Du Minshu, Meng Yao, Zhu Geju, Gao Mingze, Hsu Hsien-Yi, Liu Feng
School of Materials Science and Engineering, Northwestern Polytechnical University, Xi'an, Shaanxi, China.
Nanoscale. 2020 Nov 12;12(43):22014-22021. doi: 10.1039/d0nr05780k.
Identifying the intrinsic electrocatalytic activity of an individual nanoparticle is challenging as traditional ensemble measurements only provide average activity over a large number of nanoparticles and may be greatly affected by the ensemble properties, irrelevant to the nanoparticle itself. Here, single-particle collision electrochemistry is used to investigate the electrocatalytic activity of a single IrOx nanoparticle towards the oxygen evolution reaction (OER). The collision frequency is linearly proportional to the nanoparticle concentration. The mean peak current and transferred charge, extracted from current spikes of the collision, present a similar potential dependence relevant to IrOx intrinsic activity. The turnover frequency (TOF) is determined as 1.55 × 102 O2 s-1, which is orders of magnitude larger than TOFs of the reported ensemble systems. In addition, the deactivation of a single IrOx nanoparticle is also explored based on a half-width analysis of current spikes. This versatilely applicable method provides new insights into the intrinsic performance of a single nanoparticle, which is essential to reveal the structure-activity relations of nanoscale materials for the rational design of advanced catalysts.
识别单个纳米颗粒的本征电催化活性具有挑战性,因为传统的整体测量仅提供大量纳米颗粒的平均活性,并且可能会受到与纳米颗粒本身无关的整体性质的极大影响。在此,单颗粒碰撞电化学被用于研究单个IrOx纳米颗粒对析氧反应(OER)的电催化活性。碰撞频率与纳米颗粒浓度呈线性比例关系。从碰撞电流尖峰中提取的平均峰值电流和转移电荷呈现出与IrOx本征活性相关的类似电位依赖性。周转频率(TOF)被确定为1.55×102 O2 s-1,这比报道的整体系统的TOF大几个数量级。此外,还基于电流尖峰的半高宽分析探索了单个IrOx纳米颗粒的失活情况。这种广泛适用的方法为单个纳米颗粒的本征性能提供了新的见解,这对于揭示纳米级材料的结构-活性关系以合理设计先进催化剂至关重要。