Department of Chemical Engineering , Pohang University of Science and Technology (POSTECH) , Pohang , Gyeongbuk 37673 , Republic of Korea.
Department of Chemical and Biomolecular Engineering , Korea Advanced Institute of Science and Technology (KAIST) , Daejeon 34141 , Republic of Korea.
ACS Nano. 2019 Apr 23;13(4):4312-4321. doi: 10.1021/acsnano.8b09519. Epub 2019 Mar 27.
The work describes a carbon-based peroxidase mimic, N- and B-codoped reduced graphene oxide (NB-rGO), which shows high peroxidase-like activity without oxidase-like activity and has a catalytic efficiency nearly 1000-fold higher than that of undoped rGO. The high catalytic activity of NB-rGO is explained by density functional theory by calculating Gibbs free energy change during the peroxide decomposition reaction. Acetylcholine and C-reactive protein are successfully quantified with high sensitivity and selectivity, which were comparable to or better than those obtained using natural peroxidase. Furthermore, NB-rGO, which does not have oxidase-like activity, is proven to have higher sensitivity toward acetylcholine than Pt nanoparticles having oxidase-like activity. This work will facilitate studies on development, theoretical analysis for rational design, and bioassay applications of enzyme mimics based on nanomaterials.
该工作描述了一种基于碳的过氧化物酶模拟物，即 N 和 B 共掺杂还原氧化石墨烯（NB-rGO），它表现出高过氧化物酶样活性而没有氧化酶样活性，并且催化效率比未掺杂的 rGO 高近 1000 倍。通过计算过氧化物分解反应过程中的吉布斯自由能变化，用密度泛函理论解释了 NB-rGO 的高催化活性。成功地实现了对乙酰胆碱和 C 反应蛋白的高灵敏度和选择性定量检测，其灵敏度与使用天然过氧化物酶获得的灵敏度相当或更好。此外，已证明具有氧化酶样活性的 Pt 纳米粒子相比，不具有氧化酶样活性的 NB-rGO 对乙酰胆碱具有更高的灵敏度。这项工作将促进基于纳米材料的酶模拟物的开发、理论分析和生物测定应用的研究。
