A series of NiMoP(
x
)-Al catalysts with different
phosphorus contents were prepared by the incipient wetness co-impregnation
method. The effects of phosphorus modification on the acidity, active
phase nanostructure, and catalytic properties of the residue hydrodenitrogenation
catalysts were investigated to find the role of phosphorus in the
catalytic mechanism. The results of temperature-programmed desorption
of NH
3
and pyridine IR spectroscopy of the catalysts indicate
that phosphorus modification can increase the total acid and Brønsted
acid. Transmission electron microscopy analysis shows that phosphorus
modification increases the stacking number
N
A
, reduces the slab length
L
A
of
the active MoS
2
phase, and increases the Mo dispersion
f
Mo
, leading to the promotion of the sulfidation
degree of the active Mo phase and thus increasing the denitrification
rate. The catalyst with a 3.4 wt % P
2
O
5
loading
shows the highest Brønsted/Lewis acid ratio, the largest amount
of three-layer active phases, the smallest
L
A
, the highest
f
Mo
, the optimal
sulfurization degree, and the highest denitrification rate, 63.6%,
indicating the correlation between the nanostructure of the active
phase and its catalytic property because of the addition of phosphorus.