Microenvironmental modulation breaks intrinsic pH limitations of nanozymes to boost their activities
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...
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| Format: | Article |
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Nature Portfolio
2024-12-01
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| Series: | Nature Communications |
| Online Access: | https://doi.org/10.1038/s41467-024-55163-4 |
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| author | 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 Hui Wei |
| author_facet | 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 Hui Wei |
| author_sort | Tong Li |
| collection | DOAJ |
| description | 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. |
| format | Article |
| id | doaj-art-83c3d3c0dbd547418a899f2d537fc382 |
| institution | Kabale University |
| issn | 2041-1723 |
| language | English |
| publishDate | 2024-12-01 |
| publisher | Nature Portfolio |
| record_format | Article |
| series | Nature Communications |
| spelling | doaj-art-83c3d3c0dbd547418a899f2d537fc3822025-01-05T12:36:34ZengNature PortfolioNature Communications2041-17232024-12-0115111110.1038/s41467-024-55163-4Microenvironmental modulation breaks intrinsic pH limitations of nanozymes to boost their activitiesTong Li0Xiaoyu Wang1Yuting Wang2Yihong Zhang3Sirong Li4Wanling Liu5Shujie Liu6Yufeng Liu7Hang Xing8Ken-ichi Otake9Susumu Kitagawa10Jiangjiexing Wu11Hao Dong12Hui Wei13College of Engineering and Applied Sciences, Nanjing National Laboratory of Microstructures, Jiangsu Key Laboratory of Artificial Functional Materials, Nanjing UniversityKuang Yaming Honors School, Nanjing UniversityCollege of Engineering and Applied Sciences, Nanjing National Laboratory of Microstructures, Jiangsu Key Laboratory of Artificial Functional Materials, Nanjing UniversityCollege of Engineering and Applied Sciences, Nanjing National Laboratory of Microstructures, Jiangsu Key Laboratory of Artificial Functional Materials, Nanjing UniversityCollege of Engineering and Applied Sciences, Nanjing National Laboratory of Microstructures, Jiangsu Key Laboratory of Artificial Functional Materials, Nanjing UniversityCollege of Engineering and Applied Sciences, Nanjing National Laboratory of Microstructures, Jiangsu Key Laboratory of Artificial Functional Materials, Nanjing UniversityCollege of Engineering and Applied Sciences, Nanjing National Laboratory of Microstructures, Jiangsu Key Laboratory of Artificial Functional Materials, Nanjing UniversityCollege of Engineering and Applied Sciences, Nanjing National Laboratory of Microstructures, Jiangsu Key Laboratory of Artificial Functional Materials, Nanjing UniversityInstitute of Chemical Biology and Nanomedicine, State Key Laboratory of Chemo/Biosensing and Chemometrics, College of Chemistry and Chemical Engineering, Hunan UniversityInstitute for Integrated Cell-Material Sciences (WPI-iCeMS), Kyoto UniversityInstitute for Integrated Cell-Material Sciences (WPI-iCeMS), Kyoto UniversityCollege of Engineering and Applied Sciences, Nanjing National Laboratory of Microstructures, Jiangsu Key Laboratory of Artificial Functional Materials, Nanjing UniversityKuang Yaming Honors School, Nanjing UniversityCollege of Engineering and Applied Sciences, Nanjing National Laboratory of Microstructures, Jiangsu Key Laboratory of Artificial Functional Materials, Nanjing UniversityAbstract 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.https://doi.org/10.1038/s41467-024-55163-4 |
| spellingShingle | 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 Hui Wei Microenvironmental modulation breaks intrinsic pH limitations of nanozymes to boost their activities Nature Communications |
| title | Microenvironmental modulation breaks intrinsic pH limitations of nanozymes to boost their activities |
| title_full | Microenvironmental modulation breaks intrinsic pH limitations of nanozymes to boost their activities |
| title_fullStr | Microenvironmental modulation breaks intrinsic pH limitations of nanozymes to boost their activities |
| title_full_unstemmed | Microenvironmental modulation breaks intrinsic pH limitations of nanozymes to boost their activities |
| title_short | Microenvironmental modulation breaks intrinsic pH limitations of nanozymes to boost their activities |
| title_sort | microenvironmental modulation breaks intrinsic ph limitations of nanozymes to boost their activities |
| url | https://doi.org/10.1038/s41467-024-55163-4 |
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