ChemCatChem最新文献_第4页

“Hidden” Metal–Ligand Cooperation for Additive-Free Formic Acid Dehydrogenation 无添加甲酸脱氢过程中的 "隐藏 "金属配体合作

IF 3.8 3区化学

ChemCatChem Pub Date : 2025-03-02 DOI: 10.1002/cctc.202500094

Shang Shi, Dr. Simon Mathew, Prof. Dr. Bas de Bruin

引用次数: 0

Emerging Functionalized Lindqvist-Type Polyoxometalate-Based Compounds: Design, Synthesis, and Applications

IF 3.8 3区化学

ChemCatChem Pub Date : 2025-03-01 DOI: 10.1002/cctc.202500066

Ailing Gao, Dr. Tsukasa Iwano, Prof. Sayaka Uchida

{"title":"Emerging Functionalized Lindqvist-Type Polyoxometalate-Based Compounds: Design, Synthesis, and Applications","authors":"Ailing Gao, Dr. Tsukasa Iwano, Prof. Sayaka Uchida","doi":"10.1002/cctc.202500066","DOIUrl":"https://doi.org/10.1002/cctc.202500066","url":null,"abstract":"This concept article highlights emerging potential of Lindqvist-type polyoxometalate (POM)-based compounds, focusing on their design, synthesis, and applications in catalysis, energy, and environmental fields. POMs are anionic metal-oxo clusters, broadly classified into isopolyoxometalates and heteropolyoxometalates. This article highlights Lindqvist-type POMs [M6O19]n−, a subset of isopolyoxometalates characterized by compact, highly symmetric octahedral structures, high negative charge densities, and multielectron transfer properties. These unique features have inspired studies on their organic modifications, utilizing the high reactivity of their surface oxygen atoms. It is now timely to revisit functionalized Lindqvist-type POM-based compounds, in both solution and solid states, particularly as catalysts. Recent advancements include stabilizing Lindqvist clusters through host–guest complexes enabling their use in aqueous environments. In the solid state, they have been utilized as structural units in inorganic–organic hybrid materials, demonstrating remarkable functionality. The promising potential of Lindqvist-type POM-based compounds encourages further research to establish systematic synthetic methods, moving beyond empirical approaches or serendipity, to address challenges in sustainability and energy production.","PeriodicalId":141,"journal":{"name":"ChemCatChem","volume":"17 8","pages":""},"PeriodicalIF":3.8,"publicationDate":"2025-03-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://onlinelibrary.wiley.com/doi/epdf/10.1002/cctc.202500066","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143835954","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

Silica-Embedded Metal Oxide Nanoparticles as Epoxidation Catalysts: Batch and Continuous Flow Systems

IF 3.8 3区化学

ChemCatChem Pub Date : 2025-02-27 DOI: 10.1002/cctc.202500003

Diana M. Gomes, Xingyu Yao, Patrícia Neves, Margarida M. Antunes, Nicola Pinna, Patrícia A. Russo, Anabela A. Valente

{"title":"Silica-Embedded Metal Oxide Nanoparticles as Epoxidation Catalysts: Batch and Continuous Flow Systems","authors":"Diana M. Gomes, Xingyu Yao, Patrícia Neves, Margarida M. Antunes, Nicola Pinna, Patrícia A. Russo, Anabela A. Valente","doi":"10.1002/cctc.202500003","DOIUrl":"https://doi.org/10.1002/cctc.202500003","url":null,"abstract":"Catalytic epoxidation of olefins gives epoxide chemicals for several end-user products. With the technological advancements of these processes (especially for light olefins), which have importantly contributed to the epoxides market expansion, challenges remain in developing adequate heterogeneous catalysts for converting bulkier olefins, using simple catalyst synthesis procedures, and, on the other hand, studying the catalytic performances under different operation modes. Hence, heterogeneous epoxidation catalysts are prepared via simple one-pot procedures, with the necessary versatility to tune the material properties for batch and continuous flow operation. Specifically, silica-embedded nanoparticles of molybdenum oxide (Si/Mo(x), x = Mo loading) and silica-embedded nanoparticles of binary transition metal oxides (Si/MoM, M = Ta, Nb or W) are synthesized, and promoted the epoxidation of cis-cyclooctene with tert-butylhydroperoxide as oxidant, at 70 °C. Epoxide yields in the range of 90%–100% are reached within 4 h, at 70 °C, under batch operation. Under continuous flow, steady state conditions (fixed bed reactor), catalyst Si/MoNb led to ca. 44% epoxide yield, at 70 °C. At 90 °C, Si/MoNb exhibited multifunctionality leading to 51% cyclooctanone yield. It represents the first fully inorganic heterogeneous Mo-catalyst for continuous flow olefin epoxidation and the first heterogeneous Mo-catalyst for integrated olefins-to-cycloalkanones with hydroperoxides.","PeriodicalId":141,"journal":{"name":"ChemCatChem","volume":"17 8","pages":""},"PeriodicalIF":3.8,"publicationDate":"2025-02-27","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143836405","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

Fast Co-Catalyzed Semihydrogenation of Alkynes with Controlled E/Z-Selectivity Using Same Catalyst

IF 3.8 3区化学

ChemCatChem Pub Date : 2025-02-27 DOI: 10.1002/cctc.202500041

Dr. Dilip K. Pandey, Prof. Julia R. Khusnutdinova

引用次数: 0

Insights into the Role of Bismuth Oxidation State in Bi-Based Nanocatalysts for High Efficiency CO2 Electroreduction to Formate

IF 3.8 3区化学

ChemCatChem Pub Date : 2025-02-26 DOI: 10.1002/cctc.202402151

Xin Liu, Kejian Li, Linyu Cheng, Yang Yang, Xianming Bao, Jie Zhang, Jingjing Zhou, Sugang Meng, Xiuzhen Zheng, Liwu Zhang

{"title":"Insights into the Role of Bismuth Oxidation State in Bi-Based Nanocatalysts for High Efficiency CO2 Electroreduction to Formate","authors":"Xin Liu, Kejian Li, Linyu Cheng, Yang Yang, Xianming Bao, Jie Zhang, Jingjing Zhou, Sugang Meng, Xiuzhen Zheng, Liwu Zhang","doi":"10.1002/cctc.202402151","DOIUrl":"https://doi.org/10.1002/cctc.202402151","url":null,"abstract":"Electrocatalytic reduction of CO2 to formate (HCOO−) using Bi-based nanocatalysts shows great promise in “carbon-neutrality” and green chemical synthesis. However, the functional active species, metallic Bi or Bi-O structure responsible for CO2 reduction to HCOO− is still in debate. In this study, we found that nanodendritic Bi-metal electrocatalyst synthesized via one-step electrodeposition method, exhibited ∼100% Faradic efficiency to HCOO− at −0.98 VRHE, which was much superior to that from Bi-plasma mainly composed of Bi2O3 (Faradic efficiency, 76.7%). The in situ Raman spectra and density functional theory (DFT) calculations collectively confirmed that zero-valent Bi-metal rather than Bi-O structure is crucial for HCOO− production from CO2 electroreduction. In addition, the Bi-metal nanocatalysts exhibited high stability maintaining >95% performance over 94 h reaction and the integration with photovoltaic-electrocatalysis system achieved about 1% solar to formate conversion efficiency. This work elucidates the functional Bi-containing species in CO2 electroreduction, providing guidance onto effective Bi-based electrocatalysts design for formate production.","PeriodicalId":141,"journal":{"name":"ChemCatChem","volume":"17 8","pages":""},"PeriodicalIF":3.8,"publicationDate":"2025-02-26","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143836454","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

BINAP-Accelerated Photoinduced Trifluoromethylation of (Hetero)Aryl Iodides BINAP-光诱导的（异）芳基碘化物三氟甲基化反应

IF 3.8 3区化学

ChemCatChem Pub Date : 2025-02-26 DOI: 10.1002/cctc.202402078

Dr. Xueyan Yang, Prof. Yan Kang, Prof. Haishu Lin, Prof. Siyuan Wang

{"title":"BINAP-Accelerated Photoinduced Trifluoromethylation of (Hetero)Aryl Iodides","authors":"Dr. Xueyan Yang, Prof. Yan Kang, Prof. Haishu Lin, Prof. Siyuan Wang","doi":"10.1002/cctc.202402078","DOIUrl":"https://doi.org/10.1002/cctc.202402078","url":null,"abstract":"Trifluoromethyl groups hold significance in the bioactivity and physical properties of organic molecules. Contemporary approaches to trifluoromethylated aromatics typically involve the coupling of CuCF3 reagents with aryl halides, which is limited by the difficulty of oxidative addition of copper to organohalides. Herein, a photoinduced ligand-catalyzed trifluoromethylation/pentafluoroethylation of (hetero)aryl iodides is presented. The conversion of a C─I bond into a C─CF3 bond is enabled by the photochemistry of copper, which produces aryl radicals with in situ generated CuCF3 from Ruppert–Prakash reagent under visible light. This radical approach circumvents the challenge of oxidative addition of copper to aryl halides, and a catalytic amount of rac-BINAP substantially accelerates the whole process, allowing the reaction to complete within 1 h under very mild conditions without using any additional photo-redox catalysts. The readily availability of starting material, high efficiency, and broad utility make this transformation attractive for practitioners of synthetic and medicinal chemistry.","PeriodicalId":141,"journal":{"name":"ChemCatChem","volume":"17 8","pages":""},"PeriodicalIF":3.8,"publicationDate":"2025-02-26","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143836452","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

A Dual-Functional Approach: Temperature-Dependent Selective N-Methylation of Amines with Methanol via Skeletal Copper Catalysts

IF 3.8 3区化学

ChemCatChem Pub Date : 2025-02-25 DOI: 10.1002/cctc.202402126

Dr. Ke-Ming Li, Prof. Ti-Peng Wang, Xuan Zhang, Qun-Xing Liu, Yao Xiao, Feng-Shuo Guo, Prof. Yao-Bing Huang, Prof. Qiang Lu

{"title":"A Dual-Functional Approach: Temperature-Dependent Selective N-Methylation of Amines with Methanol via Skeletal Copper Catalysts","authors":"Dr. Ke-Ming Li, Prof. Ti-Peng Wang, Xuan Zhang, Qun-Xing Liu, Yao Xiao, Feng-Shuo Guo, Prof. Yao-Bing Huang, Prof. Qiang Lu","doi":"10.1002/cctc.202402126","DOIUrl":"https://doi.org/10.1002/cctc.202402126","url":null,"abstract":"Selective N-methylation with green methylating agents is a highly attractive yet challenging topic in organic synthesis and pharmaceutical production. Herein, a skeletal Cu-based catalyst was developed for the selective N-methylation of amines using renewable methanol under relatively mild conditions. By simply modulating the reaction temperature, the CuZnAl-1.5 catalyst enabled tunable synthesis of N-monomethylated and N,N-dimethylated amines. A wide range of amines were efficiently methylated in high yields. Kinetic and mechanistic studies revealed a borrowing hydrogen pathway, with N-monomethylation exhibiting a lower activation energy. The active Cu surface was identified as the key site for methanol activation to form aldehyde intermediate, whose concentration critically influenced product selectivity. The role of Zn in catalyst preparation and catalysis was also elucidated. The catalyst demonstrated excellent applicability in various synthetic scenarios, underscoring the potential of skeletal Cu-based systems for methylation reaction with methanol.","PeriodicalId":141,"journal":{"name":"ChemCatChem","volume":"17 8","pages":""},"PeriodicalIF":3.8,"publicationDate":"2025-02-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143836311","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

Photothermalcatalytic Hydrogen Production by Continuous Gaseous Water Splitting over Ni3N/g-C3N4

IF 3.8 3区化学

ChemCatChem Pub Date : 2025-02-25 DOI: 10.1002/cctc.202500128

Zhonghao Han, Zhiying Yang, Yingpeng Xie, Ludong Yi, Xi Yang, Guangwen Xu

{"title":"Photothermalcatalytic Hydrogen Production by Continuous Gaseous Water Splitting over Ni3N/g-C3N4","authors":"Zhonghao Han, Zhiying Yang, Yingpeng Xie, Ludong Yi, Xi Yang, Guangwen Xu","doi":"10.1002/cctc.202500128","DOIUrl":"https://doi.org/10.1002/cctc.202500128","url":null,"abstract":"The initiation of the water splitting reaction necessitates a considerable energy input and the associated energy barrier can be notably mitigated through the utilization of appropriate catalysts. Ni3N/g-C3N4 catalyst was synthesized through a combination of thermal decomposition and hydrothermal synthesis techniques for photothermal water splitting reaction. The catalyst was characterized using XRD, HRTEM, UV–vis, XPS, electrochemical impedance spectroscopy (EIS), and photoluminescence (PL). It was observed that the Ni3N promoter is uniformly dispersed on the g-C3N4 exerting no discernible influence on the surface structure and crystal phase of the g-C3N4.The incorporation of Ni3N effectively decreases the resistance of g-C3N4, enhances the photocurrent intensity, facilitates the transfer of photogenerated electrons from g-C3N4 to Ni3N, and suppresses the recombination of photogenerated carriers. Additionally, the findings from the photothermal water splitting experiments revealed that g-C3N4 decreased the activation energy to 71.23 kJ·mol−1, while the Ni3N promoter further lowered it to 19.73 kJ·mol−1.","PeriodicalId":141,"journal":{"name":"ChemCatChem","volume":"17 8","pages":""},"PeriodicalIF":3.8,"publicationDate":"2025-02-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143836324","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

Systematic Investigation of Cu-ZnO-MnOX Catalysts for CO2 Hydrogenation to Methanol

IF 3.8 3区化学

ChemCatChem Pub Date : 2025-02-25 DOI: 10.1002/cctc.202500103

Tuo Guo, Lin Wang, Dongdong Zhai, Yongning Yuan, Qingjie Guo

{"title":"Systematic Investigation of Cu-ZnO-MnOX Catalysts for CO2 Hydrogenation to Methanol","authors":"Tuo Guo, Lin Wang, Dongdong Zhai, Yongning Yuan, Qingjie Guo","doi":"10.1002/cctc.202500103","DOIUrl":"https://doi.org/10.1002/cctc.202500103","url":null,"abstract":"Currently, the doping and modification of Cu-ZnO catalysts is a research hotspot for CO2 to methanol. In this work, the impact of MnOX additive doping on the catalytic activity of Cu-ZnO catalysts for CO2 hydrogenation to methanol was systematically examined. A series of ternary Cu-ZnO-MnOX catalysts were produced by the co-precipitation method, and their physicochemical structures and catalytic activities were characterized. MnOX enhanced the dispersion of Cu and Zn species, obtained a stable crystalline phase, and formed a mesoporous structure with a larger specific surface area, which increased the effective contact area of the gas. Moreover, the appropriate amount of MnOX generated more oxygen vacancies and medium-strong basic sites in the catalyst, which effectively promoted the adsorption and conversion of CO2, and thus improved the methanol yield. The outcomes demonstrated the best activity was achieved when the molar content of MnOX was 10% (CZM-10), with a methanol space-time yield (STY) of 233.23 gMeOH/(kgcat·h) at 220 °C. In situ DRIFTS show the CO2 methanolization of CZM catalyst via a formate mechanism. This study is important to produce novel catalysts for CO2 hydrogenation to methanol.","PeriodicalId":141,"journal":{"name":"ChemCatChem","volume":"17 8","pages":""},"PeriodicalIF":3.8,"publicationDate":"2025-02-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143836313","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

Nb3VS6 Nanosheets: A Ternary Metal Sulfide That Achieves Outstanding Ampere-Level Current Density for Alkaline Electrochemical HER Activity

IF 3.8 3区化学

ChemCatChem Pub Date : 2025-02-25 DOI: 10.1002/cctc.202500183

Pallellappa Chithaiah, Divya Bhutani, C. N. R. Rao

引用次数: 0