School of Chemistry and Chemical Engineering, Institute for Energy Research, Jiangsu University, Zhenjiang 212013, China.
Chemical Sciences Division, Oak Ridge National Laboratory, Oak Ridge, Tennessee 37831, USA.
Nat Commun. 2017 Jun 9;8:15291. doi: 10.1038/ncomms15291.
Taming interfacial electronic effects on Pt nanoparticles modulated by their concomitants has emerged as an intriguing approach to optimize Pt catalytic performance. Here, we report Pt nanoparticles assembled on vacancy-abundant hexagonal boron nitride nanosheets and their use as a model catalyst to embrace an interfacial electronic effect on Pt induced by the nanosheets with N-vacancies and B-vacancies for superior CO oxidation catalysis. Experimental results indicate that strong interaction exists between Pt and the vacancies. Bader charge analysis shows that with Pt on B-vacancies, the nanosheets serve as a Lewis acid to accept electrons from Pt, and on the contrary, when Pt sits on N-vacancies, the nanosheets act as a Lewis base for donating electrons to Pt. The overall-electronic effect demonstrates an electron-rich feature of Pt after assembling on hexagonal boron nitride nanosheets. Such an interfacial electronic effect makes Pt favour the adsorption of O, alleviating CO poisoning and promoting the catalysis.
通过调控 Pt 纳米粒子的伴随物来驯服界面电子效应对优化 Pt 催化性能来说是一种很有吸引力的方法。在这里,我们报告了在富含空位的六方氮化硼纳米片上组装的 Pt 纳米粒子,并将其用作模型催化剂,以接受由具有 N 空位和 B 空位的纳米片诱导的 Pt 界面电子效应,从而实现对 CO 氧化的优异催化。实验结果表明,Pt 与空位之间存在强烈的相互作用。Bader 电荷分析表明,当 Pt 在 B 空位上时,纳米片作为路易斯酸从 Pt 接受电子,相反,当 Pt 位于 N 空位上时,纳米片作为路易斯碱向 Pt 提供电子。整体电子效应表明,Pt 在组装到六方氮化硼纳米片上后具有富电子的特征。这种界面电子效应使得 Pt 有利于 O 的吸附,减轻 CO 的中毒,并促进催化。