Dataset Information

Sunlight-driven and gram-scale vanillin production via Mn-defected γ-MnO₂ catalyst in aqueous environment.

ABSTRACT: The production of vanillin from biomass offers a sustainable route for synthesizing daily-use chemicals. However, achieving sunlight-driven vanillin synthesis through H₂O activation in an aqueous environment poses challenges due to the high barrier of H₂O dissociation. In this study, we have successfully developed an efficient approach for gram-scale vanillin synthesis in an aqueous reaction, employing Mn-defected γ-MnO₂ as a photocatalyst at room temperature. Density functional theory calculations reveal that the presence of defective Mn species (Mn³⁺) significantly enhances the adsorption of vanillyl alcohol and H₂O onto the surface of the γ-MnO₂ catalyst. Hydroxyl radical (˙OH) species are formed through H₂O activation with the assistance of sunlight, playing a pivotal role as oxygen-reactive species in the oxidation of vanillyl alcohol into vanillin. The Mn-defected γ-MnO₂ catalyst exhibits exceptional performance, achieving up to 93.4% conversion of vanillyl alcohol and 95.7% selectivity of vanillin under sunlight. Notably, even in a laboratory setting during the daytime, the Mn-defected γ-MnO₂ catalyst demonstrates significantly higher catalytic performance compared to the dark environment. This work presents a highly effective and promising strategy for low-cost and environmentally benign vanillin synthesis.

SUBMITTER: Ke Q

PROVIDER: S-EPMC10988585 | biostudies-literature | 2024 Apr

REPOSITORIES: biostudies-literature

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Sunlight-driven and gram-scale vanillin production via Mn-defected γ-MnO2 catalyst in aqueous environment.

Ke Qingping Q Zhang Yurong Y Wan Chao C Tang Jun J Li Shenglai S Guo Xu X Han Minsu M Hamada Takashi T Osman Sameh M SM Kang Yunqing Y Yamauchi Yusuke Y

Chemical science 20240219 14

The production of vanillin from biomass offers a sustainable route for synthesizing daily-use chemicals. However, achieving sunlight-driven vanillin synthesis through H2O activation in an aqueous environment poses challenges due to the high barrier of H2O dissociation. In this study, we have successfully developed an efficient approach for gram-scale vanillin synthesis in an aqueous reaction, employing Mn-defected γ-MnO2 as a photocatalyst at room temperature. De ...[more]

PMID: 38577364

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Project description:Transition metal oxides are characterized by an acute structure and composition dependent electrocatalytic activity toward the oxygen evolution (OER) and oxygen reduction (ORR) reactions. For instance, Mn containing oxides are among the most active ORR catalysts, while Ni based compounds tend to show high activity toward the OER in alkaline solutions. In this study, we show that incorporation of Ni into α-MnO2, by adding Ni precursor into the Mn-containing hydrothermal solution, can generate distinctive sites with different electronic configurations and contrasting electrocatalytic activity. The structure and composition of the Ni modified hollandite α-MnO2 phase were investigated by X-ray absorption spectroscopy (XAS), X-ray diffraction (XRD), transmission electron microscopy coupled to energy-dispersive X-ray spectroscopy (TEM-EDX), inductively coupled plasma-optical emission spectroscopy (ICP-OES), and X-ray photoelectron spectroscopy (XPS). Our analysis suggests that Mn replacement by Ni into the α-MnO2 lattice (site A) occurs up to approximately 5% of the total Mn content, while further increasing Ni content promotes the nucleation of separate Ni phases (site B). XAS and XRD show that the introduction of sites A and B have a negligible effect on the overall Mn oxidation state and bonding characteristics, while very subtle changes in the XPS spectra appear to suggest changes in the electronic configuration upon Ni incorporation into the α-MnO2 lattice. On the other hand, changes in the electronic structure promoted by site A have a significant impact in the pseudocapacitive responses obtained by cyclic voltammetry in KOH solution at pH 13, revealing the appearance of Mn 3d orbitals at the energy (potential) range relevant to the ORR. The evolution of Mn 3d upon Ni replacement significantly increases the catalytic activity of α-MnO2 toward the ORR. Interestingly, the formation of segregated Ni phases (site B) leads to a decrease in the ORR activity while increasing the OER rate.

Dataset Information

Sunlight-driven and gram-scale vanillin production via Mn-defected γ-MnO₂ catalyst in aqueous environment.

Publications

Sunlight-driven and gram-scale vanillin production <i>via</i> Mn-defected γ-MnO<sub>2</sub> catalyst in aqueous environment.

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