ChemSusChemPub Date : 2025-03-26DOI: 10.1002/cssc.202500181
Lujie Jin, Yujin Ji, Youyong Li
{"title":"High-Throughput Screening of 1D Chalcogenide Cathode Materials Beyond VS4 for Rechargeable Magnesium-ion Batteries.","authors":"Lujie Jin, Yujin Ji, Youyong Li","doi":"10.1002/cssc.202500181","DOIUrl":"https://doi.org/10.1002/cssc.202500181","url":null,"abstract":"<p><p>Owing to their high theoretical specific capacity and abundance of anodes, rechargeable Mg-ion batteries (rMIBs) have emerged as a supplement for post-Li generation. However, the strong Coulomb interactions on Mg2+ cations lead to inefficient storage and transport in the cathode, which severely restricts the actual performance of rMIBs. Herein, a virtual screening of the 1D material database (C1DB) is proposed to identify novel rMIB chalcogenide cathodes with large voids for relieving the Coulomb forces. By referring to the representative VS4 material, three potential 1D chalcogenide materials (SiS2, GeS2, and SiSe2) with optimized Coulomb interactions are ultimately screened out for rMIB cathodes. In addition, further theoretical analyses on geometry, electronic structures, and atomic charges reveal the significant roles of the large specific pore volume, low bond covalency, and mildly oxidizing anion element in optimizing rMIB cathode materials. Overall, our work may inspire future experimental and theoretical investigations, potentially accelerating breakthroughs of rMIB and other similar metal-ion batteries.</p>","PeriodicalId":149,"journal":{"name":"ChemSusChem","volume":" ","pages":"e202500181"},"PeriodicalIF":7.5,"publicationDate":"2025-03-26","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143707903","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 : 2025-03-25DOI: 10.1002/cssc.202500184
John M Saunders, Kylee Dismuke Rodriguez, Robert Lammert, Jordan Yirak, Karthik S Iyer, Bruce Howard Lipshutz, Madison J Wong
{"title":"Recent Green and Sustainable Pd-Catalyzed Aminations.","authors":"John M Saunders, Kylee Dismuke Rodriguez, Robert Lammert, Jordan Yirak, Karthik S Iyer, Bruce Howard Lipshutz, Madison J Wong","doi":"10.1002/cssc.202500184","DOIUrl":"https://doi.org/10.1002/cssc.202500184","url":null,"abstract":"<p><p>Pd-catalyzed aminations, while a powerful and commonly employed method of C-N bond construction, often relies on unsustainable technologies that utilize: egregious organic solvents, high temperatures, long reaction times, and high catalyst loadings, especially of palladium. Only recently has there been a shift towards far greener protocols based recyclable aqueous media, as well as non-traditional organic solvents. In addition, non-traditional modes for preparing the same amines have appeared, such as continuous plug flow and mechanochemistry, which also offer safe and sustainable means of chemical synthesis associated with targets in the fine chemicals industry.</p>","PeriodicalId":149,"journal":{"name":"ChemSusChem","volume":" ","pages":"e202500184"},"PeriodicalIF":7.5,"publicationDate":"2025-03-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143707904","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 : 2025-03-25DOI: 10.1002/cssc.202500462
Yongbo Fan, Lin Lei, Jingshen Cao, Weijia Wang, Huiqing Fan
{"title":"Benzene Ring Engineering of Graphitic Carbon Nitride for Enhanced Photocatalytic Dye Degradation and Hydrogen Production from Water Splitting.","authors":"Yongbo Fan, Lin Lei, Jingshen Cao, Weijia Wang, Huiqing Fan","doi":"10.1002/cssc.202500462","DOIUrl":"https://doi.org/10.1002/cssc.202500462","url":null,"abstract":"<p><p>The photocatalytic activity of graphitic carbon nitride (g-C3N4) strongly depends on its electronic structure. To design the photocatalysts with efficient charge separation and transfer property, here we report a benzene ring doped g-C3N4 via one-pot thermal polycondensation of dicyandiamide and 2,4-diaminobenzenesulfonic acid. The carbon-rich benzene ring is embedded into g-C3N4, which enables the asymmetric modification of the heptazine units in g-C3N4 and the extension of the π-conjugate system without altering its long-range order structure significantly. Such molecular structure optimization effectively improves the visible light harvesting and charge carriers' separation ability. A high photocatalytic hydrogen evolution rate and dye degradation performance is achieved under visible light irradiation (λ > 420 nm), which is about 8.4 and 4.4-fold higher than that of pristine g-C3N4, respectively. The reasons for enhanced photocatalytic performance are ascribed to a favorable optical property, suppressed charge carrier recombination, and efficient charge transfer processes. This work provides a green and economical method to functionalize g-C3N4 using low content organic carbon molecule for efficient energy conversion related applications.</p>","PeriodicalId":149,"journal":{"name":"ChemSusChem","volume":" ","pages":"e202500462"},"PeriodicalIF":7.5,"publicationDate":"2025-03-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143707899","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 : 2025-03-25DOI: 10.1002/cssc.202500318
François Jérôme, Sarah Behloul, Karine De Oliveira Vigier, Frederic Guegan, Zhen Yan
{"title":"N,N-Dimethylhydrazone as a Reversible Derivatization Agent to Promote the Hydroxymethylation of Furfural with Formaldehyde.","authors":"François Jérôme, Sarah Behloul, Karine De Oliveira Vigier, Frederic Guegan, Zhen Yan","doi":"10.1002/cssc.202500318","DOIUrl":"https://doi.org/10.1002/cssc.202500318","url":null,"abstract":"<p><p>We explore here the synthesis of HMF from concentrated feeds of two low cost and industrially abundant chemicals: furfural and formaldehyde. By adjusting the acidity of the solvent, we discovered an alternative mechanism in which the reaction selectivity stops to the hydroxymethylation step, in contrast to previously reported acid-catalyzed pathways leading to the formation of the bisfuranic dimer as major products. One of the keys of this study relies on the reversible derivation of the -CHO group of furfural with N,N-dimethylhydrazone which plays a dual role (1) it restores the nucleophilicity of the furan ring and (2) it reacts with HCHO to form in situ an electrophilic zwiterrionic species stabilized through hydrogen transfer. By means of experimental and theoretical investigations, we discovered that guaiacol can be used as a biobased and safe solvent. Under optimized conditions, the hydroxymethylation of the furan ring of furfural occurs with more than 94% selectivity, at only 50 °C and with a stoichiometric amount of HCHO. A concentrated feed of furfural as high as 25 wt% in guaiacol was employed without impacting the reaction selectivity leading to an improvement of the reactor productivity to about 25 kg/m3/h. The recycling of the N,N-dimehylhydrazone is also discussed.</p>","PeriodicalId":149,"journal":{"name":"ChemSusChem","volume":" ","pages":"e202500318"},"PeriodicalIF":7.5,"publicationDate":"2025-03-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143699259","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 : 2025-03-25DOI: 10.1002/cssc.202500029
Alberto Bianco, Francesca Mancini, Giacomo Bergamini
{"title":"A pH-Switchable System for On-Demand Solar Hydrogen Production.","authors":"Alberto Bianco, Francesca Mancini, Giacomo Bergamini","doi":"10.1002/cssc.202500029","DOIUrl":"https://doi.org/10.1002/cssc.202500029","url":null,"abstract":"<p><p>Artificial Solar-to-Fuel conversion is a pivotal pathway toward a sustainable energy future. Molecular hydrogen H₂, with its clean energy potential, emerges as a promising candidate to replace fossil fuels. Nevertheless, the intermittent nature of solar irradiation presents a formidable obstacle. Inspired by natural photosynthesis, we employed a well-known three-component system to decouple light absorption and hydrogen evolution. Our system utilizes [Ru(bpy)3]2+, triethanolamine, and methyl viologen to store solar energy as reduced viologen (MV•+). By controlling pH, we can efficiently release this stored energy to produce hydrogen on demand. Our system demonstrates superior efficiency compared to platinum-based catalysts, along with remarkable reversibility, cyclability and stability. This work significantly advances solar-to-hydrogen conversion, providing a promising solution for the intermittent nature of solar energy and paving the way to a sustainable energy future.</p>","PeriodicalId":149,"journal":{"name":"ChemSusChem","volume":" ","pages":"e202500029"},"PeriodicalIF":7.5,"publicationDate":"2025-03-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143699258","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 : 2025-03-25DOI: 10.1002/cssc.202500460
Peng Xu, Eng Liang Lim, Zhanhua Wei
{"title":"A Brief Overview of Poly(3-Hexylthiophene) as a Hole Transport Material for Perovskite Solar Cell.","authors":"Peng Xu, Eng Liang Lim, Zhanhua Wei","doi":"10.1002/cssc.202500460","DOIUrl":"https://doi.org/10.1002/cssc.202500460","url":null,"abstract":"<p><p>Perovskite solar cells (PSCs) have been widely developed and are now moving towards large-scale commercialization. Hole transporting material (HTM) is an important part of PSCs, it plays a crucial role in facilitating hole extraction to the anode and blocking electrons from passing through it. Although 2,2',7,7'-Tetrakis(N,N-di-p-methoxyphenylamine)-9,9'-spirobifluorene (Spiro-OMeTAD) and polytriarylamine (PTAA) are the commonly explored HTMs in PSCs, they need unstable hygroscopic ion dopants and additives to enhance their hole mobility, which can deteriorate the performance/stability of the device. Benefiting from the low-cost synthesis, well batch-to-batch stability, excellent hole mobility and good moisture resistance of the poly(3-hexylthiophene) (P3HT), it has then been used as an alternative HTM in PSC applications. However, the energy level mismatch and the poor interface contact between the perovskite material and P3HT have limited hole transfer to the anode, thus affecting the device performance and stability. In this review, the research progress of the P3HT HTM through interface modification, doping strategy, P3HT derivatives and, etc. is summarized to address the aforementioned problems. Finally, we also provide guidance for further improving the efficiency and stability of P3HT-based PSCs.</p>","PeriodicalId":149,"journal":{"name":"ChemSusChem","volume":" ","pages":"e202500460"},"PeriodicalIF":7.5,"publicationDate":"2025-03-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143707880","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":"A Fully Conjugated Benzo[1,2-b:4,5-b']dithiophene-Based Covalent Organic Framework Enables Efficient Blue Light-Driven Photocatalytic Sulfoxidation.","authors":"Keke Zhang, Fulin Zhang, Yuexin Wang, Kanghui Xiong, Siyu Zhang, Xianjun Lang","doi":"10.1002/cssc.202500552","DOIUrl":"https://doi.org/10.1002/cssc.202500552","url":null,"abstract":"<p><p>Covalent organic frameworks (COFs) are becoming increasingly attractive in photocatalytic transformations because of the designable structures grounded on the building blocks and the linkage. Herein, benzo[1,2-b:4,5-b']dithiophene, essential for various organic optoelectronic materials, is adopted as the building block for COFs. Hence, a fully conjugated COF BDTT-sp2c-COF and imine-linked COF BDTT-COF are constructed of 5',5''''-(benzo[1,2-b:4,5-b']dithiophene-2,6-diyl)bis([1,1':3',1''-terphenyl]-4,4''-dicarbaldehyde) with p-phenyldiacetonitrile and p-phenylenediamine, respectively. Thorough characterizations and theoretical calculations disclose that BDTT-sp2c-COF is superior to BDTT-COF in terms of specific surface area, photocarrier separation, and electron transfer. As such, BDTT-sp2c-COF enables more efficient photocatalytic sulfoxidation with oxygen than BDTT-COF. The fully conjugated structure guarantees the recyclability of BDTT-sp2c-COF. The blue light-driven sulfoxidation is generally applicable and proceeds selectively via energy and electron transfers over BDTT-sp2c-COF. The fully conjugated COFs are promising to enable photocatalytic reactions.</p>","PeriodicalId":149,"journal":{"name":"ChemSusChem","volume":" ","pages":"e202500552"},"PeriodicalIF":7.5,"publicationDate":"2025-03-24","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143690665","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 : 2025-03-23DOI: 10.1002/cssc.202500039
Jianyu Li, Junjie Yang, Xiaoqi Peng, Shuwei Sheng, Haolin Wang, Yuehao Gu, Tao Chen, Hong Wang
{"title":"Hydrothermal Deposition of Metal Sulfide Heterojunction Thin Films for Photoelectrochemical Water Splitting.","authors":"Jianyu Li, Junjie Yang, Xiaoqi Peng, Shuwei Sheng, Haolin Wang, Yuehao Gu, Tao Chen, Hong Wang","doi":"10.1002/cssc.202500039","DOIUrl":"https://doi.org/10.1002/cssc.202500039","url":null,"abstract":"<p><p>Metal sulfides represent a broad class of materials with considerable potential for applications in photovoltaic devices and energy technologies. However, the low-temperature synthesis of high-quality metal sulfide thin films remains a formidable challenge. Hydrothermal deposition, known for its versatility and cost-efficiency, has been successfully employed to synthesize a variety of materials, yet its application in the preparation of metal sulfide thin films has not been extensively explored. In this study, we develop a hydrothermal deposition method to synthesize five distinct types of metal sulfide thin films, each with well-defined phases and compositions. As a case study, CdS/Bi2S3 thin film was selected and evaluated as photoanode for photoelectrochemical water splitting. Through O-doping and the modification of an ultrathin MoO3 overlayer, the photocurrent density was significantly enhanced from 1.52 mA cm-2 (CdS/Bi2S3) to 2.27 mA cm-2 (CdS/O-Bi2S3), and further to 2.84 mA cm-2 (CdS/O-Bi2S3/MoO3) at 1.23 V vs. reversible hydrogen electrode under AM 1.5G illumination. This methodology is expected to advance both fundamental and applied research on metal sulfides.</p>","PeriodicalId":149,"journal":{"name":"ChemSusChem","volume":" ","pages":"e202500039"},"PeriodicalIF":7.5,"publicationDate":"2025-03-23","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143690683","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 : 2025-03-23DOI: 10.1002/cssc.202402737
Ziqing Wang, Charles Buddie Mullins
{"title":"Sandwich-Structured Aqueous Electrolyte with Water-Content Gradient for Enhanced Longevity and Reaction Kinetics in Zinc Metal Batteries.","authors":"Ziqing Wang, Charles Buddie Mullins","doi":"10.1002/cssc.202402737","DOIUrl":"https://doi.org/10.1002/cssc.202402737","url":null,"abstract":"<p><p>Conventional low-concentration aqueous electrolytes (AqE) for Zn metal batteries face undesirable parasitic reactions, severely deteriorating their sustainability. Although low-water-content electrolytes have shown promise in mitigating water splitting, their high viscosity and limited ion transport lead to sluggish reaction kinetics. In this work, we propose a water-content gradient electrolyte (GE) by constructing a sandwich-like structure, where two molecular crowding electrolyte (MCE) layers are applied on both electrode surfaces, while a conventional AqE occupies the space in between. The low-water-content MCE effectively suppresses electrode corrosion and dissolution, while the high-water-content AqE improves ionic conductivity. As a result, Zn/Zn symmetric cells utilizing the GE demonstrate exceptional long-term cycling for over 2000 hours at 2 mA cm-2 to 4 mAh cm-2 and over 300 hours at 7.5 mA cm-2 to 15 mAh cm-2. The Zn-vanadium and Zn-manganese full cells in GE also show remarkable longevity, with cycling lives exceeding several thousand cycles at 2 A g-1, and excellent reaction kinetics across varying current densities. Overall, the GE successfully integrates the benefits of both AqE and MCE, leading to enhanced electrode protection without compromising ion transport, thereby offering a new avenue for developing long-lasting aqueous Zn metal batteries.</p>","PeriodicalId":149,"journal":{"name":"ChemSusChem","volume":" ","pages":"e202402737"},"PeriodicalIF":7.5,"publicationDate":"2025-03-23","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143690687","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 : 2025-03-23DOI: 10.1002/cssc.202402715
Bin Zhu, Yang Zhong, Qiuge Wang, Jian Zhang, Chunlin Chen
{"title":"External Magnetic Field Enhances Biomass Electrooxidation.","authors":"Bin Zhu, Yang Zhong, Qiuge Wang, Jian Zhang, Chunlin Chen","doi":"10.1002/cssc.202402715","DOIUrl":"https://doi.org/10.1002/cssc.202402715","url":null,"abstract":"<p><p>External fields in regulating catalyst structure and tailoring catalytic performance have garnered significant attention from researchers. In this study, an external magnetic field was introduced into biomass conversion and employed as an effective means to accelerate electrocatalytic oxidation. An ox-NiCoP electrocatalyst was fabricated as an electrocatalyst for the oxidation of 2,5-bis(hydroxymethyl)furan (BHMF) to 2,5-furandicarboxylic acid (FDCA). Upon application of a 0.48 T magnetic field, the conversion of BHMF and the yield of FDCA were increased by 27.8% and 27.5%, respectively. The reaction time was shortened by 3.8 h compared to the reaction without a magnetic field. Kinetic analysis revealed that the magnetic field significantly reduced the charge transfer resistance and accelerated the kinetics of the BHMF oxidation reaction (BHMFOR), achieving a maximum reaction rate constant (k) of 2.53 h-1. The enhancement mechanism was attributed to the magnetic field-induced convection at the electrode surface via the Lorentz force, which improved BHMF diffusion between the catalytic interface and the electrolyte. This work highlights the promotive effect of an external magnetic field in the electrocatalytic conversion of organic molecules.</p>","PeriodicalId":149,"journal":{"name":"ChemSusChem","volume":" ","pages":"e202402715"},"PeriodicalIF":7.5,"publicationDate":"2025-03-23","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143690669","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}