Luo Shiqing, Sun Xiaojie, Zhang Lifang, Miao Yanming, Yan Guiqin
School of Chemistry and Materials Science, Shanxi Normal University, Taiyuan, 030000, China.
School of Chemistry and Materials Science, Shanxi Normal University, Taiyuan, 030000, China; Department of Chemistry, Xinzhou Normal University, Xinzhou, 034000, China.
Biosens Bioelectron. 2025 Jul 15;280:117423. doi: 10.1016/j.bios.2025.117423. Epub 2025 Apr 2.
Photoresponsive nanozymes are widely used in analysis and other fields owing to their controllable catalysis and low cost, but most have relatively low catalytic efficiency. In this study, room-temperature phosphorescent carbonized polymer dots (PCPDs) were optimally prepared through a one-pot hydrothermal method using polyacrylic acid and ethylenediamine as precursors. Their photoresponsive oxidase-like activity was confirmed for the first time. The sub-fluorophore and highly-crosslinked structure endow PCPDs with excellent enzymatic properties. The PCPDs have strong affinity (K = 0.1266 mM) and extremely high catalytic efficiency (V = 2.0194 × 10 M s) over 3,3',5,5'-tetramethylbenzidine (TMB), and the reaction is dozens of times faster compared with most photoresponsive oxidases (10 M s level). Uric acid (UA) is an important biomarker, and its sensitive detection is particularly critical. The PCPDs were irradiated for 1 min to oxidize TMB into dark blue, and the strong reducing property of UA faded the dark blue and enhanced the fluorescence (FL) of the system. The colorimetric/FL dual-mode method established has detection limits over UA of 77.8 and 48.1 nM, respectively, and linear ranges of 0.6-55 and 0.6-60 μM, respectively. Smartphones were also used to identify dual-mode RGB to detect UA. Finally, the PCPDs were successfully used to detect UA in human serum, urine and saliva. This study presents a natural-enzyme-free UA sensing platform based on PCPDs, and more importantly, provides a new type of highly efficient photoresponsive oxidases with great potential for analytical sensing and other fields.
光响应纳米酶因其可调控的催化性能和低成本而被广泛应用于分析等领域,但大多数光响应纳米酶的催化效率相对较低。在本研究中,以聚丙烯酸和乙二胺为前驱体,通过一锅水热法优化制备了室温磷光碳化聚合物点(PCPDs)。首次证实了其具有光响应类氧化酶活性。亚荧光团和高度交联的结构赋予了PCPDs优异的酶学性质。PCPDs对3,3',5,5'-四甲基联苯胺(TMB)具有很强的亲和力(K = 0.1266 mM)和极高的催化效率(V = 2.0194×10 M s),与大多数光响应氧化酶(10 M s水平)相比,该反应速度快几十倍。尿酸(UA)是一种重要的生物标志物,对其进行灵敏检测尤为关键。对PCPDs照射1分钟可将TMB氧化为深蓝色,而UA的强还原性可使深蓝色褪色并增强体系的荧光(FL)。所建立的比色/荧光双模式方法对UA的检测限分别为77.8和48.1 nM,线性范围分别为0.6 - 55和0.6 - 60 μM。还利用智能手机识别双模式RGB来检测UA。最后,PCPDs成功用于检测人血清、尿液和唾液中的UA。本研究提出了一种基于PCPDs的无天然酶UA传感平台,更重要的是,提供了一种新型的高效光响应氧化酶,在分析传感及其他领域具有巨大潜力。