Interfacial electronic structure and electrocatalytic performance modulation in Cu0.81Ni0.19 nanoflowers by heteroatom doping engineering using ionic liquid dopant

Abstract

Alloy is highly desirable for electrocatalysis due to its superconductivity and structural stability. However, it remains a great challenge to synthesize by a facile synthetic strategy and investigate the synergistic effect for various active components. Herein, a Cu0.81Ni0.19 alloy electrocatalyst doped with N, P, and F heteroatom is constructed by a simple liquid reduction method using ionic liquid as reducing agent and heteroatom dopant. The introduction of ionic liquid not only induces the flower-like morphological characteristics of the Cu0.81Ni0.19 alloy, but also regulates its interfacial electronic structure. This hybrid catalyst exhibits outstanding electrocatalytic performance towards the OER and HER in alkaline medium with ultralow overpotentials of 198 mV and 88 mV at 10 mA·cm−2, respectively, which is among the most efficient Cu-based alloy electrocatalysts up to now. Combined with DFT calculations indicate that both the electronic structure and the reaction energy barrier of the intermediate are regulated by these heteroatoms in electrocatalysis process. This work opens up a facile method to highly efficient and durable alloy electrocatalysts using ionic liquid as a dopant, and is a promising candidate strategy for other alloy catalysts.