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Abstract:
Converting CO2 into value-added compounds via photothermal catalysis is a promising strategy to reduce CO2 emission and might be a sustainable alternative to traditional fossil fuels. Here, we report nano-structured a Pt0.01Fe0.05-g-C3N4 hybrid catalyst synthesized via hydrothermal-method and further reduced under reaction condition for the reverse water gas shift (RWGS) reaction. Taking advantage of the photo-thermal effect caused by the near-infrared (NIR) and visible light responsive, the hybrid catalyst produces a remarkable activity (7.36 mmol.h(-1).gcat(-1)) for CO2 reduction with CO selectivity (97%) under 300 W Xe lamp irradiation and CO2/H-2 (V/V, 1/1) feed gas. The apparent activation energy of reaction decreases from 238.59 kJ/mol to 48.88 kJ/mol calculated by Arrhenius formula. In order to comprehend the good catalytic activity of Pt0.01Fe0.05-g-C3N4 in the RWGS reaction, the catalyst is characterized with powder X-ray diffraction (XRD), spherical-aberration-corrected scanning transmission electron microscopy (Cs-S/TEM) integrated with X-ray energy dispersive spectroscopy (EDS), X-ray photoelectron spectroscopy (XPS), UV-vis-NIR diffuse reflectance spectroscopy (DRS), etc. for investigating the structural information, surface state, optical properties and so on. Results show that the presence of FeOx and Pt exhibits strong absorption in a wide range from UV to NIR regions. Low photoluminescence (PL) intensity at about 460 nm shows the suppressed photogenerated carrier recombination process of Pt0.01Fe0.05-g-C3N4 due to the heterojunction between FeOx and g-C3N4. Operando diffuse reflectance infrared Fourier transform spectroscopy (DRIFTS) under different reaction conditions is employed to investigate surface species and their evolution during the conversion of CO2 into CO and a broad IR absorption is observed due to hydrogen spillover from Pt to Fe3O4. Therefore, we propose a possible mechanism of photothermal catalytic CO2 reduction, involving separate activation of CO2 and H-2 over Fe and Pt acitve sites. Our work present a high-performance Pt0.01Fe0.05-g-C3N4 catalyst for RWGS reaction and open a new vista of the design, synthesis and mechanism research of photothermal catalytic CO2 conversion in the future.
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ACTA CHIMICA SINICA
ISSN: 0567-7351
CN: 31-1320/O6
Year: 2021
Issue: 7
Volume: 79
Page: 932-940
2 . 7 8 9
JCR@2021
1 . 7 0 0
JCR@2023
ESI HC Threshold:117
JCR Journal Grade:3
CAS Journal Grade:3
Cited Count:
SCOPUS Cited Count: 7
ESI Highly Cited Papers on the List: 0 Unfold All
WanFang Cited Count:
Chinese Cited Count:
30 Days PV: 1
Affiliated Colleges: