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负载钯催化的Suzuki偶联反应研究进展 总被引:4,自引:0,他引:4
负载钯催化的Suzuki偶联反应,由于产物易分离、催化剂可重复使用,已引起人们的广泛关注.综述了近年来负载钯催化的Suzuki偶联反应研究进展,载体包括活性碳、金属氧化物、硅铝酸盐微孔分子筛、二氧化硅材料、活性粘土和聚合物等. 相似文献
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以修饰的Hummers法制备的氧化石墨烯为载体,席夫碱为配体制备了一种新型的负载型钯催化剂,采用红外光谱仪、透射电镜、X射线光电子能谱仪、热重分析仪和X射线衍射仪等手段对负载型催化剂进行了表征,并评价了其对水相Suzuki反应的催化活性.结果表明,该催化剂在较温和的实验条件下即可高效催化水相芳基卤与芳基硼酸的Suzuki反应,催化剂重复使用5次后,活性基本不变. 相似文献
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《有机化学》2015,(8)
为解决均相钯催化剂难于分离回收及循环使用问题,发展了一种廉价易行的方法合成易于原位磁分离回收的磁性纳米粒子(MNPs)负载钯催化剂Fe3O4@MOPPA-Pd.该催化剂可高效催化卤代苯的Suzuki反应及Heck反应,且对Suzuki偶联反应具有尤其高的催化活性,在温和条件下,10 mg Fe3O4@MOPPA-Pd可催化300 mmol溴苯与苯硼酸的偶联反应,联苯的分离收率达98%,转化数(TON)及转化率(TOF)分别高达77052和51368 h-1.此外,Fe3O4@MOPPA-Pd可在外加磁场存在下由反应体系中方便分离回收,循环使用4次以上催化活性无明显降低. 相似文献
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Palladium Nanoparticles Embedded into Graphene Nanosheets: Preparation,Characterization, and Nonenzymatic Electrochemical Detection of H2O2 下载免费PDF全文
A novel nonenzymatic H2O2 sensor based on a palladium nanoparticles/graphene (Pd‐NPs/GN) hybrid nanostructures composite film modified glassy carbon electrode (GCE) was reported. The composites of graphene (GN) decorated with Pd nanoparticles have been prepared by simultaneously reducing graphite oxide (GO) and K2PdCl4 in one pot. The Pd‐NPs were intended to enlarge the interplanar spacing of graphene nanosheets and were well dispersed on the surface or completely embedded into few‐layer GN, which maintain their high surface area and prevent GN from aggregating. XPS analysis indicated that the surface Pd atoms are negatively charged, favoring the reduction process of H2O2. Moreover, the Pd‐NPs/GN/GCE could remarkably decrease the overpotential and enhance the electron‐transfer rate due to the good contact between Pd‐NPs and GN sheets, and Pd‐NPs have high catalytical effect for H2O2 reduction. Amperometric measurements allow observation of the electrochemical reduction of H2O2 at 0.5 V (vs. Ag/AgCl). The H2O2 reduction current is linear to its concentration in the range from 1×10?9 to 2×10?3 M, and the detection limit was found to be 2×10?10 M (S/N=3). The as‐prepared nonenzymatic H2O2 sensor exhibits excellent repeatability, selectivity and long‐term stability. 相似文献
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Low‐Coordinated Edge Sites on Ultrathin Palladium Nanosheets Boost Carbon Dioxide Electroreduction Performance 下载免费PDF全文
Wenjin Zhu Lei Zhang Piaoping Yang Congling Hu Zhibin Luo Xiaoxia Chang Prof. Dr. Zhi‐Jian Zhao Prof. Dr. Jinlong Gong 《Angewandte Chemie (International ed. in English)》2018,57(36):11544-11548
Electrochemical conversion of carbon dioxide (CO2) to value‐added products is a possible way to decrease the problems resulting from CO2 emission. Thanks to the eminent conductivity and proper adsorption to intermediates, Pd has become a promising candidate for CO2 electroreduction (CO2ER). However, Pd‐based nanocatalysts generally need a large overpotential. Herein we describe that ultrathin Pd nanosheets effectively reduce the onset potential for CO by exposing abundant atoms with comparatively low generalized coordination number. Hexagonal Pd nanosheets with 5 atomic thickness and 5.1 nm edge length reached CO faradaic efficiency of 94 % at ?0.5 V, without any decay after a stability test of 8 h. It appears to be the most efficient among all of Pd‐based catalysts toward CO2ER. Uniform hexagonal morphology made it reasonable to build models and take DFT calculations. The enhanced activity originates from mainly edge sites on palladium nanosheets. 相似文献
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Dr. Fei Wang Yanshuai Bi Kai Hu Dr. Xuejiao Wei 《Chemistry (Weinheim an der Bergstrasse, Germany)》2020,26(21):4874-4879
A catalyst in which Pd nanoparticles are supported on triangle-shaped La2O2CO3 nanosheets exposing predominantly the (001) planes (Pd/La2O2CO3-TNS; where TNS denotes triangular nanosheets) was prepared by a facile solvothermal method. The Pd/La2O2CO3-TNS catalysts exhibited excellent catalytic activity and recycling stability for hydrogenation of cinnamaldehyde to hydrocinnamaldehyde with turnover frequency of up to 41 238 h−1. This enhanced activity of Pd/La2O2CO3-TNS results from strong metal–support interactions. Structure analysis and characterization demonstrated that surface-oxygen-enriched La2O2CO3-TNS supports exposing (001) planes are beneficial to charge transfer between the Pd nanoparticles and triangle-shaped La2O2CO3 nanosheets and increase the electron density of Pd. Moreover, the modulated electronic states of the Pd/La2O2CO3-TNS catalysts can enhance the adsorption and activation of hydrogen to enhance the hydrogenation activity. 相似文献
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Chenghui Zhang Pengjuan Ni Bo Wang Wendong Liu Yuanyuan Jiang Chuanxia Chen Jian Sun Yizhong Lu 《中国化学快报》2022,33(2):757-761
The undesirable enzymatic activity of nanozymes under near neutral p H condition and the traditional single signal output always restrict the analytical application of nanozyme-based biosensors.Herein,graphitic carbon nitride nanosheets supported palladium nanosheets composite (Pd/g-C3N4) with both oxidase-like activity and fluorescent property is synthesized.Notably,Pd/g-C3N4exhibits enhanced oxidase-like activity compared to Pd NSs under p H 7.4.By c... 相似文献
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Ekaterina S. Lokteva Vera V. Shishova Nikolay N. Tolkachev Andrey N. Kharlanov Konstantin I. Maslakov Alexey O. Kamaev Igor Yu. Kaplin Irina N. Savina Elena V. Golubina 《Molecules (Basel, Switzerland)》2021,26(1)
A mesoporous support based on silica and zirconia (ZS) was used to prepare monometallic 1 wt% Pd/ZS, 10 wt% Fe/ZS, and bimetallic FePd/ZS catalysts. The catalysts were characterized by TPR-H2, XRD, SEM-EDS, TEM, AAS, and DRIFT spectroscopy of adsorbed CO after H2 reduction in situ and tested in hydrodechlorination of environmental pollutant 4-chlorophelol in aqueous solution at 30 °C. The bimetallic catalyst demonstrated an excellent activity, selectivity to phenol and stability in 10 consecutive runs. FePd/ZS has exceptional reducibility due to the high dispersion of palladium and strong interaction between FeOx and palladium, confirmed by TPR-H2, DRIFT spectroscopy, XRD, and TEM. Its reduction occurs during short-time treatment with hydrogen in an aqueous solution at RT. The Pd/ZS was more resistant to reduction but can be activated by aqueous phenol solution and H2. The study by DRIFT spectroscopy of CO adsorbed on Pd/ZS reduced in harsh (H2, 330 °C), medium (H2, 200 °C) and mild conditions (H2 + aqueous solution of phenol) helped to identify the reasons of the reducing action of phenol solution. It was found that phenol provided fast transformation of Pd+ to Pd0. Pd/ZS also can serve as an active and stable catalyst for 4-PhCl transformation to phenol after proper reduction. 相似文献
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《Journal of molecular catalysis. A, Chemical》2007,261(1):29-35
In this study, palladium silicide was formed on the sol–gel derived SiO2 supported Pd catalysts when they were prepared by ion-exchange method using Pd(NH3)4Cl2 as a palladium precursor. No other palladium phases (PdO or Pd0) were evident after calcinations at 450 °C for 3 h. The Pd/SiO2 catalysts with Pd silicide formation were found to exhibit superior performance than commercial SiO2 supported ones in liquid-phase semihydrogenation of phenylacetylene. From XPS results, the binding energy of Pd 3d of palladium silicide on the Pd/SiO2 catalyst shifted toward larger binging energy, indicating that Pd is electron deficient. This could probably result in an inhibition of a product styrene on the Pd surface and hence high styrene selectivities were obtained at high phenylacetylene conversions. The formation of Pd silicide, however, did not have much impact on specific activity of the Pd catalysts since the TOFs were quite similar among the various catalysts with or without palladium silicides if their average particle sizes were large enough. The TOFs decreased by an order of magnitude when palladium dispersion was very high and their average particle sizes were smaller than 3–5 nm. 相似文献
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A novel palladium catalyst immobilized on polyacrylonitrile fiber mats (Pd/PAN) was prepared by electrospinning. The catalytic activity and recyclability of the microwave‐assisted Pd/PAN fiber mats were examined for the Mizoroki–Heck cross‐coupling of aryl iodides with three different acrylates in aqueous solution. The morphology of the prepared Pd/PAN fiber mats was characterized by scanning electron microscopy. The large size of the PAN fiber mat‐supported palladium catalyst enables much easier separation from the reaction mixture by simple filtration. Density functional theory calculation indicates that the chelation energy of palladium chloride (PdCl2) with propionitrile (model of PAN) is considerable smaller than that of PdCl2 with water, suggesting that the stability and reactivity of the Pd/PAN fiber mats catalyst could be improved through the surface derivatization with polar functional groups. Copyright © 2011 John Wiley & Sons, Ltd. 相似文献
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SBA-15负载Pd催化剂的制备及其在Heck反应中的应用研究 总被引:2,自引:0,他引:2
利用水热反应制备了表面离子液体功能化的SBA-15介孔材料,在丙酮溶液中与氯化钯反应,然后使用水合肼在乙醇中还原.测试了这种催化剂在Mizoroki-Heck反应中的催化活性.与直接负载在SBA-15上的钯催化剂相比,这种表面修饰的介孔SBA-15负载催化剂表现出更高的催化活性、可回收性和反应稳定性.氮气吸脱附实验和小角XRD衍射实验表明,在合成中,材料的介孔性能并没有被破坏.透视电镜也表征了该材料的表面形貌.最后,Mizoroki-Heck反应表明该催化剂具有很高的催化活性,且循环五次后,其催化活性降低并不明显. 相似文献
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A 10 w/o Pd/C catalyst from Johnson Matthey has been examined by three different techniques: chemisorption, line broadening of X-ray diffraction, and TEM (transmission electron microscopy) to investigate the size of the palladium crystallites. The dispersion of this catalyst was determined to be 20%. Among these techniques, the X-ray diffraction was found to be the most convenient method. Through this method, the dispersion of Pd was found to decrease on catalyzing hydroxylamine reactions at 330 K. The deactivation of Pd/C for these reactions was correlated to the sintering of palladium. H2 chemisorption at 373 K was found to be a good way to accurately measure the number of active palladium sites in the Pd/C catalysts. 相似文献