Department of Chemistry, Capital Normal University, Beijing 100048, China.
Energy & Catalysis Center, School of Materials Science and Engineering, Beijing Institute of Technology, Beijing 100081, China.
Anal Chem. 2022 Oct 18;94(41):14308-14316. doi: 10.1021/acs.analchem.2c02853. Epub 2022 Oct 4.
Great enthusiasm in single-atom catalysts for various catalytic reactions continues to heat up. However, the poor activity of the existing single/dual-metal-atom catalysts does not meet the actual requirement. In this scenario, the precise design of triple-metal-atom catalysts is vital but still challenging. Here, a triple-atom site catalyst of FeCoZn catalyst coordinated with S and N, which is doped in the carbon matrix (named FeCoZn-TAC/SNC), is designed. The FeCoZn catalyst can mimic the activity of oxidase by activating O into O radicals by virtue of its atomically dispersed metal active sites. Employing this characteristic, triple-atom catalysts can become a great driving force for the development of novel biosensors featuring adequate sensitivity. First, the property of FeCoZn catalyst as an oxidase-like nanozyme was explored. The obtained FeCoZn-TAC/SNC shows remarkably enhanced catalytic performance than that of FeCoZn-TAC/NC and single/dual-atom site catalysts (FeZn, CoZn, FeCo-DAC/NC and Fe, Zn, Co-SAC/NC) because of trimetallic sites, demonstrating the synergistic effect. Further, the utility of the oxidase-like FeCoZn-TAC/SNC in biosensor field is evaluated by the colorimetric sensing of ascorbic acid. The nanozyme sensor shows a wide concentration range from 0.01 to 90 μM and an excellent detection limit of 6.24 nM. The applicability of the nanozyme sensor in biologically relevant detection was further proved in serum. The implementation of TAC in colorimetric detection holds vast promise for further development of biomedical research and clinical diagnosis.
单原子催化剂在各种催化反应中引起了广泛的关注。然而,现有的单/双金属原子催化剂活性较差,无法满足实际需求。在这种情况下,精确设计三金属原子催化剂至关重要,但也极具挑战性。本文设计了一种由 S 和 N 配位的三原子位点 FeCoZn 催化剂,其掺杂在碳基质中(命名为 FeCoZn-TAC/SNC)。该 FeCoZn 催化剂可以通过其原子分散的金属活性位点将 O 激活为 O 自由基,从而模拟氧化酶的活性。利用这一特性,三原子催化剂可以成为开发具有足够灵敏度的新型生物传感器的强大动力。首先,研究了 FeCoZn 催化剂作为类氧化酶纳米酶的特性。与 FeCoZn-TAC/NC 和单/双原子位点催化剂(FeZn、CoZn、FeCo-DAC/NC 和 Fe、Zn、Co-SAC/NC)相比,所得的 FeCoZn-TAC/SNC 表现出显著增强的催化性能,这是由于三金属位点的协同作用。此外,通过对抗坏血酸的比色传感评估了类氧化酶的 FeCoZn-TAC/SNC 在生物传感器领域的应用。纳米酶传感器在 0.01 至 90 μM 的宽浓度范围内表现出优异的检测限为 6.24 nM。进一步证明了纳米酶传感器在血清中具有良好的生物相关检测适用性。TAC 在比色检测中的应用为生物医学研究和临床诊断的进一步发展提供了广阔的前景。