CaO,
as a relatively inexpensive and readily available adsorbent,
has been widely used in areas such as the removal of heavy metal pollutants,
but CaO produces sintering with an increasing temperature, which seriously
influences its adsorption capacity. This work uses the urea-assisted
Pechini sol–gel technique and innovatively combines As2O3 (g) adsorption experiments with theoretical
calculations to prepare sintering-resistant Ni/CaO adsorbents. The
experimental results showed that the Ni/Ca-2 (Ni doping mass ratio
is 2%) adsorbent exhibited excellent adsorption performance, and its
adsorption of arsenic reached 602.56 mg/kg at 700 °C, which is
2.89 times higher compared to that of pure CaO. The unique structure
formed by trace Ni doping effectively prevented the sintering phenomenon
of CaO, significantly enlarged the specific surface area of the adsorbent,
added more adsorption sites, and also helped the system to convert
the lattice oxygen into chemisorbed oxygen. In addition, the adsorption
of As2O3 on Ni/CaO adsorbent was simulated by
using a density functional theory approach. The results showed that
the main active adsorption sites of Ni/CaO were the O sites in NiO
and CaO, and the presence of Ni atoms enhanced the As2O3 adsorption energy on the CaO surface. The reason for this
is that Ni undergoes strong orbital hybridization with the O atoms
in the system, and the Ni atoms provide more free electrons to the
O atoms, which contribute to the electron redistribution on the CaO
(001) surface. This also suggests that Ni acts as a kind of bridge
for electron transfer during the reaction. The Ni/CaO adsorbent proposed
in this article provides a useful guide for the development of composite
adsorbent materials.