ChemSusChem最新文献

Valorization of Humins by Cyclic Levulinic Acid Production Using Polyoxometalates and Formic Acid.

IF 7.5 2区化学

ChemSusChem Pub Date : 2025-01-15 DOI: 10.1002/cssc.202401973

Andre Wassenberg, Tobias Esser, Maximilian J Poller, Dorothea Voß, Jakob Albert

引用次数: 0

Engineering Cascade Bio-solar Cells Inspired by the Z-Scheme of Oxygenic Photosynthesis: Layered Chlorophyll and Bacterio-chlorophyll Derivatives.

IF 7.5 2区化学

ChemSusChem Pub Date : 2025-01-15 DOI: 10.1002/cssc.202402588

Shengnan Duan, Teng Gu, Chiasa Uragami, Shin-Ichi Sasaki, Yuanqi Zhou, Ruohan Tao, Xianju Zhou, Chunbao Feng, Hitoshi Tamiaki, Xiao-Feng Wang, Zeyun Xiao, Hideki Hashimoto

{"title":"Engineering Cascade Bio-solar Cells Inspired by the Z-Scheme of Oxygenic Photosynthesis: Layered Chlorophyll and Bacterio-chlorophyll Derivatives.","authors":"Shengnan Duan, Teng Gu, Chiasa Uragami, Shin-Ichi Sasaki, Yuanqi Zhou, Ruohan Tao, Xianju Zhou, Chunbao Feng, Hitoshi Tamiaki, Xiao-Feng Wang, Zeyun Xiao, Hideki Hashimoto","doi":"10.1002/cssc.202402588","DOIUrl":"https://doi.org/10.1002/cssc.202402588","url":null,"abstract":"The natural Z-scheme of oxygenic photosynthesis efficiently drives electron transfer from photosystem II (PSII) to photosystem I (PSI) via an electron transport chain, despite the lower energy levels of PSII. Inspired by this sophisticated mechanism, we present a layered cascade bio-solar cell (CBSC) that emulates the Z-scheme. In this design, chlorophyll derivatives (Chl) act as PSI analogs, while bacteriochlorophyll derivatives (BChl) serve as PSII analogs in the active layer. The resulting photocurrent, prominently detected in the near-infrared region, is validated through external quantum efficiency measurements. Sub-nanosecond transient absorption spectroscopy reveals a prolonged charge transfer (CT) state from BChl to Chl (Chl-/BChl+ species) compared to the reverse direction (Chl+/BChl- species). This asymmetry highlights a dominant electron flow from BChl (PSII analog) to Chl (PSI analog) under simultaneous excitation, effectively replicating the natural Z-scheme electron transfer. These findings represent a significant advance in the design of bio-inspired solar cells, paving the way for artificial photosynthesis systems and offering profound insights into improving photovoltaic theory and efficiency.","PeriodicalId":149,"journal":{"name":"ChemSusChem","volume":" ","pages":"e202402588"},"PeriodicalIF":7.5,"publicationDate":"2025-01-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142982274","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

Chemical and Enzymatic Mechanosynthesis of Organocatalytic Peptide Materials Based on Proline and Phenylalanine.

IF 7.5 2区化学

ChemSusChem Pub Date : 2025-01-15 DOI: 10.1002/cssc.202402446

Alexandra Rios-Echeverri, Carlos E Puerto Galvis, Karen J Ardila-Fierro, José G Hernández

引用次数: 0

The Impact of Ligand Structure and Reaction Temperature on Ethenolysis of Fatty Acid Methyl Esters Catalyzed by Spirocyclic Alkyl Amino Carbene Ru Complexes.

IF 7.5 2区化学

ChemSusChem Pub Date : 2025-01-15 DOI: 10.1002/cssc.202402190

Anna V Afanaseva, Alexander A Vinogradov, Alexey A Vinogradov, Mikhail E Minyaev, Dmitry A Pyatakov, Alexander N Tavtorkin, Vladimir V Bagrov, Pavel V Ivchenko, Ilya Nifant'ev

{"title":"The Impact of Ligand Structure and Reaction Temperature on Ethenolysis of Fatty Acid Methyl Esters Catalyzed by Spirocyclic Alkyl Amino Carbene Ru Complexes.","authors":"Anna V Afanaseva, Alexander A Vinogradov, Alexey A Vinogradov, Mikhail E Minyaev, Dmitry A Pyatakov, Alexander N Tavtorkin, Vladimir V Bagrov, Pavel V Ivchenko, Ilya Nifant'ev","doi":"10.1002/cssc.202402190","DOIUrl":"https://doi.org/10.1002/cssc.202402190","url":null,"abstract":"Spirocyclic alkyl amino carbene (SCAAC) Ru complexes demonstrate outstanding activity and selectivity in ethenolysis of methyl oleate (MO) or fatty acid methyl esters (FAMEs), and 5,6-dimethoxyindane derivative was the most active catalyst to date. For the further catalyst design, we proposed modifying the spirocyclic fragment by fusion of saturated carbo- or heterocycle, linked to the 5,6-positions of indane or 6,7- positions of tetralin. Another suggested way of the modification of SCAAC complex was the insertion of chromane fragment to the carbene ligand. Using an alternative approach to SCAAC ligand precursors, based on hydroformylation of indenes, dihydronaphthalenes and their analogs, new SCAAC complexes were synthesized, their cis-configuration was confirmed by XRD. Comparative study of new and known selected complexes in ethenolysis of FAMEs (84 wt% MO) revealed that each of SCAAC catalysts has a temperature optimum of activity. At 60 °C 0.5 ppm of the complex containing 1,2,3,4,5,6,7,8-octahydroanthracene spirocyclic fragment provided 56% conversion of FAMEs with TON = 1.1∙106; 0.25 ppm of this complex in ethenolysis of high-purity MO demonstrated the TON ~2∙106, leading among the catalysts under study. In ethenolysis of FAMEs chromane derivative showed TON of 4-6∙105 and unprecedented temperature-independent 99.7-99.9% selectivity at 15-60 °C.","PeriodicalId":149,"journal":{"name":"ChemSusChem","volume":" ","pages":"e202402190"},"PeriodicalIF":7.5,"publicationDate":"2025-01-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142982283","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

Continuous Production of Bifunctional Platform Chemicals from Plant Oils in Water by Cyclodextrin-Mediated Hydroformylation.

IF 7.5 2区化学

ChemSusChem Pub Date : 2025-01-14 DOI: 10.1002/cssc.202402421

Thomas Friedrich Hubertus Roth, Tobias Averbeck, Marvin Daalmann, Dieter Vogt, Thomas Seidensticker

{"title":"Continuous Production of Bifunctional Platform Chemicals from Plant Oils in Water by Cyclodextrin-Mediated Hydroformylation.","authors":"Thomas Friedrich Hubertus Roth, Tobias Averbeck, Marvin Daalmann, Dieter Vogt, Thomas Seidensticker","doi":"10.1002/cssc.202402421","DOIUrl":"https://doi.org/10.1002/cssc.202402421","url":null,"abstract":"Platform chemicals from renewable resources with broad applications are highly desirable, particularly for replacing fossil-based monomers. Bifunctional aliphatic ester-aldehydes, accessible via regioselective hydroformylation of unsaturated oleochemicals, can be converted into linear ω-amino/ω-hydroxy esters and dicarboxylic acids-key building blocks for biobased aliphatic polycondensates. However, their success hinges on efficient, economically viable production, with catalyst recycling being critical. We present the Rh-catalyzed, cyclodextrin-mediated, aqueous biphasic hydroformylation of methyl 10-undecenoate (from castor oil) and methyl 9-decenoate (from rapeseed oil) to produce methyl 12-oxododecanoate and methyl 11-oxoundecanoate, respectively, with high yields and productivity. This system allows for efficient catalyst recycling via decantation, maintaining 30% of its native activity in aqueous biphasic conditions. Reaction conditions were optimized using a tailored experimental design, reducing nearly 200 experiments to 39 without sacrificing predictive accuracy. The optimized conditions were transferred to a continuous miniplant, achieving a low rhodium loss of 0.018 % h⁻¹, with excellent space-time yields of 76.5 kg h⁻¹ m⁻³. Rhodium in the product was as low as 79 ppb, with 4.4 kg of product per mg of catalyst lost, marking a significant step in combining hydroformylation-derived, bio-based platform chemicals with economic industrial potential.","PeriodicalId":149,"journal":{"name":"ChemSusChem","volume":" ","pages":"e202402421"},"PeriodicalIF":7.5,"publicationDate":"2025-01-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142977020","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

Modification strategies of bismuth-based halide perovskites for solar to fuel conversion by photocatalytic CO2 reduction.

IF 7.5 2区化学

ChemSusChem Pub Date : 2025-01-14 DOI: 10.1002/cssc.202402106

Pei Tian, Yan Ding, Fei Zhang, Yihao Zhang, Jinjia Wei, Jie Chen

{"title":"Modification strategies of bismuth-based halide perovskites for solar to fuel conversion by photocatalytic CO2 reduction.","authors":"Pei Tian, Yan Ding, Fei Zhang, Yihao Zhang, Jinjia Wei, Jie Chen","doi":"10.1002/cssc.202402106","DOIUrl":"https://doi.org/10.1002/cssc.202402106","url":null,"abstract":"In light of the increasingly pressing energy and environmental challenges, the use of photocatalysis to convert solar energy into chemical energy has emerged as a promising solution. Halide perovskites have recently attracted considerable interest as photocatalysts due to their outstanding properties. Early developments focused on Lead-based perovskites, but their use has been severely restricted due to the toxicity of Lead. Consequently, researchers have introduced non-toxic elements to replace Lead, with common substitutes being transition metals such as Tin (Sn), Bismuth (Bi), and Antimony (Sb). Among them, Bi-based perovskites have demonstrated superior photocatalytic performance. Nevertheless, the inherent instability of perovskites and the severe recombination of charge carriers have necessitated the development of various modification strategies to enhance their performance. This Review discusses the modification strategies for Bi-based halide perovskites and illustrates the impact of these strategies on the photocatalytic performance. Finally, future modification strategies of Bi-based perovskites for photocatalysis are proposed.","PeriodicalId":149,"journal":{"name":"ChemSusChem","volume":" ","pages":"e202402106"},"PeriodicalIF":7.5,"publicationDate":"2025-01-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142982278","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

Facile and Versatile Mechanochemical Synthesis of Indigoid Photoswitches.

IF 7.5 2区化学

ChemSusChem Pub Date : 2025-01-13 DOI: 10.1002/cssc.202402503

Arturo Llamosí, Oksana Danylyuk, Agnieszka Szumna

引用次数: 0

Revealing the Dynamics of Sustainable Epoxy-Acrylate Networks from Recycled Plastics Blends and Oligomeric Lignin Precursors.

IF 7.5 2区化学

ChemSusChem Pub Date : 2025-01-13 DOI: 10.1002/cssc.202402375

Marc Comi, Marlies Thys, Annelore Aerts, Stijn Geudens, Sam Vloemans, Elias Feghali, Karolien Vanbroekhoven, Richard Vendamme

{"title":"Revealing the Dynamics of Sustainable Epoxy-Acrylate Networks from Recycled Plastics Blends and Oligomeric Lignin Precursors.","authors":"Marc Comi, Marlies Thys, Annelore Aerts, Stijn Geudens, Sam Vloemans, Elias Feghali, Karolien Vanbroekhoven, Richard Vendamme","doi":"10.1002/cssc.202402375","DOIUrl":"https://doi.org/10.1002/cssc.202402375","url":null,"abstract":"The growing pursuit of carbon circularity in material fabrication has led to the increased use of recycled and biobased resources, especially in epoxy resin systems. Fossil-based bisphenols are being replaced with recycled bisphenol A (r-BPA) and lignin derivatives, both derived from previous processes. In this study, r-BPA was chemically recycled from end-of-life televisions, then converted into r-DGEBA and r-DAGBA through glycidylation and acrylic acid ring-opening. These monomers were used to create six thermosets by reacting Jeffamine D230 with r-DGEBA/r-DAGBA in varying epoxide:acrylate ratios. Acrylates introduced thermo-reversible β-amino esters, enabling dynamic bonding in the epoxy formulation. To increase biobased content, glycidylated depolymerized lignin (GDL) was added to produce five additional polymers. The crosslinked networks were thoroughly characterized, examining their thermomechanical properties and establishing a structure-property relationship. The dissociative acrylate-amine interactions allowed for reversible crosslinks under specific thermal conditions, enabling shape programming and crosslink reversibility. The study demonstrates that incorporating recycled and biobased aromatic monomers facilitates the creation of dynamic, crosslinked structures with tunable properties. This represents progress toward versatile, reusable, and circular materials.","PeriodicalId":149,"journal":{"name":"ChemSusChem","volume":" ","pages":"e202402375"},"PeriodicalIF":7.5,"publicationDate":"2025-01-13","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142968999","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

Ionogel-Based Electrodes for Non-Flammable High-Temperature Operating Electrochemical Double Layer Capacitors.

IF 7.5 2区化学

ChemSusChem Pub Date : 2025-01-13 DOI: 10.1002/cssc.202401874

Agnese Gamberini, Tobias Burton, Alix Ladam, Ahmad Bagheri, Matteo Abruzzese, Hossein Beydaghi, Valentina Mastronardi, Elena Calcagno, Samaneh Vaez, Alberto Morenghi, Teresa Gatti, Anais Falgavrat, Francesco Bonaccorso, Sebastien Fantini, Sebastiano Bellani

{"title":"Ionogel-Based Electrodes for Non-Flammable High-Temperature Operating Electrochemical Double Layer Capacitors.","authors":"Agnese Gamberini, Tobias Burton, Alix Ladam, Ahmad Bagheri, Matteo Abruzzese, Hossein Beydaghi, Valentina Mastronardi, Elena Calcagno, Samaneh Vaez, Alberto Morenghi, Teresa Gatti, Anais Falgavrat, Francesco Bonaccorso, Sebastien Fantini, Sebastiano Bellani","doi":"10.1002/cssc.202401874","DOIUrl":"https://doi.org/10.1002/cssc.202401874","url":null,"abstract":"The design of interfaces between nanostructured electrodes and advanced electrolytes is critical for realizing advanced electrochemical double-layer capacitors (EDLCs) that combine high charge-storage capacity, high-rate capability, and enhanced safety. Toward this goal, this work presents a novel and sustainable approach for fabricating ionogel-based electrodes using a renewed slurry casting method, in which the solvent is replaced by the ionic liquid (IL), namely 1-ethyl-3-methylimidazolium bis(fluorosulfonyl)imide (EMIFSI). This method avoids time-consuming and costly electrolyte-filling steps by integrating the IL directly into the electrode during slurry preparation, while improving the rate capability of EDLCs based on non-flammable ILs. The resulting ionogel electrodes demonstrate exceptional electrolyte accessibility and enable the production of symmetric EDLCs with high energy density (over 30Wh/kg based on electrode material weight) and high-rate performance. These EDLCs could operate at temperatures up to 180°C, far exceeding the limitations of traditional EDLCs based on organic electrolytes (1M TEABF4 in acetonitrile, up to 65°C). Ionogel-type EDLCs exhibit remarkable stability, retaining 88% specific capacity after 10000 galvanostatic charge/discharge cycles at 10Ag-1 and demonstrating superior retention compared to conventional EDLCs (50%), while also maintaining 92.4% energy density during 100h floating tests at 2.7V. These electrochemical properties highlight their potential for robust performance under demanding conditions.","PeriodicalId":149,"journal":{"name":"ChemSusChem","volume":" ","pages":"e202401874"},"PeriodicalIF":7.5,"publicationDate":"2025-01-13","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142968997","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

Interfacial Metal Oxides Stabilize Cu Oxidation States for Electrocatalytical CO2 Reduction.

IF 7.5 2区化学

ChemSusChem Pub Date : 2025-01-13 DOI: 10.1002/cssc.202402510

Yajie Zhao, Haoyuan Wang, Chunxiao Liu, Yuan Ji, Xu Li, Qiu Jiang, Chuan Xia, Tingting Zheng

{"title":"Interfacial Metal Oxides Stabilize Cu Oxidation States for Electrocatalytical CO2 Reduction.","authors":"Yajie Zhao, Haoyuan Wang, Chunxiao Liu, Yuan Ji, Xu Li, Qiu Jiang, Chuan Xia, Tingting Zheng","doi":"10.1002/cssc.202402510","DOIUrl":"https://doi.org/10.1002/cssc.202402510","url":null,"abstract":"Modulating the oxidation state of copper (Cu) is crucial for enhancing the electrocatalytic CO2 reduction reaction (CO2RR), particularly for facilitating deep reductions to produce methane (CH4) or multi-carbon (C2+) products. However, Cuδ+ sites are thermodynamically unstable, fluctuating their oxidation states under reaction conditions, which complicates their functionality. Incorporating interfacial metal oxides has emerged as an effective strategy for stabilizing these oxidation states. This review provides an in-depth examination of the reaction mechanisms occurring at oxide-modified Cuδ+ sites, offering a comprehensive understanding of their behavior. We explore how Cu/metal oxide interfaces stabilize Cu oxidation states, showing that oxides-modified Cu catalysts often enhance selectivity for C2+ or CH4 products by stabilizing Cu+ or Cu2+ sites. In addition, we discuss innovative strategies for the rational design of efficient Cu catalytic sites tailored for specific deep CO2RR products. The review concludes with an outlook on current challenges and future directions, offering new insights into the rational design of selective and efficient CO2RR catalysts.","PeriodicalId":149,"journal":{"name":"ChemSusChem","volume":" ","pages":"e202402510"},"PeriodicalIF":7.5,"publicationDate":"2025-01-13","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142968995","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