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Selective Photocatalytic Transformation of Lignin to Aromatic Chemicals by Crystalline Carbon Nitride in Water-Acetonitrile Solutions.

ABSTRACT: The photocatalytic conversion of lignin to aromatic compounds in aqueous solutions is a promising approach. We herein report a crystalline carbon nitride prepared by high-temperature thermal polymerization and alkali-metal molten salt treatment, which was then applied in the selective conversion of lignin to aromatic compounds. The results showed that the tri-s-tri-C₃N₄ presented a relatively high activity and selectivity for the conversion of lignin in aqueous solutions. In a 95% water-acetonitrile solution, it achieved a relatively high conversation rate of lignin, reaching 62.00%, and the selectivity of the C-C bond cleavage was high, at 86.8%. The characterization results obtained by TEM, UV-vis/DRS, PL, and transient photocurrent response showed that the ultra-high activity of tri-s-tri-C₃N₄ was mainly due to the improvements in crystallinity and light absorption. Mechanism studies showed that the dispersion of the catalyst and the combination of lignin and catalyst in aqueous solvents with different acetonitrile ratios were the main factors affecting lignin conversion. As the water content in the solutions increased, the primary active sites were converted from h⁺ to ·O₂^-. This study revealed the interactions between lignin, photocatalysts, and reaction solutions, providing a theoretical basis for the photocatalytic conversion of lignin in aqueous solutions.

SUBMITTER: Huang M

PROVIDER: S-EPMC9736535 | biostudies-literature | 2022 Nov

REPOSITORIES: biostudies-literature

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Selective Photocatalytic Transformation of Lignin to Aromatic Chemicals by Crystalline Carbon Nitride in Water-Acetonitrile Solutions.

Huang Meirou M Guo Huiqin H Zeng Zhenxing Z Xiao Hong H Hu Hong H He Liu L Li Kexin K Liu Xiaoming X Yan Liushui L

International journal of environmental research and public health 20221125 23

The photocatalytic conversion of lignin to aromatic compounds in aqueous solutions is a promising approach. We herein report a crystalline carbon nitride prepared by high-temperature thermal polymerization and alkali-metal molten salt treatment, which was then applied in the selective conversion of lignin to aromatic compounds. The results showed that the tri-s-tri-C<sub>3</sub>N<sub>4</sub> presented a relatively high activity and selectivity for the conversion of lignin in aqueous solutions. I ...[more]

PMID: 36497780

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Project description:Graphical abstract Highlights • The ultrasound was successfully utilized as a mean of precipitated synthesis of TiO2.• The ultrasound assisted synthesized TiO2 samples showed the formation of nanostructures.• The optimization of utilized frequencies and different amplitudes is necessary to alter/tuned the photoactivity.• The additive free photocatalytic selective oxidation of aromatic alcohols to corresponding products was studied.• Our novel ultrasound assisted synthesized TiO2 showed higher selectivity of products. The research for “green” and economically feasible approaches such as (photo)catalysis especially for biomass valorization such as selective oxidation of biomass derived compounds like aromatic alcohols to corresponding aldehyde by avoiding the harsh reaction conditions and the addition of reagents concentrate the focus of attention the last years. Hence, design and development of novel photocatalyst for the partial selective oxidation is highly desirable. In this research work, ultrasonication of different frequencies (22, 40, 80 kHz) and different amplitudes was utilized as synthesis tool in order to obtain novel materials by precipitation method. The synthesized samples were characterized by using different techniques such as N2 sorption, TEM, XPS, XRD, thermal analysis, and diffuse reflectance spectroscopy. The synthesized sample by using low ultrasound frequency (22 kHz) and amplitude showed a mixed morphological and structural nature consisting of asymmetric 1-dimensional (nanorods-like), layered nano-structures and not well-defined areas, leading to elevate for metal oxide specific surface areas up to 155 m2/g. The observed 1-D nanostructures have diamentions in the range of 20–60 nm. This sample revealed the highest photo-oxidation efficiency for the selective conversion of two biomass-derived, and more specifically lignin-inspired model compounds, benzyl alcohol and cinnamyl alcohol to benzaldehyde and cinnamyl aldehyde, respectively, and hence the highest yield towards the desired aldehydes. The selective photo-oxidation activity was retained even after 5 photocatalytic cycles, while no leaching of Ti was recorded.

Dataset Information

Selective Photocatalytic Transformation of Lignin to Aromatic Chemicals by Crystalline Carbon Nitride in Water-Acetonitrile Solutions.

Publications

Selective Photocatalytic Transformation of Lignin to Aromatic Chemicals by Crystalline Carbon Nitride in Water-Acetonitrile Solutions.

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