Zhang Bin-Wei, Zheng Tao, Wang Yun-Xiao, Du Yi, Chu Sheng-Qi, Xia Zhenhai, Amal Rose, Dou Shi-Xue, Dai Liming
Australian Carbon Materials Centre (A-CMC), School of Chemical Engineering, The University of New South Wales Sydney, Sydney, NSW, 2052, Australia.
Department of Materials Science and Engineering, Department of Chemistry, University of North Texas, Denton, TX, 76203, USA.
Commun Chem. 2022 Mar 28;5(1):43. doi: 10.1038/s42004-022-00645-z.
Electrochemical oxygen reduction provides an eco-friendly synthetic route to hydrogen peroxide (HO), a widely used green chemical. However, the kinetically sluggish and low-selectivity oxygen reduction reaction (ORR) is a key challenge to electrochemical production of HO for practical applications. Herein, we demonstrate that single cobalt atoms anchored on oxygen functionalized graphene oxide form Co-O-C@GO active centres (abbreviated as Co@GO for simplicity) that act as an efficient and durable electrocatalyst for HO production. This Co@GO electrocatalyst shows excellent electrochemical performance in O-saturated 0.1 M KOH, exhibiting high reactivity with an onset potential of 0.91 V and HO production of 1.0 mg cm h while affording high selectivity of 81.4% for HO. Our combined experimental observations and theoretical calculations indicate that the high reactivity and selectivity of Co@GO for HO electrogeneration arises from a synergistic effect between the O-bonded single Co atoms and adjacent oxygen functional groups (C-O bonds) of the GO present in the Co-O-C active centres.
电化学氧还原为过氧化氢（HO）提供了一条环保的合成路线，过氧化氢是一种广泛使用的绿色化学品。然而，动力学迟缓且选择性低的氧还原反应（ORR）是将HO电化学制备用于实际应用的关键挑战。在此，我们证明了锚定在氧官能化氧化石墨烯上的单钴原子形成了Co-O-C@GO活性中心（为简单起见简称为Co@GO），该活性中心可作为用于制备HO的高效且耐用的电催化剂。这种Co@GO电催化剂在O饱和的0.1 M KOH中表现出优异的电化学性能，起始电位为0.91 V，HO生成量为1.0 mg cm h，同时对HO的选择性高达81.4%。我们结合实验观察和理论计算表明，Co@GO对HO电生成的高反应性和选择性源于Co-O-C活性中心中与O键合的单个Co原子和GO相邻的氧官能团（C-O键）之间的协同效应。
