Unlocking the Potential of Mn‐based Catalyst for Durable Two‐electron Oxygen Reduction in Acid at High Current Densities
Abstract
Abstract Electrochemical synthesis of H 2 O 2 by two‐electron oxygen reduction (2e − ORR) often shows limited stability at high current densities in acidic media. Mn‐based catalysts have been demonstrated highly stable for four‐electron ORR thanks to their intrinsically low rate constant for Fenton‐like reactions. However, their activity toward acidic 2e − ORR remains low because of too strong adsorption to *OOH. Here, we report a diatomic Mn catalyst with high‐spin Mn II centers to enable high onset potential (0.69 V), high selectivity (>90%), and outstanding stability (240 h under 300 mA cm −2 ) toward H 2 O 2 electrosynthesis in acid. Theoretical calculations and in situ spectroscopies reveal that the diatomic Mn sites have downshifted d ‐band center and thus weakened adsorption strength for *OOH. Moreover, the inertia of the Mn II sites toward the troublesome Fenton‐like reactions leads to the long‐term stability at high current densities. We further demonstrate the functionalization of waste polyethylene (PE) using the high‐concentration H 2 O 2 as produced, which provides a sustainable route toward on‐site upcycling of plastic waste.
Article Details
Authors (19)
Helai Huang
State Key Laboratory of Chemical Engineering Department of Chemical Engineering Tsinghua University Beijing 100084 P.R. China
Mingze Sun
Kai Chen
Yizhen Che
State Key Laboratory of Chemical Engineering, Department of Chemical Engineering
Xin Tang
Zhengwen Li
Department of Chemical Engineering
Kaiqi Nie
Department of Chemical Engineering
Shuairen Qian
Department of Chemical Engineering
Jinjie Fang
State Key Lab of Organic−Inorganic Composites, Beijing University of Chemical Technology, 100029 Beijing, China
Haiyong Wang
State Key Laboratory of Organic−Inorganic Composites and Beijing Advanced Innovation Center for Soft Matter Science and Engineering Beijing University of Chemical Technology Beijing 100084 P.R. China
Yanfen Wu
Qikun Hu
State Key Laboratory of Chemical Engineering, Department of Chemical Engineering
Yuqi Wang
Xiaohang Sun
Junliang He
State Key Laboratory of Chemical Engineering Department of Chemical Engineering Tsinghua University Beijing 100084 P.R. China
Yu‐Xiao Zhang
State Key Laboratory of Chemical Engineering Department of Chemical Engineering Tsinghua University Beijing 100084 P.R. China
Zhongbin Zhuang
Liang Zhang
Zhiqiang Niu
State Key Laboratory of Chemical Engineering, Department of Chemical Engineering