Single‐Atomic Site Catalyst with Heme Enzymes‐Like Active Sites for Electrochemical Sensing of Hydrogen Peroxide

Ding, Shichao; Lyu, Zhaoyuan; Fang, Lingzhe; Li, Tao; Zhu, Wenlei; Li, Suiqiong; Li, Xin; Li, Jin‐Cheng; Du, Dan; Lin, Yuehe

doi:10.1002/smll.202100664

Single‐Atomic Site Catalyst with Heme Enzymes‐Like Active Sites for Electrochemical Sensing of Hydrogen Peroxide

Journal Article · Mon May 24 00:00:00 EDT 2021 · Small

DOI:https://doi.org/10.1002/smll.202100664· OSTI ID:1784442

^[1]; Lyu, Zhaoyuan ^[1]; Fang, Lingzhe ^[2]; Li, Tao ^[3]; ^[1]; Li, Suiqiong ^[4]; Li, Xin ^[1]; ^[1]; ^[1]; ^[1]

School of Mechanical and Materials Engineering Washington State University Pullman WA 99164 USA
Department of Chemistry and Biochemistry Northern Illinois University DeKalb IL 60115 USA
Department of Chemistry and Biochemistry Northern Illinois University DeKalb IL 60115 USA, X‐ray Science Division Argonne National Laboratory Lemont IL 60439 USA
DL ADV‐Tech Pullman WA 99163 USA

Abstract

Heme enzymes, with the pentacoordinate heme iron active sites, possess high catalytic activity and selectivity in biosensing applications. However, they are still subject to limited catalytic stability in the complex environment and high cost for broad applications in electrochemical sensing. It is meaningful to develop a novel substitute that has a similar structure to some heme enzymes and mimics their enzyme activities. One emerging strategy is to design the Fe‐N‐C based single‐atomic site catalysts (SASCs). The obtained atomically dispersed Fe‐N _x active sites can mimic the active sites of heme enzymes effectively. In this work, a SASC (Fe‐SASC/NW) is synthesized by doping single iron atoms in polypyrrole (PPy) derived carbon nanowire via a zinc‐atom‐assisted method. The proposed Fe‐SASC/NW shows high heme enzyme‐like catalytic performance for hydrogen peroxide (H ₂ O ₂ ) with a specific activity of 42.8 U mg ⁻¹ . An electrochemical sensor based on Fe‐SASC/NW is developed for the detection of H ₂ O ₂ . This sensor exhibits a wide detection concentration range from 5.0 × 10 ⁻¹⁰ m to 0.5 m and an excellent limit of detection (LOD) of 46.35 × 10 ⁻⁹ m . Such excellent catalytic activity and electrochemical sensing sensitivity are attributed to the isolated Fe‐N _x active sites and their structural similarity with natural metalloproteases.

View Accepted Manuscript (Publisher)

Sponsoring Organization:: USDOE

Grant/Contract Number:: AC02-06CH11357

OSTI ID:: 1784442

Journal Information:: Small, Journal Name: Small Journal Issue: 25 Vol. 17; ISSN 1613-6810

Publisher:: Wiley Blackwell (John Wiley & Sons)Copyright Statement

Country of Publication:: Germany

Language:: English

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