Herein, by modulating trivalent/tetravalent metallic
elements,
NiMLDHs (M = Al, Co, Fe, Mn, and Ti) were successfully prepared and
evaluated in photocatalytic CO2 reduction reaction (PCRR).
Photocatalytic results declared that the electronic yields followed
the order of NiTiLDH > NiCoLDH > NiFeLDH > NiMnLDH > NiAlLDH.
Multiple
characterizations affirmed that the introduction of various trivalent/tetravalent
metallic elements could visibly affect the three critical aspects:
(i) light harvesting; (ii) charge separation and transfer; and (iii)
surface reactions, thus governing PCRR performance. Importantly, an
in-depth mechanistic investigation was conducted by in situ diffuse
reflectance infrared Fourier transform spectroscopy (DRIFTS) experiments.
These layered double hydroxides (LDHs) exhibited different adsorption/activation
behaviors toward CO2 molecule: NiAlLDH primarily converted
CO2 into b-CO3
2– species;
NiCoLDH, NiFeLDH, and NiMnLDH could induce c-CO3
2– intermediate; NiTiLDH could generate a higher proportion of •CO2
– species, which was
an important intermediate to produce CO. More favorable carries separation
and adsorption/activation process was presented upon NiTiLDH, thus
more markedly enhancing photoactivity.
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