微纤复合硼掺杂碳纳米管膜催化剂的制备及其对苯酚的降解性能

doi:10.11901/1005.3093.2023.609

材料研究学报

2024, Vol. 38

Issue (12): 893-901 DOI: 10.11901/1005.3093.2023.609

研究论文

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微纤复合硼掺杂碳纳米管膜催化剂的制备及其对苯酚的降解性能

庄超君, 胡俊辉, 鄢瑛(

)

华南理工大学化学与化工学院广州 510640

Preparation of Paper-like Stainless Steel Fiber Coated with Boron-doped Carbon Nanotubes Catalyst and Its Application for Phenol Degradation

ZHUANG Chaojun, HU Junhui, YAN Ying(

)

School of Chemistry and Chemical Engineering, South China University of Technology, Guangzhou 510640, China

引用本文:

庄超君, 胡俊辉, 鄢瑛. 微纤复合硼掺杂碳纳米管膜催化剂的制备及其对苯酚的降解性能[J]. 材料研究学报, 2024, 38(12): 893-901.
Chaojun ZHUANG, Junhui HU, Ying YAN. Preparation of Paper-like Stainless Steel Fiber Coated with Boron-doped Carbon Nanotubes Catalyst and Its Application for Phenol Degradation[J]. Chinese Journal of Materials Research, 2024, 38(12): 893-901.

全文: PDF(10341 KB) HTML

摘要:

以苯硼酸为前驱体用化学气相沉积(CVD)法在纸状烧结不锈钢微纤载体(PSSF)表面生长出硼掺杂碳纳米管(B-CNT)膜，构成了具有梯度多孔结构的微纤复合硼掺杂碳纳米管膜无金属催化剂(B-CNTs/PSSF)。使用FE-SEM、TEM、Raman、TG和XPS等手段对其表征，研究催化剂对苯酚的湿式催化降解性能。结果表明，B-CNTs/PSSF对苯酚的降解性能比CNTs/PSSF优异，苯酚的转化率为100%，总有机碳(TOC)的转化率达到68%。根据密度泛函理论(DFT)的研究发现，产生催化性能差异的原因是，B-CNT对H₂O₂的吸附性能比CNT更强以及片段间的电子转移。

关键词 ：复合材料, 硼掺杂碳纳米管, 湿式催化氧化, 密度泛函理论, 无金属催化剂

Abstract：

A new type of boron-doped carbon nanotube (B-CNT) film was successfully grown on the surface of paper- sintered stainless steel fiber (PSSF) carrier via chemical vapor deposition (CVD) method with phenylboronic acid as precursor, constituting a metal-free composite catalyst of boron-doped carbon nanotube membrane with gradient porous structure on PSSF (B-CNTs/PSSF). The B-CNTs/PSSF was characterized by means of FE-SEM, TEM, Raman, TG and XPS, and then applied to the degradation of phenol. The results showed that the prepared B-CNTs/PSSF had a better phenol degradation performance than CNTs/PSSF without B doping, with a phenol conversion rate of 100%, a total organic carbon conversion rate of 68%. Based on the density functional theory (DFT), it was found that the difference in catalytic performance comes from the stronger adsorption and mutual electron transfer of H₂O₂ by B-CNT than CNT.

Key words： composite boron doped carbon nanotubes catalytic wet peroxide oxidation density functional theory metal-free catalyst

收稿日期: 2023-12-26

ZTFLH:

TQ032

基金资助:国家自然科学基金(22178122)

通讯作者: 鄢瑛，副研究员，yingyan@scut.edu.cn，研究方向为吸附与催化

Corresponding author: YAN Ying, Tel: 13902490801, E-mail: yingyan@scut.edu.cn

作者简介: 庄超君，男，1999年生，硕士生

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https://www.cjmr.org/CN/10.11901/1005.3093.2023.609 或 https://www.cjmr.org/CN/Y2024/V38/I12/893

图1 CVD法制备B-CNTs/PSSF的示意图

图2 苯酚在结构化固定床反应器上湿式催化氧化实验流程图

图3 二次煅烧的PSSF、CNTs/PSSF、B-CNTs/PSSF的SEM图和B-CNTs/PSSF的TEM像

图4 CNTs/PSSF和B-CNTs/PSSF的FTIR谱

图5 B-CNTs/PSSF和CNTs/PSSF的Raman谱

图6 B-CNTs/PSSF和CNTs/PSSF的TG曲线

图7 B-CNTs/PSSF的XPS全谱、C1s、B1s和O1s的高分辨谱

图8 不同催化剂对苯酚CWPO的催化性能

图9 CNT对H2O2的吸附构型、吸附能和电子密度差图以及B-CNT对H2O2的吸附构型和电子密度差图

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