The design of active and stable Pt-based nanoscale electrocatalysts for the oxygen reduction reaction (ORR) plays the central role in ameliorating the efficiency of proton exchange membrane fuel-cells towards future energy applications. On that front, theoretical studies have contributed significantly to this research area by gaining deeper insights and understanding of the ongoing processes. In this work, we present an approach capable of characterizing differently-shaped platinum nanoparticles undergoing thermally- and adsorbate-induced restructuring of the surface. Further, by performing ReaxFF-Grand Canonical Molecular Dynamics simulations we explored the water formation on these roughened (“realistic”) nanoparticles in a H₂/O₂ environment. Taking into consideration the coverage of oxygen-containing intermediates and occurring surface roughening the nanoparticles’ activities were explored. Hereby, we succeeded in locally resolving the water formation on the nanoparticles’ surfaces, allowing an allocation of the active sites for H₂O production. We observed that exposed, low-coordinated sites as well as pit-shaped sites originating from roughening of vertices and edges are most active towards H₂O formation.

用于氧还原反应（ORR）的活性和稳定的基于Pt的纳米级电催化剂的设计在改善质子交换膜燃料电池对未来能源应用的效率方面起着核心作用。在这一方面，理论研究通过获得更深刻的见识和对正在进行的过程的理解，为该研究领域做出了重大贡献。在这项工作中，我们提出了一种能够表征经历热和吸附物诱导的表面重构的不同形状的铂纳米粒子的方法。此外，通过执行ReaxFF-Grand Canonical分子动力学模拟，我们探索了在H ₂ / O _2中这些粗糙（“现实”）纳米粒子上的水形成。环境。考虑到含氧中间体的覆盖和发生的表面粗糙化，研究了纳米粒子的活性。因此，我们成功地局部解决了纳米颗粒表面的水形成问题，从而为H ₂ O生产分配了活性位点。我们观察到，暴露的，低配位的部位以及源自顶点和边缘变粗糙的凹坑状部位对H ₂ O的形成最为活跃。