Atomic-scale strain engineering of atomically resolved Pt clusters transcending natural enzymes
Strain engineering plays an important role in tuning electronic structure and improving catalytic capability of biocatalyst, but it is still challenging to modify the atomic-scale strain for specific enzyme-like reactions. Here, we systematically design Pt single atom (Pt<sub>1</sub>), several Pt atoms (Pt<sub>n</sub>) and atomically-resolved Pt clusters (Ptc) on PdAu biocatalysts to investigate the correlation between atomic strain and enzyme-like catalytic activity by experimental technology and in-depth Density Functional Theory calculations. It is found that Ptc on PdAu (Ptc-PA) with reasonable atomic strain upshifts the d-band center and exposes high potential surface, indicating the sufficient active sites to achieve superior biocatalytic performances. Besides, the Pd shell and Au core serve as storage layers providing abundant energetic charge carriers. The Ptc-PA exhibits a prominent peroxidase (POD)-like activity with the catalytic efficiency (K<sub>cat</sub>/K<sub>m</sub>) of 1.50 × 10<sup>9</sup> mM<sup>-1</sup> min<sup>-1</sup>, about four orders of magnitude higher than natural horseradish peroxidase (HRP), while catalase (CAT)-like and superoxide dismutase (SOD)-like activities of Ptc-PA are also comparable to those of natural enzymes. Biological experiments demonstrate that the detection limit of the Ptc-PA-based catalytic detection system exceeds that of visual inspection by 132-fold in clinical cancer diagnosis. Besides, Ptc-PA can reduce multi-organ acute inflammatory damage and mitigate oxidative stress disorder.
Authors
- Changlong Liu (ORCID: https://orcid.org/0000-0001-8516-2436)
- Qinjuan Ren
- Yuxing Yan
- Jin Chang (ORCID: https://orcid.org/0000-0002-6752-8526)
- Xiaoyu Mu (ORCID: https://orcid.org/0000-0002-6053-9775)
- Jingkai Yang
- Shuang Zhao (ORCID: https://orcid.org/0000-0002-1803-3017)
- Yikai Fu (ORCID: https://orcid.org/0009-0003-2362-6751)
- Shu‐Lin Liu (ORCID: https://orcid.org/0000-0002-1043-4238)
- Xiaodong Zhang (ORCID: https://orcid.org/0000-0002-7212-0138)
- Xiaoqun Gong (ORCID: https://orcid.org/0000-0002-0481-9756)
- Li Guo (ORCID: https://orcid.org/0000-0003-0575-6715)
- Ruoli Zhao (ORCID: https://orcid.org/0000-0003-4395-6902)
- Ling Liu (ORCID: https://orcid.org/0009-0003-1110-9239)
- Bo Zhang (ORCID: https://orcid.org/0000-0001-8745-2752)
- Qingshan Liu
- Yonghui Li (ORCID: https://orcid.org/0000-0002-6105-6484)
- Ke Chen (ORCID: https://orcid.org/0000-0002-3855-8363)
- Yuan Li (ORCID: https://orcid.org/0009-0000-5683-3835)
- Wei Long (ORCID: https://orcid.org/0000-0002-5365-9111)
- Junying Wang (ORCID: https://orcid.org/0000-0002-9289-7702)
- Yaoyao Ren (ORCID: https://orcid.org/0000-0001-8273-6895)
- Xin Qi (ORCID: https://orcid.org/0009-0007-4351-9186)
- Haitao Dai
- Shu Hua Zhang (ORCID: https://orcid.org/0000-0002-8517-2199)
- Peiyu Yao
- Ran Luo (ORCID: https://orcid.org/0000-0002-2470-2088)
- Jianning Zhang
- Qiong Qin
- Yang Cao (ORCID: https://orcid.org/0000-0003-3111-5751)
Institutions
- University of North Carolina at Chapel Hill (US)
- Tianjin University of Technology (CN)
- Tianjin University (CN)
- Chinese Academy of Medical Sciences & Peking Union Medical College (CN)
- Nankai University (CN)
- Tianjin Medical University General Hospital (CN)
- Southern University of Science and Technology (CN)
- Tianjin Medical University (CN)
Publication Details
- Journal
- Nature Communications
- Published
- 2024-09-27
- DOI
- https://doi.org/10.1038/s41467-024-52684-w
- Citations
- 28
- Primary Topic
- Nanocluster Synthesis and Applications
- Type
- article
- Field-Weighted Citation Impact
- 3.28
Funders
- National Natural Science Foundation of China
- Tianjin University
- Natural Science Foundation of Tianjin City
- National Key Research and Development Program of China