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Title: Unprecedented peroxidase-mimicking activity of single-atom nanozyme with atomically dispersed Fe–Nx moieties hosted by MOF derived porous carbon

Abstract

Due to robustness, easy large-scale preparation and low cost, nanomaterials with enzyme-like characteristics (defined as ‘nanozymes’) are attracting increasing interest for various applications. However, most of currently developed nanozymes show much lower activity in comparison with natural enzymes, and the deficiency greatly hinders their use in sensing and biomedicine. Single-atom catalysts (SACs) offer the unique feature of maximum atomic utilization, providing a potential pathway to improve the catalytic activity of nanozymes. Herein, we propose a Fe-N-C single-atom nanozyme (SAN) that exhibits unprecedented peroxidase-mimicking activity. The SAN consists of atomically dispersed Fe-Nx moieties hosted by metal–organic frameworks (MOF) derived porous carbon. Thanks to the 100% single-atom active Fe dispersion and the large surface area of the porous support, the Fe-N-C SAN provided a specific activity of 57.76 U mg-1, which was almost at the same level as natural horseradish peroxidase (HRP). Attractively, the SAN presented much better storage stability and robustness against harsh environments. As a proof-of-concept application, highly sensitive biosensing of butyrylcholinesterase (BChE) activity using the Fe-N-C SAN as a substitute for natural HRP was further verified.

Authors:
 [1];  [1];  [1];  [1];  [1];  [1];  [1];  [1];  [2];  [3]; ORCiD logo [3]
  1. Washington State University
  2. BATTELLE (PACIFIC NW LAB)
  3. WASHINGTON STATE UNIV
Publication Date:
Research Org.:
Pacific Northwest National Lab. (PNNL), Richland, WA (United States)
Sponsoring Org.:
USDOE
OSTI Identifier:
1577052
Report Number(s):
PNNL-SA-145442
DOE Contract Number:  
AC05-76RL01830
Resource Type:
Journal Article
Journal Name:
Biosensors and Bioelectronics
Additional Journal Information:
Journal Volume: 142
Country of Publication:
United States
Language:
English

Citation Formats

Niu, Xiangheng, Shi, Qiurong, Zhu, Wenlei, Liu, Dong, Tian, Hangyu, Fu, Shaofang, Cheng, Nan, Li, Suiqiong, Smith, Jordan N., Du, Dan, and Lin, Yuehe. Unprecedented peroxidase-mimicking activity of single-atom nanozyme with atomically dispersed Fe–Nx moieties hosted by MOF derived porous carbon. United States: N. p., 2019. Web. doi:10.1016/j.bios.2019.111495.
Niu, Xiangheng, Shi, Qiurong, Zhu, Wenlei, Liu, Dong, Tian, Hangyu, Fu, Shaofang, Cheng, Nan, Li, Suiqiong, Smith, Jordan N., Du, Dan, & Lin, Yuehe. Unprecedented peroxidase-mimicking activity of single-atom nanozyme with atomically dispersed Fe–Nx moieties hosted by MOF derived porous carbon. United States. https://doi.org/10.1016/j.bios.2019.111495
Niu, Xiangheng, Shi, Qiurong, Zhu, Wenlei, Liu, Dong, Tian, Hangyu, Fu, Shaofang, Cheng, Nan, Li, Suiqiong, Smith, Jordan N., Du, Dan, and Lin, Yuehe. 2019. "Unprecedented peroxidase-mimicking activity of single-atom nanozyme with atomically dispersed Fe–Nx moieties hosted by MOF derived porous carbon". United States. https://doi.org/10.1016/j.bios.2019.111495.
@article{osti_1577052,
title = {Unprecedented peroxidase-mimicking activity of single-atom nanozyme with atomically dispersed Fe–Nx moieties hosted by MOF derived porous carbon},
author = {Niu, Xiangheng and Shi, Qiurong and Zhu, Wenlei and Liu, Dong and Tian, Hangyu and Fu, Shaofang and Cheng, Nan and Li, Suiqiong and Smith, Jordan N. and Du, Dan and Lin, Yuehe},
abstractNote = {Due to robustness, easy large-scale preparation and low cost, nanomaterials with enzyme-like characteristics (defined as ‘nanozymes’) are attracting increasing interest for various applications. However, most of currently developed nanozymes show much lower activity in comparison with natural enzymes, and the deficiency greatly hinders their use in sensing and biomedicine. Single-atom catalysts (SACs) offer the unique feature of maximum atomic utilization, providing a potential pathway to improve the catalytic activity of nanozymes. Herein, we propose a Fe-N-C single-atom nanozyme (SAN) that exhibits unprecedented peroxidase-mimicking activity. The SAN consists of atomically dispersed Fe-Nx moieties hosted by metal–organic frameworks (MOF) derived porous carbon. Thanks to the 100% single-atom active Fe dispersion and the large surface area of the porous support, the Fe-N-C SAN provided a specific activity of 57.76 U mg-1, which was almost at the same level as natural horseradish peroxidase (HRP). Attractively, the SAN presented much better storage stability and robustness against harsh environments. As a proof-of-concept application, highly sensitive biosensing of butyrylcholinesterase (BChE) activity using the Fe-N-C SAN as a substitute for natural HRP was further verified.},
doi = {10.1016/j.bios.2019.111495},
url = {https://www.osti.gov/biblio/1577052}, journal = {Biosensors and Bioelectronics},
number = ,
volume = 142,
place = {United States},
year = {2019},
month = {10}
}