具有新型结构的RuNiCo基催化剂构筑及其催化加氢协同机理研究

提高贵金属利用率，并保证高催化活性、选择性及稳定性是含贵金属催化剂研究的核心问题。本项目提出利用贵金属-过渡金属-过渡金属氢氧化物的协同效应，以炭黑为载体，构筑具有“小岛状钌纳米团簇负载于过渡金属/过渡金属氢氧化物纳米颗粒”新型结构的催化剂，记作Ru/TM/TMOH/C，其中TM为Ni、Co或NiCo；TMOH 为Ni(OH)2、Co(OH)2或Ni(OH)2-Co(OH)2。本项目将研究上述催化剂纳米结构调控规律；以芳烃加氢为模型反应，探究其纳米结构及各表面物种比例与其催化加氢性能的关系；采用程序升温脱附质谱、原位和频光谱与原位同步辐射X射线吸收等技术阐明该新型纳米结构催化剂催化加氢协同效应机理（“多活性位分工协同”或“界面电子效应协同机制”）。本研究将为合成低成本、高效率、高稳定性、多元金属协同的加氢催化剂提供理论依据和技术支持，也可丰富多元金属催化基础理论，具有重要的理论与应用价值。

The core problem in the research of catalysts containing noble metal is to improve the utilization efficiency of precious metal and keep their high catalytic performance, selectivity and stability. In this project, it is proposed to effectively use the synergetic effect among noble metal - transition metal - transition metal hydroxide related species, and the catalyst with the novel structure - Ru nanoclusters islands supported on transition metal/transition metal hydroxides nanoparticles is constructed, using carbon black as catalyst support, denoted as Ru/TM/TMOH/C, where TM = Ni, Co or NiCo; TMOH = Ni(OH)2, Co(OH)2 or Ni(OH)2-Co(OH)2. The principle of regulating nanostructure of above-mentioned catalysts is investigated; with the hydrogenation of aromatics as the model reaction, the relationship between their nanostructures as well as the ratio of surface species and their catalytic performance in aromatic hydrogenation is explored; the accurate mechanism of synergetic effect (“mechanism of specialization and cooperation of multiple active sites” or “synergetic effect of interface electrons”) in the catalyst with novel nanostructure for hydrogenation reaction is further illustrated by such techniques as temperature programmed desorption mass spectrometry (TPD-MS), in-situ sum frequency generation vibrational spectroscopy (in-situ SFG) and in-situ synchrotron radiation X-ray absorption (in-situ XAS). This study can serve as theoretical basis and technical support for the synthesis of low-cost novel multi-metallic synergetic hydrogenation catalysts with high catalytic performance and selectivity, and also enrich the fundamental theory of multi-metallic catalysis, and thus has significant values in theory and applications.