ChemCatChem最新文献_第3页

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

Insights for the Hydrogen-Mediated Deoxydehydration (DODH) with Cp*ReO3 and Alkene Extrusion of Related Re(V)-Diolates

IF 3.8 3区化学

ChemCatChem Pub Date : 2025-02-14 DOI: 10.1002/cctc.202402010

Dr. Yannick Stöckl, Dr. Frank Rominger, Prof. Dr. A. Stephen K. Hashmi, Prof. Dr. Thomas Schaub

引用次数: 0

Identification and Engineering of Novel N-Methyltransferases

IF 3.8 3区化学

ChemCatChem Pub Date : 2025-02-14 DOI: 10.1002/cctc.202401929

Florian Heinz, Hannes Meinert, Ina Somvilla, Dr. Marian J. Menke, Dr. Mark Doerr, Dr. Thomas Bayer, Prof. Uwe T. Bornscheuer

引用次数: 0

Visible Light-Promoted Enantioselective Catalytic Alkylation of α-Ketoamides with Hydrocarbons

IF 3.8 3区化学

ChemCatChem Pub Date : 2025-02-14 DOI: 10.1002/cctc.202402112

Han Yu, Zun Yang, Hongda Wu, Yao Luo, Weidi Cao, Prof. Dr. Xiaohua Liu, Prof. Dr. Xiaoming Feng

引用次数: 0

Quantitative Basicity-Activity Correlation in Ru-Imidazolium Ionic Liquid-Catalyzed Acetylene Hydrochlorination

IF 3.8 3区化学

ChemCatChem Pub Date : 2025-02-12 DOI: 10.1002/cctc.202401873

Linfeng Li, Bao Wang, Tiantong Zhang, Xinyuan Wang, Dingqiang Feng, Wei Li, Jiangjiexing Wu, Jinli Zhang

{"title":"Quantitative Basicity-Activity Correlation in Ru-Imidazolium Ionic Liquid-Catalyzed Acetylene Hydrochlorination","authors":"Linfeng Li, Bao Wang, Tiantong Zhang, Xinyuan Wang, Dingqiang Feng, Wei Li, Jiangjiexing Wu, Jinli Zhang","doi":"10.1002/cctc.202401873","DOIUrl":"https://doi.org/10.1002/cctc.202401873","url":null,"abstract":"Ionic liquids (ILs), as liquid-phase media in acetylene hydrochlorination, not only optimize the mixing environment of reactants but also stabilize the active sites of metal catalysts. Nevertheless, research in this field is still in its early stages, and systematic analysis and in-depth study of liquid-phase media-ionic liquids are still insufficient. In this study, imidazolium-based ILs ([Bmim]X) with different hydrogen bond basicity (β) values were used to fine-tune the Ru-based liquid-phase catalytic system (Ru-[Bmim]X). It was found that as the β value of [Bmim]X increased, its solubility in HCl and C2H2 also increased, resulting in a volcanic trend in the activity of the Ru-[Bmim]X catalysts. Through systematic characterization and theoretical calculations, we identified the active site of the Ru-[Bmim]Cl catalyst as the [RuCl4]− anion and confirmed that the reaction is a two-step mechanism. Various anions of [Bmim]X influence the adsorption of reactants and reactive energy barriers by modulating the electronic and steric effects at the active sites. In particular, the Ru-[Bmim]Cl catalyst showed a remarkable conversion rate of 86.8% and high stability even at a low temperature of 110 °C. These results provide the scientific basis for the development of novel and efficient liquid-phase catalytic systems.","PeriodicalId":141,"journal":{"name":"ChemCatChem","volume":"17 7","pages":""},"PeriodicalIF":3.8,"publicationDate":"2025-02-12","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143778180","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

Nickel Single Atoms Anchored on Pyridinic N Dominated Porous Carbon for Enhanced Electrochemical 4-Electron Oxygen Reduction

IF 3.8 3区化学

ChemCatChem Pub Date : 2025-02-12 DOI: 10.1002/cctc.202401934

Dr. Shanshan Niu, Dr. Ji Yang, Haifeng Qi, Dr. Lei-Lei Qian, Asst. Prof. Pan Du, Nan Si, Dr. Xiaomin Gu, Asst. Prof. Dawei Jiang, Asst. Prof. Yan Feng

{"title":"Nickel Single Atoms Anchored on Pyridinic N Dominated Porous Carbon for Enhanced Electrochemical 4-Electron Oxygen Reduction","authors":"Dr. Shanshan Niu, Dr. Ji Yang, Haifeng Qi, Dr. Lei-Lei Qian, Asst. Prof. Pan Du, Nan Si, Dr. Xiaomin Gu, Asst. Prof. Dawei Jiang, Asst. Prof. Yan Feng","doi":"10.1002/cctc.202401934","DOIUrl":"https://doi.org/10.1002/cctc.202401934","url":null,"abstract":"The four-electron oxygen reduction reaction (ORR) is at the heart of key renewable energy technologies including fuel cells and rechargeable metal-air batteries, but its wide use necessitates the development of efficient yet inexpensive catalysts. In this study, we have engineered single Ni atoms supported on nitrogen-doped porous carbon with a high content of pyridinic nitrogen (referred to as Ni1–NC–G–NH3). This was accomplished by pyrolyzing a Zn–Ni-ZIF–glucose composite and subsequently treating it with ammonia. Remarkably, the glucose facilitates the formation of isolated Ni atoms within an ammonia reduction atmosphere. Furthermore, we have attained a substantial nitrogen doping level of up to 13 atomic percent, with a significant enrichment of pyridinic nitrogen, constituting 39.5% of the total nitrogen content. Owing to the synergistic interaction between the pyridinic nitrogen and the Ni–Nx sites within the ZIF-derived porous carbon matrix, the Ni1–NC–G–NH3 catalyst demonstrates exceptional ORR catalytic activity and a nearly four-electron selectivity that rivals the commercial Pt/C catalyst in alkaline environments.","PeriodicalId":141,"journal":{"name":"ChemCatChem","volume":"17 7","pages":""},"PeriodicalIF":3.8,"publicationDate":"2025-02-12","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143778179","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

Positive Effect of Carbon Monolith Porosity Sealing with MgO in the CO2 Hydrogenation to CH4 Using NiO-CeO2 Active Phase

IF 3.8 3区化学

ChemCatChem Pub Date : 2025-02-12 DOI: 10.1002/cctc.202401806

Iván Martínez-López, Arantxa Davó-Quiñonero, Esteban Guillén-Bas, Iris Martín-García, Esther Bailón-García, Dolores Lozano-Castelló, Agustín Bueno-López

{"title":"Positive Effect of Carbon Monolith Porosity Sealing with MgO in the CO2 Hydrogenation to CH4 Using NiO-CeO2 Active Phase","authors":"Iván Martínez-López, Arantxa Davó-Quiñonero, Esteban Guillén-Bas, Iris Martín-García, Esther Bailón-García, Dolores Lozano-Castelló, Agustín Bueno-López","doi":"10.1002/cctc.202401806","DOIUrl":"https://doi.org/10.1002/cctc.202401806","url":null,"abstract":"Carbon monolith supports have been manufactured using 3D printed channels template and resorcinol-formaldehyde carbonizable resin. These carbon monoliths were loaded with NiO-CeO2 nanoparticles (Np) as the active phase and tested for CO2 hydrogenation to CH4, focusing on the effect of sealing the carbon porosity with MgO. The MgO coating improves CO2 conversion to CH4 by preventing the NiO-CeO2 nanoparticles from settling within the microporous structure of the carbon support, where gas diffusion limitations hinder access to the active phase. This was confirmed by SEM images, which evidence the introduction of NiO-CeO2 (Np) into the carbon matrix of the bare carbon monolith support and the accumulation of the active phase at the surface of the monolith channels once the porosity is sealed. Other characterization techniques like N2 adsorption and Hg porosimetry, confirm that the porosity is blocked by MgO. On the other hand, it has been demonstrated that there is not a relevant chemical effect of MgO on the NiO-CeO2 (Np) catalytic performance for the carbon monoliths supported catalysts, because the contact between the MgO and NiO-CeO2 phases is poor due to the dispersing effect of carbon.","PeriodicalId":141,"journal":{"name":"ChemCatChem","volume":"17 7","pages":""},"PeriodicalIF":3.8,"publicationDate":"2025-02-12","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143778359","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

Designed Catalytic Templates for the Universal Synthesis of Metal/Nitrogen-Doped Carbon Nanotubes with Hierarchical Architectures for Enhanced Oxygen Reduction 设计催化模板，用于普遍合成具有分层结构的金属/氮掺杂碳纳米管，以增强氧气还原能力

IF 3.8 3区化学

ChemCatChem Pub Date : 2025-02-12 DOI: 10.1002/cctc.202402145

Hong Huang, Xiaoyuan Sun, Mingming Wang, Jizheng Feng, Xinyi Li, Zhongfeng Wang, Yanjiao Chen, Wenting Lu, Prof. Xiao Zhao

{"title":"Designed Catalytic Templates for the Universal Synthesis of Metal/Nitrogen-Doped Carbon Nanotubes with Hierarchical Architectures for Enhanced Oxygen Reduction","authors":"Hong Huang, Xiaoyuan Sun, Mingming Wang, Jizheng Feng, Xinyi Li, Zhongfeng Wang, Yanjiao Chen, Wenting Lu, Prof. Xiao Zhao","doi":"10.1002/cctc.202402145","DOIUrl":"https://doi.org/10.1002/cctc.202402145","url":null,"abstract":"Hierarchical nitrogen-doped carbon nanotubes (NCNTs) with embedded metal species (M/NCNTs) offer broad applications yet are challenging to synthesize controllably. We report a universal one-step strategy leveraging the designed catalytic templates that catalyze the growth of NCNTs and concurrently direct their assembly into diverse hierarchical architectures. This method applies to various precursors from metal hydroxides to metal-organic frameworks and metal nanoparticles/carbon, yielding M/NCNTs with morphologies from plates to flowers, spheres, and NCNTs-grafted dodecahedrons. The Co/NCNTs with hierarchical architecture exhibits superior oxygen reduction reaction (ORR) performance with a half-wave potential of 0.851 V and high durability (negligible decay after 10,000 cycles) in alkaline relative to commercial Pt/C. Electrochemical impedance spectroscopy analysis implies that the hierarchical architecture reduces the mass transfer resistance. Consequently, this Co/NCNTs enables the zinc-air battery with a peak power density of 234.1 mW cm−2 and a specific capacity of 798.8 mAh g−1 Zn.","PeriodicalId":141,"journal":{"name":"ChemCatChem","volume":"17 7","pages":""},"PeriodicalIF":3.8,"publicationDate":"2025-02-12","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143778178","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