Reversible Redox Property of Co(III) in Amorphous Co-doped SiO2/γ-Al2O3 Layered Composites
Abstract
:1. Introduction
2. Experimental Procedures
2.1. Sample Synthesis
2.1.1. Co-Doped SiO2/γ-Al2O3 Layered Composite Sample
2.1.2. Co-Doped SiO2/γ-Al2O3 Composite Powder Sample
2.1.3. Homogeneous Co-Doped Aluminosilicate Powder Sample
2.1.4. γ-Al2O3/Co-Doped SiO2/γ-Al2O3 Layered Composite Membrane Sample
2.2. Characterizations
2.2.1. Characterization Techniques
2.2.2. In Situ Characterizations
- heat-treatment to remove adsorbed water at 500 °C for 8 h under a flow of Ar (4 mL·min−1).
- subsequent heat treatment at 500 °C for 0.5 h under a flow of H2 (4 mL·min−1).
- final heat treatment at 500 °C for 8 h under a flow of Ar (4 mL·min−1).
3. Results and Discussion
3.1. Distribution of Co Cations within the Co-Doped SiO2/γ-Al2O3 Layered Composite Sample
3.2. Properties of Co-Doped SiO2/γ-Al2O3 Composites
3.3. Redox Behavior of Co Species
- The reduction-oxidation of Co cation species in the CoSiOAlpow sample is associated with the formation-deformation of OH groups.
- The redox reactions begin to proceed at relatively low temperatures around 250–350 °C.
- The redox reactions are reversible and governed by the H2 partial pressure at T ≥ 250 °C.
3.4. Gas Permeation Properties of γ-Al2O3/Co-doped SiO2/γ-Al2O3 Layered Composite Membrane
4. Conclusions
- XPS depth profile analyses for the Co-doped SiO2/mesoporous γ-Al2O3 layered composite sample revealed preferential Co diffusion from the SiO2 top-layer matrix to the γ-Al2O3 surface, and the equilibrium chemical composition of the Al, Si, and Co within the mesoporous γ-Al2O3 layer was determined as Al:Si:Co = 85:10:5.
- XRD, HRTEM, and HAADF-STEM analyses revealed that the Co-doped SiO2/γ-Al2O3 composite powder sample with the equilibrium composition of Al:Si:Co = 85:10:5 kept its amorphous state without crystallization of Co oxides after H2 treatment at 500 °C.
- In situ XANES spectroscopic analyses during the 500 °C heat treatment under H2 flow and subsequent cooling to RT under Ar flow exhibited reversible redox properties of Co cations in the Co-doped SiO2/γ-Al2O3 composite powder sample.
- XPS and DRIFT spectroscopic analyses and cyclic TPR/TPD measurements concluded the reversible Co(III)/Co(II) redox reactions were associated with OH formation (hydrogenation)-deformation (dehydrogenation) within amorphous aluminosilicate, which was governed by the H2 partial pressure at 250–500 °C.
- The Co(III) cations in the present composite samples formed via the Fenton reaction in the presence of H2O2 during the sample syntheses.
- Gas permeation measurements for the γ-Al2O3/Co-doped SiO2/γ-Al2O3 layered composite membrane under the cyclic He–H2–He flow suggested that H2 triggered a chemical valve property: micropores under He flow (closure) and mesopores under H2 flow (open), which could be explained by the reversible redox reactions of Co(III)/(II) associated with bond cleavage (hydrogenation)-regeneration (dehydrogenation) of the Si–O–Al amorphous network formed in situ at the hetero interface of the Co-doped SiO2/γ-Al2O3.
Supplementary Materials
Author Contributions
Funding
Acknowledgments
Conflicts of Interest
References
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Tada, S.; Saito, S.; Mori, A.; Mizuno, H.; Ando, S.; Asaka, T.; Daiko, Y.; Honda, S.; Bernard, S.; Iwamoto, Y. Reversible Redox Property of Co(III) in Amorphous Co-doped SiO2/γ-Al2O3 Layered Composites. Materials 2020, 13, 5345. https://doi.org/10.3390/ma13235345
Tada S, Saito S, Mori A, Mizuno H, Ando S, Asaka T, Daiko Y, Honda S, Bernard S, Iwamoto Y. Reversible Redox Property of Co(III) in Amorphous Co-doped SiO2/γ-Al2O3 Layered Composites. Materials. 2020; 13(23):5345. https://doi.org/10.3390/ma13235345
Chicago/Turabian StyleTada, Shotaro, Shota Saito, Akito Mori, Hideki Mizuno, Shiori Ando, Toru Asaka, Yusuke Daiko, Sawao Honda, Samuel Bernard, and Yuji Iwamoto. 2020. "Reversible Redox Property of Co(III) in Amorphous Co-doped SiO2/γ-Al2O3 Layered Composites" Materials 13, no. 23: 5345. https://doi.org/10.3390/ma13235345