研磨-焙烧法制备La2O3/BiOCl复合光催化剂及其对高浓度染料降解性能

doi:10.15541/jim20150075

无机材料学报 ›› 2015, Vol. 30 ›› Issue (9): 943-949.DOI: 10.15541/jim20150075

研磨-焙烧法制备La₂O₃/BiOCl复合光催化剂及其对高浓度染料降解性能

陈建钗¹, 余长林¹, 李家德^{1, 2}, 方稳¹, 何洪波¹

(1. 江西理工大学冶金与化学工程学院, 赣州 341000; 2. 福州大学能源与环境光催化国家重点实验室, 福州350002)

收稿日期:2015-02-02 修回日期:2015-05-13 出版日期:2015-09-20 网络出版日期:2015-08-19
作者简介:陈建钗(1988–), 女, 硕士. E-mail: chenjianchai3719@126.com
基金资助:
国家自然科学基金 (21067004, 21263005);江西省自然科学基金青年科学基金(20133BAB21003);江西省教育厅高等学校科技落地计划项目(KJLD14046);江西省青年科学家培养项目(20122BCB23015);江西省远航工程

Preparation by Grinding-calcination and Photocatalytic Performance of La₂O₃/BiOCl Composite Photocatalysts

CHEN Jian-Chai¹, YU Chang-Lin¹, LI Jia-De^{1, 2}, FANG Wen¹, HE Hong-Bo¹

(1. School of Metallurgy and Chemical Engineering, Jiangxi University of Science and Technology, Ganzhou 341000, China; 2.?State Key Laboratory of Photocatalysis on Energy and Environment, Fuzhou University, Fuzhou 350002, China)

Received:2015-02-02 Revised:2015-05-13 Published:2015-09-20 Online:2015-08-19
About author:CHEN Jian-Chai. E-mail: chenjianchai3719@126.com
Supported by:
National Natural Science Foundation of China (21067004, 21263005);Young Science and Technology Project of Jiangxi Province Natural Science Foundation China (20133BAB21003);The Landing Project of Science and Technology of Colleges and Universities in Jiangxi Province (KJLD14046);Young Scientist Training Project of Jiangxi Province China (20122BCB23015);Yuan Hang Gong Cheng Project of Jiangxi Province

摘要/Abstract

摘要：

首先利用沉淀法合成了BiOCl纳米片, 然后利用研磨-焙烧法将La₂O₃纳米颗粒复合到BiOCl纳米片中, 制备了一系列La₂O₃/BiOCl复合光催化剂(La₂O₃: 1wt%、2wt%、4wt%、8wt%)。运用X射线粉末衍射(XRD)、扫描电镜(SEM)、透射电镜(TEM)、光电子能谱(XPS)、紫外-可见漫反射光谱(UV-Vis DRS)、傅里叶红外光谱(FT-IR)和光致发光(PL)谱等对样品的晶相、光吸收和表面性能等进行了表征。以紫外灯(λ = 254 nm)为光源, 评价了所制备样品光催化降解高浓度染料酸性橙II(40×10^-6)的活性。结果表明, 经过研磨-焙烧后该系列催化剂均具有较好的结晶性能, 同时2~5 nm的La₂O₃纳米粒子粘附在BiOCl纳米片表面。200℃焙烧制备的1wt%La₂O₃/BiOCl催化剂具有丰富的表面羟基, 对染料表现出较强的吸附性能。该催化剂表现了最高的光催化活性, 活性为纯BiOCl的2.4倍。另外, La₂O₃/BiOCl中的La³⁺提供的氧化-还原势阱可能捕获光生电子, 从而阻止了光生电子(e^-)和空穴(h⁺)的复合, 有利于光催化活性的提高。

关键词: La2O3/BiOCl, 光催化, 稀土, 高浓度染料, 研磨-煅烧

Abstract:

BiOCl nanoplates were firstly prepared by precipitation method and then La₂O₃/BiOCl composite photocatalysts with different La₂O₃ contents (1wt%, 2wt%, 4wt%, 8wt%) were synthesized by grinding-calcination procedure. The physical chemistry properties of the as-prepared photocatalysts were characterized by powder X-ray diffraction (XRD), scanning electron microscope (SEM), transmission electron microscope (TEM), UV-Vis diffuse reflectance spectroscope (DRS), X-ray photoelectron spectroscope (XPS), Fourier transformed infrared spectroscope (FT-IR), and photoluminescence (PL) spectroscope. The photocatalytic activity of the samples was evaluated by photocatalytic degradation of high concentration acid orange II (40×10^-6) under UV light (λ=254 nm) irradiation. Results showed that the as-prepared samples have good crystallinity. La₂O₃ particles with the size of 2-5 nm were closely combined with BiOCl nanoplate after grinding-calcination treatment. La₂O₃/BiOCl composite photocatalysts with 1wt% La₂O₃ calcined at 200℃ displayed the best photocatalytic activity which is 2.4 times of that of pure BiOCl. The produced La₂O₃/BiOCl has abundant surface OH groups and highly suitable adsorption of dye. Moreover, La³⁺ could capture the photon-generated electrons (e^-) and prevent the recombination of photon-generated and holes (h⁺).

Key words: La2O3/BiOCl, photocatalysis, rare earth, high concentration dye, grinding-calcination

中图分类号:

TB321
O643

陈建钗, 余长林, 李家德, 方稳, 何洪波. 研磨-焙烧法制备La₂O₃/BiOCl复合光催化剂及其对高浓度染料降解性能[J]. 无机材料学报, 2015, 30(9): 943-949.

CHEN Jian-Chai, YU Chang-Lin, LI Jia-De, FANG Wen, HE Hong-Bo. Preparation by Grinding-calcination and Photocatalytic Performance of La₂O₃/BiOCl Composite Photocatalysts[J]. Journal of Inorganic Materials, 2015, 30(9): 943-949.

图/表 10

图1 所制备BiOCl和La2O3/BiOCl样品的XRD图谱

Fig. 1 XRD patterns of the prepared BiOCl and La2O3/BiOCl samples (a) La2O3/BiOCl with different La2O3 contents calcined at 200℃; (b) 1wt% La2O3/BiOCl calcined at different temperatures

图2 所制备BiOCl和La2O3/BiOCl样品的扫描电镜照片

Fig. 2 SEM images of the prepared BiOCl and La2O3/BiOCl samples (a) 1wt% La2O3/BiOCl(200℃); (b) 4wt% La2O3/BiOCl (200℃); (b) 8wt% La2O3/BiOCl (200℃); (d) 1wt% La2O3/BiOCl(500℃)

图3 BiOCl和2wt% La2O3/BiOCl(200℃)的透射电镜照片

Fig. 3 TEM images of BiOCl (a) and 2wt% La2O3/BiOCl (200℃) (b)

图4 2wt% La2O3/BiOCl(200℃)的EDX图谱

Fig. 4 EDX pattern of the La2O3/BiOCl(200℃) sample

图5 所制备BiOCl和La2O3/BiOCl样品的紫外-可见漫反射吸收光谱

Fig. 5 UV-Vis DRS spectra of the prepared BiOCl and La2O3/BiOCl samples (a) La2O3/BiOCl with different La2O3 contents calcined at 200℃; (b) 1wt% La2O3/BiOCl calcined at different temperatures

图6 所制备BiOCl和La2O3/BiOCl样品的FT-IR图谱

Fig. 6 FT-IR spectra of the prepared BiOCl and La2O3/BiOCl samples (a) La2O3/BiOCl with different La2O3 content calcined at 200℃; (b) 1wt% La2O3/BiOCl calcined at different temperatures

图7 200 ℃焙烧1wt%La2O3/BiOCl的XPS图谱

Fig. 7 XPS spectra of 1wt%La2O3/BiOCl calcined at 200 ℃ (a) Full survey spectrum; (b) La3d; (c) Bi4f; (d) O1s; (e) Cl2p

图8 200℃焙烧制备的La2O3/BiOCl样品降解染料的活性比较

Fig. 8 Activity comparison of the La2O3/BiOCl samples calcined at 200℃

图9 不同焙烧温度制备的1wt% La2O3/BiOCl样品降解染料的活性比较

Fig. 9 Activity comparison of the 1wt% La2O3/BiOCl samples calcined at different temperatures

图10 1%La2O3/BiOCl(200℃)及BiOCl样品在0.01 mol/L香豆素溶液中的光致发光谱图

Fig. 10 PL spectra of BiOCl and 1wt% La2O3/BiOCl (200℃) dispersed in 0.01 mol/L coumarin aqueous solution

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研磨-焙烧法制备La₂O₃/BiOCl复合光催化剂及其对高浓度染料降解性能

Preparation by Grinding-calcination and Photocatalytic Performance of La₂O₃/BiOCl Composite Photocatalysts

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