MOE Key Laboratory of Bioinorganic and Synthetic Chemistry, School of Chemistry, Sun Yat-sen University, Guangzhou, 510006, China.
Guangzhou Municipal and Guangdong Provincial Key Laboratory of Molecular Target & Clinical Pharmacology, the NMPA and State Key Laboratory of Respiratory Disease, School of Pharmaceutical Sciences and the Fifth Affiliated Hospital, Guangzhou Medical University, Guangzhou, 511436, China.
Angew Chem Int Ed Engl. 2023 Mar 20;62(13):e202218661. doi: 10.1002/anie.202218661. Epub 2023 Feb 15.
Mimicking the bioactivity of native enzymes through synthetic chemistry is an efficient means to advance the biocatalysts in a cell-free environment, however, remains long-standing challenges. Herein, we utilize structurally explicit hydrogen-bonded organic frameworks (HOFs) to mimic photo-responsive oxidase, and uncover the important role of pore environments on mediating oxidase-like activity by means of constructing isostructural HOFs. We discover that the HOF pore with suitable geometry can stabilize and spatially organize the catalytic substrate into a favorable catalytic route, as with the function of the native enzyme pocket. Based on the desirable photo-responsive oxidase-like activity, a visual and sensitive HOFs biosensor is established for the detection of phosphatase, an important biomarker of skeletal and hepatobiliary diseases. This work demonstrates that the pore environments significantly influence the nanozymes' activity in addition to the active center.
通过合成化学模拟天然酶的生物活性是在无细胞环境中推进生物催化剂的有效手段，但仍然存在长期存在的挑战。在此，我们利用结构明确的氢键有机框架（HOFs）模拟光响应氧化酶，并通过构建同构的 HOFs 揭示孔环境在调节氧化酶样活性方面的重要作用。我们发现具有合适几何形状的 HOF 孔可以稳定和空间组织催化底物进入有利的催化途径，就像天然酶口袋的功能一样。基于理想的光响应氧化酶样活性，我们建立了一种可视化和敏感的 HOFs 生物传感器，用于检测磷酸酶，这是骨骼和肝胆疾病的重要生物标志物。这项工作表明，除了活性中心外，孔环境还会显著影响纳米酶的活性。
