Bionanofiber Assisted Decoration of Few‐Layered MoSe2 Nanosheets on 3D Conductive Networks for Efficient Hydrogen Evolution

Abstract

Molybdenum diselenide (MoSe₂) has emerged as a promising electrocatalyst for hydrogen evolution reaction (HER). However, its properties are still confined due to the limited active sites and poor conductivity. Thus, it remains a great challenge to synergistically achieve structural and electronic modulations for MoSe₂-based HER catalysts because of the contradictory relationship between these two characteristics. Herein, bacterial cellulose-derived carbon nanofibers are used to assist the uniform growth of few-layered MoSe₂ nanosheets, which effectively increase the active sites of MoSe₂ for hydrogen atom adsorption. Meanwhile, carbonized bacterial cellulose (CBC) nanofibers provide a 3D network for electrolyte penetration into the inner space and accelerate electron transfer as well, thus leading to the dramatically increased HER activity. In acidic media, the CBC/MoSe₂ hybrid catalyst exhibits fast hydrogen evolution kinetics with onset overpotential of 91 mV and Tafel slope of 55 mV dec⁻¹, which is much more outstanding than both bulk MoSe₂ aggregates and CBC nanofibers. Furthermore, the fast HER kinetics are well supported by theoretical calculations of density-functional-theory analysis with a low activation barrier of 0.08 eV for H₂ generation. Hence, this work highlights an efficient solution to develop high-performance HER catalysts by incorporating biotemplate materials, to simultaneously achieve increased active sites and conductivity.