论文标题
在PTAU中的结晶缺陷处的化学分配是稳定电催化剂的途径
Chemical Partitioning at Crystalline Defects in PtAu as a Pathway to Stabilize Electrocatalysts
论文作者
论文摘要
在长期和动态操作中,电催化剂在能量转化和储存设备(例如燃料电池和电解液)中的挑战性问题。为了开发稳定的电催化剂,我们采用了隔离工程的设计概念,该设计概念使用容易发生的溶质分离来在内部缺陷(即晶界和脱位)下进行电化学溶解。我们通过稳定模型PT催化剂来展示这种方法的可行性,并添加了更多贵族AU(约5个原子百分比)。我们表征了缺陷的纳米级结构和化学,并通过在线电感耦合等离子体质谱法监测了PT和PTAU合金的电化学溶解。一旦隔离到缺陷,AU原子就可以稳定并因此钝化了针对电化学溶解的最脆弱的部位,并提高了PT电催化剂的稳定性和寿命,而不是数量级。这为使用溶质隔离以开发更稳定的纳米级电催化剂的途径打开了途径,这是一种适用于各种催化系统的概念。
Dissolution of electrocatalysts during long-term and dynamic operation is a challenging problem in energy conversion and storage devices such as fuel cells and electrolyzers. To develop stable electrocatalysts, we adopt the design concept of segregation engineering, which uses solute segregation prone to electrochemical dissolution at internal defects, i.e., grain boundaries and dislocations. We showcase the feasibility of this approach by stabilizing a model Pt catalyst with an addition of more noble Au (approximately 5 atomic percent). We characterized the defects' nanoscale structure and chemistry, and monitored the electrochemical dissolution of Pt and PtAu alloys by online inductively coupled plasma mass spectrometry. Once segregated to defects, Au atoms can stabilize and hence passivate the most vulnerable sites against electrochemical dissolution and improve the stability and longevity of the Pt electrocatalysts by more than an order of magnitude. This opens pathways to use solute segregation to defects for the development of more stable nanoscale electrocatalysts, a concept applicable for a wide range of catalytic systems.