ChemCatChem最新文献_第7页

Oxidative Dehydrogenation of Propane on Vanadium Catalysts: Role of V Site Isolation 钒催化剂上丙烷氧化脱氢：V位分离的作用

IF 3.9 3区化学

ChemCatChem Pub Date : 2025-07-10 DOI: 10.1002/cctc.202500728

Małgorzata Smoliło-Utrata, Mariusz Gackowski, Ewa Madej, Agnieszka Drzewiecka-Matuszek, Katarzyna Samson, Małgorzata Ruggiero-Mikołajczyk, Jerzy Podobiński, Jerzy Datka, Marcin Zając, Dorota Rutkowska-Zbik

{"title":"Oxidative Dehydrogenation of Propane on Vanadium Catalysts: Role of V Site Isolation","authors":"Małgorzata Smoliło-Utrata, Mariusz Gackowski, Ewa Madej, Agnieszka Drzewiecka-Matuszek, Katarzyna Samson, Małgorzata Ruggiero-Mikołajczyk, Jerzy Podobiński, Jerzy Datka, Marcin Zając, Dorota Rutkowska-Zbik","doi":"10.1002/cctc.202500728","DOIUrl":"10.1002/cctc.202500728","url":null,"abstract":"The aim of the study was to test the hypothesis that an isolation of the vanadium active sites is pivotal for high activity in oxidative dehydrogenation (ODH) of propane. A series of materials in which isolated vanadium ions were introduced into faujasite was synthetized. The nature of the VOx species was confirmed by different physicochemical techniques showing that they constitute highly dispersed VOx species of tetrahedral/square pyramid coordination. The samples were tested in ODH in air in the temperature range 400–500 °C under atmospheric pressure. Their activity was compared with analogous systems in which nonisolated, polymeric vanadium species were introduced into the same zeolite by wet impregnation. The resulting catalysts with isolated vanadium ions exhibited higher propylene selectivity than those containing polymeric species in temperature range 425–500 °C (23.6%–31.7% vs. 3.6%–10.5%), confirming the hypothesis. Additionally, the reaction mechanism was proposed based on density functional theory calculations, indicating that the first C─H bond breaking in propane is the rate determining step (the energy barrier equals to 27.5 kcal/mol). The formed propyl radical diffuses then to reach the new vanadium site, where the second C─H bond breaking occurs (the energy barrier equals to 10.5 kcal/mol).","PeriodicalId":141,"journal":{"name":"ChemCatChem","volume":"17 17","pages":""},"PeriodicalIF":3.9,"publicationDate":"2025-07-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144999127","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"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

Upcycling CO2 into Long Chain Fatty Acids by Decoupled Microbial Electrochemical Systems 解耦微生物电化学系统将二氧化碳升级为长链脂肪酸

IF 3.9 3区化学

ChemCatChem Pub Date : 2025-07-10 DOI: 10.1002/cctc.202500398

Xiang Xia, Yudong Wu, Xiao Liu, Yajie Liang, Kai Liu

{"title":"Upcycling CO2 into Long Chain Fatty Acids by Decoupled Microbial Electrochemical Systems","authors":"Xiang Xia, Yudong Wu, Xiao Liu, Yajie Liang, Kai Liu","doi":"10.1002/cctc.202500398","DOIUrl":"10.1002/cctc.202500398","url":null,"abstract":"The heavy reliance on fossil fuels results in excessive greenhouse emissions, exacerbating environmental change, and global warming. CO2 electrocatalysis has been widely studied and the products are limited to C1-2. Herein, we reported the integration of electrocatalysis and microbial catalysis for the synthesis of fatty acids from CO2. Here, we compared two decoupled MESs for fatty acid production, electrocatalysis-purification system (System I), and direct-electrocatalysis system (System II). Firstly, an upstream electrolysis was used to reduce CO2 to formate using KHCO3 and medium as electrolyte, respectively, with carbon nanofiber supported bismuth (Bi@PCF) catalyst. The results indicated that KHCO3 as electrolyte had higher formate yield and Faraday efficiency than that of medium. Subsequently, a downstream microbial catalysis composed of Cupriavidus species was employed to synthesize fatty acids from formate in System I and System II, respectively. It was demonstrated that System I with the yield of 1.006 mg L−1 was more favorable for the synthesis of fatty acids than System II with the yield of 0.349 mg L−1. These results suggested that decoupled electrochemical and microbial catalysis were an efficient approach for fixing CO2, indicating the great potential of a renewable energy driving artificial photosynthesis.","PeriodicalId":141,"journal":{"name":"ChemCatChem","volume":"17 17","pages":""},"PeriodicalIF":3.9,"publicationDate":"2025-07-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144999139","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"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

Halide Perovskite Photocatalysts for Solar Energy Harvesting: Concept, Major Advances, and Challenges 用于太阳能收集的卤化物钙钛矿光催化剂：概念、主要进展和挑战

IF 3.9 3区化学

ChemCatChem Pub Date : 2025-07-10 DOI: 10.1002/cctc.202500410

Dr. Jinsun Lee, Dr. Juan Carlos Babón Molina, Laura Rosso, Prof. Dr. Harun Tüysüz

引用次数: 0

Synergistic Dual-Active Sites Engineering in ZIF-Derived CoOx/B-Modified g-C3N4 for Efficient CO2 Cycloaddition Under Mild Conditions zif衍生CoOx/ b修饰g-C3N4在温和条件下高效CO2环加成的协同双活性位点工程

IF 3.9 3区化学

ChemCatChem Pub Date : 2025-07-10 DOI: 10.1002/cctc.202500759

Tianao Zhang, Haolong Huang, Yunchong Wang, Qianqian Zhao, Rui Han, Qingling Liu

{"title":"Synergistic Dual-Active Sites Engineering in ZIF-Derived CoOx/B-Modified g-C3N4 for Efficient CO2 Cycloaddition Under Mild Conditions","authors":"Tianao Zhang, Haolong Huang, Yunchong Wang, Qianqian Zhao, Rui Han, Qingling Liu","doi":"10.1002/cctc.202500759","DOIUrl":"10.1002/cctc.202500759","url":null,"abstract":"The carbon dioxide (CO2) cycloaddition reaction provides an efficient route to achieve resource utilization of CO2. However, the inherent chemical stability of CO2 itself hinders its efficient transformation into cyclic carbonates. Herein, the CoOx/BCN catalyst was successfully prepared by a simple deposition method. The CoOx/BCN exhibited excellent catalytic performance in the CO2 cycloaddition reaction synergistically catalyzed with the nucleophilic reagent KI under solvent-free and mild reaction conditions (80 °C, 0.8 MPa, 6 h). The yield of cyclic carbonate was 98% and the selectivity was 99%, which was significantly superior to CoOx/CN catalyst (with a cyclic carbonate yield of 73.7%). Furthermore, after six cyclic reactions, CoOx/BCN still maintained a yield of over 93%. It was found that after boron (B) was doped into graphitic carbon nitride (g-C3N4), the generated ─NB(OH)2 group on CoOx/BCN effectively activated the epoxide. Importantly, the interaction between B-doped g-C3N4 and CoOx induced the generation of abundant oxygen vacancies, which provided sufficient active sites for CO2 adsorption and activation. In addition, carbonates were identified as the main reaction intermediates by in situ DRIFTS, and the possible reaction pathways of the CoOx/BCN catalyst were proposed. Therefore, this work provides new idea for the design of catalysts for CO2 cycloaddition.","PeriodicalId":141,"journal":{"name":"ChemCatChem","volume":"17 17","pages":""},"PeriodicalIF":3.9,"publicationDate":"2025-07-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144998983","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"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

CO and CH4 Oxidation Reactions on Pt/CeO2 Catalysts: Experimental Study and Mathematical Modeling Pt/CeO2催化剂上CO和CH4氧化反应的实验研究和数学模型

IF 3.9 3区化学

ChemCatChem Pub Date : 2025-07-03 DOI: 10.1002/cctc.202500616

Dr. Elena A. Lashina, Dr. Elena M. Slavinskaya, Prof. Dr. Andrei I. Boronin

{"title":"CO and CH4 Oxidation Reactions on Pt/CeO2 Catalysts: Experimental Study and Mathematical Modeling","authors":"Dr. Elena A. Lashina, Dr. Elena M. Slavinskaya, Prof. Dr. Andrei I. Boronin","doi":"10.1002/cctc.202500616","DOIUrl":"10.1002/cctc.202500616","url":null,"abstract":"CO and CH4 oxidation reactions on Pt/CeO2 catalysts were studied with the aid of experimental kinetic methods of temperature-programmed reactions with CO and CH4 in combination with modeling of the reaction kinetics. The comparison of results obtained for catalysts with low and high Pt content made it possible to differentiate the features of CO and CH4 interaction with different active centers of the catalyst surface, namely, single atoms and PtOx clusters. The presence of PtOx clusters in catalysts leads to the implementation of low-temperature reactions CO + O2 and CH4 + O2. The developed scheme of reactions at the boundary and internal centers of clusters made it possible to explain the implementation of both partial and complete oxidation of methane. When modeling the methane oxidation reaction on PtOx clusters, it was established that the active centers are the boundary centers of clusters modified with OH-groups, which are formed by the dissociation of methane on Pt-O-Ce centers. The experimentally observed increase in the catalytic activity of the methane oxidation reaction in the presence of CO is associated with an additional CO-assisted O2 dissociation mechanism, which is realized only on PtOx cluster centers and not realized on single atom sites.","PeriodicalId":141,"journal":{"name":"ChemCatChem","volume":"17 17","pages":""},"PeriodicalIF":3.9,"publicationDate":"2025-07-03","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144998655","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"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

Substrate Adaptability Enabled by Remote Noncovalent Interactions: How Far Are We? 远距离非共价相互作用使底物适应性成为可能：我们走了多远？

IF 3.9 3区化学

ChemCatChem Pub Date : 2025-07-03 DOI: 10.1002/cctc.202500291

Yuhao Zhu, Dr. Ye Zhu

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Advancing Biocatalysis: Using Siloxanes to Solubilize and Stabilize Enzymes in Organic Solvents 推进生物催化：使用硅氧烷在有机溶剂中溶解和稳定酶

IF 3.9 3区化学

ChemCatChem Pub Date : 2025-07-03 DOI: 10.1002/cctc.202500606

Najibeh Alizadeh, Zain Ahmed, Paul M. Zelisko

{"title":"Advancing Biocatalysis: Using Siloxanes to Solubilize and Stabilize Enzymes in Organic Solvents","authors":"Najibeh Alizadeh, Zain Ahmed, Paul M. Zelisko","doi":"10.1002/cctc.202500606","DOIUrl":"10.1002/cctc.202500606","url":null,"abstract":"Biocatalysis presents an interesting opportunity for addressing the need for sustainability in chemical processes, especially as a means of supplanting catalysts based on nonrenewable metals. However, a significant challenge facing this strategy is the propensity for biological molecules to function optimally in aqueous environments while many chemical transformations occur in organic solvents, an environment that is typically antithetical to the functioning of enzymes. To address this challenge, we have modified proteins with siloxane oligomers in an effort to generate biocatalytic systems that can be used in homogeneous reaction systems rather than as heterogeneous catalysts where the biocatalyst is immobilized on a solid support. The siloxane-modified proteins displayed activity and stability in organic solvents that is comparable to that observed with unmodified proteins in aqueous environments and demonstrated excellent solubility in organic solvents. Modification of the proteins was a straightforward process that demonstrated a high level of efficiency. The covalent modification of human serum albumin (HSA) and trypsin with siloxanes was examined using matrix assisted laser desorption ionisation time of flight mass spectrometry (MALDI-TOF-MS) and the Michaelis-Menton activity of the enzyme was studied using standard assays.","PeriodicalId":141,"journal":{"name":"ChemCatChem","volume":"17 17","pages":""},"PeriodicalIF":3.9,"publicationDate":"2025-07-03","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://chemistry-europe.onlinelibrary.wiley.com/doi/epdf/10.1002/cctc.202500606","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144997926","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Encapsulating Enzymes Within Pickering Emulsion-Derived Microcapsules for Continuous-Flow Epoxidation of Vegetable Oils 在皮克林乳液衍生的微胶囊内包封酶用于植物油的连续流环氧化

IF 3.9 3区化学

ChemCatChem Pub Date : 2025-07-03 DOI: 10.1002/cctc.202500658

Yuan Li, Xiaolan Tang, Wei Li, Ming Zhang, Hengquan Yang

{"title":"Encapsulating Enzymes Within Pickering Emulsion-Derived Microcapsules for Continuous-Flow Epoxidation of Vegetable Oils","authors":"Yuan Li, Xiaolan Tang, Wei Li, Ming Zhang, Hengquan Yang","doi":"10.1002/cctc.202500658","DOIUrl":"10.1002/cctc.202500658","url":null,"abstract":"Enzyme-catalyzed transformation of vegetable oils into epoxidized vegetable oils (EVOs) is of significant importance for sustainable and green industrial production. However, challenges such as enzyme inactivation, low efficiency, and poor stability hinder its large-scale implementation. In this study, a continuous-flow catalytic system based on enzyme-encapsulated Pickering emulsion microcapsules was developed to address these issues. Candida antarctica lipase B (CALB) was encapsulated within microcapsules featuring porous silica shells, forming a stable aqueous microenvironment that maintains enzyme conformation and activity. This design also prevents droplet agglomeration and ensures stability in polar reaction media. By adjusting the structure of microcapsules and reaction conditions, including microcapsules size, shells thickness, enzyme content, and hydrogen peroxide concentration, the optimal conditions for the epoxidation reaction are identified. Utilizing these conditions, the system achieved 80%–92% conversion for the epoxidation of various vegetable oils, maintained long-term operational stability for up to 700 h, and exhibited a fivefold increase in specific activity compared to traditional batch systems. This study provides a novel and industrially viable approach to the epoxidation reaction of vegetable oils.","PeriodicalId":141,"journal":{"name":"ChemCatChem","volume":"17 17","pages":""},"PeriodicalIF":3.9,"publicationDate":"2025-07-03","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144997927","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"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

Insight into the Selectivity Mechanism During Formaldehyde Decomposition: Hydrogen or Methanol Production 深入了解甲醛分解过程中的选择性机制：氢气或甲醇的生产

IF 3.9 3区化学

ChemCatChem Pub Date : 2025-07-03 DOI: 10.1002/cctc.202500800

Zeling Yang, Tianyu Tang, Huanzhi Fang, Yi Cai, Yulu Zhan, Dr. Yangbin Shen

引用次数: 0

Unprecedented Chiral Functionalized Biochar for Asymmetric PTC 空前的手性功能化生物炭用于不对称PTC

IF 3.9 3区化学

ChemCatChem Pub Date : 2025-07-03 DOI: 10.1002/cctc.202500707

Dr. Rosaria Schettini, Mr. Bernardo Franzese, Dr. Aida Kiani, Dr. Paola Giudicianni, Dr. Corinna Maria Grottola, Prof. Maria Rosaria Acocella

引用次数: 0