/cssc.202401523

Chunyan Ma, Mona Mohamoud, Tiaan Punt, Jinlong Li, Michael Svärd, Kerstin Forsberg

引用次数: 0

Two-Dimensional π-d Conjugated Conductive Metal-Organic Framework with Triple Active Centers as High-Performance Cathodes for Flexible Zinc Batteries. 具有三重活性中心的二维 π-d 共轭导电金属有机框架作为柔性锌电池的高性能阴极。

IF 7.5 2区化学

ChemSusChem Pub Date : 2024-11-16 DOI: 10.1002/cssc.202401606

Hong Ding, Ping Liu, Chengyu Liu, Tiantian Li, Wen Guo, Haijiao Xie, Gang Wang, Tiantian Gu

{"title":"Two-Dimensional π-d Conjugated Conductive Metal-Organic Framework with Triple Active Centers as High-Performance Cathodes for Flexible Zinc Batteries.","authors":"Hong Ding, Ping Liu, Chengyu Liu, Tiantian Li, Wen Guo, Haijiao Xie, Gang Wang, Tiantian Gu","doi":"10.1002/cssc.202401606","DOIUrl":"https://doi.org/10.1002/cssc.202401606","url":null,"abstract":"Conductive metal-organic frameworks (C-MOFs) have received extensive interest in high-performance zinc-ion batteries (ZIBs) owing to multi-redox sites and high electrical conductivity. Here, we present a π-d C-MOF by coordinating 2,3,5,6-tetraaminobenzoquinone (TABQ) ligands with Cu2+ ions (2D Cu-TABQ) acting as cathodes for ZIBs. Benefiting from a triple active center (Cu2+, C=O, and C=N), 2D Cu-TABQ shows an ultra-high reversible capacity of 297.7 mAh g-1at 0.2 A g-1. Meanwhile, 2D Cu-TABQ also has superior cycle stability with a capacity of up to 98.2 mAh g-1 after 1000 times at 2.0 A g-1. Considering the instability of the ligand bonds of C-MOFs in aqueous electrolytes,this work uses gel electrolytes to reduce the dissolution of organic ligands into the electrolyte, thus suppressing the shuttle effect, significantly improving the cycling stability of 2D Cu-TABQ. The flexible battery assembled by 2D Cu-TABQ shows excellent capacity retention (64.4%) after 50 times at 0.2 A g-1, which is significantly better than 36.4% in the common electrolyte, as well as outstanding bending resistance and electrochemical properties at different folding angles. This investigation will highlight the electrochemical application of C-MOFs in flexible zinc ion batteries and offer novel ideas for the structural design of cathodes with multiple active centers.","PeriodicalId":149,"journal":{"name":"ChemSusChem","volume":" ","pages":"e202401606"},"PeriodicalIF":7.5,"publicationDate":"2024-11-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142643542","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

Progress on Photo-, Electro-, and Photoelectro-Catalytic Conversion of Recalcitrant Polyethylene, Polypropylene, and Polystyrene - A Review. 光催化、电催化和光电催化转化难降解聚乙烯、聚丙烯和聚苯乙烯的研究进展--综述。

IF 7.5 2区化学

ChemSusChem Pub Date : 2024-11-15 DOI: 10.1002/cssc.202401714

Bhanupriya Boruah, Juan A Lopez-Ruiz

引用次数: 0

Steering Acid-base Site Distribution and Hydrophobicity of Bioresourced Bifunctional Hybrid Materials for Direct Synthesis of γ-Valerolactone from Biomass-based Furfural. 引导生物质双功能杂化材料的酸碱位点分布和疏水性，从生物质糠醛直接合成γ-戊内酯

IF 7.5 2区化学

ChemSusChem Pub Date : 2024-11-15 DOI: 10.1002/cssc.202402165

Mei Wu, Wenping Liu, Fengjuan Deng, Shima Liu, Ke Song, Xianwu Zhou, Jie Guo, Jian He, Hu Li

{"title":"Steering Acid-base Site Distribution and Hydrophobicity of Bioresourced Bifunctional Hybrid Materials for Direct Synthesis of γ-Valerolactone from Biomass-based Furfural.","authors":"Mei Wu, Wenping Liu, Fengjuan Deng, Shima Liu, Ke Song, Xianwu Zhou, Jie Guo, Jian He, Hu Li","doi":"10.1002/cssc.202402165","DOIUrl":"https://doi.org/10.1002/cssc.202402165","url":null,"abstract":"The direct production of value-added chemicals from biomass via multiple conversion processes with a sole renewable solid catalyst is promising for carbon-neutral development while challenging. Herein, a series of novel bioresourced organic-inorganic hybrid materials were synthesized from bio-based ascorbic acid (Vc), zirconium chloride (ZrCl4) and p-toluenesulfonic acid (p-TSA) through a facile solvothermal process. The as-prepared Zr-Vc-3 catalyst with Vc, ZrCl4, and p-TSA in the 1:1:0.5 molar ratio displayed outstanding performance in direct furfural-to-γ-valerolactone (GVL) transformation, giving an ultrahigh GVL yield of 76.2%, with an ideal activation energy (55.46 kJ mol-1), outperforming state-of-the-art catalysts. The superior performance of Zr-Vc-3 could be ascribed to its good reusability, relatively large pore size, suitable amount of acid-base sites, and good hydrophobicity. Mechanistic studies unveiled that Lewis acid-base sites facilitate the conversion of furfural to furfuryl alcohol and isopropyl levulinate (IPL) to 4-hydroxypentanoate via transfer hydrogenation process, while Brønsted acid sites are instrumental in the ring-opening of furfuryl alcohol to IPL and the lactonization of 4-hydroxypentanoate to GVL, overall contributing to the multi-step conversion of furfural to GVL in a single pot. This work provides a valuable reference for precisely constructing bio-based OIHMs with tailored functionalities for one-pot valorization of biomass feedstocks via tandem reactions.","PeriodicalId":149,"journal":{"name":"ChemSusChem","volume":" ","pages":"e202402165"},"PeriodicalIF":7.5,"publicationDate":"2024-11-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142637961","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

Unfolding Electrolyzer Characteristics to Reveal Solar-to-Chemical Efficiency Potential: Rapid Analysis Method Bridging Electrochemistry and Photovoltaics. 揭示电解槽特性，揭示太阳能转化为化学能的潜力：连接电化学与光伏学的快速分析方法。

IF 7.5 2区化学

ChemSusChem Pub Date : 2024-11-15 DOI: 10.1002/cssc.202402027

Oleksandr Astakhov, Thérèse Cibaka, Lars Wieprecht, Uwe Rau, Tsvetelina Merdzhanova

{"title":"Unfolding Electrolyzer Characteristics to Reveal Solar-to-Chemical Efficiency Potential: Rapid Analysis Method Bridging Electrochemistry and Photovoltaics.","authors":"Oleksandr Astakhov, Thérèse Cibaka, Lars Wieprecht, Uwe Rau, Tsvetelina Merdzhanova","doi":"10.1002/cssc.202402027","DOIUrl":"https://doi.org/10.1002/cssc.202402027","url":null,"abstract":"Development of photovoltaic-electrochemical (PV-EC) systems for energy storage and industry decarbonization requires multidisciplinary collaborative efforts of different research groups from both photovoltaic and electrochemical research communities. Consequently, the evaluation of the solar-to-chemical or solar-to-fuel efficiency of a new electrolyzer (EC) as a part of a PV-EC system is a time-consuming task that is challenging in a routine optimization loop. To address this issue, a new rapid assessment method is proposed. This method employs power balance requirements to unfold the input EC characteristics into the parameter space of PV-EC systems. The system parameters, composed with the EC output characteristics, yield the solar-to-chemical efficiency attainable by the electrolyzer in combination with any PV device under any irradiance at any relative PV-to-EC scaling and any mode of power coupling. This comprehensive overview is achieved via a mathematically simple conversion of the EC characteristics in any spreadsheet software. The method, designed to streamline the development and minimize the efforts of both the photovoltaic and electrochemical communities, is demonstrated via the analysis of CO2-reduction electrolyzer characteristics and verified with dedicated PV-EC experiments.","PeriodicalId":149,"journal":{"name":"ChemSusChem","volume":" ","pages":"e202402027"},"PeriodicalIF":7.5,"publicationDate":"2024-11-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142637962","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

Influence of Process Conditions During Aqueous and Direct Recycling of NMC811 Cathodes. NMC811 阴极水循环和直接循环过程中工艺条件的影响。

IF 7.5 2区化学

ChemSusChem Pub Date : 2024-11-14 DOI: 10.1002/cssc.202401803

Felix Nagler, Leonhard Kolb, Nino Christian, Andreas Flegler, Michael Hofmann, Guinevere A Giffin

{"title":"Influence of Process Conditions During Aqueous and Direct Recycling of NMC811 Cathodes.","authors":"Felix Nagler, Leonhard Kolb, Nino Christian, Andreas Flegler, Michael Hofmann, Guinevere A Giffin","doi":"10.1002/cssc.202401803","DOIUrl":"https://doi.org/10.1002/cssc.202401803","url":null,"abstract":"This study investigated the impact of various process conditions on the aqueous, direct recycling of LiNi0.8Mn0.1Co0.1O2 (NMC811) cathodes. Three model systems were used. The first system assumes that the current collector delamination is performed in a dry environment without the use of water as a process medium. Consequently, the NMC811 is only exposed to water during classification, where no aluminum foil is present. The second model system assumes that the current collector delamination occurs in water. Therefore, the NMC811 is exposed to water in the presence of aluminum foil. Due to the pH increase caused by the Li+/H+ exchange reaction, the pH value surpasses the stability window of the aluminum-oxide passivation layer (pH 4.5-8.5), resulting in the deposition of aluminum-containing species on the NMC811 surface. The third model system is identical to the second, with the exception that H3PO4 is added. This causes the pH to decrease and prevents corrosion of the aluminum foil. The findings reveal that process conditions significantly affect the surface chemistry on NMC811, influencing electrochemical performance. Notably, aluminum-containing species increase polarization. Heat treatment simulating regeneration led to cation mixing as surface species diffused into the NMC811 bulk structure, highlighting the need to control recycling process conditions.","PeriodicalId":149,"journal":{"name":"ChemSusChem","volume":" ","pages":"e202401803"},"PeriodicalIF":7.5,"publicationDate":"2024-11-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142611836","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