School of Health Science and Engineering, University of Shanghai for Science and Technology, Shanghai, 200093, China.
Collaborative Research Center, Shanghai University of Medicine & Health Sciences, Shanghai, 201318, China.
Appl Biochem Biotechnol. 2022 Jul;194(7):3044-3065. doi: 10.1007/s12010-022-03861-4. Epub 2022 Mar 25.
Porous carbon sphere materials have a large variety of applications in several fields due to the large surface area, adaptable porosity, and good conductivity they possess. Obtaining a steady carbon sphere using the green synthesis method remains a significant challenge. In this experiment, covalent organic frameworks (COFs) were used as a precursor and FeONPs were integrated into the precursor in order to synthesize a porous carbon sphere material using the one-step pyrolysis method. COFs have an ordered porous structure, perpetual porosity, large surface area, and low density and display good environmental tolerance. These properties make them an excellent precursor for synthesizing porous carbon sphere, which maintains good morphology at high temperatures, and it is not involved in the removal of dangerous reagent and small size restrictions during the synthesis process. In addition to the formation of a porous carbon sphere, transition metal carbon material that contains N element can be an active catalyst. The composites exhibit better activity when Fe is doped into carbon materials containing N element than that of other doped transition metals including Mn and Co. In this situation, the integration of FeONPs and N element in the COF precursor exposed the active sites of the composites and the two substances synergistically improved the electrocatalytic properties, and the composites were named FeO@NPCS. The constructed FeO@NPCS/GCE immunosensor was applied as a means of detecting CA19-9 antigen and presented a wide linear range from 0.00001 to 10 U/mL with a low detection limit of 2.429 μU/mL (S/N = 3). In addition, the prepared immunosensor was utilized for detecting CA19-9 antigen in the real human serum, and the recovery rates were in the range from 95.24% to 106.38%. Therefore, a porous carbon sphere prepared by COFs as a precursor can be applied for the detection of CA19-9 antigen in real samples, which could be an excellent strategy for CA19-9 antigen detection and could potentially promote the development of COF materials in various electrochemical fields.
多孔碳球材料因其具有较大的比表面积、可调节的孔隙率和良好的导电性，在多个领域得到了广泛的应用。使用绿色合成方法获得稳定的碳球仍然是一个重大挑战。在本实验中，我们使用共价有机骨架（COFs）作为前体，并将 FeONPs 整合到前体中，通过一步热解法合成多孔碳球材料。COFs 具有有序的多孔结构、永久的孔隙率、大的比表面积和低密度，并且表现出良好的环境耐受性。这些特性使它们成为合成多孔碳球的理想前体，在高温下保持良好的形态，并且在合成过程中不涉及危险试剂的去除和小尺寸的限制。除了形成多孔碳球之外，含有 N 元素的过渡金属碳材料也可以作为活性催化剂。与 Mn 和 Co 等其他掺杂的过渡金属相比，Fe 掺杂到含 N 元素的碳材料中时，复合材料表现出更好的活性。在这种情况下，将 FeONPs 和 N 元素整合到 COF 前体中暴露了复合材料的活性位点，两种物质协同提高了电催化性能，该复合材料被命名为 FeO@NPCS。构建的 FeO@NPCS/GCE 免疫传感器被用作检测 CA19-9 抗原的手段，其线性范围从 0.00001 到 10 U/mL，检测限低至 2.429 μU/mL（S/N=3）。此外，该制备的免疫传感器用于检测真实人血清中的 CA19-9 抗原，回收率在 95.24%至 106.38%之间。因此，以 COFs 为前体制备的多孔碳球可用于检测真实样品中的 CA19-9 抗原，这可能是 CA19-9 抗原检测的一种极好策略，并有可能促进 COF 材料在各个电化学领域的发展。
