Steering CO resistance and catalytic activity of PtRu alloy in methanol oxidation with atomically dispersed Ni

Abstract

The effective design and construction of high-performance methanol oxidation reaction (MOR) electrocatalysts are crucial for the advancement of direct methanol fuel cells. However, the active sites of MOR electrocatalysts are prone to poisoning by CO, leading to severely decayed durability. Herein, a Ni-atomically dispersed PtRu alloy catalyst is prepared via electrodeposition on stainless steel mesh (PtRuNi/SS) for CO-resistant MOR. DFT calculations reveal that the PtRu alloy with atomically dispersed Ni could adjust the electronic configuration of Pt and facilitate bond breaking between hydrogen and carbon, decreasing the binding energy of *CO. The calculation results could be clearly verified by the electrochemical attenuated total reflection infrared spectroscopy and CO stripping experiments. Consequently, PtRuNi/SS exhibits a mass activity of 0.95 A mg⁻¹_Pt for the MOR, which is 1.9 and 4.3 times that of PtRu/SS (0.51 A mg⁻¹_Pt) and commercial Pt/C (0.22 A mg⁻¹_Pt), respectively. Moreover, PtRuNi/SS demonstrates promising MOR stability, retaining 86.4% of its current density in comparison with 68.9% for PtRu/SS and 53.8% for Pt/C during accelerated durability tests. The excellent CO resistance even endows PtRuNi with robust activity in the oxidation of other alcohols like ethanol.