One-Dimensional van der Waals Heterostructures as Efficient Metal-Free Oxygen Electrocatalysts

材料科学 异质结 金属 氧气 纳米技术 范德瓦尔斯力 化学物理 光电子学 化学 有机化学 分子 冶金
作者
Chang Liu,Fei Liu,Hao Li,Junsheng Chen,Jingyuan Fei,Zixun Yu,Ziwen Yuan,Chaojun Wang,Huiling Zheng,Zongwen Liu,Meiying Xu,Graeme Henkelman,Li Wei,Yuan Chen
出处
期刊:ACS Nano [American Chemical Society]
卷期号:15 (2): 3309-3319 被引量:117
标识
DOI:10.1021/acsnano.0c10242
摘要

Two-dimensional covalent organic frameworks (2D-COFs) may serve as an emerging family of catalysts with well-defined atomic structures. However, the severe stacking of 2D nanosheets and large intrinsic bandgaps significantly impair their catalytic performance. Here, we report coaxial one-dimensional van der Waals heterostructures (1D vdWHs) comprised of a carbon nanotube (CNT) core and a thickness tunable thienothiophene-pyrene COF shell using a solution-based in situ wrapping method. Density functional theory calculations and operando and ex situ spectroscopic analysis indicate that carbon–sulfur regions in thienothiophene groups in the COF serve as an active catalytic site for oxygen reduction and evolution reactions. The coaxial structure enables n-doping from the CNT core to the COF shell, which is controllable by varying COF shell thickness. The charge transfer from CNTs lowers COF's bandgap and work function, which reduces the charge transfer barrier between the active catalytic sites and adsorbed oxygen intermediates, resulting in dramatically enhanced catalytic activity. The 1D vdWHs were applied as a bifunctional oxygen electrocatalyst in rechargeable zinc–air batteries, delivering a high specific capacity of 696 mAh gZn–1 under a high current density of 40 mA cm–2 and excellent cycling stability. The 1D vdWHs based on the coaxial structure of 2D COF wrapped around CNT cores may be further used as versatile building units to create multidimensional vdWHs for exploring fundamental physics and chemistry as well as practical applications in electrochemistry, electronics, photonics, and beyond.
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