Highly efficient photo-thermal synergistic catalysis of CO2 methanation over La1−xCexNiO3 perovskite-catalyst
Solar-driven photo-thermal catalytic CO 2 methanation reaction is a promising technology to alleviate the problems posed by greenhouse gases emissions. However, designing advanced photo-thermal catalysts remains a research challenge for CO 2 methanation reaction. In this work, a series of ABO 3 (A =...
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Published in | Nano research Vol. 17; no. 9; pp. 7945 - 7956 |
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Main Authors | , , , , , , , |
Format | Journal Article |
Language | English |
Published |
Beijing
Tsinghua University Press
01.09.2024
Springer Nature B.V |
Subjects | |
Online Access | Get full text |
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Summary: | Solar-driven photo-thermal catalytic CO
2
methanation reaction is a promising technology to alleviate the problems posed by greenhouse gases emissions. However, designing advanced photo-thermal catalysts remains a research challenge for CO
2
methanation reaction. In this work, a series of ABO
3
(A = lanthanide, B = transition metal) perovskite catalysts with Ce-substituted LaNiO
3
(La
1−
x
Ce
x
NiO
3
,
x
= 0, 0.2, 0.5, 0.8, 1) were synthesized for CO
2
methanation. The La
0.2
Ce
0.8
NiO
3
exhibited the highest CH
4
formation rate of 258.9 mmol·g
−1
·h
cat
−1
, CO
2
conversion of 55.4% and 97.2% CH
4
selectivity at 300 °C with the light intensity of 2.9 W·cm
−2
. Then the catalysts were thoroughly analyzed by physicochemical structure and optical properties characterizations. The partial substitution of the A-site provided more active sites for the adsorption and activation of CO
2
/H
2
. The sources of the active sites were considered to be the oxygen vacancies (O
v
) created by lattice distortions due to different species of ions (La
3+
, Ce
4+
, Ce
3+
) and exsolved Ni
0
by H
2
reduction. The catalysts have excellent light absorption absorbance and low electron–hole (e
−
/h
+
) recombination rate, which greatly contribute to the excellent performance in photo-thermal synergistic catalysis (PTC) CO
2
methanation. The results of
in situ
irradiated electron paramagnetic resonance spectrometer (ISI-EPR) and ISI-X-ray photoelectron spectroscopy (XPS) indicated that the aggregation of unpaired electrons near the defects and Ni metal (from La and Ce ions to O
v
and Ni
0
) accelerated adsorption and activation of CO
2
/H
2
. At last, the catalyst properties and structure were correlated with the proposed reaction mechanism from the
in situ
diffuse reflection infrared Fourier transform spectrum (DRIFTS) measurements. The
in situ
precipitation of the B-site enhanced the dispersion of Ni, while its enriched photoelectrons upon illumination further promote hydrogen dissociation. More H* spillover accelerated the rate-determining step (RDS) of HCOO* hydrogenation. This work provides the theoretical basis for the development of catalysts and industrial application. |
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ISSN: | 1998-0124 1998-0000 |
DOI: | 10.1007/s12274-024-6796-x |