Effect of interlayer anions in layered double hydroxides on the photothermocatalytic CO2 methanation of derived Ni–Al2O3 catalysts

IF 10.8 2区 化学 Q1 CHEMISTRY, PHYSICAL 物理化学学报 Pub Date : 2025-01-01 DOI:10.3866/PKU.WHXB202309002
Lina Guo , Ruizhe Li , Chuang Sun , Xiaoli Luo , Yiqiu Shi , Hong Yuan , Shuxin Ouyang , Tierui Zhang
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Abstract

The concentration of carbon dioxide (CO2) in the atmosphere is progressively increasing due to industrial development, leading to environmental concerns such as the greenhouse effect. Consequently, it is crucial to decrease dependence on the fossil fuels and mitigate the CO2 emissions. Photothermocatalysis technology facilitates the conversion of light energy into heat energy on the surface of catalysts, thereby driving chemical reactions. This catalytic approach effectively harnesses ample solar energy, consequently reducing non-renewable energy consumption. Solar-driven CO2 methanation is an important route to simultaneously mitigate excessive carbon emissions and produce fuels. Layered double hydroxides (LDH) can be reduced at high temperature in a reductive atmosphere of a hydrogen/argon (H2/Ar) mixture to prepare metal-loaded oxide (MO) catalysts, which are widely used in CO2 hydrogenation reactions as excellent photothermal catalysts. However, there is limited study on how the interlayer anion type of LDH affects the activity of CO2 methanation. Herein, a series of LDH precursors, intercalated with various anions, were synthesized using a co-precipitation method. The LDH precursors were reduced in a H2/Ar atmosphere to acquire a group of nickel (Ni) loaded on alumina (Al2O3) catalysts, referred to as NiAl-x-MO (x = CO3, NO3, Cl, and SO4, which represents carbonate, nitrate, chloride, and sulfate anions, respectively). Energy dispersive spectrometer (EDS) elemental mapping and X-ray photoelectron spectroscopy (XPS) results revealed the presence of nitrogen (N), chlorine (Cl), and sulfur (S) species on the surfaces of NiAl–NO3-MO, NiAl–Cl-MO, and NiAl–SO4-MO catalysts, respectively. Photothermocatalytic tests were conducted on the catalysts to assess the potential influence of the residual species on CO2 methanation. Among them, the NiAl–CO3-MO catalyst demonstrated a CO2 conversion of 50.1 %, methane (CH4) selectivity of 99.9 %, along with a CH4 production rate of 94.4 mmol g−1 h−1. The performance of the NiAl–NO3-MO catalyst was found to be comparable to that of the NiAl–CO3-MO catalyst. In contrast, the CO2 methanation activity of the NiAl–Cl-MO and NiAl–SO4-MO catalysts were negligible. CO2 temperature programmed desorption (CO2-TPD) analysis demonstrated that the presence of N, Cl, and S species had a negligible effect on the adsorption of CO2. H2 temperature programmed desorption (H2-TPD) and density functional theory (DFT) results suggested that the strong coordination bond between residual Cl or S species and metallic Ni impeded the absorption and activation of H2, which was responsible for the low CO2 conversion. Hence, the significant role of the interlayer anion in LDH should be preferentially considered when designing LDH-derived catalysts, especially the Ni-based catalysts for hydrogenation reactions.

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物理化学学报
物理化学学报 化学-物理化学
CiteScore
16.60
自引率
5.50%
发文量
9754
审稿时长
1.2 months
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