Microenvironmental modulation breaks intrinsic pH limitations of nanozymes to boost their activities

Tong Li, Xiaoyu Wang, Yuting Wang, Yihong Zhang, Sirong Li, Wanling Liu, Shujie Liu, Yufeng Liu, Hang Xing, Ken-ichi Otake, Susumu Kitagawa, Jiangjiexing Wu (), Hao Dong () and Hui Wei ()
Additional contact information
Tong Li: Nanjing University
Xiaoyu Wang: Nanjing University
Yuting Wang: Nanjing University
Yihong Zhang: Nanjing University
Sirong Li: Nanjing University
Wanling Liu: Nanjing University
Shujie Liu: Nanjing University
Yufeng Liu: Nanjing University
Hang Xing: Hunan University
Ken-ichi Otake: Kyoto University
Susumu Kitagawa: Kyoto University
Jiangjiexing Wu: Nanjing University
Hao Dong: Nanjing University
Hui Wei: Nanjing University

Nature Communications, 2024, vol. 15, issue 1, 1-11

Abstract: Abstract Functional nanomaterials with enzyme-mimicking activities, termed as nanozymes, have found wide applications in various fields. However, the deviation between the working and optimal pHs of nanozymes has been limiting their practical applications. Here we develop a strategy to modulate the microenvironmental pHs of metal–organic framework (MOF) nanozymes by confining polyacids or polybases (serving as Brønsted acids or bases). The confinement of poly(acrylic acid) (PAA) into the channels of peroxidase-mimicking PCN-222-Fe (PCN = porous coordination network) nanozyme lowers its microenvironmental pH, enabling it to perform its best activity at pH 7.4 and to solve pH mismatch in cascade systems coupled with acid-denatured oxidases. Experimental investigations and molecular dynamics simulations reveal that PAA not only donates protons but also holds protons through the salt bridges between hydroniums and deprotonated carboxyl groups in neutral pH condition. Therefore, the confinement of poly(ethylene imine) increases the microenvironmental pH, leading to the enhanced hydrolase-mimicking activity of MOF nanozymes. This strategy is expected to pave a promising way for designing high-performance nanozymes and nanocatalysts for practical applications.

Date: 2024
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DOI: 10.1038/s41467-024-55163-4

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