纳米纤维素/氮化碳复合气凝胶的制备及应用

doi:10.3969/j.issn.1673-5854.2023.04.002

摘要/Abstract

摘要：

以三聚氰胺(M)和三聚氰酸(C)为原料, 在水相中充分混合制备得到富含氢键的前驱体; 随后通过高温聚合反应制备得到三维状片层卷曲堆叠的多孔氮化碳(g-C₃N₄)材料(MC-s-CN)。探讨了聚合过程中前躯体内氢键对催化性能的影响, 结果表明氢键的引入很大程度减少了g-C₃N₄的块状堆叠, 提升了其比表面积, 使表面积达到74.111 9 m²/g, 为传统氮化碳M-CN的8.7倍。通过荧光光谱、光电流和电化学阻抗测试, 进一步证明MC-s-CN具有更好的光生载流子传输速率和更低的复合速率, 最终降解罗丹明染料模拟废水的效果相较传统方法提升了12.52倍。以2, 2, 6, 6-四甲基哌啶氧化物氧化的纳米纤维素(TCNF)为骨架材料, 依靠分子间氢键交联作用, 将MC-s-CN倒入TCNF悬浮液中通过定向冷冻的方式成功制备得到大比表面积和良好吸附性能的复合气凝胶材料(CN-TCA)。经测试, CN-TCA具有良好的光催化降解性能, 在120 min可见光照射下对罗丹明溶液的降解率达到91%, 同时其循环使用性能优异, 在5次循环后仍具有原始状态94.08%的降解效果。

关键词: 类石墨相氮化碳, 光催化, 纳米纤维素, 气凝胶

Abstract:

The hydrogen bond-riched precursors were prepared by mixing melamine and cyanuric acid in aqueous phase. Subsequently, the porous carbon nitride(g-C₃N₄) materials(MC-s-CN) with three-dimensional lamellar curl stacks were prepared by high temperature polymerization. The effect of hydrogen bonds within the precursor on the catalytic performance during the polymerization process was investigated. The results showed that the introduction of hydrogen bonding greatly reduced the blocky stacking of g-C₃N₄ material and increased its specific surface area to 74.111 9 m²/g, which was 8.7 times that of traditional carbon nitride M-CN. The better photogenerated carrier transport rate and lower complexation rate of MC-s-CN were further proved by fluorescence spectroscopy, photocurrent and electrochemical impedance tests. Finally, the degradation effect of simulated rhodamine dye wastewater was 12.52 times higher than that of traditional method. Then, the nanocelluloses oxidized by 2, 2, 6, 6-tetramethylpiperidine oxide were used as the skeleton materials, and the composite aerogel materials(CN-TCA) with large specific surface area and excellent adsorption performance were successfully prepared by directional freezing relying on the cross-linking of intermolecular hydrogen bonds. The CN-TCA was tested to has good photocatalytic degradation performance, and the degradation rate of rhodamine solution reached 91% under 120 min visible light irradiation. Additionally, the CN-TCA had great recycling performance, and the degradation effect was still 94.08% in the original state after five cycles.

Key words: g-C₃N₄, photocatalysis, nano cellulose, aerogel

中图分类号:

TQ35
TS72

曾劲松, 张泽新, 刘冰洋, 李鹏飞. 纳米纤维素/氮化碳复合气凝胶的制备及应用[J]. 生物质化学工程, 2023, 57(4): 17-26.

Jinsong ZENG, Zexin ZHANG, Bingyang LIU, Pengfei LI. Preparation and Application of Nanocellulose Carbon Nitride Composite Aerogel[J]. Biomass Chemical Engineering, 2023, 57(4): 17-26.

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样品samples	比表面积specific surface area/(m²·g^-1)¹⁾			总孔体积pore volume/(cm³·g^-1)
样品samples	S_total	S_mic	S_ext	总孔体积pore volume/(cm³·g^-1)
U-CN	9.877 5	0.950 7	8.926 8	0.061 58
M-CN	8.519 0	1.288 3	7.230 7	0.069 78
MC-g-CN	17.650 3	3.124 9	14.525 5	0.117 99
MC-s-CN	74.111 9	8.412 5	65.699 4	0.512 03

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