聚卟啉<strong>/MXene</strong>基自支撑复合薄膜的光催化降解性能

doi:10.11901/1005.3093.2024.050

材料研究学报

2024, Vol. 38

Issue (12): 950-960 DOI: 10.11901/1005.3093.2024.050

研究论文

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聚卟啉/MXene基自支撑复合薄膜的光催化降解性能

霍朝晖(

), 吴豪杰, 何泳淇, 郑明秀, 詹曼姿, 张绮彤, 廖晓琳

广东第二师范学院化学与材料科学学院广州 510303

Polyporphyrin/MXene-based Self-supporting Composite Films and Photocatalytic Degradation of Pollutants

HUO Zhaohui(

), WU Haojie, HE Yongqi, ZHENG Mingxiu, ZHAN Manzi, ZHANG Qitong, LIAO Xiaolin

School of Chemistry and Materials Science, GuangDong University of Education, Guangzhou 510303, China

引用本文:

霍朝晖, 吴豪杰, 何泳淇, 郑明秀, 詹曼姿, 张绮彤, 廖晓琳. 聚卟啉/MXene基自支撑复合薄膜的光催化降解性能[J]. 材料研究学报, 2024, 38(12): 950-960.
Zhaohui HUO, Haojie WU, Yongqi HE, Mingxiu ZHENG, Manzi ZHAN, Qitong ZHANG, Xiaolin LIAO. Polyporphyrin/MXene-based Self-supporting Composite Films and Photocatalytic Degradation of Pollutants[J]. Chinese Journal of Materials Research, 2024, 38(12): 950-960.

全文: PDF(11543 KB) HTML

摘要:

以八乙基卟啉锌和4,4-联吡啶为单体、以多层Ti₃C₂ (MXene自支撑膜)为载体，用阳极氧化法制备聚卟啉/MXene基自支撑复合薄膜光催化剂，使用扫描电子显微镜(SEM）、傅立叶变换红外光谱仪(FTIR)、X射线衍射仪(XRD)、X射线光电子能谱(XPS)、电化学阻抗谱(EIS)、光电化学测试(I-t)等手段对其表征，研究了这种光催化剂对亚甲基蓝的降解性能。结果表明：将聚卟啉负载在MXene薄膜上可促进光生电子对的分离从而提高其催化效率和回收重复使用。用阳极氧化法将聚卟啉负载在MXene上，可增大MXene层间距、避免MXene重堆叠和提高MXene的孔洞率。在聚卟啉/MXene基复合薄膜的面积为1 cm²、亚甲基蓝的初始浓度为10 mg/L的条件下，光照80 min后复合薄膜对亚甲基蓝的降解率高达98.00%。在光催化降解亚甲基蓝过程中，这种光催化剂中起主要作用的是自由基h⁺。

关键词 ：复合材料, 卟啉, MXene自支撑膜, 阳极氧化法, 光催化, 亚甲基蓝

Abstract：

Herein, photocatalyst composite films of polyporphyrin/MXene were prepared via anodic oxidation method with octaethyl porphyrin zinc and 4,4-bipyridine as monomers, and multi-layered Ti₃C₂ as MXene self-supporting film, with the aim to prepare a novel material with high-photocatalysis efficiency for degradation of dyestuffs wastewaters. The prepared catalyst was characterized by scanning electron microscopy, Fourier transform infrared spectroscopy, X-ray powder diffraction, X-ray photoelectron spectroscopy, electrochemical impedance spectroscopy, photoelectrochemical testing etc. The photocatalytic degradation effect of the synthesized self-supporting composite film photocatalyst on methylene blue was assessed through photocatalytic degradation testing. The results indicate that loading polyporphyrin onto MXene thin films can promote the separation of photo generated electron pairs, improve the efficiency of polyporphyrin photocatalysis, and achieve reusable recycling of materials. The increase in interlayer spacing of MXene was achieved by loading polyporphyrin onto the MXene through anodic oxidation, effectively solving the problem related with restacking and increasing the porosity of MXene. When the area of the polyporphyrin/MXene based composite film is 1 cm² and the initial concentration of methylene blue is 10 mg/L, the degradation rate of methylene blue by the composite material reaches 98% after 80 minutes of illumination. The capture experiment shows that the main free radical playing a role in the photocatalytic degradation of methylene blue is h⁺.

Key words： composite material porphyrin MXene self-supporting membrane anodic oxidation method photocatalytic Methylene blue

收稿日期: 2024-01-22

ZTFLH:

O643.36

基金资助:广东省基础与应用基础研究基金(粤穗联合基金)(2023A1515111132);广州市基础与应用基础项目(202102020424);大学生创新创业训练计划(202414278081);广东省普通高校重点领域专项(2023ZDZX4043)

通讯作者: 霍朝晖，副教授，huozhaohui@gdei.edu.cn，研究方向为光电催化、电分析

Corresponding author: HUO Zhaohui, Tel: 13422197623, E-mail: huozhaohui@gdei.edu.cn

作者简介: 霍朝晖，女，1986年生，博士

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https://www.cjmr.org/CN/10.11901/1005.3093.2024.050 或 https://www.cjmr.org/CN/Y2024/V38/I12/950

图1 聚卟啉/MXene复合薄膜的合成示意图

图2 Ti3AlC2、Ti3C2、MXene(Ti3C2)膜截面形貌图、MXene薄膜截面形貌图和聚卟啉/MXene复合薄膜截面的SEM照片

图3 聚卟啉/MXene复合薄膜的FT-IR谱

图4 聚卟啉/MXene复合薄膜的XRD谱

图5 Ti 2p、O 1s、N 1s、C 1s、Zn 2p的XPS谱

图6 聚卟啉/MXene复合薄膜的EIS谱和I-t测试曲线

表1 亚甲基蓝在卟啉/MXene基复合膜上的吸附动力学拟合数据

图7 吸附动力学拟合曲线及其表达式

图8 亚甲基蓝的标准曲线和自降解

图9 H2O2对光催化剂降解性能的影响、不同材料对亚甲基蓝的光催化降解率、不同材料对亚甲基蓝的光催化降解性能以及不同自由基捕获剂存在下聚卟啉/MXene复合薄膜对亚甲基蓝的降解率

图10 聚卟啉/MXene复合薄膜对亚甲基蓝的光催化降解机理

图11 聚卟啉/MXene复合薄膜的循环使用寿命

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