Yoo Su-Hyun, Aota Leonardo Shoji, Shin Sangyong, El-Zoka Ayman A, Kang Phil Woong, Lee Yonghyuk, Lee Hyunjoo, Kim Se-Ho, Gault Baptiste
Max-Planck Institut für Eisenforschung GmbH, 40237 Düsseldorf, Germany.
Department of Materials, Imperial College London, SW7 2AZ London, United Kingdom.
ACS Energy Lett. 2023 Jul 14;8(8):3381-3386. doi: 10.1021/acsenergylett.3c00842. eCollection 2023 Aug 11.
Introduction of interstitial dopants has opened a new pathway to optimize nanoparticle catalytic activity for, e.g., hydrogen evolution/oxidation and other reactions. Here, we discuss the stability of a property-enhancing dopant, B, introduced through the controlled synthesis of an electrocatalyst Pd aerogel. We observe significant removal of B after the hydrogen oxidation reaction. calculations show that the high stability of subsurface B in Pd is substantially reduced when H is adsorbed/absorbed on the surface, favoring its departure from the host nanostructure. The destabilization of subsurface B is more pronounced, as more H occupies surface sites and empty interstitial sites. We hence demonstrate that the H fuel itself favors the microstructural degradation of the electrocatalyst and an associated drop in activity.
间隙掺杂剂的引入为优化纳米颗粒的催化活性开辟了一条新途径，例如用于析氢/氧化反应及其他反应。在此，我们讨论通过电催化剂钯气凝胶的可控合成引入的性能增强掺杂剂硼（B）的稳定性。我们观察到在氢氧化反应后硼有显著去除。计算表明，当氢吸附/吸收在钯表面时，钯中次表面硼的高稳定性会大幅降低，这有利于硼离开主体纳米结构。随着更多氢占据表面位点和空的间隙位点，次表面硼的失稳更加明显。因此，我们证明氢燃料本身有利于电催化剂的微观结构降解及相关的活性下降。
