A single-atom Cu–N2 catalyst eliminates oxygen interference for electrochemical sensing of hydrogen peroxide in a living animal brain†

Received: 12 Feb 2021, Revised: 23 Mar 2021, Accepted: 07 Aug 2021, Available online: 08 Sep 2021, Version of Record: 08 Sep 2021

Xiaolong Gao,‡ac Wenjie Ma,‡ac Junjie Mao,‡d Chun-Ting He e , Wenliang Ji,a Zheng Chen d , Wenxing Chen f , Wenjie Wu,a Ping Yu ac , and Lanqun Mao *abc

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* Corresponding authors
a Beijing National Laboratory for Molecular Sciences, Key Laboratory of Analytical Chemistry for Living Biosystems, Institute of Chemistry, The Chinese Academy of Sciences (CAS), Beijing, China
E-mail: lqmao@bnu.edu.cn
b College of Chemistry, Beijing Normal University, Xinjiekouwai Street 19, Beijing, China
c University of Chinese Academy of Sciences, Beijing, China
d Key Laboratory of Functional Molecular Solids, Ministry of Education, College of Chemistry and Materials Science, Anhui Normal University, Wuhu, China
e MOE Key Laboratory of Functional Small Organic Molecule, College of Chemistry and Chemical Engineering, Jiangxi Normal University, Nanchang, China
f Beijing Key Laboratory of Construction Tailorable Advanced Functional Materials and Green Applications, School of Materials Science and Engineering, Beijing Institute of Technology, Beijing, China

Abstract


Hydrogen peroxide (H2O2) plays essential roles in various physiological and pathological processes. The electrochemical hydrogen peroxide reduction reaction (HPRR) has been recognized as an efficient approach to H2O2 sensing; however, the HPRR has always suffered from low tolerance against the oxygen reduction reaction (ORR), resulting in poor selectivity of the HPRR-based sensing platform. In this study, we find that the electrochemical HPRR occurs preferentially compared to the ORR when isolated Cu atoms anchored on carbon nitride (Cu1/C3N4) are used as a single-atom electrocatalyst, which is theoretically attributed to the lower energy barrier of the HPRR than that of the ORR on a Cu1/C3N4 single-atom catalyst (SAC). With the Cu1/C3N4 SAC as the electrocatalyst, we fabricated microsensors that have a good response to H2O2, but not to O2 or other electroactive neurochemicals. When implanted into a living rat brain, the microsensor shows excellent in vivo sensing performance, enabling its application in real-time quantitative investigation of the dynamics of H2O2 production induced by mercaptosuccinate and glutathione monoethyl ester in a living animal brain.
Graphical abstract: A single-atom Cu–N2 catalyst eliminates oxygen interference for electrochemical sensing of hydrogen peroxide in a living animal brain



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