Integrated CO2 capture and utilization (ICCU)
has been
regarded as an innovative strategy to realize large-scale CO2 emission reduction. The rational design of robust dual-function
materials (DFMs) and the optimization of operating parameters are
essential for the intensification of the ICCU process. In this work,
Ni-CaO DFMs pellets with Ni loadings varying in the 1–20 wt
% range are prepared for CO production via integrated CO2 capture and reversed water gas shift (RWGS) reaction. The effect
of Ni loading on the structure–reactivity relationships of
the Ni-CaO DFMs pellets is investigated. CO2 capture capacity
decreases noticeably at higher loadings of 15 and 20 wt % due to reduced
surface basicity. Increased Ni loading enhances reducibility but results
in increased Ni particle size, decreased Ni specific surface area,
and inferior Ni dispersion, and CO yield thus increases first and
then declines. CO2 conversion and CO selectivity are almost
free from the Ni loading effect. The influences of operating parameters
on the ICCU performance of the 5Ni-CaO-P DFMs pellets are investigated
using an orthogonal experimental design. The influencing degree of
the operating parameters on CO2 capture capacity follows
the order of H2 concentration for catalyst reduction >
reaction temperature > CO2 concentration > weight
hourly
space velocity (WHSV). Reaction temperature and H2 concentration
in the RWGS stage represent the two primary factors affecting the
CO2 conversion performance. Multiple linear regression
analyses are performed, and regression equations for describing the
relationships between the various attributes and predictors are acquired.
The optimal combination of the operating variables is identified as
the reaction temperature of 650 °C, WHSV of 135 000 mL/(h·gcat), 25% H2 for catalyst reduction, 10% CO2 for capture, and 5% H2 for in situ RWGS. The desired
5Ni-CaO-P sample exhibits a high CO2 uptake of 16.05 mmol
of CO2/g, a great CO yield of 5.77 mmol of CO/g, a remarkable
CO2 conversion of ∼99%, a great CO selectivity of
∼90%, and good stability in multiple cycles under optimized
working conditions. These results will guide the rational design of
DFMs pellets and lay the groundwork for their scale-up applications
in ICCU.