Metal organic polymers with dual catalytic sites for oxygen reduction and oxygen evolution reactions  

作　　者：Sijia Liu Minghao Liu Xuewen Li Shuai Yang Qiyang Miao Qing Xu Gaofeng Zeng 

机构地区：[1]CAS Key Laboratory of Low-Carbon Conversion Science and Engineering,Shanghai Advanced Research Institute(SARI),Chinese Academy of Sciences(CAS),Shanghai,China [2]School of Physical Science and Technology,ShanghaiTech University,Shanghai,China [3]School of Chemical Engineering,University of Chinese Academy of Sciences,Beijing,China

出　　处：《Carbon Energy》2023年第5期127-137,共11页碳能源（英文）

基　　金：support from the Natural Science Foundation of Shanghai (20ZR1464000);G.Zeng acknowledges the support from the National Natural Science Foundation of China (21878322,22075309);the Science and Technology Commission of Shanghai Municipality (19ZR1479200,22ZR1470100)。

摘　　要：Metal-organic frameworks and covalent organic frameworks have been widely employed in electrochemical catalysis owing to their designable skeletons,controllable porosities,and well-defined catalytic centers.However,the poor chemical stability and low electron conductivity limited their activity,and single-functional sites in these frameworks hindered them to show multifunctional roles in catalytic systems.Herein,we have constructed novel metal organic polymers(Co-HAT-CN and Ni-HAT-CN)with dual catalytic centers(metal-N_(4) and metal-N_(2))to catalyze oxygen reduction reaction(ORR)and oxygen evolution reaction(OER).By using different metal centers,the catalytic activity and selectivity were well-tuned.Among them,Co-HAT-CN catalyzed the ORR in a 4e^(-)pathway,with a half-wave potential of 0.8 V versus RHE,while the Ni-HAT-CN catalyze ORR in a 2e^(-)pathway with H_(2)O_(2) selectivity over 90%.Moreover,the Co-HAT-CN delivered an overpotential of 350 mV at 10 mA cm^(-2) with a corresponding Tafel slope of 24 mV dec^(-1) for OER in a 1.0 M KOH aqueous solution.The experimental results revealed that the activities toward ORR were due to the M-N_(4) sites in the frameworks,and both M-N_(4) and M-N_(2) sites contributed to the OER.This work gives us a new platform to construct bifunctional catalysts.

关 键 词：covalent organic frameworks metal organic polymers oxygen evolution reaction oxygen reduction reaction single atom catalysts 

分 类 号：O643.36[理学—物理化学]