ChemSusChemPub Date : 2025-03-27DOI: 10.1002/cssc.202500297
Chaozheng Zhou, Haozhe Jia, Pengfei Yan, Chenglong Yang, Song Xu, Guangyu An, Baorui Song, Qun Xu
{"title":"Electrocatalytic Conversion of Glucose into Renewable Formic Acid Using \"Electron-Withdrawing\" MoO<sub>3</sub> Support under Mild Conditions.","authors":"Chaozheng Zhou, Haozhe Jia, Pengfei Yan, Chenglong Yang, Song Xu, Guangyu An, Baorui Song, Qun Xu","doi":"10.1002/cssc.202500297","DOIUrl":"10.1002/cssc.202500297","url":null,"abstract":"<p><p>Electrocatalysis is a sustainable and effective approach to produce value-added chemical commodities from biomass, where highly effective catalyst is required. Since transition metal hydroxide is a feasible catalyst for electrochemical biomass conversion, rational optimization of its electrocatalytic activity is highly desired. Herein, electrocatalytic activity of glucose oxidation is significantly optimized by reducing the electron density at Ni active sites, which is achieved by depositing Ni(OH)<sub>2</sub> at \"electron-withdrawing\" MoO<sub>3</sub> support (Ni(OH)<sub>2</sub>MoO<sub>3-x</sub>). As results, the formation of active sites (NiOOH) and the adsorption of glucose are simultaneously facilitated in Ni(OH)<sub>2</sub>MoO<sub>3-x</sub>, which effectively converts glucose to formic acid (FA) with remarkable yield and Faraday efficiency (≈90.5 and 98%, respectively), far superior to conventional β-Ni(OH)<sub>2</sub> catalyst (≈22.5 and 58.9%, respectively). In addition to a novel strategy for efficient FA production from glucose, this work offers valuable insights into the rational optimization of electrocatalytic oxidation of biomass-based substrates.</p>","PeriodicalId":149,"journal":{"name":"ChemSusChem","volume":" ","pages":"e2500297"},"PeriodicalIF":7.5,"publicationDate":"2025-03-27","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143717781","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":"Progress and Perspectives for Efficient Electrochemical Carbon Dioxide Reduction to Methane.","authors":"Fang Huang, Huanhuan Sun, Siyu He, Xiangyu Chen, Dong Wei, Aihao Xu, Boran Wang, Xucai Yin, Jing Xu, Huibing He","doi":"10.1002/cssc.202402568","DOIUrl":"10.1002/cssc.202402568","url":null,"abstract":"<p><p>The electrochemical carbon dioxide reduction reaction (ECO<sub>2</sub>RR) provides a promising route for synthesizing high-value chemicals and fuels for sustainable economic development. Methane, one of the potential reduction products of ECO<sub>2</sub>RR, plays a crucial role in chemical production and energy storage. Recent advancements in ECO<sub>2</sub>RR have led to significant progress in methane production. However, existing research findings remain substantially distant from practical industrial applications. In this article, the recent research progress in ECO<sub>2</sub>RR for methane production is systematically reviewed. First, the theoretical foundations of ECO<sub>2</sub>RR and the key reaction mechanisms involved in methane production are elaborated upon. Then, catalyst design strategies are summarized aimed at enhancing methane selectivity and activity, including 1) fine tuning of crystal surface, morphology, and size; (2) defects engineering; and (3) tandem catalysis. In addition, the role of modulating microenvironment is reviewed, focusing on the effects of pH, ionic effects, and CO<sub>2</sub> concentration. Finally, some insights into the industrial application of ECO<sub>2</sub>RR to methane are presented in light of existing studies and practical needs.</p>","PeriodicalId":149,"journal":{"name":"ChemSusChem","volume":" ","pages":"e2402568"},"PeriodicalIF":7.5,"publicationDate":"2025-03-26","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143717785","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 : 2025-03-26DOI: 10.1002/cssc.202402766
Mingjie Song, Wutao Wei, Zhao Liu, Xuyan Qin, Li Wei, Zhikai Wang, Xi Jia, Yanjie Wang, Liwei Mi
{"title":"Ni3S4/Co3S4 HeterojunctionTailored by Liquid-Assisted Sintering Strategy for High-Performance Supercapacitors.","authors":"Mingjie Song, Wutao Wei, Zhao Liu, Xuyan Qin, Li Wei, Zhikai Wang, Xi Jia, Yanjie Wang, Liwei Mi","doi":"10.1002/cssc.202402766","DOIUrl":"https://doi.org/10.1002/cssc.202402766","url":null,"abstract":"<p><p>Nanostructures composed of transition metal sulfides (TMS) exhibit excellent electrochemical properties, rendering them well-suited for use in supercapacitor applications. Nevertheless, the conventional synthesis method restricts the synthesis of nanostructures in TMS and the investigation of the synthesis mechanism. In view of the above considerations, we propose a novel synthesis method: liquid-assisted sintering. This approach retains the advantages of solvothermal synthesis of nanomaterials while providing insight into the reaction mechanism and avoiding densification from sintering. The synthesis mechanism of this method is also revealed by the synthesis of Ni3S4/Co3S4. The synthesis process is influenced by Le Chatelier's principle, forming a three-step cyclic reaction. This in turn leads to cathode materials with heterojunction structures The cathode material possesses excellent electrochemical properties. The best devices can achieve an energy density of 57.7 W h kg-1 at a power density of 102.4 W kg-1 and maintain an energy density of 21.7 W h kg-1 at a power density of 3547.8 W kg-1. This work provides a new way to make nanomaterials and develop electrode materials for supercapacitors.</p>","PeriodicalId":149,"journal":{"name":"ChemSusChem","volume":" ","pages":"e202402766"},"PeriodicalIF":7.5,"publicationDate":"2025-03-26","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143717783","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 : 2025-03-26DOI: 10.1002/cssc.202402779
Alae Eddine Lakraychi, Ifeanyi Emmanuel Udom, Ren Wen, Yan Yao
{"title":"Air stable High-Voltage Li-ion Organic Cathode Enabled by Localized High-Concentration Electrolyte.","authors":"Alae Eddine Lakraychi, Ifeanyi Emmanuel Udom, Ren Wen, Yan Yao","doi":"10.1002/cssc.202402779","DOIUrl":"https://doi.org/10.1002/cssc.202402779","url":null,"abstract":"<p><p>While lithium-ion batteries (LIBs) have revolutionized the field of energy storage, their reliance on critical minerals such as cobalt and nickel raises significant concerns over resource availability and supply chain uncertainty. In this study, we revisit dithiin fused dilithium naphthazarin (5,8-dihydroxy-1,4-naphthoquinone) (DNP-Li) as a high-voltage Li-ion organic cathode and evaluate its performance in conjunction with localized high-concentration electrolyte (LHCE). DNP-Li exhibits remarkable air and thermal stability, a high operating potential of 3.55 V vs. Li+/Li, and a specific capacity of 232 mAh g⁻¹, positioning it as one of the most promising candidates among Li-ion organic cathodes. Furthermore, the electrochemical behavior of DNP-Li is strongly influenced by the electrolyte composition, giving distinct two-plateaus or four-plateaus voltage profiles accompanied with reversible or irreversible phase transition in carbonate-based or LHCE electrolyte formulations, respectively. The reduced solubility of DNP-Li-based redox intermediates in LHCE enhances cycling stability, achieving a capacity retention of 85% after 50 cycles at 0.1C and 75% after 160 cycles at 0.5C, demonstrating a significant improvement compared to the carbonate-based electrolyte. This work highlights the critical role of solute-electrolyte interactions in modulating the electrochemical performance of multi-electron small molecule organic cathodes, offering new pathways for advancing sustainable and high-efficiency energy storage technologies.</p>","PeriodicalId":149,"journal":{"name":"ChemSusChem","volume":" ","pages":"e202402779"},"PeriodicalIF":7.5,"publicationDate":"2025-03-26","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143717779","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 : 2025-03-26DOI: 10.1002/cssc.202500181
Lujie Jin, Yujin Ji, Youyong Li
{"title":"High-Throughput Screening of 1D Chalcogenide Cathode Materials Beyond VS<sub>4</sub> for Rechargeable Magnesium-Ion Batteries.","authors":"Lujie Jin, Yujin Ji, Youyong Li","doi":"10.1002/cssc.202500181","DOIUrl":"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 Mg<sup>2+</sup> 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 VS<sub>4</sub> material, three potential 1D chalcogenide materials (SiS<sub>2</sub>, GeS<sub>2</sub>, and SiSe<sub>2</sub>) 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, this 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":"e2500181"},"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":"10.1002/cssc.202500462","url":null,"abstract":"<p><p>The photocatalytic activity of graphitic carbon nitride (g-C<sub>3</sub>N<sub>4</sub>) strongly depends on its electronic structure. To design the photocatalysts with efficient charge separation and transfer property, here a benzene ring-doped g-C<sub>3</sub>N<sub>4</sub> via one-pot thermal polycondensation of dicyandiamide and 2,4-diaminobenzenesulfonic acid is reported. The carbon-rich benzene ring is embedded into g-C<sub>3</sub>N<sub>4</sub>, which enables the asymmetric modification of the heptazine units in g-C<sub>3</sub>N<sub>4</sub> 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-C<sub>3</sub>N<sub>4</sub>, respectively. The reason for enhanced photocatalytic performance is 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-C<sub>3</sub>N<sub>4</sub> using low-content organic carbon molecule for efficient energy conversion-related applications.</p>","PeriodicalId":149,"journal":{"name":"ChemSusChem","volume":" ","pages":"e2500462"},"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
Sarah Behloul, Zhen Yan, Karine De Oliveira Vigier, Frederic Guégan, François Jérôme
{"title":"N,N-Dimethylhydrazine as a Reversible Derivatization Agent to Promote the Hydroxymethylation of Furfural with Formaldehyde.","authors":"Sarah Behloul, Zhen Yan, Karine De Oliveira Vigier, Frederic Guégan, François Jérôme","doi":"10.1002/cssc.202500318","DOIUrl":"10.1002/cssc.202500318","url":null,"abstract":"<p><p>In this report, the synthesis of 5-hydroxymethylfurfural from concentrated feeds of two low-cost and industrially abundant chemicals: Furfural and formaldehyde is explored. By adjusting the acidity of the solvent, an alternative mechanism is discovered 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 a major product. One of the keys of this study relies on the reversible derivation of the -CHO group of furfural with N,N-Dimethylhydrazine 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, this reaction is optimized and it is discovered that guaiacol can be used as a bio-based and safe solvent. Under optimized conditions, the hydroxymethylation of the furan ring of furfural occurs with more than 95% selectivity, at only 50 °C and with a stoichiometric amount of HCHO. A concentrated feed of furfural as high as 40 wt% in guaiacol can be employed without impacting the reaction selectivity, leading to an improvement of the reactor productivity to about 25 kg m<sup>-3</sup> h<sup>-1</sup>. The recovery of the reaction products and the recycling of the N,N-dimehylhydrazone are also discussed.</p>","PeriodicalId":149,"journal":{"name":"ChemSusChem","volume":" ","pages":"e2500318"},"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":"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 H<sub>2</sub>, 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, a well-known three-component system is employed to decouple light absorption and hydrogen evolution. The system utilizes [Ru(bpy)<sub>3</sub>]<sup>2+</sup>, triethanolamine, and methyl viologen to store solar energy as reduced viologen (MV<sup>•+</sup>). By controlling pH, this stored energy can be efficiently released to produce hydrogen on demand. The 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":"e2500029"},"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}