石墨烯-铁酸铋纳米晶复合材料的制备及其催化性能研究

doi:10.15541/jim20200594

无机材料学报 ›› 2021, Vol. 36 ›› Issue (7): 725-732.DOI: 10.15541/jim20200594 CSTR: 32189.14.10.15541/jim20200594

石墨烯-铁酸铋纳米晶复合材料的制备及其催化性能研究

李铁¹(), 李玥¹, 王颖异², 张珽¹

1.中国科学院苏州纳米技术与纳米仿生研究所, 苏州 215123
2.西交利物浦大学, 苏州 215123

收稿日期:2020-10-19 修回日期:2021-01-27 出版日期:2021-07-20 网络出版日期:2021-03-01
作者简介:李铁(1984-), 男, 副研究员. E-mail:tli2014@sinano.ac.cn
基金资助:
国家重点研发计划(2017YFA0701101);国家重点研发计划(2020YFB2008501);国家自然科学基金(62071462);国家自然科学基金(51702354);中国科学院青年促进会(2020320);江苏省基础研究计划面上项目(BK20201195);苏州市重点产业技术创新项目(SYG202029)

Preparation and Catalytic Properties of Graphene-Bismuth Ferrite Nanocrystal Nanocomposite

LI Tie¹(), LI Yue¹, WANG Yingyi², ZHANG Ting¹

1. Suzhou Institute of Nano-Tech and Nano-Bionics, Chinese Academy of Sciences, Suzhou 215123, China
2. Xi’an Jiao-tong Liverpool University, Suzhou 215123, China

Received:2020-10-19 Revised:2021-01-27 Published:2021-07-20 Online:2021-03-01
About author:LI Tie(1984-), male, associate professor. E-mail:tli2014@sinano.ac.cn
Supported by:
National Key R&D Program of China(2017YFA0701101);National Key R&D Program of China(2020YFB2008501);National Natural Science Foundation of China(62071462);National Natural Science Foundation of China(51702354);Youth Promotion Association of Chinese Academy of Sciences(2020320);Foundation Research Project of Jiangsu Province(BK20201195);Suzhou Key Industrial Technology Innovation Project(SYG202029)

摘要/Abstract

摘要：

BiFeO₃(BFO)是一种新型可回收光响应催化剂, 但较高的光生电子/空穴对复合率和较低的量子产率限制了其实际应用。本研究通过水热法制备出还原氧化石墨烯-BFO(RGO-BFO)纳米晶复合材料, 表征与测试结果表明, 相比于BFO颗粒, 复合材料的禁带宽度E_g为2.0 eV, 降低约10%; 40 min对亚甲基蓝吸附-催化效率接近100%, 远高于BFO颗粒(28%), 这主要由于复合体系中光生电子/空穴对复合率更低。通过本征磁性回收并重复利用6次后, 复合材料仍保持89.1%催化效率, 表现出优异催化性能。

关键词: 铁酸铋, 纳米晶, 石墨烯, 催化降解

Abstract:

BiFeO₃ (BFO) is a novel recyclable photocatalyst which benefits from its appropriate theoretical band gap and room temperature ferromagnetism, yet the relatively high recombination rate of photogenerated electron-hole pairs and low quantum yield limit its practical catalytic performance. Here, a composite material of reduced graphene oxide and BiFeO₃ nanocrystals (RGO-BFO) was successfully prepared via a hydrothermal self-assembly process with about 10wt% RGO loaded 85wt% BFO nanocrystalline (~10 nm). Specific surface area of the composite is about 5 times of that of pure BFO particles. Furthermore, this nanocomposite demonstrates the enhanced ultraviolet absorption behavior as well as its intrinsic visible light absorption, with an energy gap (E_g) of 2.0 eV, which is about 10% lower than BFO particles (2.3 eV). As a result, a significantly higher catalytic efficiency of nearly 100% of the RGO-BFO was obtained as compared to the 25% value of BFO after a 40-min process of adsorption and photodegradation for methylene blue. The improved performances may be attributed to the additional photogenerated electron-hole pairs and lower recombination ratio, which can be proved by the result of photoelectric response. As an intrinsically ferromagnetic material, it could be easily recycled from the solvent system, and its repetitive catalytic efficiency maintained 89.1% after 6 cycles, showing a good catalytic stability.

Key words: bismuth ferrite, nanocrystals, graphene, catalytic degradation

中图分类号:

O643

李铁, 李玥, 王颖异, 张珽. 石墨烯-铁酸铋纳米晶复合材料的制备及其催化性能研究[J]. 无机材料学报, 2021, 36(7): 725-732.

LI Tie, LI Yue, WANG Yingyi, ZHANG Ting. Preparation and Catalytic Properties of Graphene-Bismuth Ferrite Nanocrystal Nanocomposite[J]. Journal of Inorganic Materials, 2021, 36(7): 725-732.

图/表 6

图1 RGO-BFO制备流程示意图

Fig. 1 Preparation process illustration of the RGO-BFO nanocrystal nanocomposite

图2 RGO-BFO纳米晶复合材料的形貌和成分分析结果

Fig. 2 Morphology and composition characterizations of RGO-BFO nanocrystal nanocomposite (a) SEM/EDX; (c-d) TEM/SEAD and (e-f) AFM

表1 RGO-BFO复合体系与BFO的比表面积对比表

Table 1 Comparision of specific surface area between RGO-BFO composite and BFO

Sample	S_BET/(m²·g^-1)	S_Langmuir/(m²·g^-1)	S_T-method/(m²·g^-1)	V_{pore, HK method}/(cm³·g^-1)	D_{pore, HK method}/nm
RGO-BFO	23.124	39.536	23.1240	0.00651	0.3675
BFO	4.763	7.237	1.8463	0.15020	1.9020

图3 RGO-BFO纳米晶复合材料的结构和组成

Fig. 3 Structure and composition analysis of RGO-BFO nanocrystal nanocomposite (a) XRD patterns; (b) FT-IR spectra; (c) Raman spectra; (d) TG curves; (e-f) XPS peaks

图4 RGO-BFO纳米晶复合材料性质及紫外光催化降解MB性能图

Fig. 4 Physical properties and photocatalytic MB degradation performances of RGO-BFO nanocrystal nanocomposite (a) M-H magnetic curve; (b-c) UV-Vis absorption spectra and calculated result of optical band gap; (d) Absorption spectra of MB solution under various time nodes; (e) Degradation effects of various controlled samples; (f) Cyclic performance of the composite

图5 RGO-BFO纳米晶复合材料光电响应机制

Fig. 5 Photoelectric response mechanism of RGO-BFO nanocrystal nanocomposite (a) Photogenerated currents of the controlled sample; (b) Degradation mechanism of the nanocrystal composite

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石墨烯-铁酸铋纳米晶复合材料的制备及其催化性能研究

Preparation and Catalytic Properties of Graphene-Bismuth Ferrite Nanocrystal Nanocomposite

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