Wuya College of Innovation, Shenyang Pharmaceutical University, No. 103, Wenhua Road, Shenyang 110016, China.
Wuya College of Innovation, Shenyang Pharmaceutical University, No. 103, Wenhua Road, Shenyang 110016, China.
J Hazard Mater. 2024 Mar 5;465:133424. doi: 10.1016/j.jhazmat.2024.133424. Epub 2024 Jan 4.
Heavy metal pollution poses a major threat to human health, and developing a user-deliverable heavy metal detection strategy remains a major challenge. In this work, two-mode Hg sensing platforms based on the tunable cobalt metal-organic framework (Co-MOF) active site strategy are constructed, including a colorimetric, and an electrochemical assay using a personal glucose meter (PGM) as the terminal device. Specifically, thymine (T), a single, adaptable nucleotide, is chosen to replace typical T-rich DNA aptamers. The catalytic sites of Co-MOF are tuned competitively by the specific binding of T-Hg-T, and different signal output platforms are developed based on the different enzyme-like activities of Co-MOF. DFT calculations are utilized to analyze the interaction mechanism between T and Co-MOF with defect structure. Notably, the two-mode sensing platforms exhibit outstanding detection performance, with LOD values as low as 0.5 nM (colorimetric) and 3.69 nM (PGM), respectively, superior to recently reported nanozyme-based Hg sensors. In real samples of tap water and lake water, this approach demonstrates an effective recovery rate and outstanding selectivity. Surprisingly, the method is potentially versatile and, by exchanging out T-Hg-T, can also detect Ag. This simple, portable, and user-friendly Hg detection approach shows plenty of promise for application in the future.
重金属污染对人类健康构成重大威胁，开发用户可交付的重金属检测策略仍然是一个重大挑战。在这项工作中，构建了两种基于可调钴金属有机骨架（Co-MOF）活性位点策略的双模 Hg 传感平台，包括比色法和使用个人血糖仪（PGM）作为终端设备的电化学测定法。具体来说，选择胸腺嘧啶（T）作为单个适应性核苷酸，替代典型的富含 T 的 DNA 适体。T-Hg-T 的特异性结合竞争性地调节 Co-MOF 的催化位点，并基于 Co-MOF 的不同酶样活性开发不同的信号输出平台。利用 DFT 计算分析 T 与具有缺陷结构的 Co-MOF 的相互作用机制。值得注意的是，这两种双模传感平台表现出出色的检测性能，LOD 值分别低至 0.5 nM（比色法）和 3.69 nM（PGM），优于最近报道的基于纳米酶的 Hg 传感器。在自来水和湖水的实际样品中，该方法表现出有效的回收率和出色的选择性。令人惊讶的是，该方法具有潜在的多功能性，通过替换 T-Hg-T，还可以检测 Ag。这种简单、便携和用户友好的 Hg 检测方法具有广阔的应用前景。
