Lin Yifan, Wan Hao, Wu Dan, Chen Gen, Zhang Ning, Liu Xiaohe, Li Junhui, Cao Yijun, Qiu Guanzhou, Ma Renzhi
Henan Province Industrial Technology Research Institute of Resources and Materials, Zhengzhou University, Zhengzhou, Henan 450001, People's Republic of China.
International Center for Materials Nanoarchitectonics, National Institute for Materials Science, Namiki 1-1, Tsukuba, Ibaraki 305-0044, Japan.
J Am Chem Soc. 2020 Apr 22;142(16):7317-7321. doi: 10.1021/jacs.0c01916. Epub 2020 Apr 9.
Rational design and bottom-up synthesis based on the structural topology is a promising way to obtain two-dimensional metal-organic frameworks (2D MOFs) in well-defined geometric morphology. Herein, a topology-guided bottom-up synthesis of a novel hexagonal 2D MOF nanoplate is realized. The hexagonal channels constructed via the distorted (3,4)-connected Ni(BDC)(DABCO) (BDC = 1,4-benzenedicarboxylic acid, DABCO = 1,4-diazabicyclo[2.2.2]octane) framework serve as the template for the specifically designed morphology. Under the inhibition and modulation of pyridine through a substitution-suppression process, the morphology can be modified from hexagonal nanorods to nanodisks and to nanoplates with controllable thickness tuned by the dosage of pyridine. Subsequent pyrolysis treatment converts the nanoplates into a N-doped Ni@carbon electrocatalyst, which exhibits a small overpotential as low as 307 mV at a current density of 10 mA cm in the oxygen evolution reaction.
基于结构拓扑的合理设计和自下而上的合成是获得具有明确几何形态的二维金属有机框架（2D MOF）的一种有前途的方法。在此，实现了一种拓扑引导的自下而上合成新型六边形2D MOF纳米片的方法。通过扭曲的（3,4）连接的Ni（BDC）（DABCO）（BDC = 1,4-苯二甲酸，DABCO = 1,4-二氮杂双环[2.2.2]辛烷）框架构建的六边形通道作为特定设计形态的模板。在吡啶通过取代抑制过程的抑制和调节下，形态可以从六边形纳米棒转变为纳米盘，再到通过吡啶用量可控制厚度的纳米片。随后的热解处理将纳米片转化为N掺杂的Ni@碳电催化剂，该催化剂在析氧反应中，在电流密度为10 mA cm时表现出低至307 mV的小过电位。
