ChemSusChem最新文献_第2页

Heteroatom-Based Ligand Engineering of Metal Organic Frameworks for Efficient and Robust Electrochemical Water Oxidation.

IF 7.5 2区化学

ChemSusChem Pub Date : 2024-12-13 DOI: 10.1002/cssc.202402112

Hong-Yi Tan, Bing-Hao Wang, Meng-Yi Xu, Zhi-Yong Peng, Wen-Juan Wu, Sheng Shen, Shuangfeng Yin

{"title":"Heteroatom-Based Ligand Engineering of Metal Organic Frameworks for Efficient and Robust Electrochemical Water Oxidation.","authors":"Hong-Yi Tan, Bing-Hao Wang, Meng-Yi Xu, Zhi-Yong Peng, Wen-Juan Wu, Sheng Shen, Shuangfeng Yin","doi":"10.1002/cssc.202402112","DOIUrl":"https://doi.org/10.1002/cssc.202402112","url":null,"abstract":"Metal-organic frameworks (MOFs) are promising catalysts for the electrochemical oxygen evolution reaction (OER) due to their high surface area, tunable pore structures, and abundant active sites. Ligand engineering is an important strategy to optimize their performance. Here, we report the synthesis of NiFe-MOFs based on three different ligands: 1,4-terephthalic acid (BDC), 2,4-thiophene dicarboxylic acid (TDC), and 2,5-furandicarboxylic acid (FDC), to investigate the effects of heteroatom-based aromatic rings on OER performance. It is revealed that by incorporating electronegative sulfur and oxygen atoms into the ligands, the electron density at the metal sites is reduced, leading to enhanced metal-oxygen covalency and improved charge transfer kinetics. The NiFe-FDC/NF catalyst demonstrates an overpotential of 189 mV at 10 mA·cm-2 and stable performance over 1300 hours at 1 A·cm-2. In situ infrared spectroscopy reveal minimal structural reconstruction in NiFe-FDC/NF, contributing to its superior stability. The NiFe-FDC/NF were then subjected to 3600 hours of OER operation and it's metal elution was monitored. These findings offer a novel approach to ligand design for high-performance MOF-based OER catalysts, highlighting the potential of furan-based ligands for MOF ligand engineering.","PeriodicalId":149,"journal":{"name":"ChemSusChem","volume":" ","pages":"e202402112"},"PeriodicalIF":7.5,"publicationDate":"2024-12-13","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142816856","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

Direct Ink Writing Additive Manufacturing of Silica Aerogels.

IF 7.5 2区化学

ChemSusChem Pub Date : 2024-12-12 DOI: 10.1002/cssc.202402119

Bo Chen, Qiyang Jiang, Jing Tu, Xinhong Xiong, Jiaxi Cui

{"title":"Direct Ink Writing Additive Manufacturing of Silica Aerogels.","authors":"Bo Chen, Qiyang Jiang, Jing Tu, Xinhong Xiong, Jiaxi Cui","doi":"10.1002/cssc.202402119","DOIUrl":"https://doi.org/10.1002/cssc.202402119","url":null,"abstract":"Silica aerogels (SAs) have garnered significant attention due to their high porosity, low density, hydrophobic properties, low thermal conductivity, and optical transparency. The traditional method for producing SAs, known as \"sol-gel\" technology, involves precursor preparation, aging, and drying processes. However, aerogels produced through this method often exhibit drawbacks such as poor processability and low precision, which prevent them from fully leveraging their potential properties, including catalysis, adsorption, insulation, and sensing. In contrast, direct ink writing (DIW) technology offers a promising avenue for creating functional structures from SAs. This technique enables the production of inks with shear-thinning behavior, facilitating the high-precision printing of complex SA structures. This review summarizes the advancements in DIW additive manufacturing (AM) of SAs and the challenges currently faced in this field. Briefly, we first introduce the ink preparation, 3D printing process, drying and heat treatment suitable for DIW 3D printing silica aerogels, followed by the discussion of the current state of research and key challenges of DIW 3D printing SAs.","PeriodicalId":149,"journal":{"name":"ChemSusChem","volume":" ","pages":"e202402119"},"PeriodicalIF":7.5,"publicationDate":"2024-12-12","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142811672","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

Cover Feature: Decarboxylation of Hydroxybenzoic Acids to Phenol Via Deep Eutectic Solvents (ChemSusChem 23/2024)

IF 7.5 2区化学

ChemSusChem Pub Date : 2024-12-11 DOI: 10.1002/cssc.202482302

Da Hae Oh, Md. Al Mamunur Rashid, Chun-Jae Yoo, Jeong-Myeong Ha, Bonwook Koo, Jungkyu Choi, Keunhong Jeong, Kwang Ho Kim

引用次数: 0

Cover Feature: Graphene-Based Material Supports for Ni− and Ru− Catalysts in CO2 Hydrogenation: Ruling out Performances and Impurity Role (ChemSusChem 23/2024)

IF 7.5 2区化学

ChemSusChem Pub Date : 2024-12-11 DOI: 10.1002/cssc.202482304

Sina Ebrahim Atakoohi, Paola Riani, Elena Spennati, Letizia Savio, Luca Vattuone, Jacopo De Maron, Gabriella Garbarino

引用次数: 0

Boosting Photocatalytic Selective Oxidation of 5-Hydroxymethylfurfural to 2,5-Diformylfuran via Atomically Bridged Indium in In-SnS2.

IF 7.5 2区化学

ChemSusChem Pub Date : 2024-12-11 DOI: 10.1002/cssc.202402197

Akkammagari Putta Rangapppa, Wenhua Xue, Anirban Chowdhury, Yixuan Liu, Jong-Min Lee, Jun Zhao

{"title":"Boosting Photocatalytic Selective Oxidation of 5-Hydroxymethylfurfural to 2,5-Diformylfuran via Atomically Bridged Indium in In-SnS2.","authors":"Akkammagari Putta Rangapppa, Wenhua Xue, Anirban Chowdhury, Yixuan Liu, Jong-Min Lee, Jun Zhao","doi":"10.1002/cssc.202402197","DOIUrl":"https://doi.org/10.1002/cssc.202402197","url":null,"abstract":"The photocatalytic conversion of biomass-based platform molecules, such as 5-hydroxymethylfurfural (HMF), holds significant importance for the utilization of biomass resources. This study focuses on the unique ability of atomically bridged indium (In) atoms that encourages inactive SnS2 surface and steer the selective HMF oxidation process under solar light. Experimental results suggest that In confined SnS2 structure provides not only favorable sites and electronic structures for the synergistic activation of HMF/O2 but also benefit in charge carrier dynamics, thus influencing the overall activity and selectivity of the SnS2 catalyst. In addition, in-situ spectroscopy and density functional theory (DFT) analysis uncovered the multifunctional role of In sites in promoting the key steps of the catalytic process, from ROS generation to regulated adsorption/activation of *HMF which serves as the rate limiting step of the overall HMF oxidation process. Consequently, the optimized In-SnS2-0.75 photocatalyst demonstrated excellent photo oxidation performance, reaching a high HMF conversion efficiency, yield, and selectivity of 91.2, 73 and 80% respectively, in just two hours of the reaction. This study highlights the strategic approach of rationally designed catalytic systems in order to tune the ROS and the product distribution of the HMF oxidation process.","PeriodicalId":149,"journal":{"name":"ChemSusChem","volume":" ","pages":"e202402197"},"PeriodicalIF":7.5,"publicationDate":"2024-12-11","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142805655","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

Front Cover: Towards Sustainable Production of Polybutylene Adipate Terephthalate: Non-Biological Catalytic Syntheses of Biomass-Derived Constituents (ChemSusChem 23/2024)

IF 7.5 2区化学

ChemSusChem Pub Date : 2024-12-11 DOI: 10.1002/cssc.202482301

Jechan Lee, Chanyeong Park, Yiu Fai Tsang, Kun-Yi Andrew Lin

引用次数: 0

Cover Feature: Influence of Complex Multiphasic Flow on the Thiuram Electrosynthesis in a Microchannel Reactor (ChemSusChem 23/2024)

IF 7.5 2区化学

ChemSusChem Pub Date : 2024-12-11 DOI: 10.1002/cssc.202482303

Dr. Siyuan Zheng, Prof. Kai Wang

引用次数: 0

Enhancing Stability of Microwave-Synthesized Cs₂Sn_xTi_1-xBr₆ Perovskite by Cation Mixing.

IF 7.5 2区化学

ChemSusChem Pub Date : 2024-12-10 DOI: 10.1002/cssc.202402073

Emmanuel Reyes-Francis, Beatriz Julián-López, Carlos Echeverría-Arrondo, Jhonatan Rodríguez-Pereira, Diego Esparza, Tzarara López-Luke, Jaime Espino-Valencia, Daniel Prochowicz, Iván Mora-Seró, Silver-Hamill Turren-Cruz

{"title":"Enhancing Stability of Microwave-Synthesized Cs2SnxTi1-xBr6 Perovskite by Cation Mixing.","authors":"Emmanuel Reyes-Francis, Beatriz Julián-López, Carlos Echeverría-Arrondo, Jhonatan Rodríguez-Pereira, Diego Esparza, Tzarara López-Luke, Jaime Espino-Valencia, Daniel Prochowicz, Iván Mora-Seró, Silver-Hamill Turren-Cruz","doi":"10.1002/cssc.202402073","DOIUrl":"10.1002/cssc.202402073","url":null,"abstract":"The double-perovskite material Cs2TiBr6 shows excellent photovoltaic potential, making it a promising alternative to lead-based materials. However, its high susceptibility to degradation in air has raised concerns about its practical application. This study introduces an interesting synthesis approach that significantly enhances the stability of Cs2TiBr6 powder. We implemented a gradual cation exchange process by substituting Ti4+ with Sn4+ in the efficient microwave-assisted synthesis method, developing a double perovskite Cs2SnxTi1-xBr6 type. A systematic study of increasing concentration of Sn4+ in Cs2TiBr6 perovskite has been performed to analyze the effect of Sn-doping degree on the chemical and thermal stability of the material and the optical features in both nitrogen and ambient atmospheres, significantly increasing the stability of the material in the air for over a week. Furthermore, introducing Sn4+ results in a more uniform polygonal crystal morphology of the powders and a slight band gap broadening. We show that microwave-assisted synthesis is highly efficient and cost-effective in producing more sustainable lead-free perovskite materials with enhanced stability and desirable electrical characteristics. This work suggests a promising method for synthesizing perovskite materials, opening new routes for scientific research and applications.","PeriodicalId":149,"journal":{"name":"ChemSusChem","volume":" ","pages":"e202402073"},"PeriodicalIF":7.5,"publicationDate":"2024-12-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142798753","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

Multifunctional Heterogeneous Cobalt Catalyst for the One-Pot Synthesis of Benzimidazoles by Reductive Coupling of Dinitroarenes with Aldehydes in Water.

IF 7.5 2区化学

ChemSusChem Pub Date : 2024-12-09 DOI: 10.1002/cssc.202402141

José Luis Del Río-Rodríguez, Silvia Gutiérrez-Tarriño, Lidia E Chinchilla, Juan Pedro Holgado, Ignacio J Villar-García, Virginia Pérez-Dieste, Jose J Calvino, Pascual Oña-Burgos

{"title":"Multifunctional Heterogeneous Cobalt Catalyst for the One-Pot Synthesis of Benzimidazoles by Reductive Coupling of Dinitroarenes with Aldehydes in Water.","authors":"José Luis Del Río-Rodríguez, Silvia Gutiérrez-Tarriño, Lidia E Chinchilla, Juan Pedro Holgado, Ignacio J Villar-García, Virginia Pérez-Dieste, Jose J Calvino, Pascual Oña-Burgos","doi":"10.1002/cssc.202402141","DOIUrl":"10.1002/cssc.202402141","url":null,"abstract":"The endeavor of sustainable chemistry has led to significant advancements in green methodologies aimed at minimizing environmental impact while maximizing efficiency. Herein, a straightforward synthesis of benzimidazoles by reductive coupling of o-dinitroarenes with aldehydes is reported for the first time in aqueous media while using a non-noble metal catalyst. This work demonstrates that the combination of nitrogen and phosphorous ligands in the synthesis of supported heteroatom-incorporated Co nanoparticles is crucial for obtaining the desired benzimidazoles. The process achieves >99 % conversion, >99 % chemoselectivity and stability for the reduction of dinitroarenes using water as the solvent and hydrogen as the reductant under mild reaction conditions. The robustness of the catalyst has been investigated using several advanced techniques such as HRTEM, HAADF-STEM, XEDS, EELS, and NAP-XPS. In fact, we have shown that the introduction of N and P dopants prevents metal leaching and the sintering of the cobalt nanoparticles. Finally, to explore the general catalytic performance, a wide range of substituted dinitroarenes and benzaldehydes were evaluated, yielding benzimidazoles with competitive and scalable results, including MBIB (94 % yield), which is a compound of pharmaceutical interest.","PeriodicalId":149,"journal":{"name":"ChemSusChem","volume":" ","pages":"e202402141"},"PeriodicalIF":7.5,"publicationDate":"2024-12-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142798758","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

Dynamic release electrolyte design for stable proton batteries.

IF 7.5 2区化学

ChemSusChem Pub Date : 2024-12-09 DOI: 10.1002/cssc.202402105

Jian Zhang, Qing Lang, Jiayuan Yu, Yixiao Yang, Jiulong Che, Liang Chen, Gang Wang

{"title":"Dynamic release electrolyte design for stable proton batteries.","authors":"Jian Zhang, Qing Lang, Jiayuan Yu, Yixiao Yang, Jiulong Che, Liang Chen, Gang Wang","doi":"10.1002/cssc.202402105","DOIUrl":"https://doi.org/10.1002/cssc.202402105","url":null,"abstract":"Aqueous proton batteries (APBs) have recently demonstrated unprecedented advantages in the fields of ultralow temperature and high-power energy applications due to kinetically favorable proton chemistry. Proton acids (e.g. H2SO4, H3PO4) as the common proton-conducting electrolyte, however, seriously corrode electrode materials and current collectors, resulting in limited cycle life of APBs. Here we reported protonated amine as a feasible proton transport mediator and releasing source for APBs based on its dynamic chemical dissociation equilibrium. Free protons in the electrolyte are limited to a quite low level. Consequently, the optimized electrolyte with a nearly neutral pH value significantly suppresses corrosion and broadens material selection option for APBs. The CuFe-TBA electrode exhibited a long cycle performance over 40000 cycles with only ~0.0004% attenuation rate per cycle in the optimized electrolyte. The WO3 and VO2(B) electrode also displayed high cycling stability. Benefiting from enhanced electrode stability in the optimized electrolyte, the resultant CuFe-TBA/WO3 and CuFe-TBA/VO2(B) full batteries display impressive long-term cycling performance with high-capacity retention. Our work presents a proton dynamic-release electrolyte for durable APBs which is highly promising for scalable energy systems.","PeriodicalId":149,"journal":{"name":"ChemSusChem","volume":" ","pages":"e202402105"},"PeriodicalIF":7.5,"publicationDate":"2024-12-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142798751","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