Institute of Nanochemistry and Nanobiology, School of Environmental and Chemical Engineering, Shanghai University, Shanghai, 200444, China.
Institute for Sustainable Energy/College of Sciences, Shanghai University, Shanghai, 200444, China.
Anal Chim Acta. 2023 May 8;1254:341091. doi: 10.1016/j.aca.2023.341091. Epub 2023 Mar 20.
Single-atom catalyst (SAC), one of the most attractive catalysts in the field of energy conversion and storage, was proven as efficient accelerator for luminol-dissolved oxygen electrochemiluminescence (ECL) via the catalysis of oxygen reduction reaction (ORR). In this work, we synthesized heteroatom doping SACs of Fe-N/P-C for the catalysis of cathodic luminol ECL. The doping of P could lower the reaction energy barrier of the OH* reduction, and promote catalytic efficiency toward ORR. The formation of reactive oxygen species (ROS) during ORR triggered cathodic luminol ECL. Greatly enhanced ECL emission catalyzed by SACs proved that Fe-N/P-C exhibited higher catalytic activity to ORR compared with Fe-N-C. Since the system was highly dependent on oxygen, an ultra-sensitive detection of a typical antioxidant, ascorbic acid, was achieved with detection limit of 0.03 nM. This study provides possibility to greatly enhance the performance of ECL platform through rational tailoring of SACs via heteroatom doping.
单原子催化剂（SAC）作为能量转换和存储领域最具吸引力的催化剂之一，通过催化氧还原反应（ORR）被证明是鲁米诺溶解氧电化学发光（ECL）的有效加速剂。在这项工作中，我们合成了用于催化阴极鲁米诺 ECL 的杂原子掺杂 Fe-N/P-C SAC。P 的掺杂可以降低 OH*还原的反应能垒，并提高 ORR 的催化效率。ORR 过程中形成的活性氧物种（ROS）触发了阴极鲁米诺 ECL。SAC 极大地增强了 ECL 发射，证明了 Fe-N/P-C 对 ORR 的催化活性高于 Fe-N-C。由于该体系高度依赖氧气，因此可以实现对典型抗氧化剂抗坏血酸的超灵敏检测，检测限低至 0.03 nM。本研究通过杂原子掺杂对 SAC 进行合理设计，为极大地提高 ECL 平台的性能提供了可能。
