2 research outputs found
Manipulating the Morphology and Electronic State of a Two-Dimensional Coordination Polymer as a Hydrogen Evolution Cocatalyst Enhances Photocatalytic Overall Water Splitting
To
achieve efficacious photocatalytic overall water splitting,
surface modification of photocatalysts with proficient cocatalysts
for hydrogen evolution reaction (HER) is imperative. NiBHT, a conductive
two-dimensional coordination polymer (2D CP), or a 2D metal–organic framework (2D MOF), endowed
with remarkable chemical stability and HER selectivity, emerged as
a promising candidate for an HER cocatalyst. However, the bulky morphology
of NiBHT hampered its performance. Here, we demonstrate a strategy
to miniaturize NiBHT by incorporating the benzene-1,2-dithiol (BDT)
ligand, yielding NiBHT nanoparticles (NiBHT-NP). Beyond morphology,
empirical evidence unveiled alterations in the electronic state and
catalytic activity of NiBHT-NP, and the ramifications of BDT modulation
on intrinsic characteristics are elucidated through density functional
theory (DFT) calculations. As a model system, CoOx/SrTiO3:Al photocatalyst with NiBHT-NP modification
exhibited an apparent quantum efficiency (AQE) of 10.3% at 365 nm
for overall water splitting. This pioneering work showcases that a
modulator ligand may manipulate the morphology, electronic state,
and catalytic behavior of 2D CPs, holding prodigious potential for
developing more effective CP-based HER
cocatalysts