Natural Protein Photon Upconversion Supramolecular Assemblies for Background-Free Biosensing

光子上转换 化学 肌氨酸 纳米探针 生物传感器 纳米技术 材料科学 生物化学 有机化学 纳米颗粒 离子 甘氨酸 氨基酸
作者
Hongjuan Feng,Le Zeng,Jiayao Li,Wen-Yue Lin,Fang Qi,Lin‐Han Jiang,Ming‐Yu Zhang,Yang Zhao,Ling Huang,Dai‐Wen Pang
出处
期刊:Journal of the American Chemical Society [American Chemical Society]
卷期号:146 (31): 21791-21805 被引量:1
标识
DOI:10.1021/jacs.4c06012
摘要

The diagnosis of disease biomarkers is crucial for the identification, monitoring, and prognostic assessment of malignant disease. However, biological samples with autofluorescence, complex components, and heterogeneity pose major challenges to reliable biosensing. Here, we report the self-assembly of natural proteins and the triplet–triplet annihilation upconversion (TTA-UC) pair to form upconverted protein clusters (∼8.2 ± 1.1 nm), which were further assembled into photon upconversion supramolecular assemblies (PUSA). This PUSA exhibited unique features, including a small size (∼44.1 ± 4.1 nm), oxygen tolerance, superior biocompatibility, and easy storage via lyophilization, all of which are long sought after for photon upconversion materials. Further, we have revealed that the steric hindrance of the annihilator suppresses the stacking of the annihilator in PUSA, which is vital for maintaining the water dispersibility and enhancing the upconversion performance of PUSA. In conjunction with sarcosine oxidase, this near infrared (NIR)-excitable PUSA nanoprobe could perform background-free biosensing of urinary sarcosine, which is a common biomarker for prostatic carcinoma (PCa). More importantly, this nanoprobe not only allows for qualitative identification of urinary samples from PCa patients by the unaided eye under NIR-light-emitting diode (LED) illumination but also quantifies the concentration of urinary sarcosine. These remarkable findings have propelled photon upconversion materials to a new evolutionary stage and expedited the progress of upconversion biosensing in clinical diagnostics.
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