ChemCatChem最新文献_第7页

Blue-LED Oxidative Coupling of Amines to N-Alkyl Imines by Metal-Free Meso-Tetraphenyl Porphyrin/Lignin-Nanoparticles

IF 3.8 3区化学

ChemCatChem Pub Date : 2025-02-18 DOI: 10.1002/cctc.202402097

Dr. Natalia Ceccotti Vlas, Dr. Fabiana Fosso, Dr. Elisa De Marchi, Dr. Sofia Gabellone, Dr. Eliana Capecchi, Dr. Davide Piccinino, Prof. Lorenzo Botta, Prof. Raffaele Saladino

引用次数: 0

Enhanced Targeted Deoxygenation Catalytic Pyrolysis of Lignin to Aromatic Hydrocarbons over Oxygen Vacancies Pt-MoOx/TiO2

IF 3.8 3区化学

ChemCatChem Pub Date : 2025-02-17 DOI: 10.1002/cctc.202401727

Yi Gao, Jiajun Yu, Bo Zhang, Wei Jin, Huiyan Zhang

{"title":"Enhanced Targeted Deoxygenation Catalytic Pyrolysis of Lignin to Aromatic Hydrocarbons over Oxygen Vacancies Pt-MoOx/TiO2","authors":"Yi Gao, Jiajun Yu, Bo Zhang, Wei Jin, Huiyan Zhang","doi":"10.1002/cctc.202401727","DOIUrl":"https://doi.org/10.1002/cctc.202401727","url":null,"abstract":"Catalytic pyrolysis technology has been widely used in the conversion of lignin to aromatics, but the catalysts still suffer from poor stability and low product yields due to the lack of oxygen vacancy design. In this study, we report a multi-active site synergistic strategy to enhance the cleavage of lignin aryl carbon-oxygen bonds. Pt-MoOx/TiO2 has a large specific surface area and pore volume, showing a significant medium mesopore size, which was favorable for trapping macromolecular oxides. Meanwhile, a significant synergistic effect was found between hydrogen-activated metallic Pt and molybdenum oxide, which both inhibited the hydrogenation of the aryl ring and promoted the dissociation of hydrogen, thus providing more active sites. More importantly, the defective oxygen vacancies played a key role in the adsorption and activation of oxygen-containing groups, facilitating the absorption of active hydrogen formed by hydrogen spillover. Under the conditions of atmospheric pressure and 400 °C, the high efficiency conversion (100%) of m-cresol was achieved, and guaranteed a high yield of aromatics (98%) and high selectivity (98%). Extending to lignin, the yield of aromatics can reach 5 wt.%. The catalyst remained highly active after 6 h of continuous operation, and there was no significant decrease in yield after two regenerations.","PeriodicalId":141,"journal":{"name":"ChemCatChem","volume":"17 7","pages":""},"PeriodicalIF":3.8,"publicationDate":"2025-02-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143778195","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

Deciphering the Electrochemical Activity and Selectivity of Earth-Abundant Transition Metal-Based Catalysts for the Alcohol Electrooxidation—Current Status

IF 3.8 3区化学

ChemCatChem Pub Date : 2025-02-17 DOI: 10.1002/cctc.202402013

Michael Braun, Corina Andronescu

{"title":"Deciphering the Electrochemical Activity and Selectivity of Earth-Abundant Transition Metal-Based Catalysts for the Alcohol Electrooxidation—Current Status","authors":"Michael Braun, Corina Andronescu","doi":"10.1002/cctc.202402013","DOIUrl":"https://doi.org/10.1002/cctc.202402013","url":null,"abstract":"Since alternative anode reactions such as the electrochemical alcohol oxidation reaction (AOR) are becoming increasingly important for water electrolysis in the course of a sustainable defossilization and electrification of the energy and chemical industry, this paper reviews the progress in understanding the electrocatalytic activity and selectivity of non-noble metal-based (non-NMB) catalysts regarding AOR and especially, the glycerol oxidation reaction (GOR). Starting from Ni-based catalysts, the review aims to consolidate the current state of knowledge for improving electrocatalytic activity based on mechanistic models and to transfer it to Co- and Cu-based materials. Several main influences on the catalytic activity can be identified via the involvement of metal ions (metal redox reactions) or oxygen species (oxygen redox reactions), which lead to the importance of M─O motifs for the electrocatalytically active ensemble on the surface of an electrically conductive non-NMB catalyst. In addition to the electrocatalytic activity, this work delves into possibilities for influencing the selectivity during AOR, which include the catalyst itself, electrode potential, or the pH value of the electrolyte. Furthermore, the chemical structure of the alcohol proves to be crucial, especially when oxidizing vicinal alcohols, because differentiating products from oxidative (pseudo)glycol cleavage and hydrogen atom transfer can complicate understanding selectivity influences.","PeriodicalId":141,"journal":{"name":"ChemCatChem","volume":"17 8","pages":""},"PeriodicalIF":3.8,"publicationDate":"2025-02-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://onlinelibrary.wiley.com/doi/epdf/10.1002/cctc.202402013","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143836257","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

Ethylene Glycol Partial Aqueous Oxidation on Co3O4 (001) Surfaces: Pathways to Two- and Four-Electron Products in Neutral and Oxidative Conditions

IF 3.8 3区化学

ChemCatChem Pub Date : 2025-02-17 DOI: 10.1002/cctc.202401885

Msc Falonne Bertholde Sharone Nkou, PhD Stephane Kenmoe

{"title":"Ethylene Glycol Partial Aqueous Oxidation on Co3O4 (001) Surfaces: Pathways to Two- and Four-Electron Products in Neutral and Oxidative Conditions","authors":"Msc Falonne Bertholde Sharone Nkou, PhD Stephane Kenmoe","doi":"10.1002/cctc.202401885","DOIUrl":"https://doi.org/10.1002/cctc.202401885","url":null,"abstract":"The catalytic oxidation of ethylene glycol (EG) on the Co3O4 (001) surface is investigated by AIMD simulations in the presence of a water layer for the A- and B- terminations. In addition to the surface structure and composition, the chemical state of the aqueous environment plays a crucial role in the oxidation process. Specifically, it depends on the concentration of surface hydroxyl groups, which can act both as proton donors and acceptors. Reference surfaces, which are generated by bringing the unhydrogenated A- and B-terminated surfaces in contact with a stoichiometric water layer, show some spontaneous water dissociation, which produces a number of surface hydroxyl groups. On such an A-terminated reference surface, the EG molecule is barely reactive. This holds even in a more oxidative state. On the B-terminated surface, EG's decomposition into ethylenedioxy species occurs already in the reference state. Under the more oxidative hydrogen-deficient conditions obtained by removing eight hydrogen atoms, the reaction proceeds to the formation of the two-electron oxidation product glycolaldehyde. Removal of altogether 16 hydrogen atoms facilitates the formation of four-electron oxidation products, such as glycolic acid and glyoxal and the observation of a transient H2O2 species, which subsequently evolves to form dioxygen.","PeriodicalId":141,"journal":{"name":"ChemCatChem","volume":"17 7","pages":""},"PeriodicalIF":3.8,"publicationDate":"2025-02-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://onlinelibrary.wiley.com/doi/epdf/10.1002/cctc.202401885","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143778194","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

Recent Progress in the Electrocatalytic Synthesis of H2O2 from Graphite-Based Materials

IF 3.8 3区化学

ChemCatChem Pub Date : 2025-02-16 DOI: 10.1002/cctc.202402062

Hengjun Shang, Yaning Zhang, Yuming Dong, Prof. Yongfa Zhu, Prof. Chengsi Pan

{"title":"Recent Progress in the Electrocatalytic Synthesis of H2O2 from Graphite-Based Materials","authors":"Hengjun Shang, Yaning Zhang, Yuming Dong, Prof. Yongfa Zhu, Prof. Chengsi Pan","doi":"10.1002/cctc.202402062","DOIUrl":"https://doi.org/10.1002/cctc.202402062","url":null,"abstract":"Graphite-based catalysts, with their abundant availability, low cost, excellent electrical conductivity, and chemical stability, serve as an ideal candidate for eletrocatalytical synthesis of hydrogen peroxide (H2O2). This review explores the fundamental principles of H₂O₂ production via the electrochemical oxygen reduction reaction (ORR) and the theoretical basis for evaluating catalyst selectivity. It summarizes the structural characteristics, classifications, and developmental history of graphite-based catalysts, with a focus on recent advancements. The discussion highlights strategies such as heteroatom doping, defect engineering, and surface oxygen functionalization, analyzing their effectiveness in designing novel high-performance catalysts. By rationally designing catalyst components and fine-tuning the microenvironment of active sites, it is possible to develop efficient and highly stable catalysts, narrowing the gap between experimental outcomes and theoretical predictions. This work aims to advance the scalable application of graphite-based materials in green chemistry and energy fields.","PeriodicalId":141,"journal":{"name":"ChemCatChem","volume":"17 7","pages":""},"PeriodicalIF":3.8,"publicationDate":"2025-02-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143778433","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

Decarboxylative Cross-Dehydrogenative Coupling of Tetrahydroisoquinoline and Alkynoic Acids Using Recyclable Carbon Nanotube Supported Copper/Nickel Oxide Catalysts

IF 3.8 3区化学

ChemCatChem Pub Date : 2025-02-16 DOI: 10.1002/cctc.202401821

Robin Prakash Sirvin Rajan, Ji Dang Kim, Hyun Chul Choi, Sunwoo Lee

引用次数: 0

Electrocatalytic Syngas Production Using Metalloporphyrins with Controllable H2/CO Ratios 利用具有可控 H2/CO 比率的金属卟啉电催化合成气生产

IF 3.8 3区化学

ChemCatChem Pub Date : 2025-02-16 DOI: 10.1002/cctc.202402090

Zhimeng Wang, Benxing Mei, Yuhan Xu, Yuze Liu, Dr. Xialiang Li, Prof. Dr. Rui Cao

{"title":"Electrocatalytic Syngas Production Using Metalloporphyrins with Controllable H2/CO Ratios","authors":"Zhimeng Wang, Benxing Mei, Yuhan Xu, Yuze Liu, Dr. Xialiang Li, Prof. Dr. Rui Cao","doi":"10.1002/cctc.202402090","DOIUrl":"https://doi.org/10.1002/cctc.202402090","url":null,"abstract":"Electrochemical methods to produce syngas present a promising strategy for energy conservation and environmental protection. The H₂/CO ratio of syngas is crucial for its applications. However, few catalysts can achieve catalytic generation of syngas that can be directly used because the H₂/CO ratio is difficult to be controlled. To address this issue, bicomponent electrocatalysts are utilized to produce syngas with controllable H₂/CO ratios. These two catalysts in the bicomponent electrocatalysts can efficiently and selectively catalyze CO2 reduction reaction (CO2RR) to generate CO and hydrogen evolution reaction (HER) to generate H2 respectively. Metalloporphyrins are promising electrocatalysts for both CO2RR and HER. A series of metalloporphyrins 1-M (M = Fe, Co, Ni, Cu) were synthesized as electrocatalysts to produce syngas with different H2/CO ratios. Among these metalloporphyrins, 1-Co and 1-Cu can selectively produce CO and H2, respectively, through CO2RR and HER in KHCO3 aqueous solutions. The ratio of 1-Co and 1-Cu in bicomponent electrocatalysts 1-Co/1-Cu is adjusted to achieve the regulation of H2/CO ratio (0.1–6.4) at high catalytic currents. This work provides a new approach for designing more efficient syngas catalysts with tunable H2/CO ratios.","PeriodicalId":141,"journal":{"name":"ChemCatChem","volume":"17 8","pages":""},"PeriodicalIF":3.8,"publicationDate":"2025-02-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143836353","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

Characterization of Recombinant Unspecific Peroxygenase from Candolleomyces aberdarensis Through Crystallographic and Substrate Selectivity Studies

IF 3.8 3区化学

ChemCatChem Pub Date : 2025-02-16 DOI: 10.1002/cctc.202402015

Andrea Menés-Rubio, Angela Fernandez-Garcia, Dianelis T. Monterrey, Patricia Gomez de Santos, Israel Sánchez-Moreno, Julia Sanz-Aparicio, Miguel Alcalde

{"title":"Characterization of Recombinant Unspecific Peroxygenase from Candolleomyces aberdarensis Through Crystallographic and Substrate Selectivity Studies","authors":"Andrea Menés-Rubio, Angela Fernandez-Garcia, Dianelis T. Monterrey, Patricia Gomez de Santos, Israel Sánchez-Moreno, Julia Sanz-Aparicio, Miguel Alcalde","doi":"10.1002/cctc.202402015","DOIUrl":"https://doi.org/10.1002/cctc.202402015","url":null,"abstract":"Fungal unspecific peroxygenases (UPOs) are remarkable biocatalysts for the selective oxygenation of non-activated C─H bonds. Here, we describe a crystallographic and substrate selectivity study of an UPO ortholog from Candolleomyces (Psathyrella) aberdarensis (PabUPO-II). The recombinant enzyme produced in yeast was crystallized and complexed with a representative panel of substrates, including alkanes, fatty acids, and norisoprenoids; the crystals diffracted at a resolution up to 2 Å. PabUPO-II combines structural features of canonical long and short UPOs, presenting a hybrid heme channel and a flexible catalytic Glu212 that adopts two alternate conformations, proximal and distal to the substrates. The positioning of substrates at the heme channel in soaking experiments was complemented with a characterization of the enzymatic reactions. With alkanes and fatty acids, PabUPO-II carried out oxygenations at ω-2 and ω-1, but when forcing the reaction with dicarboxylic acids, α- and β-hydroxylations were detected. Reactions with the α-ionone and α-damascone norisoprenoids produced major oxygenations at the cyclohexene and at the vinylic aliphatic chain, respectively. Taken together, PabUPO-II shares structural and functional similarities with both long and short UPOs, opening avenues for future engineering endeavors.","PeriodicalId":141,"journal":{"name":"ChemCatChem","volume":"17 7","pages":""},"PeriodicalIF":3.8,"publicationDate":"2025-02-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143778435","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

Single Co Atom Catalyst Derived from Terpolymer Pyrolysis for Hydrogenation of Nitroarenes

IF 3.8 3区化学

ChemCatChem Pub Date : 2025-02-16 DOI: 10.1002/cctc.202401902

Yanan Zhou, Anni Guo, Huawei Shen, Yue Wang, Fuxing Zhang, Xuejiao Rong, Yang Li, Xilong Yan, Ligong Chen, Bowei Wang

{"title":"Single Co Atom Catalyst Derived from Terpolymer Pyrolysis for Hydrogenation of Nitroarenes","authors":"Yanan Zhou, Anni Guo, Huawei Shen, Yue Wang, Fuxing Zhang, Xuejiao Rong, Yang Li, Xilong Yan, Ligong Chen, Bowei Wang","doi":"10.1002/cctc.202401902","DOIUrl":"https://doi.org/10.1002/cctc.202401902","url":null,"abstract":"Recently, single atom catalysts (SACs) with isolated metal atom as the active site have received extensive attention for their excellent catalytic performance. However, limited by the strong aggregation tendency of monometallic atoms, the construction of SACs remains a formidable challenge. Herein, we developed a facile ternary copolymerization-pyrolysis approach to synthesize a single cobalt atom catalyst (Co1@NC) by employing amino-functionalized cobalt phthalocyanine (CoPc(NH2)4) as the metal precursor. Specially, CoPc(NH2)4 was copolymerized with melamine and 1,4-phthalaldehyde to yield a terpolymer, thereby allowing CoPc to be more uniformly and stably distributed in the polymer network. Subsequently, the obtained terpolymer was pyrolyzed to afford Co1@NC. Aberration-corrected high-angle annular dark-field scanning transmission electron microscopy (AC HAADF-STEM) and X-ray absorption spectroscopy (XAS) directly confirmed that the catalyst Co1@NC was a single cobalt atom catalyst. Furthermore, the large specific surface area (SBET = 418.8 m2/g) and high cobalt content (2.71 wt%) of Co1@NC provided more cobalt active sites and therefore displayed excellent catalytic activity in the hydrogenation of nitrobenzene. In addition, the catalyst showed remarkable cyclic stability in five cycles and remained as the single atom catalyst.","PeriodicalId":141,"journal":{"name":"ChemCatChem","volume":"17 7","pages":""},"PeriodicalIF":3.8,"publicationDate":"2025-02-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143778434","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

Advancing Spin Controlled Electrocatalysis Using Chiral Gold Nanoparticles Functionalized Bimetallic Spinel Oxide

IF 3.8 3区化学

ChemCatChem Pub Date : 2025-02-15 DOI: 10.1002/cctc.202401695

Anujit Balo, Utkarsh Utkarsh, Mive Yasmin, Utpal Kumar Gosh, Koyel Banerjee Ghosh

{"title":"Advancing Spin Controlled Electrocatalysis Using Chiral Gold Nanoparticles Functionalized Bimetallic Spinel Oxide","authors":"Anujit Balo, Utkarsh Utkarsh, Mive Yasmin, Utpal Kumar Gosh, Koyel Banerjee Ghosh","doi":"10.1002/cctc.202401695","DOIUrl":"https://doi.org/10.1002/cctc.202401695","url":null,"abstract":"Oxygen reduction reaction (ORR) and oxygen evolution reaction (OER) are the foundations of renewable energy technology. However, both processes have significant activation barriers, severely limiting the overall performance of energy conversion devices that utilize ORR/OER. Though traditional catalyst design prioritizes crystal and electronic structure, understanding the detailed mechanism requires consideration of spin selection rules as the ground electronic state of diatomic oxygen is a triplet. Here, we demonstrate the enhancement of the electrocatalytic performance of Mn and Co-based bimetallic spinel oxides by functionalizing with chiral gold nanoparticles. Chiral gold nanoparticles impart spin selective charge transfer during oxygen reduction, resulting in higher current density in comparison with the achiral composite catalyst. Furthermore, the onset potential gets reduced by 120 mV at 2.5 mA cm−2 current density toward the OER activity of the chiral gold nanoparticle functionalized catalyst, attributed to the spin polarization mechanisms via chiral induced spin selectivity effect. This work emphasizes the use of chirality in the transition metal-based oxide to induce the spin polarization in the oxide-based catalysts in advancing ORR and OER efficiencies that are very essential for the application in renewable energy technology.","PeriodicalId":141,"journal":{"name":"ChemCatChem","volume":"17 7","pages":""},"PeriodicalIF":3.8,"publicationDate":"2025-02-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143778431","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