Recycling valuable cobalt from spent lithium ion batteries for controllably designing a novel sea-urchin-like cobalt nitride-graphene hybrid catalyst: towards efficient overall water splitting

Abstract

Abstract Along with the continuous consumption in lithium-ion batteries (LIBs), the price of cobalt is inevitably going up in recent years. Therefore, recycling valuable Co element from spent devices, and boosting its service efficiency are becoming two indispensable approaches to promote the utilization of Co in various energy conversion/storage devices. Herein, we realize the recovery of Co from spent LIBs and synthesize a three–dimensional (3D) sea-urchin-like cobalt nitride composite material (labeled as CoN-Gr-2), which is used as a bi-functional catalyst for water splitting. Benefiting from the intrinsic high conductivity, larger surface area and unique 3D sea–urchin–like architecture, CoN-Gr-2 shows an excellent electron transfer efficiency, highly exposed active sites as well as the superior mass transport capacity. The CoN-Gr-2 catalyst exhibits low overpotentials of 128.9 mV and 280 mV for hydrogen evolution reaction (HER) and oxygen evolution reaction (OER), which are comparable to the commercial 20 wt% Pt/C and RuO2 catalysts. Moreover, when adopting CoN-Gr-2 as both anode and cathode materials for overall water splitting (in 1.0 M KOH electrolyte), the assembled cell achieves a current density of 10 mA cm-2 at 1.61 V, which almost close to that of Pt/C||RuO2 benchmark (1.60 V), demonstrating its superior water-splitting efficiency. Meanwhile, the CoN catalysts exhibit strong chemical interaction with the Gr support, suppressing the aggregation of CoN catalysts and maintains their high activity during HER and OER reactions. So, the cell exhibits a high current retention of 97.3% after 40 h. This work successfully develops an industrial chain from recycling Co wastes in spent energy devices to controllably designing 3D sea-urchin-like CoN-Gr with high water splitting efficiency. Therefore, it could further promote the efficient utilization of valuable Co element in various energy devices.