Vertical Growth of 2D Covalent Organic Framework Nanoplatelets on a Macroporous Scaffold for High-Performance Electrodes.

Abstract

Hierarchically structural engineering of electrodes is critical to achieving high energy density and high power density in electrochemical energy storage (EES). However, rational regulation of the mesoscopic structure that coordinates microscopic and macroscopic structural features simultaneously remains a significant challenge. Here, the construction of electrodes with well-defined hierarchical pores spanning multiple length scales from 1nm to 50µm is reported. Vertically aligned 2D covalent organic framework (COF) nanoplatelets with a thickness around 30nm are insitu grown on macroporous graphene aerogel scaffold by a reversible polycondensation-termination strategy. The obtained electrode thus combines abundant accessible active sites and efficient transport expressways for both ions and electrons. When used for supercapacitors, a superior gravimetric capacitance of 289Fg-1 as well as outstanding capacitance retention at both high charge/discharge rates of 77% from 0.5to 50Ag-1 and high mass loading of 74% from 1.2to 10.4mgcm-2 are achieved. Hierarchical engineering of mesostructured 2D COF units on the macroporous scaffold will bring unprecedented structural designability and performance enhancement for EES electrodes.