ChemSusChemPub Date : 2025-04-08DOI: 10.1002/cssc.202402488
Aby Cheruvathoor Poulose, Hugo Bares, Dagmar Zaoralová, Ivan Dědek, Michal Otyepka, Aristides Bakandritsos, Radek Zboril
{"title":"Amino-Sulfonated Graphene as a Catalyst for Efficient Production of Biodiesel from Fatty Acids and Crude Vegetable Oils.","authors":"Aby Cheruvathoor Poulose, Hugo Bares, Dagmar Zaoralová, Ivan Dědek, Michal Otyepka, Aristides Bakandritsos, Radek Zboril","doi":"10.1002/cssc.202402488","DOIUrl":"https://doi.org/10.1002/cssc.202402488","url":null,"abstract":"<p><p>Climate change and the depletion of fossil fuels increase the demand for sustainable energy. Biodiesel, synthesized with heterogeneous acid catalysts, is a promising chemical carrier of clean energy, adhering to circular carbon economy . Here, we report the particularly effective synthesis of biodiesel using a reusable, solid-state acid graphene catalyst functionalized with a natural aminosulfonic acid. Experimental and theoretical studies unveil the key role of the functionalities containing simultaneously an amino and sulfonate group, ascribing superior acidity. Excellent activity and selectivity for oleic acid conversion to oleic acid methyl esters (a sustainable biofuel) were obtained, offering a strategy for achieving improved catalytic performance compared to earlier or benchmark catalysts in the field. Notably, the catalyst is also highly effective in converting commonly available vegetable oils to biodiesel through trans-esterification, and in carbohydrate dehydration to value-added chemicals, demonstrating its general applicability. Two more variants of aminosulfonic acid‑functionalized graphenes demonstrated very similar activities, validating the key role of such functionalities on the high acidity and activity. The development of such potent, recyclable catalysts is crucial since acid catalysis is arguably the most general and versatile approach for organic reactions, ubiquitous in an extraordinary range of biological and synthetic transformations.</p>","PeriodicalId":149,"journal":{"name":"ChemSusChem","volume":" ","pages":"e202402488"},"PeriodicalIF":7.5,"publicationDate":"2025-04-08","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143801978","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":"Solvent-Swing CO2 Capture with Aralkylamines.","authors":"Ryo Murakami, Hiroto Tanishima, Risa Otsuka, Ayaka Uchida, Narumi Iwamoto, Fuyuhiko Inagaki","doi":"10.1002/cssc.202500112","DOIUrl":"https://doi.org/10.1002/cssc.202500112","url":null,"abstract":"<p><p>A critical bottleneck in CO2 capture technologies is the substantial energy requirement for CO2 release and concentration during the separation process. This study introduces a novel CO2 emission system that overcomes this challenge through retro-neutralization due to the solubility difference. The simple addition of a solvent, requiring no external energy, enables the release of CO2 from aralkylamine-CO2 complexes at room temperature.</p>","PeriodicalId":149,"journal":{"name":"ChemSusChem","volume":" ","pages":"e202500112"},"PeriodicalIF":7.5,"publicationDate":"2025-04-08","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143802018","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":"Efficient One-Step Synthesis of Lactide with High Yield and Selectivity Using Brønsted Acid Catalysis.","authors":"Yingjie Zhao, Wenqi Qiu, Yukang Liu, Yufei Zhang, Xiaotao Wang, Yuman Guo, Hui Liu, Canbin Ouyang, Zongxia Guo","doi":"10.1002/cssc.202500100","DOIUrl":"https://doi.org/10.1002/cssc.202500100","url":null,"abstract":"<p><p>In this work, a one-step method synthesis of lactide was reported instead of the traditional two-step method. The selection of a suitable acid catalyst polyphosphoric acid (PPA) and optimization of reaction conditions resulted in a yield of 97%. Moreover, this new one-step strategy eliminates the need for metal catalysts and does not require high-temperature conditions, thereby avoiding the issue of racemization. The simple one-step strategy offers a combination of efficiency, sustainability, and product quality improvements, making it a modern, practical approach to lactide synthesis.</p>","PeriodicalId":149,"journal":{"name":"ChemSusChem","volume":" ","pages":"e202500100"},"PeriodicalIF":7.5,"publicationDate":"2025-04-08","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143801986","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":"Electrostatic Self-Assembly of NiTiO3 on Carbon Nitride as a Photocatalyst for Visible-Light-Driven Overall Water Splitting.","authors":"Long Wang, Haihua Wu, Yifan Lin, Mingyue Wang, Zilong Wang, Wandong Xing, Sibo Wang, Yuanxing Fang","doi":"10.1002/cssc.202500338","DOIUrl":"https://doi.org/10.1002/cssc.202500338","url":null,"abstract":"<p><p>Achieving intimate contact is crucial for the efficiency of a photocatalyst that includes both reduction and oxidation compartments, as it directly influences charge carrier transfer between them. However, traditional metal oxide-based photocatalysts often face intrinsic limitations in integrating these two functional components due to the difficulty in adjusting their surfaces. Herein, protonated polymeric carbon nitride nanosheets (CNNS) with controlled electrostatic property was integrated with NiTiO3 (NTO). Among them, CNNS functions as the hydrogen evolution photocatalyst (HEP), and NTO nanoparticles served as the oxygen evolution photocatalyst (OEP), resulting in a photocatalytic system for OWS. The system exhibits H₂ and O₂ evolution rates of 35.6 and 17.7 μmol·h⁻¹, respectively, and the corresponding apparent quantum yield is 2.7% at an incident wavelength of 365 nm, outperforming those of individual photocatalysts. This study introduces an applicable electrostatic self-assembly strategy for using carbon nitride to construct redox-mediator-free heterojunctions, thereby advancing applications in various fields, particularly the hydrogen evolution reaction via photocatalytic OWS.</p>","PeriodicalId":149,"journal":{"name":"ChemSusChem","volume":" ","pages":"e202500338"},"PeriodicalIF":7.5,"publicationDate":"2025-04-07","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143794107","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 : 2025-04-07DOI: 10.1002/cssc.202500180
Ida Dinges, Markus Pyschik, Julian Schütz, Selina Schneider, Elias Klemm, Siegfried R Waldvogel, Markus Stöckl
{"title":"All Electrochemical Synthesis of Performic Acid Starting from CO2, O2 and H2O.","authors":"Ida Dinges, Markus Pyschik, Julian Schütz, Selina Schneider, Elias Klemm, Siegfried R Waldvogel, Markus Stöckl","doi":"10.1002/cssc.202500180","DOIUrl":"https://doi.org/10.1002/cssc.202500180","url":null,"abstract":"<p><p>Driven by anthropogenic climate change, innovative approaches to defossilise the chemical industry are required. With this study, the first all-electrochemical feasibility study for the complete electrosynthesis of the strong oxidiser and effective disinfectant performic acid is presented. Its synthesis was achieved solely from CO2, O2 and H2O in a two-step process. Initially, CO2 is electrochemically reduced to formate employing Bi2O3 based gas diffusion electrodes in a phosphate buffered electrolyte. Thereby, high formate concentration (500.7 ± 0.6 mmol L-1) and high Faradaic efficiency (86.3 ± 0.3%) were achieved at technically relevant current density (150 mA cm-2). Subsequently, the formate acts as (storable) feed electrolyte for the second electrolysis step. Employing carbon based gas diffusion electrodes, O2 is reduced to H2O2 and performic acid is directly formed in-situ. As before, high H2O2 concentration (1.27 ± 0.06 mol L-1) and high Faradaic efficiency (85.3 ± 5.4%) were achieved. Furthermore, performic acid concentration suitable for disinfection was obtained (82 ± 11 mmol L-1). In summary, this innovative feasibility study highlights the potential of combining electrochemical CO2 reduction with H2O2 electrosynthesis, which could provide sustainable access to performic acid in the future.</p>","PeriodicalId":149,"journal":{"name":"ChemSusChem","volume":" ","pages":"e202500180"},"PeriodicalIF":7.5,"publicationDate":"2025-04-07","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143794273","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 : 2025-04-07DOI: 10.1002/cssc.202500350
Xingjie Cheng, Hong Li, Jinchen Fan, Weiju Hao, Qingyuan Bi, Guisheng Li
{"title":"Phosphorus-Modified High-Entropy Layered Double Hydroxide for Enhanced Electrocatalytic Oxygen Evolution via d-Band Center Modulation.","authors":"Xingjie Cheng, Hong Li, Jinchen Fan, Weiju Hao, Qingyuan Bi, Guisheng Li","doi":"10.1002/cssc.202500350","DOIUrl":"https://doi.org/10.1002/cssc.202500350","url":null,"abstract":"<p><p>Developing cost-effective, high-performance electrocatalysts for the oxygen evolution reaction (OER) is crucial but challenging. High-entropy layered double hydroxides (HE-LDHs) show promise due to their multi-metal synergy and structural complexity, yet their OER performance is limited by electronic and surface properties. This study combines theoretical and experimental methods to enhance OER by incorporating phosphorus (P) atoms in HE-LDHs, optimizing oxygen intermediate adsorption, and boosting OER activity and stability. A P-modified FeNiCoCuZn LDH catalyst (P-FeNiCoCuZn LDH) was synthesized via hydrothermal and low-temperature phosphatization processes, featuring phosphate anion intercalation and surface metal phosphides. The phosphate anions improve conductivity and stability, while surface P atoms adjust the electronic structure of metal sites, particularly Ni and Fe, reducing the energy barrier for the rate-determining step (*O→*OOH). The P-FeNiCoCuZn LDH achieves a low overpotential of 290 mV at 100 mA cm-2 and maintains stability for 100 hours in 1 M KOH. In-situ Raman spectroscopy shows the formation of highly active Ni(Fe)-OOH species during OER. This work offers a novel strategy for designing efficient water-splitting catalysts through in-situ heteroatom modification, advancing high-entropy materials in electrocatalysis.</p>","PeriodicalId":149,"journal":{"name":"ChemSusChem","volume":" ","pages":"e202500350"},"PeriodicalIF":7.5,"publicationDate":"2025-04-07","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143794175","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 : 2025-04-07DOI: 10.1002/cssc.202500364
Jun Wang, Lijuan Chen, Lan Huang, Tengfei Chen, Juqin Zeng, Wenbo Ju
{"title":"Direct Carbonate Reduction on Sn Oxide Surface.","authors":"Jun Wang, Lijuan Chen, Lan Huang, Tengfei Chen, Juqin Zeng, Wenbo Ju","doi":"10.1002/cssc.202500364","DOIUrl":"https://doi.org/10.1002/cssc.202500364","url":null,"abstract":"<p><p>Direct reduction of carbonate (CO32‒) to value-added chemicals presents several advantages for integrating CO2 capture from air with electrochemical conversion at near-unity efficiency. However, a critical challenge lies in effectively adsorbing CO32‒ as a reactive intermediate for sequential reduction. Density functional theory calculations indicate that the presence of oxygen vacancies (VO) on a SnO2 surface significantly enhances its reactivity toward CO32‒ adsorption, with the resulting adsorbed species (*CO3) detectable by Raman spectroscopy. Operando electrochemical Raman spectra have confirmed the formation of *CO3 on the partially reduced SnO2-xVO surface. Pulsed electrolysis has successfully converted CO32‒ to CO at a constant flow rate in an electrolyzer featuring a gas diffusion electrode configuration. A reaction cycle, encompassing SnO2 partial reduction, CO32‒ adsorption and reduction, and SnO2 regeneration, has been proposed as a viable approach for continuous direct CO32‒ reduction.</p>","PeriodicalId":149,"journal":{"name":"ChemSusChem","volume":" ","pages":"e202500364"},"PeriodicalIF":7.5,"publicationDate":"2025-04-07","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143794188","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 : 2025-04-07DOI: 10.1002/cssc.202500347
Wen Yan, Chi Wang, Xiaoyue Li, Ying Jiang
{"title":"Coupling Agents in Lithium Batteries: Impact on Enhancing Interfacial Bonding and Stability.","authors":"Wen Yan, Chi Wang, Xiaoyue Li, Ying Jiang","doi":"10.1002/cssc.202500347","DOIUrl":"https://doi.org/10.1002/cssc.202500347","url":null,"abstract":"<p><p>Lithium-ion and lithium metal batterie are the cornerstone of modern energy storage but face significant challenges related to interfacial stability, including solid-electrolyte interphase (SEI) formation, lithium dendrite growth, and electrode degradation. Coupling agents offer a promising solution to address these issues by enhancing interfacial bonding, improving compatibility, and reducing resistance. This review provides a comprehensive overview of the role of coupling agents in optimizing battery interfaces, focusing on their functions as adhesion promoters, protective surface layers, and precursors for electrode material synthesis. We also discuss their applications in composite solid electrolytes, gel polymer electrolytes, and protective coatings for metallic lithium anodes and current collectors. The impacts of coupling agents on interfacial bonding and stability, as well as the interaction mechanisms, are examined at the molecular level. By highlighting recent advancements and challenges, this review aims to guide future research in interfacial engineering for high-performance composite materials and optimized interfaces in batteries.</p>","PeriodicalId":149,"journal":{"name":"ChemSusChem","volume":" ","pages":"e202500347"},"PeriodicalIF":7.5,"publicationDate":"2025-04-07","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143801982","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 : 2025-04-07DOI: 10.1002/cssc.202500044
Long Pan, Xiong Xiong Liu, Pengcheng Yuan, Haotian Zhang, Yuan Zhang, Mufan Cao, Min Gao, Yaping Wang, Tomasz Wejrzanowski, Wei Zhang, ZhengMing Sun
{"title":"Garnets Initiate Grafting of Methyl Methacrylate Brushes onto Fluoropolymers for Electrochemically Stable and Fast-Ion-Conducting Composite Solid-State Electrolytes.","authors":"Long Pan, Xiong Xiong Liu, Pengcheng Yuan, Haotian Zhang, Yuan Zhang, Mufan Cao, Min Gao, Yaping Wang, Tomasz Wejrzanowski, Wei Zhang, ZhengMing Sun","doi":"10.1002/cssc.202500044","DOIUrl":"https://doi.org/10.1002/cssc.202500044","url":null,"abstract":"<p><p>Fluoropolymer-based solid-state electrolytes (SSEs) promise next-generation all-solid-state Li metal batteries but suffer poor stability against Li metal anodes and sluggish Li+ transport. Here, we propose garnet-type Li6.4La3Zr1.4Ta0.6O12 (LLZTO) as a bifunctional mediator to enable the in-situ grafting and compositing for poly(vinylidene fluoride-co-hexafluoropropylene) (PVH), aiming at electrochemically stable and superionic SSEs. The LLZTO not only induces the formation of C=C bonds as active sites for effectively grafting methyl methacrylate (MMA) brush chains to PVH, but also acts as an ion-conducting filler to enhance mechanical properties and ion transport. In addition, the grafted MMA brush chains improve electrochemical stability against Li metal anodes and weaken polymer crystallinity to create amorphous domains for Li+ transport. Therefore, the resulting composite SSEs, PVH-graft-MMA/LLZTO (PVHML), achieves an impressive ionic conductivity of 0.94 mS cm-1 at 25 °C, high mechanical strength (2.02 MPa), and exceptional cycling stability in Li symmetric cells (2800 h at 0.1 mA cm-1, 25 °C). Furthermore, PVHML-based all-solid-state LiFePO4|Li full cells demonstrate superior cyclability with 89.8% capacity retention at 0.2C after 200 cycles (25 °C). This strategy provides an efficient solution to the challenges of fluoropolymer-based SSEs, paving the way for their practical applications in high-performance all-solid-state lithium metal batteries.</p>","PeriodicalId":149,"journal":{"name":"ChemSusChem","volume":" ","pages":"e202500044"},"PeriodicalIF":7.5,"publicationDate":"2025-04-07","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143801992","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 : 2025-04-07DOI: 10.1002/cssc.202500570
Ganesh D Sharma, Pengfei Li, Tingting Gu, Yi Fu, Xu Liang, Haijun Xu, Rahul Singhal
{"title":"BODIPY-coumarin triad as acceptor for ternary Non-Fullerene Solar Cells with over 15% Efficiency.","authors":"Ganesh D Sharma, Pengfei Li, Tingting Gu, Yi Fu, Xu Liang, Haijun Xu, Rahul Singhal","doi":"10.1002/cssc.202500570","DOIUrl":"https://doi.org/10.1002/cssc.202500570","url":null,"abstract":"<p><p>Herein, we synthesized a new non-fused fullerene-free acceptor based on the BODIPY-coumarin triad, BDP-2C, which exhibits a medium optical bandgap of about 1.51 eV, and HOMO and LUMO energy levels about -5.50 eV and -4.00 eV, respectively. Employing BDP-2C as a guest component in PM6:Y6, the resulting optimized ternary organic solar cells attained a power conversion efficiency (PCE) of about 15.09% with a low energy loss of 0.503 eV. The balanced charge transport and suppressed charge recombination, shorter charge extraction time, and prolonged charge carrier lifetime are the factors that enhance the PCE of ternary organic solar cells.</p>","PeriodicalId":149,"journal":{"name":"ChemSusChem","volume":" ","pages":"e202500570"},"PeriodicalIF":7.5,"publicationDate":"2025-04-07","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143794274","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}