Yu Haoran, Zachman Michael J, Reeves Kimberly S, Park Jae Hyung, Kariuki Nancy N, Hu Leiming, Mukundan Rangachary, Neyerlin Kenneth C, Myers Deborah J, Cullen David A
Center for Nanophase Materials Sciences, Oak Ridge National Laboratory, Oak Ridge, Tennessee 37831, United States.
Chemical Sciences and Engineering Division, Argonne National Laboratory, Lemont, Illinois 60439, United States.
ACS Nano. 2022 Aug 23;16(8):12083-12094. doi: 10.1021/acsnano.2c02307. Epub 2022 Jul 22.
Nanoparticles are an important class of materials that exhibit special properties arising from their high surface area-to-volume ratio. Scanning transmission electron microscopy (STEM) has played an important role in nanoparticle characterization, owing to its high spatial resolution, which allows direct visualization of composition and morphology with atomic precision. This typically comes at the cost of sample size, potentially limiting the accuracy and relevance of STEM results, as well as the ability to meaningfully track changes in properties that vary spatially. In this work, automated STEM data acquisition and analysis techniques are employed that enable physical and compositional properties of nanoparticles to be obtained at high resolution over length scales on the order of microns. This is demonstrated by studying the localized effects of potential cycling on electrocatalyst degradation across proton exchange membrane fuel cell cathodes. In contrast to conventional, manual STEM measurements, which produce particle size distributions representing hundreds of particles, these high-throughput automated methods capture tens of thousands of particles and enable nanoparticle size, number density, and composition to be measured as a function of position within the cathode. Comparing the properties of pristine and degraded fuel cells provides statistically robust evidence for the inhomogeneous nature of catalyst degradation across electrodes. These results demonstrate how high-throughput automated STEM techniques can be utilized to investigate local phenomena occurring in nanoparticle systems employed in practical devices.
纳米颗粒是一类重要的材料,因其高比表面积与体积比而展现出特殊性质。扫描透射电子显微镜(STEM)在纳米颗粒表征中发挥了重要作用,这得益于其高空间分辨率,能够以原子精度直接观察成分和形态。然而,这通常以牺牲样品尺寸为代价,可能会限制STEM结果的准确性和相关性,以及有意义地追踪空间变化性质的能力。在这项工作中,采用了自动化的STEM数据采集和分析技术,能够在微米量级的长度尺度上以高分辨率获取纳米颗粒的物理和成分性质。通过研究电势循环对质子交换膜燃料电池阴极电催化剂降解的局部影响来证明这一点。与传统的手动STEM测量不同,传统测量产生的是代表数百个颗粒的粒径分布,而这些高通量自动化方法能够捕获数万个颗粒,并能够测量纳米颗粒的尺寸、数密度和成分随阴极内位置的变化。比较原始燃料电池和降解燃料电池的性质,为电极间催化剂降解的不均匀性质提供了具有统计学说服力的证据。这些结果表明了高通量自动化STEM技术如何能够用于研究实际装置中使用的纳米颗粒系统中发生的局部现象。