Su Fabing, Lv Lu, Lee Fang Yin, Liu Tao, Cooper Andrew I, Zhao Xiu Song
Department of Chemical and Biomolecular Engineering, National University of Singapore, 4 Engineering Drive 4, Singapore 117576.
J Am Chem Soc. 2007 Nov 21;129(46):14213-23. doi: 10.1021/ja072697v. Epub 2007 Oct 31.
We report here a thermal reduction method for preparing Ru catalysts supported on a carbon substrate. Mesoporous SBA-15 silica, surface-carbon-coated SBA-15, templated mesoporous carbon, activated carbon, and carbon black with different pore structures and compositions were employed as catalyst supports to explore the versatility of the thermal reduction method. Nitrogen adsorption, X-ray diffraction, field-emission scanning electron microscopy, transmission electron microscopy, scanning transmission electron microscopy, thermogravimetric analysis, and X-ray absorption near-edge structure techniques were used to characterize the samples. It was observed that carbon species that could thermally reduce Ru species at high temperatures played a vital role in the reduction process. Ru nanoparticles supported on various carbon-based substrates exhibited good dispersion with an appropriate particle size, high crystallinity, strong resistance against oxidative atmosphere, less leaching, lack of aggregation, and avoidance of pore blocking. As such, these catalysts display a remarkably high catalytic activity and stability in the hydrogenation of benzene and toluene (up to 3-24-fold compared with Ru catalysts prepared by traditional methods). It is believed that the excellent catalytic performance of the thermally reduced Ru nanoparticles is related to the intimate interfacial contact between the Ru nanoparticles and the carbon support.
我们在此报告一种用于制备负载在碳载体上的钌催化剂的热还原方法。使用具有不同孔结构和组成的介孔SBA-15二氧化硅、表面碳包覆的SBA-15、模板介孔碳、活性炭和炭黑作为催化剂载体,以探索热还原方法的通用性。采用氮气吸附、X射线衍射、场发射扫描电子显微镜、透射电子显微镜、扫描透射电子显微镜、热重分析和X射线吸收近边结构技术对样品进行表征。观察到在高温下能够热还原钌物种的碳物种在还原过程中起着至关重要的作用。负载在各种碳基载体上的钌纳米颗粒表现出良好的分散性,具有合适的粒径、高结晶度、对氧化气氛的强抗性、较少的浸出、无团聚以及避免孔堵塞。因此,这些催化剂在苯和甲苯的氢化反应中表现出非常高的催化活性和稳定性(与通过传统方法制备的钌催化剂相比高达3至24倍)。据信,热还原的钌纳米颗粒优异的催化性能与钌纳米颗粒和碳载体之间紧密的界面接触有关。