ChemCatChem最新文献_第10页

Photothermal Dry Reforming of Methane on Yolk-Shell Co–Ni Alloy@SiO2 Catalyst

IF 3.8 3区化学

ChemCatChem Pub Date : 2024-10-28 DOI: 10.1002/cctc.202401396

Hamada A. El-Naggar, Daichi Takami, Hisashi Asanuma, Takafumi Hirata, Hisao Yoshida, Akira Yamamoto

{"title":"Photothermal Dry Reforming of Methane on Yolk-Shell Co–Ni Alloy@SiO2 Catalyst","authors":"Hamada A. El-Naggar, Daichi Takami, Hisashi Asanuma, Takafumi Hirata, Hisao Yoshida, Akira Yamamoto","doi":"10.1002/cctc.202401396","DOIUrl":"https://doi.org/10.1002/cctc.202401396","url":null,"abstract":"Photothermal dry reforming of methane (PT-DRM) is an appealing pathway to convert carbon dioxide and methane into synthesis gas, a mixture of carbon monoxide and hydrogen, via photothermal heating induced by concentrated sunlight. However, coke formation and sintering of active metal nanoparticles are key issues for catalyst stability. In the present study, we demonstrated Co–Ni alloy nanoparticles encapsulated with a porous SiO2 shell exhibited improved catalytic activity and stability for PT-DRM using visible/near-IR light irradiation without any other external heating. The addition of a tiny amount of Co (1–5 mol% relative to total metal) and SiO2 encapsulation enhanced the stability by simultaneously suppressing coke formation and sintering of the metal nanoparticles. Furthermore, we revealed that the position of the light irradiation spot has a crucial role in the conversions of methane and carbon dioxide and product selectivity, presumably due to the large temperature gradient under the light irradiation. These findings would contribute to designing effective PT-DRM catalysts with improved activity and enhanced resistance for both coke formation and sintering and emphasize the significant contribution of the temperature gradients to the performance of PT-DRM.","PeriodicalId":141,"journal":{"name":"ChemCatChem","volume":"17 3","pages":""},"PeriodicalIF":3.8,"publicationDate":"2024-10-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143363069","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

Synthesis of Ru-PNPC Pincer Complexes and Applications in Catalytic Hydrogenation and Dehydrogenation Reactions

IF 3.8 3区化学

ChemCatChem Pub Date : 2024-10-28 DOI: 10.1002/cctc.202401481

Hendrik A. Kempf, Germán López Robledo, Dr. Anke Spannenberg, Dr. Kathrin Junge, Dr. Haijun Jiao, Dr. Henrik Junge, Prof. Dr. Matthias Beller

引用次数: 0

Catalytic Ammonia Synthesis by Supported Molybdenum Nitride: Insight into the Support Effect

IF 3.8 3区化学

ChemCatChem Pub Date : 2024-10-28 DOI: 10.1002/cctc.202400494

Amanda Sfeir, Camila A. Teles, Hervé Vezin, Maya Marinova, Jean-Philippe Dacquin, Said Laassiri, Sébastien Royer

{"title":"Catalytic Ammonia Synthesis by Supported Molybdenum Nitride: Insight into the Support Effect","authors":"Amanda Sfeir, Camila A. Teles, Hervé Vezin, Maya Marinova, Jean-Philippe Dacquin, Said Laassiri, Sébastien Royer","doi":"10.1002/cctc.202400494","DOIUrl":"https://doi.org/10.1002/cctc.202400494","url":null,"abstract":"The influence of the support on the performance of Mo nitrides has been investigated in ammonia synthesis and decomposition. A series of Mo–N catalysts supported on different materials, namely SiO2 (commercial, SBA-15), Al2O3, and CeO2, were prepared. The results indicated that, despite the high dispersion of Mo species in all catalysts, large disparities in the activity for ammonia synthesis exist. Initial rates of ∼1208, ∼481, and ∼372 µmol gactive phase−1 h−1 are obtained over 10-Mo–N/SBA-15, 10-Mo–N/SiO2, and 10-Mo–N/Al2O3 respectively. However, no catalytic activity was registered when Mo species were supported on CeO2. Furthermore, 10-Mo–N/Al2O3 deactivated after few hours of reaction. The surface composition was studied by means of XPS to probe the origin of the catalytic activity differences, and the results indicated that a range of various oxidation states of Mo was detected depending on the support. The difference in catalytic behavior could not be solely explained by the differences in Mo–N species concentrations. In situ EPR analysis exhibited that the mechanism of MoO3 nitridation could differ depending on the support, leading to the formation of different Mo–N species. The effect of support was, however, not as severe in ammonia decomposition as it was the case of ammonia synthesis.","PeriodicalId":141,"journal":{"name":"ChemCatChem","volume":"17 3","pages":""},"PeriodicalIF":3.8,"publicationDate":"2024-10-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://onlinelibrary.wiley.com/doi/epdf/10.1002/cctc.202400494","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143363067","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

Construction of Magnetic FeP/CdS Composites as Photo-Fenton-Like Catalysts to Realize High-Efficiency Degradation of Tetracycline Hydrochloride

IF 3.8 3区化学

ChemCatChem Pub Date : 2024-10-28 DOI: 10.1002/cctc.202401364

Haixia Li, Dan Li, Chuanqiang Yin, Feigao Xu

{"title":"Construction of Magnetic FeP/CdS Composites as Photo-Fenton-Like Catalysts to Realize High-Efficiency Degradation of Tetracycline Hydrochloride","authors":"Haixia Li, Dan Li, Chuanqiang Yin, Feigao Xu","doi":"10.1002/cctc.202401364","DOIUrl":"https://doi.org/10.1002/cctc.202401364","url":null,"abstract":"Photocatalysis is an efficient technology for the degradation of pollutants. However, it still needs to be improved. In this study, magnetic Z-scheme FeP/CdS composites heterojunction photocatalysts were prepared by a facile hydrothermal method, and the structure, morphology, optical, and photocatalytic properties of the prepared composites were investigated in detail. The efficiency of tetracycline hydrochloride (TCH) removal by FeP/CdS composites was investigated under different reaction conditions (including different FeP and CdS ratios, catalyst dosage, hydrogen peroxide consumption, temperature, and initial pH). FeP/CdS composites exhibited better catalytic performance compared with pure components. The F1Cd1 composite (mass ratio of FeP to CdS is 1:1) achieved 92.7% removal efficiency of TCH; moreover, the F1Cd1 composite still exhibits a high stability after five consecutive cycles. The capture experiments on the active material showed that the removal of TCH by the F1Cd1 composite was mainly dominated by •OH; however, •O2−, e−, and h+ played a minor role, and the degradation mechanism was revealed by combining various characterization techniques. The introduction of cadmium sulfide formed an effective photogenerated carrier transport channel at the interface with the iron phosphide surface, which could accelerate the transfer and separation of photo-excited e−/h+ pairs, thus improving the degradation performance of TCH.","PeriodicalId":141,"journal":{"name":"ChemCatChem","volume":"17 3","pages":""},"PeriodicalIF":3.8,"publicationDate":"2024-10-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143363068","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

Fusion of Hydrophobic Anchor Peptides Promotes the Hydrolytic Activity of PETase but not the Extent of PET Depolymerization

IF 3.8 3区化学

ChemCatChem Pub Date : 2024-10-28 DOI: 10.1002/cctc.202401252

Yongjie Wang, Ekram Akram, Yujing Ding, Chengzhi He, Yifei Zhang

{"title":"Fusion of Hydrophobic Anchor Peptides Promotes the Hydrolytic Activity of PETase but not the Extent of PET Depolymerization","authors":"Yongjie Wang, Ekram Akram, Yujing Ding, Chengzhi He, Yifei Zhang","doi":"10.1002/cctc.202401252","DOIUrl":"https://doi.org/10.1002/cctc.202401252","url":null,"abstract":"Enzymatic recycling of polyethylene terephthalate (PET) has attracted significant attention in recent years. While the fusion of anchor peptides to PET hydrolases is believed to enhance PET hydrolytic activity, a quantitative analysis is yet lacking. Here, we construct four fusion enzymes by fusing anchor peptides (including hydrophobic LCI, LCIM1 and TA2, and hydrophilic EK4) to the C terminus of HotPETase, one of the most active PET hydrolases for high-crystallinity PET (HC-PET). Single-molecule force spectroscopy (SMFS) demonstrates that hydrophobic anchor peptides promote adhesive interactions between the fusion enzymes and the PET surface. This is also validated by the adsorption kinetics and isotherms, and the saturated adsorption capacity remains unaltered compared to HotPETase. At low substrate loadings, the apparent hydrolytic activity of these fusion enzymes is positively related to the hydrophobicity of the anchor peptides. Among them, HotPETase-LCI stands out as the most effective enzyme for HC-PET degradation, demonstrating a 1.5-fold increase in hydrolytic activity. At high substrate loadings, the advantages of fusion with anchor peptides diminish. We conclude that fusion enzymes only facilitate the hydrolytic rates of reactions for HC-PET but have little effect on the final conversion extent.","PeriodicalId":141,"journal":{"name":"ChemCatChem","volume":"17 3","pages":""},"PeriodicalIF":3.8,"publicationDate":"2024-10-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143363070","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

Recent Advances in the Development of Targeted Activation Strategies for Organoboron Prodrugs

IF 3.8 3区化学

ChemCatChem Pub Date : 2024-10-27 DOI: 10.1002/cctc.202401609

Moyi Liu, Taotao Zou

{"title":"Recent Advances in the Development of Targeted Activation Strategies for Organoboron Prodrugs","authors":"Moyi Liu, Taotao Zou","doi":"10.1002/cctc.202401609","DOIUrl":"https://doi.org/10.1002/cctc.202401609","url":null,"abstract":"Elevated levels of reactive oxygen species (ROS) are a hallmark of varieties of diseases such as cancer, inflammation, and neurodegenerative disorders. Inspired by the discrepancy of ROS concentrations between pathological tissues and the normal counterparts, an increasing number of ROS-responsive theragnostic prodrugs are developed in past years, with particularly high proportions of organoboron-based prodrugs that can respond to H2O2. Unfortunately, increasing studies have demonstrated that the intrinsic ROS (H2O2) levels in most pathological tissue are only slightly higher than normal tissues and are not adequate to activate organoboron prodrugs; in contrast, several organoboron compounds have been clinically approved in which boronic acid acts as electrophilic warhead. To this end, developing more robust and universal approaches for boronic acid-prodrug activation becomes highly attractive. In this context, we discuss the recently reported activation strategies for boron-caged prodrugs with a particular focus on their design principles and activation mechanisms. The perspectives on the future directions for this important research area are discussed as well.","PeriodicalId":141,"journal":{"name":"ChemCatChem","volume":"17 3","pages":""},"PeriodicalIF":3.8,"publicationDate":"2024-10-27","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143362977","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

Pyrene-4,5,9,10-Tetraone-Based Porous Aromatic Frameworks for Photocatalytic Production of Hydrogen Peroxide

IF 3.8 3区化学

ChemCatChem Pub Date : 2024-10-27 DOI: 10.1002/cctc.202401141

Miao Cheng, He Wang, Linzhu Cao, Jingjing Shao, Yuxuan He, Xin Tao, Guangshan Zhu

引用次数: 0

Correlating Heterogeneities in Support Fragmentation to Polymer Morphology in Metallocene-Based Propylene Polymerization Catalysis

IF 3.8 3区化学

ChemCatChem Pub Date : 2024-10-27 DOI: 10.1002/cctc.202401183

Joren M. Dorresteijn, Dr. Roozbeh Valadian, Dr. Yuntao Ji, Dr. Silvia Zanoni, Dr. Koen W. Bossers, Dr. Nikolaos Nikolopoulos, Dr. Virginie Cirriez, Dr. Alexandre Welle, Dr. Daniel Curulla-Ferré, Prof. Eelco T.C. Vogt, Prof. Florian Meirer, Prof. Bert M. Weckhuysen

{"title":"Correlating Heterogeneities in Support Fragmentation to Polymer Morphology in Metallocene-Based Propylene Polymerization Catalysis","authors":"Joren M. Dorresteijn, Dr. Roozbeh Valadian, Dr. Yuntao Ji, Dr. Silvia Zanoni, Dr. Koen W. Bossers, Dr. Nikolaos Nikolopoulos, Dr. Virginie Cirriez, Dr. Alexandre Welle, Dr. Daniel Curulla-Ferré, Prof. Eelco T.C. Vogt, Prof. Florian Meirer, Prof. Bert M. Weckhuysen","doi":"10.1002/cctc.202401183","DOIUrl":"https://doi.org/10.1002/cctc.202401183","url":null,"abstract":"In the field of olefin polymerization catalysis, metallocenes are heterogenized with methylaluminoxane onto silica supports to yield active catalysts. During olefin polymerization, these silica supports act as a framework to control the fragmentation stage, thereby influencing the final polymer product and preventing reactor fouling and fines formation. This study investigates the influence of different silica supports induced on the final polymer product. To study a broad range of silica supports from an industrial silica database, we utilize a hierarchical clustering method to cluster the supports based on their physical properties. From the clustering method, five supports representing the clusters and an industrial benchmark were analyzed at different polymerization stages using focused ion beam–scanning electron microscopy (FIB–SEM) and microcomputed tomography (microCT). This combined FIB-SEM/microCT methodology revealed differences in both fragmentation behavior and polymer morphologies based on structural features, including macropores, mesopores, spray-dried shells, spray-dried spheres, and denser shells. The heterogeneity and ideal fragmentation behavior was further assessed by calculating the replication factor of each support, indicating that silica materials containing macropores and spray-dried shells have an almost ideal replication phenomenon. This multiscale analysis revealed new understanding of catalyst fragmentation for different supports. This understanding could in the future be further developed by the addition of more supports or additional analysis of the supports to the industrial database.","PeriodicalId":141,"journal":{"name":"ChemCatChem","volume":"17 3","pages":""},"PeriodicalIF":3.8,"publicationDate":"2024-10-27","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://onlinelibrary.wiley.com/doi/epdf/10.1002/cctc.202401183","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143362979","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

Balanced Rh+-Rh0 Sites over Rh Clusters Enhance Heterogeneous Hydroformylation of Aldehyde

IF 3.8 3区化学

ChemCatChem Pub Date : 2024-10-27 DOI: 10.1002/cctc.202401392

Qi Yang, Ying Zheng, Yi Feng, Jie Ding, Maoshuai Li, Shouying Huang, Mei-Yan Wang, Xinbin Ma

{"title":"Balanced Rh+-Rh0 Sites over Rh Clusters Enhance Heterogeneous Hydroformylation of Aldehyde","authors":"Qi Yang, Ying Zheng, Yi Feng, Jie Ding, Maoshuai Li, Shouying Huang, Mei-Yan Wang, Xinbin Ma","doi":"10.1002/cctc.202401392","DOIUrl":"https://doi.org/10.1002/cctc.202401392","url":null,"abstract":"Controlling the metal geometric and electronic structure is of significance in developing efficient catalysts for heterogeneous hydroformylation. This study examines the structural sizes of Rh and Rh+-Rh0 distribution to construct a highly active catalyst for formaldehyde hydroformylation. The active sites for hydroformylation require several Rhn atoms, while single-atom Rh can solely catalyze hydrogenation. The highest activity was achieved on Rh nanoclusters (0.95 nm), giving a TOF of 191 h−1 and selectivity of 82% for glycolaldehyde formation. The tunability of the electronic properties of Rh nanoclusters and the synergistic interaction between Rh+ and Rh0 are essential for enhanced activity. Pseudo-in situ FT-IR analysis elucidated that formaldehyde adsorbed on Rh nanocluster prefers to produce glycolaldehyde via hydroformylation, while formaldehyde adsorbed on isolated Rhδ+ sites tends to form methanol via hydrogenation. This study provides a new insight into the design of heterogeneous catalysts and guidance for understanding the reaction mechanism for aldehydes/olefins hydroformylation.","PeriodicalId":141,"journal":{"name":"ChemCatChem","volume":"17 3","pages":""},"PeriodicalIF":3.8,"publicationDate":"2024-10-27","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143362981","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

Step Towards Enzymatic Bioelectrorefinery: Design of a Ligninolytic Hybrid Air-Breathing Biocathode

IF 3.8 3区化学

ChemCatChem Pub Date : 2024-10-27 DOI: 10.1002/cctc.202401537

Dr. Vladyslav Mishyn, Juliette Floret, Dr. Brigitte Chabbert, Dr. Véronique Aguié-Béghin, David Crônier, Nunzio Giorgio G. Carducci, Dr. David P. Hickey, Dr. Sofiene Abdellaoui

{"title":"Step Towards Enzymatic Bioelectrorefinery: Design of a Ligninolytic Hybrid Air-Breathing Biocathode","authors":"Dr. Vladyslav Mishyn, Juliette Floret, Dr. Brigitte Chabbert, Dr. Véronique Aguié-Béghin, David Crônier, Nunzio Giorgio G. Carducci, Dr. David P. Hickey, Dr. Sofiene Abdellaoui","doi":"10.1002/cctc.202401537","DOIUrl":"https://doi.org/10.1002/cctc.202401537","url":null,"abstract":"Lignins, abundant aromatic biopolymers and one of the major components of lignocellulosic biomass, remain the most underutilized renewable bioresources of aromatics and hydrocarbons on the Earth. Numerous physical and chemical processes have been developed for lignin valorization; however, they generally suffer from environmentally unfriendly, harsh conditions and lack reaction specificity. On the other hand, milder methods involving biocatalysts exist but are impeded by many limitations, such as cofactor regeneration, deleterious enzyme–lignin interactions, and low stability. In this work, we attempt to eliminate the constrains encountered in enzyme-based lignin valorization processes through the development of a novel electrochemically assisted bioprocess. This “all-in-one” biocathode incorporates a hybrid electrocatalytic interface combining a hydrogen peroxide-generating passive air-breathing gas diffusion electrode with an immobilized hydrogen peroxide-consuming lignin peroxidase on a single surface and catalyzing the depolymerization of lignins. The ligninolytic potential of this bioelectrochemical device is demonstrated using both lignin models (veratryl alcohol and veratrylglycerol β-guaiacyl ether) and a technical lignin at room temperature in aqueous media with the reaction efficiency of 14.9% per hour.","PeriodicalId":141,"journal":{"name":"ChemCatChem","volume":"17 3","pages":""},"PeriodicalIF":3.8,"publicationDate":"2024-10-27","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://onlinelibrary.wiley.com/doi/epdf/10.1002/cctc.202401537","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143362980","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