A Battery Process Activated Highly Efficient Carbon Catalyst toward Oxygen Reduction by Stabilizing Lithium–Oxygen Bonding

Abstract Graphene oxide (GO) has shown broad prospects in various practical applications, but it has been considered as a non‐active catalyst for the oxygen reduction reaction (ORR) unless a pretreatment such as high temperature heteroatoms‐doping is applied. Here, an interdisciplinary strategy is reported by utilizing lithium‐ion battery as a pretreatment processing to activate GO. The electrochemical battery process endows the GO with boosted ORR catalytic activity, exceeding that of nitrogen‐doped graphene at high temperature, a well‐recognized carbon catalyst. A series of control experiments point to that the carbon–oxygen–lithium bonding (C–O–Li) is possibly the origin of the activity. Further theoretical simulation tells that the lithium species stabilize the COO groups that help maintain the catalytic activity of the catalyst. Different from traditional chemical synthesis, this method provides a way to realize the lithium doping that has rarely been achieved for the heteroatoms‐doped carbon catalysts and also the control of the catalytic performance. Moreover, the proposed catalytic mechanism inspires researchers to pay more attention to the interaction of metallic heteroatoms and the oxygen‐containing functional groups in carbon. Such an interdisciplinary research combining the batteries and catalysis brings a broader vision to the field of carbon‐based electrochemistry.