Microenvironmental modulation breaks intrinsic pH limitations of nanozymes to boost their activities
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.
Authors
- Ken‐ichi Otake (ORCID: https://orcid.org/0000-0002-7904-5003)
- Jiangjiexing Wu (ORCID: https://orcid.org/0000-0003-1652-4047)
- Hui Wei (ORCID: https://orcid.org/0000-0003-0870-7142)
- Susumu Kitagawa (ORCID: https://orcid.org/0000-0001-6956-9543)
- Shujie Liu (ORCID: https://orcid.org/0000-0003-0012-5199)
- Hang Xing (ORCID: https://orcid.org/0000-0003-3917-8343)
- Yufeng Liu (ORCID: https://orcid.org/0000-0002-2355-4706)
- Hao Dong (ORCID: https://orcid.org/0000-0001-7280-7506)
- Sirong Li
- Tong Li (ORCID: https://orcid.org/0000-0002-2341-3372)
- Yihong Zhang (ORCID: https://orcid.org/0000-0002-6432-3840)
- Wanling Liu (ORCID: https://orcid.org/0000-0003-4584-105X)
- Yuting Wang (ORCID: https://orcid.org/0000-0003-3894-4536)
- Xiaoyu Wang (ORCID: https://orcid.org/0009-0009-8943-131X)
Institutions
- Tianjin University of Science and Technology (CN)
- Nanjing Tech University (CN)
- Tianjin University of Technology (CN)
- Hunan University (CN)
- Kyoto University (JP)
- Nanjing Brain Hospital (CN)
- Collaborative Innovation Center of Advanced Microstructures (CN)
- Ministry of Education and Child Care (CA)
- Nanjing University (CN)
Publication Details
- Journal
- Nature Communications
- Published
- 2024-12-30
- DOI
- https://doi.org/10.1038/s41467-024-55163-4
- Citations
- 73
- Primary Topic
- Advanced Nanomaterials in Catalysis
- Type
- article
- Field-Weighted Citation Impact
- 8.55
Funders
- National Natural Science Foundation of China
- Hunan Provincial Science and Technology Department
- Nanjing University
- Priority Academic Program Development of Jiangsu Higher Education Institutions
- Japan Science and Technology Agency
- Fundamental Research Funds for the Central Universities
- Sakura Science Exchange Program