ABSTRACT
The surging demand for environmental-friendly and safe electrochemical energy storage systems has driven the development of aqueous zinc (Zn)-ion batteries (ZIBs). However, metallic Zn anodes suffer from severe dendrite growth and large volume change, resulting in a limited lifetime for aqueous ZIB applications. Here, it is shown that 3D mesoporous carbon (MC) with controlled carbon and defect configurations can function as a highly reversible and dendrite-free Zn host, enabling the stable operation of aqueous ZIBs. The MC host has a structure-controlled architecture that contains optimal sp2 -carbon and defect sites, which results in an improved initial nucleation energy barrier and promotes uniform Zn deposition. As a consequence, the MC host shows outstanding Zn plating/stripping performance over 1000 cycles at 2 mA cm-2 and over 250 cycles at 6 mA cm-2 in asymmetric cells. Density functional theory calculations further reveal the role of the defective sp2 -carbon surface in Zn adsorption energy. Moreover, a full cell based on Zn@MC900 anode and V2 O5 cathode exhibits remarkable rate performance and cycling stability over 3500 cycles. These results establish a structure-mechanism-performance relationship of the carbon host as a highly reversible Zn anode for the reliable operation of ZIBs.
ABSTRACT
To date, carbon-based materials including various carbon nanostructured materials have been extensively used as an electrocatalyst support for proton exchange membrane fuel cell (PEMFC) applications due to their practical nature. However, carbon dissolution or corrosion caused by high electrode potential in the presence of O2 and/or water has been identified as one of the main failure modes for the device operation. Here, we report the first TiN nanofiber (TNF)-based nonwoven structured materials to be constructed via electrospinning and subsequent two-step thermal treatment processes as a support for the PEMFC catalyst. Pt catalyst nanoparticles (NPs) deposited on the TNFs (Pt/TNFs) were electrochemically characterized with respect to oxygen reduction reaction (ORR) activity and durability in an acidic medium. From the electrochemical tests, the TNF-supported Pt catalyst was better and more stable in terms of its catalytic performance compared to a commercially available carbon-supported Pt catalyst. For example, the initial oxygen reduction performance was comparable for both cases, while the Pt/TNF showed much higher durability from an accelerated degradation test (ADT) configuration. It is understood that the improved catalytic roles of TNFs on the supported Pt NPs for ORR are due to the high electrical conductivity arising from the extended connectivity, high inertness to the electrochemical environment and strong catalyst-support interactions.
