The defect engineering of low-dimensional
nanostructured
materials
has led to increased scientific efforts owing to their high efficiency
concerning high-performance electrocatalysts that play a crucial role
in renewable energy technologies. Herein, we report an efficient methodology
for fabricating atomically thin, holey metal-phosphide nanosheets
with excellent electrocatalyst functionality. Two-dimensional, subnanometer-thick,
holey Ru2P nanosheets containing crystal defects were synthesized
via the phosphidation of monolayer RuO2 nanosheets. Holey
Ru2P nanosheets exhibited superior electrocatalytic activity
for the hydrogen evolution reaction (HER) compared to that exhibited
by nonholey Ru2P nanoparticles. Further, holey Ru2P nanosheets exhibited overpotentials of 17 and 26 mV in acidic and
alkaline electrolytes, respectively. Thus, they are among the best-performing
Ru–P-based HER catalysts reported to date. In situ spectroscopic
investigations indicated that the holey nanosheet morphology enhanced
the accumulation of surface hydrogen through the adsorption of protons
and/or water, resulting in an increased contribution of the Volmer–Tafel
mechanism toward the exceptional HER activity of these ultrathin electrocatalysts.