利用杂原子调控纳米碳材料催化剂催化能力的初步探索  

Computational exploration on effects of heteroatom doping for nanostructured carbon catalysts

作　　者：李波[1] 苏党生[1] 

机构地区：[1]中国科学院金属研究所沈阳材料科学国家(联合)实验室,辽宁沈阳110016

出　　处：《化工学报》2014年第7期2657-2667,共11页CIESC Journal

基　　金：中国科学院金属研究所资助项目(Y3NBA211A1);国家自然科学基金项目(21133010;51221264;21261160487);国家重点基础研究发展计划项目(2011CBA00504);中国科学院战略先导项目(XDA09030103)~~

摘　　要：纳米碳材料已经成为一类重要的非金属催化剂。通过在纳米碳材料催化剂中引入杂原子可以有效地改变催化剂的性能。通过3个研究实例分别说明了杂原子硼和氮在甲烷部分氧化、氧化脱氢反应中乙烯选择性和乙炔卤化反应中的作用和机理。通过研究表明硼和氮杂原子可以优化纳米碳材料的催化效果,改变催化剂的电子结构和酸碱性,揭示了碳材料与金属催化剂的不同作用机理。当前计算结果可为进一步提高纳米碳材料催化剂催化能力奠定基础。Nanostructured carbon materials have become an important class of non-metal catalysts. One of the effective ways to tailor the properties of nanostructured carbon catalysts is heteroatoms doping. In the current study, three cases were selected to demonstrate the effects of heteroatoms doping with boron or nitrogen. They were partial oxidation of methane, selectivity in oxidative dehydrogenation reaction, and halogenation of acetylene. Computational studies revealed that doping did enhance the catalytic capabilities of nanostructured carbon catalysts. Moreover it could modulate the electronic structure and acidfbase properties of the catalysts. The reaction mechanism was different from metal catalyst. Overall, the current study is crucial for the further development of nanostructured carbon catalysts and sheds light on the new strategy for optimization of catalytic performance.

关 键 词：计算化学 部分氧化 催化剂活化 纳米碳材料 杂原子 

分 类 号：O643.3[理学—物理化学]