{"title":"固定在富含吡啶 N 的碳纳米片上的钯纳米颗粒用于促进铃木交叉偶联反应。","authors":"Shihao Cui, Dejian Xu, Zhiyuan Wang, Libo Wang, Yikun Zhao, Wei Deng, Qingshan Zhao, Mingbo Wu","doi":"10.3390/nano14211690","DOIUrl":null,"url":null,"abstract":"<p><p>Palladium (Pd) catalysts play a crucial role in facilitating Suzuki cross-coupling reactions for the synthesis of valuable organic compounds. However, conventional heterogeneous Pd catalysts often encounter challenges such as leaching and deactivation during reactions, leading to reduced catalytic efficiency. In this study, we employed an innovative intercalation templating strategy to prepare two-dimensional carbon nanosheets with high nitrogen doping derived from petroleum asphalt, which were utilized as a versatile support for immobilizing Pd nanoparticles (Pd/N-CNS) in efficient Suzuki cross-coupling reactions. The results indicate that the anchoring effect of high-pyridinic N species on the two-dimensional carbon nanosheets enhances interactions between Pd and the support, effectively improving both the dispersibility and stability of the Pd nanoparticles. Notably, the Pd/N-CNS catalyst achieved an overall turnover frequency (TOF) of 2390 h<sup>-1</sup> for the Suzuki cross-coupling reaction under mild conditions, representing approximately a nine-fold increase in activity compared to commercial Pd/C catalysts. Furthermore, this catalyst maintained an overall TOF of 2294 h<sup>-1</sup> even after five reaction cycles, demonstrating excellent stability. Theoretical calculations corroborate these observed enhancements in catalytic performance by attributing them to improved electron transfer from Pd to the support facilitated by abundant pyridinic N species. This work provides valuable insights into feasible strategies for developing efficient catalysts aimed at sustainable production of biaromatic compounds.</p>","PeriodicalId":18966,"journal":{"name":"Nanomaterials","volume":"14 21","pages":""},"PeriodicalIF":4.4000,"publicationDate":"2024-10-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.ncbi.nlm.nih.gov/pmc/articles/PMC11548024/pdf/","citationCount":"0","resultStr":"{\"title\":\"Pd Nanoparticles Immobilized on Pyridinic N-Rich Carbon Nanosheets for Promoting Suzuki Cross-Coupling Reactions.\",\"authors\":\"Shihao Cui, Dejian Xu, Zhiyuan Wang, Libo Wang, Yikun Zhao, Wei Deng, Qingshan Zhao, Mingbo Wu\",\"doi\":\"10.3390/nano14211690\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"<p><p>Palladium (Pd) catalysts play a crucial role in facilitating Suzuki cross-coupling reactions for the synthesis of valuable organic compounds. 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Furthermore, this catalyst maintained an overall TOF of 2294 h<sup>-1</sup> even after five reaction cycles, demonstrating excellent stability. Theoretical calculations corroborate these observed enhancements in catalytic performance by attributing them to improved electron transfer from Pd to the support facilitated by abundant pyridinic N species. 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引用次数: 0
摘要
钯(Pd)催化剂在促进合成有价值有机化合物的铃木交叉偶联反应中发挥着至关重要的作用。然而,传统的异质钯催化剂经常会在反应过程中遇到浸出和失活等难题,导致催化效率降低。在本研究中,我们采用了一种创新的插层模板策略,从石油沥青中制备出高氮掺杂的二维碳纳米片,并将其作为固定钯纳米颗粒(Pd/N-CNS)的多功能载体,用于高效的铃木交叉偶联反应。研究结果表明,二维碳纳米片上的高吡啶基 N 物种的锚定效应增强了 Pd 与支撑物之间的相互作用,从而有效提高了 Pd 纳米粒子的分散性和稳定性。值得注意的是,在温和条件下,Pd/N-CNS 催化剂进行铃木交叉偶联反应的总周转频率 (TOF) 达到 2390 h-1,与商用 Pd/C 催化剂相比,活性提高了约九倍。此外,这种催化剂在经过五个反应循环后仍能保持 2294 h-1 的总体 TOF,显示出极佳的稳定性。理论计算证实了所观察到的催化性能的提高,并将其归因于丰富的吡啶 N 物种促进了电子从钯到载体的转移。这项工作为开发高效催化剂的可行策略提供了宝贵的见解,从而实现生物芳香化合物的可持续生产。
Pd Nanoparticles Immobilized on Pyridinic N-Rich Carbon Nanosheets for Promoting Suzuki Cross-Coupling Reactions.
Palladium (Pd) catalysts play a crucial role in facilitating Suzuki cross-coupling reactions for the synthesis of valuable organic compounds. However, conventional heterogeneous Pd catalysts often encounter challenges such as leaching and deactivation during reactions, leading to reduced catalytic efficiency. In this study, we employed an innovative intercalation templating strategy to prepare two-dimensional carbon nanosheets with high nitrogen doping derived from petroleum asphalt, which were utilized as a versatile support for immobilizing Pd nanoparticles (Pd/N-CNS) in efficient Suzuki cross-coupling reactions. The results indicate that the anchoring effect of high-pyridinic N species on the two-dimensional carbon nanosheets enhances interactions between Pd and the support, effectively improving both the dispersibility and stability of the Pd nanoparticles. Notably, the Pd/N-CNS catalyst achieved an overall turnover frequency (TOF) of 2390 h-1 for the Suzuki cross-coupling reaction under mild conditions, representing approximately a nine-fold increase in activity compared to commercial Pd/C catalysts. Furthermore, this catalyst maintained an overall TOF of 2294 h-1 even after five reaction cycles, demonstrating excellent stability. Theoretical calculations corroborate these observed enhancements in catalytic performance by attributing them to improved electron transfer from Pd to the support facilitated by abundant pyridinic N species. This work provides valuable insights into feasible strategies for developing efficient catalysts aimed at sustainable production of biaromatic compounds.
期刊介绍:
Nanomaterials (ISSN 2076-4991) is an international and interdisciplinary scholarly open access journal. It publishes reviews, regular research papers, communications, and short notes that are relevant to any field of study that involves nanomaterials, with respect to their science and application. Thus, theoretical and experimental articles will be accepted, along with articles that deal with the synthesis and use of nanomaterials. Articles that synthesize information from multiple fields, and which place discoveries within a broader context, will be preferred. There is no restriction on the length of the papers. Our aim is to encourage scientists to publish their experimental and theoretical research in as much detail as possible. Full experimental or methodical details, or both, must be provided for research articles. Computed data or files regarding the full details of the experimental procedure, if unable to be published in a normal way, can be deposited as supplementary material. Nanomaterials is dedicated to a high scientific standard. All manuscripts undergo a rigorous reviewing process and decisions are based on the recommendations of independent reviewers.