High-performance Pt0.01Fe0.05-g-C3N4 Catalyst for Photothermal Catalytic CO2 Reduction

doi:10.6023/A21030118

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 Pt_0.01Fe_0.05-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•g_cat^-1) for CO₂ reduction with CO selectivity (97%) under 300 W Xe lamp irradiation and CO₂/H₂ (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 Pt_0.01Fe_0.05-g-C₃N₄in 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 FeO _x 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 Pt_0.01Fe_0.05-g-C₃N₄ due to the heterojunction between FeO _x 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 H₂ over Fe and Pt acitve sites. Our work present a high-performance Pt_0.01Fe_0.05-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.

Key words: g-C₃N₄, photothermal catalysis, CO₂ reduction reaction, operando diffuse reflectance infrared Fourier transform spectroscopy

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Ruizhao Wang, Yunjie Zou, Sheng Hong, Mingkai Xu, Lan Ling. High-performance Pt_0.01Fe_0.05-g-C₃N₄ Catalyst for Photothermal Catalytic CO₂ Reduction[J]. Acta Chimica Sinica, 2021, 79(7): 932-940.

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Fig. & Tab. 11

Figure 1. XRD patterns of 5Fe1Pt AR, 5Fe1Pt BR and 5Fe0Pt

Figure 2. Full XPS pattern of 5Fe1Pt AR, and 5Fe0Pt, g-C3N4 (a), XPS pattern of high-spin Fe 2p for 5Fe1Pt BR (b) and 5Fe1Pt AR (c), Pt 4f for 5Fe1Pt BR and 5Fe1Pt AR (d), N 1s for 5Fe0Pt and 5Fe1Pt AR (e)

Figure 3. HRTEM of 5Fe1Pt BR (a) and STEM-EDS elemental mapping of 5Fe1Pt BR (b)

Figure 4. The position of the EDS line scan (a) and EDS line scan profile (b) of FeOx particle on 5Fe1Pt AR

Figure 5. N2 absorption-desorption isotherm (a) and DFT desorption pore size distribution plot (b) of 5Fe1Pt AR

Figure 6. CH4 and CO evolution rates over 5Fe1Pt, 5Fe0Pt, 0Fe1Pt, and 0.5Fe1Pt (a), and apparent photothermal-thermal activation energy contrast (b)

Figure 7. Thermal equilibrium temperatures for 5Fe1Pt, 5Fe0Pt and 0.5Fe1Pt at different power levels

Figure 8. The DRS spectra (a) and photoluminescence (PL) spectra (b) of samples

Figure 9. Photocurrent of 5Fe1Pt, 5Fe0Pt and g-C3N4

Figure 10. IR spectra of 5Fe1Pt AR under H2 (a). Operando DRIFTS for 5Fe1Pt AR following exposure to CO2/H2 (V/V, 1/1) feed gas after pretreatment with pure CO2 (b, c), following exposure to H2 after pretreatment with pure CO2 (d), and absorption changes under different reaction conditions (e)

Figure 11. Illustration of possible mechanism of photothermal CO2 reduction

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Pt_0.01Fe_0.05-g-C₃N₄催化剂高效光热催化二氧化碳还原

High-performance Pt_0.01Fe_0.05-g-C₃N₄ Catalyst for Photothermal Catalytic CO₂ Reduction

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Pt0.01Fe0.05-g-C3N4催化剂高效光热催化二氧化碳还原