Preparation and Photothermal Catalytic Application of Powder-form Cobalt Plasmonic Superstructures

doi:10.15541/jim20210458

Abstract

Abstract:

Highly light absorptive photocatalysts are of great significance to boost the photothermal conversion efficiency. Light trapping effect of nanoarray structured photothermal catalysts can enhance the light absorption and improve the photothermal conversion efficiency. However, the practical applications of array-based catalysts are hindered by very low loadings of active metal catalysts per unit illumination area. Herein, we develop a SiO₂-protected MOFs pyrolysis method for the preparation of powder-form cobalt plasmonic superstructures that enable a 90% absorption efficiency of sunlight and tunable metal loading per unit area. Its high light absorption capacity was confirmed by time-domain finite-difference simulation calculations due to the plasmonic hybridization effect of nanoparticles. Compared with nanoarray-structured plasmonic superstructures, the powder-form catalyst exhibit enhanced catalytic activity and stability, resulting in the increase of CO₂ conversion efficiency from 0.9% to 26.2%. This study lays the foundation for the practical application of non-precious metal photothermal catalysts.

Key words: photothermal catalysis, carbon dioxide hydrogenation, plasmonic superstructure, strong light absorptive catalyst, solar-to-chemical energy conversion

CLC Number:

TQ174

WANG Xiao, ZHU Zhijie, WU Zhiyi, ZHANG Chengcheng, CHEN Zhijie, XIAO Mengqi, LI Chaoran, HE Le. Preparation and Photothermal Catalytic Application of Powder-form Cobalt Plasmonic Superstructures[J]. Journal of Inorganic Materials, 2022, 37(1): 22-28.

Figures/Tables 7

Fig. 1 Preparation and characterization of Co-SiO2 (a) Schematic illustration of preparation of Co and Co-SiO2 catalysts, TEM images of (b) ZIF-67-SiO2, (c) Co and (d) Co-SiO2, (e) HRTEM, (f) SAED and (g-j) elemental mappings of Co-SiO2

Fig. 2 XRD patterns of (a) ZIF-67, ZIF-67-SiO2, and (b) Co and Co-SiO2

Fig. 3 (a) Diffuse reflectance spectra of Co-SiO2 and Co (insets showing photographs of two catalysts), (b) dependence of calculated normalized extinction cross-section of Co nanostructures on the number of Co nanoparticles (n) in the chain, and surface temperature of (c) Co catalyst and (d) Co-SiO2 catalyst

Fig. 4 Catalytic activity and CO selectivity of Co-SiO2 under different light intensities

Table 1 CO2 conversion efficiencies of different catalysts in photothermal hydrogenation of carbon dioxide

Sample	Metal mass per unit area /(mg·cm^-2)	Size of Co/nm	CO₂ conversion /%	CO selectivity /%
Co-SiO₂-1	0.41	27	11.9	61.0
Co-SiO₂-2	0.86	27	17.6	34.9
Co-SiO₂-3	1.4	27	26.2	29.7
Co-SiO₂-4	1.7	27	24.8	27.2
Co-PS@SiO₂	0.32	25	0.9	70.4

Fig. 5 Stability of Co-SiO2 and Co in thermocatalytic CO2 hydrogenation at 300 ℃ (a) CO2 conversion rate; (b) CO selectivity

Fig. 6 (a) TEM image and (b) particle size distribution of spent Co-SiO2

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