Journal of Catalysis最新文献

筛选
英文 中文
A highly stable metallosalen-based metal–organic framework electrocatalyst for versatile oxidative organic transformations 一种高度稳定的金属盐基金属有机框架电催化剂,用于多功能氧化有机转化
IF 7.3 1区 化学
Journal of Catalysis Pub Date : 2025-05-30 DOI: 10.1016/j.jcat.2025.116252
Lei-Yan Lyu, Fa-Xue Ma, Xin-Ling Xie, Meng-Jiao Sun, Tao Huang, Teng Zhang
{"title":"A highly stable metallosalen-based metal–organic framework electrocatalyst for versatile oxidative organic transformations","authors":"Lei-Yan Lyu, Fa-Xue Ma, Xin-Ling Xie, Meng-Jiao Sun, Tao Huang, Teng Zhang","doi":"10.1016/j.jcat.2025.116252","DOIUrl":"https://doi.org/10.1016/j.jcat.2025.116252","url":null,"abstract":"Production of epoxides and aldehydes as key intermediates for organic synthesis usually suffers from the consumption of toxic, corrosive or explosive oxidants. Electrochemical oxidation of alkenes and alcohols have been proposed as alternative green, atom-economic and sustainable synthetic methods, yet the lack of efficient electrocatalysts severely limits potential industrial applications due to the low selectivity and poor stability. We herein present the synthesis of FICN-24, a chemically stable metal–organic framework constructed from Ni<sub>8</sub>-pyrazolate secondary building units and Mn(salen)-derived ligands, as active and selective electrocatalyst for alkene epoxidation and alcohol oxidation reactions. FICN-24 showed high yields and selectivity up to &gt; 90 % towards the desired epoxide and aldehyde products in the electrochemical oxidation of a broad scope of alkene and primary alcohol substrates, respectively, and retained its structural integrity and catalytic activity upon recycling. This work establishes MOF-based electrocatalysis as a promising platform for selective organic transformations, advancing sustainable synthesis in alignment with green chemistry principles.","PeriodicalId":346,"journal":{"name":"Journal of Catalysis","volume":"121 1","pages":""},"PeriodicalIF":7.3,"publicationDate":"2025-05-30","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144176707","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"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
Easily synthesized self-nitrogen doped carbon-supported nickel bio-based sustainable catalyst for hydrogenation of benzylamine from benzonitrile 易于合成自氮掺杂碳负载镍生物基苯甲腈加氢苯胺催化剂
IF 7.3 1区 化学
Journal of Catalysis Pub Date : 2025-05-30 DOI: 10.1016/j.jcat.2025.116251
Weidong Liu, Jianguo Liu
{"title":"Easily synthesized self-nitrogen doped carbon-supported nickel bio-based sustainable catalyst for hydrogenation of benzylamine from benzonitrile","authors":"Weidong Liu, Jianguo Liu","doi":"10.1016/j.jcat.2025.116251","DOIUrl":"https://doi.org/10.1016/j.jcat.2025.116251","url":null,"abstract":"Benzylamine production from the hydrogenation of nitrile is attractive, but most of the catalysts are complicated and costly. In this paper, a simple synthesis of self-nitrogen-doped carbon-supported nickel biobased sustainable catalyst (Ni-JKS-600) for benzylamine hydrogenation with benzonitrile has been reported. The catalyst has high specific surface area, abundant micro-mesoporous structure and nickel hydrogenation active site. By optimizing the reaction conditions, a mild reaction condition (120 ℃, 2 MPa H<sub>2</sub>, 3 h) was determined, and it was found that the solvent had a significant effect on the selectivity of benzylamine, and the selectivity of benzylamine could reach 97.08 % when ammonia methanol was used as the solvent. Ni-JKS-600 catalyst is superior to precious metal catalysts (Ru, Pt, Ir, Pd) in aniline selectivity, and is comparable to Raney nickel catalyst, which shows its potential application in industrial production of amines. The catalyst uses cheap and widely available chitin as carbon and nitrogen source, and has the characteristics of green economy with simple preparation method and low cost. It is expected to replace precious metal catalyst for efficient production of benzylamine in the future.","PeriodicalId":346,"journal":{"name":"Journal of Catalysis","volume":"49 12 1","pages":""},"PeriodicalIF":7.3,"publicationDate":"2025-05-30","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144176706","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"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
Tailored and recyclable ppm levels of Pd nanoparticles for chemoselective hydrogenation of nitroarenes in water 定制和可回收的ppm水平的钯纳米粒子的化学选择性氢化硝基芳烃在水中
IF 7.3 1区 化学
Journal of Catalysis Pub Date : 2025-05-30 DOI: 10.1016/j.jcat.2025.116249
Xia Wang, Ming-Hui Su, Jia-Yong Zhou, Jin-Wei Yuan, Liang-Ru Yang, Dong-Pu Zhao, Meng Yan, Ya-Xin Li, Yun-Tao Xia
{"title":"Tailored and recyclable ppm levels of Pd nanoparticles for chemoselective hydrogenation of nitroarenes in water","authors":"Xia Wang, Ming-Hui Su, Jia-Yong Zhou, Jin-Wei Yuan, Liang-Ru Yang, Dong-Pu Zhao, Meng Yan, Ya-Xin Li, Yun-Tao Xia","doi":"10.1016/j.jcat.2025.116249","DOIUrl":"https://doi.org/10.1016/j.jcat.2025.116249","url":null,"abstract":"For the first time, a hitherto unreported green synthesis of anilines by the non-loading type ppm nanopalladium-catalyzed reduction of nitro compounds is described. The reaction and post-treatment purification processes can produce high-purity target products without the use of organic solvents. The catalytic turnover frequency was as high as 27062 h<sup>−1</sup>, which greater than that of the Pd/C catalyst under the same conditions. This even outperforms state-of-the-art Pd-, Pt-, and Ru-based catalysts for the nitrobenzene hydrogenation reported previously. Key to success was the design and utilization of the palladium nanoparticle with strong lipophilicity and highly stable, which permits the ppm palladium-catalyzed selective hydrogenation in water at room temperature without dispersant, providing a general preparation of functionalized anilines in good-to-high yields. The unprecedented high activity of the palladium nanoparticles is attributed to the support, which interacts strongly with the metal to maintain the oxidation–reduction states of the metals and accelerate the reaction. This work avoids the use of phase transfer reagents, as well as strong reductants, organic acids, and high-pressurized hydrogen gas as hydrogen sources, providing a promising concept for developing green catalytic systems. Benefitting from the heterogeneous manner, successful recycling in water of the catalysts was further achieved with high reaction efficiency maintained, and the total palladium leaching was less than 0.1 ppm after five cycles of the catalysts.","PeriodicalId":346,"journal":{"name":"Journal of Catalysis","volume":"33 1","pages":"116249"},"PeriodicalIF":7.3,"publicationDate":"2025-05-30","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144184036","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"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
Rational design of selective catalysts for ethylene hydroformylation via microkinetic modeling and universal neural network potentials 基于微动力学模型和通用神经网络电位的乙烯氢甲酰化选择性催化剂的合理设计
IF 7.3 1区 化学
Journal of Catalysis Pub Date : 2025-05-29 DOI: 10.1016/j.jcat.2025.116253
Kento Sakai, Ippei Furikado, Andrew J. Medford
{"title":"Rational design of selective catalysts for ethylene hydroformylation via microkinetic modeling and universal neural network potentials","authors":"Kento Sakai, Ippei Furikado, Andrew J. Medford","doi":"10.1016/j.jcat.2025.116253","DOIUrl":"https://doi.org/10.1016/j.jcat.2025.116253","url":null,"abstract":"Rapid prediction of the activity and selectivity of catalysts is essential for advancing catalyst development. Computational chemistry offers a promising approach for achieving this aim by enabling such predictions without experimentation. However, traditional methods, such as density functional theory calculations, can be computationally expensive. In this study, we report a descriptor-based microkinetic model that describes the selectivity and activity trends in ethylene hydroformylation on close-packed metal facets using a universal neural network potential. By incorporating adsorbate–adsorbate interactions, our model successfully reproduced the experimental trends in both catalyst activity and selectivity, including the higher production rates of propionaldehyde for Rh and Ir. Furthermore, a high-throughput screening approach was used to evaluate the efficacy of various Rh-based candidates, providing insights into potential improvements through the addition of secondary components. Overall, this study highlights the potential of integrating neural network potentials with microkinetic modeling to advance the rational design of heterogeneous catalysts.","PeriodicalId":346,"journal":{"name":"Journal of Catalysis","volume":"36 1","pages":""},"PeriodicalIF":7.3,"publicationDate":"2025-05-29","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144176708","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"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
Atomically dispersed noble metal-free Cu(I) sites in Ce-MOF-808 with enhanced catalytic hydrogenation performance Ce-MOF-808原子分散无贵金属Cu(I)位点,增强催化加氢性能
IF 6.5 1区 化学
Journal of Catalysis Pub Date : 2025-05-28 DOI: 10.1016/j.jcat.2025.116246
Juan Chen , Linmeng Wang , Hongyi Gao , Rushuo Li , Zhiyuan Liu , Tao Ban , Shunzheng Zhao , Jichao Yang , Ge Wang
{"title":"Atomically dispersed noble metal-free Cu(I) sites in Ce-MOF-808 with enhanced catalytic hydrogenation performance","authors":"Juan Chen ,&nbsp;Linmeng Wang ,&nbsp;Hongyi Gao ,&nbsp;Rushuo Li ,&nbsp;Zhiyuan Liu ,&nbsp;Tao Ban ,&nbsp;Shunzheng Zhao ,&nbsp;Jichao Yang ,&nbsp;Ge Wang","doi":"10.1016/j.jcat.2025.116246","DOIUrl":"10.1016/j.jcat.2025.116246","url":null,"abstract":"<div><div>Single-atom catalysts (SACs) catalysts have unique electronic properties and geometric structures, offering maximum atom-utilization efficiency. Noble metal-free SACs anchored within metal–organic frameworks (MOFs) enable precise tuning of electronic structures and significantly enhance catalytic activity beyond conventional porous materials. Herein, we synthesized the synthesis of Cu(I)/Ce-MOF-808-EA by anchoring atomically dispersed Cu(II) species onto the open Ce<sub>6</sub> nodes of the Ce-MOF-808 framework, followed by in situ reduction to Cu(I) via ethanol treatment and thermal activation processes. The atomic dispersion and valence transformation of Cu sites on Ce-MOF-808 were confirmed by X-ray Absorption Spectroscopy (XAS), high-angle annular dark-field scanning transmission electron microscopy (HAADF-STEM), and X-ray photoelectron spectroscopy (XPS). The resulting Cu(I)/Ce-MOF-808-EA exhibited outstanding catalytic performance for the hydrogenation of Dicyclopentadiene (DCPD), achieving 100 % conversion, 91.54 % selectivity toward Dihydrodicyclopentadiene (DHDCPD), and 8.45 % selectivity toward Tetrahydrodicyclopentadiene (THDCPD) at 100 °C, 2 MPa. Notably, Cu(I)/Ce-MOF-808-EA outperformed other transition metal catalysts (Co/Ce-MOF-808-EA, Ni/Ce-MOF-808-EA and Zn/Ce-MOF-808-EA). For the first time, Density Functional Theory (DFT) calculations, combined with experimental investigations, revealed a low-energy reaction pathway for DCPD hydrogenation, wherein Cu(I) sites, in cooperation with adjacent oxygen atoms, act as bi-active centers to heterolytically cleave H<sub>2</sub> into proton and hydride species (*H<sup>δ+</sup>-H<sup>δ-</sup>) for subsequent hydrogenation. This study underscores the potential of MOFs as versatile platforms for engineering single-atom catalysts with enhanced catalytic properties.</div></div>","PeriodicalId":346,"journal":{"name":"Journal of Catalysis","volume":"450 ","pages":"Article 116246"},"PeriodicalIF":6.5,"publicationDate":"2025-05-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144165016","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"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
Is silicalite-1 inert or reactive towards alkene oligomerization? 硅石-1对烯烃低聚反应是惰性的还是活性的?
IF 6.5 1区 化学
Journal of Catalysis Pub Date : 2025-05-28 DOI: 10.1016/j.jcat.2025.116247
Nibras Hijazi , Jose Luis Cerrillo , Alla Dikhtiarenko , Rushana Khairova , Jorge Gascon
{"title":"Is silicalite-1 inert or reactive towards alkene oligomerization?","authors":"Nibras Hijazi ,&nbsp;Jose Luis Cerrillo ,&nbsp;Alla Dikhtiarenko ,&nbsp;Rushana Khairova ,&nbsp;Jorge Gascon","doi":"10.1016/j.jcat.2025.116247","DOIUrl":"10.1016/j.jcat.2025.116247","url":null,"abstract":"<div><div>Brønsted acid zeolites such as ZSM-5 catalyze alkene oligomerization primarily over strongly acidic bridging hydroxyl groups (Si–OH–Al). Turnover rates of alkene oligomerization have been widely interpreted in terms of the quantity of these bridging hydroxyl groups. In this study, we investigate whether weakly acidic hydroxyl groups such as H-bonded silanol groups catalyze alkene oligomerization. The investigation was based on reacting propene over silicalite-1, a siliceous variant of ZSM-5, at 598–648 K and 0.5 MPa of propene pressure. Results show that vicinal silanols and silanol nests in silicalite-1 catalyze propene oligomerization at mild initial turnover rates (0.0017–0.027 mol mol<sub>SiOH</sub><sup>−1</sup> s<sup>−1</sup>). Results also show that by alkaline treating silicalite-1 silanol nests are healed by reinsertion of dissolved Si species, while new mesopores are formed. These newly formed mesopores shorten diffusion paths to vicinal silanols and lead to significantly improved initial propene oligomerization turnover rates (0.25–0.70 mol mol<sub>SiOH</sub><sup>−1</sup> s<sup>−1</sup>).</div></div>","PeriodicalId":346,"journal":{"name":"Journal of Catalysis","volume":"450 ","pages":"Article 116247"},"PeriodicalIF":6.5,"publicationDate":"2025-05-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144165017","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"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
Microenvironment-coordinated P1CoN3 single-atom sites for selective photocatalytic CO2 reduction to C2 products 微环境配位P1CoN3单原子位点选择性光催化CO2还原为C2产物
IF 6.5 1区 化学
Journal of Catalysis Pub Date : 2025-05-27 DOI: 10.1016/j.jcat.2025.116245
Cheng Huang, Qingshan Wang, Xuping Wei, Guiqing Bai, Junying Tang
{"title":"Microenvironment-coordinated P1CoN3 single-atom sites for selective photocatalytic CO2 reduction to C2 products","authors":"Cheng Huang,&nbsp;Qingshan Wang,&nbsp;Xuping Wei,&nbsp;Guiqing Bai,&nbsp;Junying Tang","doi":"10.1016/j.jcat.2025.116245","DOIUrl":"10.1016/j.jcat.2025.116245","url":null,"abstract":"<div><div>Gaining a comprehensive understanding of the C–C coupling process involving metal active sites and their local coordination environments remains a significant challenge. In this study, we developed a Co<sub>sac</sub>P-CN/MA photocatalyst by incorporating the nonmetal p-block element phosphorus (P) to precisely tailor the coordination environment of individual cobalt (Co) atoms, followed by hybridization with MgAl-LDH. The resulting single-atom catalyst, characterized by a P<sub>1</sub>CoN<sub>3</sub> coordination structure, demonstrates remarkable performance for C<sub>2</sub>H<sub>6</sub> production with nearly 60% selectivity. The asymmetric P<sub>1</sub>CoN<sub>3</sub> single-atom site significantly enhances CO<sub>2</sub> activation, stabilizes CO intermediates, and improves the utilization of photogenerated electrons, offering both thermodynamic and kinetic advantages for the deep reduction of CO<sub>2</sub>. This work offers valuable insights into the precise engineering of the coordination environment of single-atom metal centers to optimize the selective production of C<sub>2</sub> products.</div></div>","PeriodicalId":346,"journal":{"name":"Journal of Catalysis","volume":"450 ","pages":"Article 116245"},"PeriodicalIF":6.5,"publicationDate":"2025-05-27","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144154055","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"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
Machine learning accelerated interfacial fluxionality in Ni-supported metal nitride ammonia synthesis catalysts 机器学习加速了ni负载金属氮氨合成催化剂的界面流动性
IF 7.3 1区 化学
Journal of Catalysis Pub Date : 2025-05-27 DOI: 10.1016/j.jcat.2025.116224
Pranav Roy, Brandon C. Bukowski
{"title":"Machine learning accelerated interfacial fluxionality in Ni-supported metal nitride ammonia synthesis catalysts","authors":"Pranav Roy, Brandon C. Bukowski","doi":"10.1016/j.jcat.2025.116224","DOIUrl":"https://doi.org/10.1016/j.jcat.2025.116224","url":null,"abstract":"The development of energy-efficient catalysts for ammonia synthesis under mild conditions is crucial for reducing the energy demands and carbon footprint of the industrial Haber-Bosch process. In this study, we investigated ammonia synthesis via the associative Mars-van Krevelen (MvK) mechanism using B1-structured metal nitrides, focusing on manganese nitride (MnN) due to its low vacancy formation energy and potential as a metal-support interface. Density functional theory (DFT) calculations identified the MnN (100) facet as the most stable, with a nickel (Ni) nanowire implemented on the surface to facilitate H<sub>2</sub> dissociation while surface nitrogen vacancies activate N<sub>2</sub>. A free energy diagram for Ni-MnN (100) at 400 °C was and a dual-site microkinetic model was developed to determine reaction orders, apparent activation energies and the rate limiting step (RDS). To capture temperature-induced catalyst restructuring, ab initio molecular dynamics (AIMD) simulations and machine learning interatomic potentials (MLPs) were employed to improve the sampling of interfacial active sites over longer timescales. We found significant active site fluxionality leading to active site structural rearrangements that reduced vacancy formation energies. A hydrogen coverage analysis at reaction temperatures revealed coverage-dependent dynamic restructuring of Ni active sites, with lowered free energy change of the RDS that correlates with Ni p-Band center. MLPs were observed to predict coverage-dependent fluxionality with training data exclusive to high coverage regimes. By integrating DFT, AIMD, and MLP-based molecular dynamics, we established a computational framework for understanding dynamic metal-support interactions in transition metal nitride catalysts, demonstrating its applicability not only to ammonia synthesis under mild conditions but also to broader classes of supported catalysts and reactions.","PeriodicalId":346,"journal":{"name":"Journal of Catalysis","volume":"35 1","pages":""},"PeriodicalIF":7.3,"publicationDate":"2025-05-27","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144154057","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"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
Unravelling the mechanism for the mono-alkoxycarbonylation of butadiene: what is the role of the base? 揭示丁二烯单烷氧羰基化的机理:碱的作用是什么?
IF 6.5 1区 化学
Journal of Catalysis Pub Date : 2025-05-22 DOI: 10.1016/j.jcat.2025.116235
Mohammad Ameskal, Lionel Magna, Juan M. Asensio, Pascal Raybaud
{"title":"Unravelling the mechanism for the mono-alkoxycarbonylation of butadiene: what is the role of the base?","authors":"Mohammad Ameskal,&nbsp;Lionel Magna,&nbsp;Juan M. Asensio,&nbsp;Pascal Raybaud","doi":"10.1016/j.jcat.2025.116235","DOIUrl":"10.1016/j.jcat.2025.116235","url":null,"abstract":"<div><div>The mechanism of catalytic alkoxycarbonylation of alkenes has been extensively studied and it is generally accepted that it elapses through three elementary steps: (i) alkene insertion into a Pd<img>H bond, (ii) carbonylation, and (iii) alcoholysis. In the case of butadiene methoxycarbonylation catalyzed by [Pd(d<sup>t</sup>bpx)H]<sup>+</sup>, we have identified the formation of a highly stable Pd(<em>η</em><sup>3</sup>-allyl) intermediate by Density Functional Theory (DFT) calculations and Nuclear Magnetic Resonance (NMR). This intermediate makes the apparent kinetic barrier of the mechanism incompatible with experimental observations (ca. 200 kJ·mol<sup>−1</sup>). Upon coupling DFT calculations and experimental analysis, we proposed a revised mechanism founded on a “base assisted” pathway where the mono-alkoxycarbonylation of dienes exhibits a significantly decreased free energy of activation (ca. 100 kJ mol<sup>−1</sup>). Hence, we proposed that the base coming from the Pd precursor is non-innocent and participates in the reaction upon acting as proton shuttle during the alcoholysis step. By considering various acid/base pairs, we further refined these findings and demonstrated that an optimum balance between the acid and the base must be found, regarding strengths and concentrations, to maximize the catalytic activity.</div></div>","PeriodicalId":346,"journal":{"name":"Journal of Catalysis","volume":"450 ","pages":"Article 116235"},"PeriodicalIF":6.5,"publicationDate":"2025-05-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144122591","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"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
Carbon dioxide hydrogenation to formate catalyzed by highly active Ru-tris(pyrazolyl)methane complexes 高活性ru -三(吡唑基)甲烷配合物催化二氧化碳加氢生成甲酸酯
IF 6.5 1区 化学
Journal of Catalysis Pub Date : 2025-05-21 DOI: 10.1016/j.jcat.2025.116231
Sylwia Kostera , Alberto Gobbo , Massimo Guelfi , Stefano Zacchini , Gabriele Manca , Fabio Marchetti , Luca Gonsalvi
{"title":"Carbon dioxide hydrogenation to formate catalyzed by highly active Ru-tris(pyrazolyl)methane complexes","authors":"Sylwia Kostera ,&nbsp;Alberto Gobbo ,&nbsp;Massimo Guelfi ,&nbsp;Stefano Zacchini ,&nbsp;Gabriele Manca ,&nbsp;Fabio Marchetti ,&nbsp;Luca Gonsalvi","doi":"10.1016/j.jcat.2025.116231","DOIUrl":"10.1016/j.jcat.2025.116231","url":null,"abstract":"<div><div>In the quest for novel, active ruthenium(II) complexes for homogeneous catalytic CO<sub>2</sub> hydrogenation to formate, a small library of cationic Ru(κ<sup>3</sup>-tpm) complexes [tpm = tris(pyrazolyl)methane] bearing different ancillary ligands were tested under various reaction conditions, with and without the addition of a Lewis acid co-catalyst. Under optimized conditions (80 bar, 120 °C) and in the presence of LiOTf, TONs &gt; 54000 were obtained in single batch runs with the complex [RuCl(κ<sup>3</sup>-tpm)(PPh<sub>3</sub>)(CH<sub>3</sub>CN)]Cl (<strong>1</strong>). Mechanistic studies using NMR spectroscopy and DFT calculations were also carried out to elucidate key steps and the energies associated with the reaction pathway, which allowed for the proposal of a catalytic mechanism.</div></div>","PeriodicalId":346,"journal":{"name":"Journal of Catalysis","volume":"450 ","pages":"Article 116231"},"PeriodicalIF":6.5,"publicationDate":"2025-05-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144113524","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"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
0
×
引用
GB/T 7714-2015
复制
MLA
复制
APA
复制
导出至
BibTeX EndNote RefMan NoteFirst NoteExpress
×
提示
您的信息不完整,为了账户安全,请先补充。
现在去补充
×
提示
您因"违规操作"
具体请查看互助需知
我知道了
×
提示
确定
请完成安全验证×
相关产品
×
本文献相关产品
联系我们:info@booksci.cn Book学术提供免费学术资源搜索服务,方便国内外学者检索中英文文献。致力于提供最便捷和优质的服务体验。 Copyright © 2023 布克学术 All rights reserved.
京ICP备2023020795号-1
ghs 京公网安备 11010802042870号
Book学术文献互助
Book学术文献互助群
群 号:481959085
Book学术官方微信