Thursday, 2 June 2022: 09:00
West Meeting Room 218 (Vancouver Convention Center)
Controllable synthesis of graphene-coated metal nanoparticles (NPs) presents a big challenge because the shell thickness plays a key role in activity of these catalysts. Herein, we use silica as a radical sieve to grow graphene over cobalt NPs via chemical vapor deposition. As-prepared single-layer graphene-coated cobalt NPs with and without N doping (Co@N-SG and Co@SG) exhibit noticeable oxygen evolution reaction (OER) activity of 316 and 334 mV, respectively at a current density of 10 mA cm-2. Furthermore, a magnet-assisted binder-free Co@N-SG electrode illustrates much improved OER activity and stability over conventional binder-assisted counterparts, suggesting this as an effective way to overcome the recognized issues of high electron transfer resistance and poor adhesion of binder-based electrodes in practical applications. Interestingly, the graphene shell possesses varying defects and major OER active sites are found around the defects in the shell. On the other hand, separately isolated Co@SG with a defect-free shell, despite exhibiting a slightly lower initial activity, illustrates a much-improved durable OER performance. The underlying Co affects the electron density of the graphene shell through dipole interaction and the electron density is optimized for adsorption of reaction intermediates, hence accelerating OER performance. This work will provide new clues to design efficient and durable electrocatalysts with further enhanced OER performance.