Interfacial Electronic Modulation of Dual-Monodispersed Pt–Ni3S2 as Efficacious Bi-Functional Electrocatalysts for Concurrent H2 Evolution and Methanol Selective Oxidation
Qianqian Zhao, Bin Zhao, Xin Long, Renfei Feng, Mohsen Shakouri, Alisa R. Paterson, Qunfeng Xiao, Yu Zhang, Xian‐Zhu Fu, Jing‐Li Luo
Abstract
Abstract Constructing the efficacious and applicable bi-functional electrocatalysts and establishing out the mechanisms of organic electro-oxidation by replacing anodic oxygen evolution reaction (OER) are critical to the development of electrochemically-driven technologies for efficient hydrogen production and avoid CO 2 emission. Herein, the hetero-nanocrystals between monodispersed Pt (~ 2 nm) and Ni 3 S 2 (~ 9.6 nm) are constructed as active electrocatalysts through interfacial electronic modulation, which exhibit superior bi-functional activities for methanol selective oxidation and H 2 generation. The experimental and theoretical studies reveal that the asymmetrical charge distribution at Pt–Ni 3 S 2 could be modulated by the electronic interaction at the interface of dual-monodispersed heterojunctions, which thus promote the adsorption/desorption of the chemical intermediates at the interface. As a result, the selective conversion from CH 3 OH to formate is accomplished at very low potentials (1.45 V) to attain 100 mA cm −2 with high electronic utilization rate (~ 98%) and without CO 2 emission. Meanwhile, the Pt–Ni 3 S 2 can simultaneously exhibit a broad potential window with outstanding stability and large current densities for hydrogen evolution reaction (HER) at the cathode. Further, the excellent bi-functional performance is also indicated in the coupled methanol oxidation reaction (MOR)//HER reactor by only requiring a cell voltage of 1.60 V to achieve a current density of 50 mA cm −2 with good reusability.