纺织学报 ›› 2022, Vol. 43 ›› Issue (03): 58-63.doi: 10.13475/j.fzxb.20201201106

• 纤维材料 • 上一篇    下一篇

负载MIL-53(Fe)的改性聚丙烯腈纤维光催化剂的制备及其性能

邓杨1, 石现兵1, 王涛1, 刘利伟2, 韩振邦1()   

  1. 1.天津工业大学 纺织科学与工程学院, 天津 300387
    2.天津市远大工贸有限公司, 天津 301600
  • 收稿日期:2020-12-04 修回日期:2021-12-30 出版日期:2022-03-15 发布日期:2022-03-29
  • 通讯作者: 韩振邦
  • 作者简介:邓杨(1996—),女,硕士生。主要研究方向为光催化纤维材料。
  • 基金资助:
    国家自然科学基金青年基金项目(52003192);天津市技术创新引导专项基金项目(20YDTPJC00920);天津市应用基础与前沿技术研究计划青年项目(15JCQNJC06300)

Preparation and performance of modified polyacrylonitrile fibers photocatalyst with MIL-53(Fe)

DENG Yang1, SHI Xianbing1, WANG Tao1, LIU Liwei2, HAN Zhenbang1()   

  1. 1. School of Textile Science and Engineering, Tiangong University, Tianjin 300387, China
    2. Tianjin Yunda Industry and Trade Co., Ltd., Tianjin 301600, China
  • Received:2020-12-04 Revised:2021-12-30 Published:2022-03-15 Online:2022-03-29
  • Contact: HAN Zhenbang

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摘要：

针对MIL-53(Fe)粉末作为光催化剂的光响应范围窄、催化效率低和难回收利用等问题,以偕胺肟改性聚丙烯腈(PAN)纤维作为载体,通过表面原位合成法制备了负载不规则MIL-53(Fe)的纤维MIL-53(Fe)-PAN。借助扫描电子显微镜、X射线衍射仪、红外光谱仪和紫外-可见漫反射光谱仪对其表面形态、微观结构和光吸收性能进行表征,并对其在染料降解中的光催化性能进行了研究。结果表明:原位合成的MIL-53(Fe)能够均匀分布于改性PAN纤维表面,部分MIL-53(Fe)呈现出一定的结晶性能,且纤维配体的电荷转移(LMCT)效应将其光谱响应范围拓宽至800 nm;由于纤维配体和对苯二甲酸配体的协同作用,使得MIL-53(Fe)-PAN在染料降解中显示出极高的可见光催化活性,远优于MIL-53(Fe)粉末及其直接负载改性PAN纤维催化剂,为高效金属有机框架材料(MOFs)光催化剂的结构调控提供了新的思路。

关键词: 金属有机框架材料, 改性聚丙烯腈纤维, 原位合成, 光催化剂, 染料降解, 废水处理

Abstract:

MIL-53(Fe) powder suffers from limited photoabsorption, low catalytic efficiency and poor recycling ability in the application of photocatalysis. A highly efficient MIL-53(Fe) photocatalyst was constructed with irregular structure via an in-situ synthesis method using amidoximated polyacryloni-trile(PAN) fiber as the support. The surface morphology, microstructure and light absorption performance of the photocatalyst were characterized and analyzed by scanning electron microscope, X-ray diffraction, Fourier transform infrared spectroscopy and UV-Vis diffuse reflectance spectroscopy, and the photocatalytic performance was evaluated by the degradation of an organic dye. The results indicate that the in-situ synthesized MIL-53(Fe) are evenly distributed on the modified PAN fibrous support, and partial MIL-53(Fe) exhibit certain crystalline properties. Furthermore, the fibrous ligand greatly extends the spectral response of MIL-53(Fe) to 800 nm through ligand-to-metal charge transfer (LMCT) effect. Benefiting from the synergistic effect of fiber ligand and terephthalic acid ligand, the in-situ produced MIL-53(Fe) shows high photocatalytic activity for dye degradation under visible light irradiation, much superior to the MIL-53(Fe) powder and the fiber supported MIL-53(Fe) using a direct combination method. The findings provide a novel approach to design high-efficiency photocatalysts based on metal organic framework materials.

Key words: metal organic frameworks, modified polyacrylonitrile fiber, in-situ synthesis, photocatalyst, dye degradation, wastewater treatment

中图分类号: 

  • TQ619.2

图1

AO-PAN和MIL-53(Fe)-PAN的扫描电镜照片及MIL-53(Fe)-PAN的元素分布图(×1 000)"

图2

AO-PAN及MIL-53(Fe)系列催化剂的XRD谱图"

图3

AO-PAN及MIL-53(Fe)系列催化剂的红外谱图"

图4

AO-PAN及MIL-53(Fe)系列催化剂的紫外-可见漫反射光谱谱图"

图5

MIL-53(Fe)系列催化剂对RhB的降解曲线"

图6

AO-PAN氰基转化率对MIL-53(Fe)-PAN催化活性的影响"

图7

捕捉剂对MIL-53(Fe)-PAN光催化染料降解率的影响"

图8

溶液pH值对MIL-53(Fe)-PAN光催化活性的影响"

[1] 谢艳新, 刘海娟, 尚磊, 等. 染料废水处理最新研究进展[J]. 印染助剂, 2020,37(7):11-16.
XIE Yanxin, LIU Haijuan, SHANG Lei, et al. The latest research progress of dye wastewater treatment[J]. Textile Auxiliaries, 2020,37(7):11-16.
[2] 任南琪, 周显娇, 郭婉茜, 等. 染料废水处理技术研究进展[J]. 化工学报, 2013,64(1):84-94.
REN Nanqi, ZHOU Xianjiao, GUO Wanqian, et al. Research progress of dye wastewater treatment technology[J]. CIESC Journal, 2013,64(1):84-94.
[3] 钱怡帆, 周堂, 张礼颖, 等. 聚丙烯腈/醋酸纤维素/TiO2复合纳米纤维膜的制备及其光催化降解性能[J]. 纺织学报, 2020,41(5):8-14.
QIAN Yifan, ZHOU Tang, ZHANG Liying, et al. Preparation of polyacrylonitrile/cellulose acetate/TiO2 composite nanofiber membrane and its photocatalytic degradation performance[J]. Journal of Textile Research, 2020,41(5):8-14.
[4] 李庆, 管斌斌, 王雅, 等. 光敏剂敏化Cu-有机骨架对活性深蓝K-R 的高效光催化降解[J]. 纺织学报, 2020,41(10):87-93.
LI Qing, GUAN Binbin, WANG Ya, et al. Photosensitizers sensitized Cu-organic framework for highly efficient photocatalytic degradation of Reactive Dark Blue K-R[J]. Journal of Textile Research, 2020,41(10):87-93.
[5] 张金水, 王博, 王心晨. 氮化碳聚合物半导体光催化[J]. 化学进展, 2014,26(1):19-29.
ZHANG Jinshui, WANG Bo, WANG Xinchen. Carbon nitride polymer semiconductor photocatalysis[J]. Progress in Chemistry, 2014,26(1):19-29.
[6] HAN Z B, DENG Y, FEI J W, et al. Facile synjournal of amidoximated PAN fiber-supported TiO2 for visible light driven photocatalysis[J]. Colloids and Surfaces A-Physicochemical and Engineering Aspects, 2020,600:10.
[7] ZHANG Y, ZHOU J, CHEN J, et al. Rapid degradation of tetracycline hydrochloride by heterogeneous photocatalysis coupling persulfate oxidation with MIL-53(Fe) under visible light irradiation[J]. Journal of Hazardous Materials, 2020,392:122315.
doi: 10.1016/j.jhazmat.2020.122315
[8] YANG C, YOU X, CHENG J H, et al. A novel visible-light-driven in-based MOF/graphene oxide composite photocatalyst with enhanced photocatalytic activity toward the degradation of amoxicillin[J]. Applied Catalysis B-Environmental, 2017,200:673-680.
doi: 10.1016/j.apcatb.2016.07.057
[9] LIANG R, JING F, SHEN L, et al. MIL-53(Fe) as a highly efficient bifunctional photocatalyst for the simultaneous reduction of Cr(VI) and oxidation of dyes[J]. Journal of Hazardous Materials, 2015,287:364-372.
doi: 10.1016/j.jhazmat.2015.01.048
[10] HAN Z, HAN X, ZHAO X, et al. Iron phthalocyanine supported on amidoximated PAN fiber as effective catalyst for controllable hydrogen peroxide activation in oxidizing organic dyes[J]. Journal of Hazardous Materials, 2016,320:27-35.
doi: 10.1016/j.jhazmat.2016.08.004
[11] HAN Z, GUO J, LI W. Fe(bpy)32+ supported on amidoximated PAN fiber as effective catalyst for the photodegradation of organic dye under visible light irradiation[J]. Chemical Engineering Journal, 2013,228:36-44.
doi: 10.1016/j.cej.2013.05.006
[12] HAN Z, DONG Y, DONG S. Copper-iron bimetal modified PAN fiber complexes as novel heterogeneous Fenton catalysts for degradation of organic dye under visible light irradiation[J]. Journal of Hazardous Materials, 2011,189(1/2):241-248.
doi: 10.1016/j.jhazmat.2011.02.026
[13] 韩旭. 基于铁系金属配合物的负载型纤维集合体的构筑及其光催化性能研究[D]. 天津:天津工业大学, 2018: 1-200.
HAN Xu. Study on the construction and photocatalytic performance of supported fiber aggregates based on iron-based metal complexes[D]. Tianjin: Tiangong University, 2018: 1-200.
[14] 韩磊. 聚丙烯腈非均相偕胺肟化及其对铀酰离子吸附行为的研究[D]. 哈尔滨:哈尔滨工程大学, 2019: 1-88.
HAN Lei. Study on heterogeneous amidoximation of polyacrylonitrile and its adsorption behavior for uranyl ions[D]. Harbin: Harbin Engineering University, 2019: 1-88.
[15] 闫增元. MIL-53(Fe)光催化去除废水中典型核化污染物研究[D]. 北京: 军事科学院, 2019: 1-85.
YAN Zengyuan. Photocatalytic removal of typical nuclear pollutants from wastewater by MIL-53 (Fe)[D]. Beijing: Academy of Military Sciences, 2019: 1-85.
[16] LIU N, ZHENG Y J, JING C W, et al. Boosting catalytic degradation efficiency by incorporation of MIL-53(Fe) with Ti3C2Tx nanosheeets[J]. Journal of Molecular Liquids, 2020,311:113201.
doi: 10.1016/j.molliq.2020.113201
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