Abstract
AbstractSelf‐standing two‐dimensional P‐doped molybdenum diselenide (MoSe2) nanosheets were synthesized on carbon fiber paper (CFP) (P‐doped MoSe2/CFP) using a hydrothermal reaction followed by phosphorization and were subsequently used as a high‐efficiency hydrogen evolution reaction (HER) electrocatalyst. Nanosheet aggregation was remarkably inhibited, and numerous active sites were exposed. The H adsorption and desorption capacities of MoSe2 were optimized by doping P atoms in the MoSe2 lattice. Electrochemical testing indicated that the overpotential (η50) required by P‐doped MoSe2/CFP was only 186 mV, which was much lower than that of the as‐prepared MoSe2/CFP (237 mV). The Tafel slope of P‐doped MoSe2/CFP was 54.3 mV ⋅ dec−1, which was remarkably lower than that of the as‐prepared MoSe2/CFP (79.8 mV ⋅ dec−1). The Gibbs energy of the H atoms adsorbed on P‐doped MoSe2 (ΔGH*) reached the lowest value (0.202 eV) when the hydrogen coverage (θH) was 75 %. For MoSe2, the lowest ΔGH* value was 0.296 eV when θH was 25 %. The adsorption and desorption of H atoms at the active sites of P‐doped MoSe2 occurred easier than at the active sites of MoSe2. Moreover, the P doping effect facilitated the formation of more Hads species during the Volmer reaction and substantially accelerated the kinetics of the HER.
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