一种可见光活性的等离子体纳米Au-Cu(I)@Na2Ti6O13光催化滤膜的制备和对乙醛的降解

doi:10.1016/S1872-2067(17)62954-1

催化学报 ›› 2017, Vol. 38 ›› Issue (12): 2048-2055.DOI: 10.1016/S1872-2067(17)62954-1

一种可见光活性的等离子体纳米Au-Cu(I)@Na₂Ti₆O₁₃光催化滤膜的制备和对乙醛的降解

杨静静, 刘保顺, 赵修建

武汉理工大学硅酸盐建筑国家重点实验室, 湖北武汉 430070

收稿日期:2017-10-01 修回日期:2017-10-31 出版日期:2017-12-18 发布日期:2017-12-29
通讯作者: 刘保顺, 赵修建
基金资助:
国家自然科学基金（51772230，51461135004）；湖北省对外科技合作项目（2017AHB059）；日本学术振兴会外籍邀请研究员基金（L16531）.

A visible-light-active Au-Cu(I)@Na₂Ti₆O₁₃ nanostructured hybrid pasmonic photocatalytic membrane for acetaldehyde elimination

Jingjing Yang, Baoshun Liu, Xiujian Zhao

State Key Laboratory of Silicate Materials for Architectures, Wuhan University of Technology, Wuhan 430070, Hubei, China

Received:2017-10-01 Revised:2017-10-31 Online:2017-12-18 Published:2017-12-29
Supported by:
This work was supported by the National Natural Science Foundation of China (51772230, 51461135004), Hubei Foreign Science and Technology Cooperation Project (2017AHB059), and the Japan Society for the Promotion of Science (JSPS) for an Invitation Fellowship for Foreign Researchers (L16531).

摘要/Abstract

摘要：

室内环境的空气质量对人们生活和健康的影响很大.其中挥发性有机物（VOCs）如乙醛、甲醛、丙酮、苯和甲苯等是室内环境污染的主要来源之一，它们会引起机体免疫力水平失调，影响中枢神经功能，还可影响消化系统，严重时可损伤肝脏和造血功能等.因此，消除这些VOCs变得刻不容缓.
本文报道了一种新型等离子体纳米Au-Cu（I）@Na₂Ti₆O₁₃光催化薄膜.钛酸盐材料容易制备，且具有良好的化学和机械性能，目前多应用于电容器、传感器和光催化领域.此薄膜采用水热法制备并进一步热处理得到，该法简单易操作，水热时间较短且成本低廉.另外通过热置沉积的方法分别将Au纳米颗粒和Cu（I）成功负载到Na₂Ti₆O₁₃滤膜上.分别使用场发射扫描电子显微镜（FE-SEM）、透射电子显微镜（TEM）、X射线光电子光谱仪（XPS）、X射线衍射仪（XRD）和UV-Vis光谱仪研究了薄膜的形态结构、元素组成、晶相组成和光学性能.
SEM和TEM结果表明，Na₂Ti₆O₁₃滤膜由超长的Na₂Ti₆O₁₃纳米纤维组成.纳米纤维之间存在较大的孔，可以使空气自由通过.XRD，XPS和UV-Vis结果发现，Au纳米颗粒和铜纳米簇成功地负载在Na₂Ti₆O₁₃滤膜上，且铜呈无定形态，价态为+1.相应的催化结果表明，在可见光照射下，相比于纯Na₂Ti₆O₁₃滤膜，Au-Cu（I）@Na₂Ti₆O₁₃滤膜显示出非常高的降解乙醛活性.结果发现，Na₂Ti₆O₁₃滤膜的可见光活性随着负载的Au纳米颗粒含量的增加呈现先增加后降低的趋势，当Au纳米颗粒的含量为2.85 wt%时达到最大.使用超长Na₂Ti₆O₁₃纳米纤维作为支撑材料，Au纳米颗粒的等离子体可见光吸附导致电子从Au纳米颗粒迁移到Na₂Ti₆O₁₃的导带，并被表面负载的Cu（I）俘获，有效地避免了Na₂Ti₆O₁₃中导带电子和留在Au纳米颗粒上空穴的复合，延长了电子和空穴的寿命，进而提高了滤膜的可见光催化活性.Na₂Ti₆O₁₃滤膜可以有效地避免粉体在光催化反应过程中发生团聚，因而在实际应用过程中易分离，避免了二次污染，且可以循环使用，因此成本低，有望用作空气净化的功能材料.

null

关键词: Na₂Ti₆O₁₃, Au负载, Cu (I)纳米簇负载, 协同效应, 光催化

Abstract:

The present article reports a novel self-standing nanostructured Au-Cu(I)@Na₂Ti₆O₁₃ plasmonic photocatalytic membrane, which is prepared by a hydrothermal reaction followed by a simple subsequent heat treatment process. The morphological structure, elemental composition, crystalline phases, and optical properties of the membrane were studied in detail by field-emission scanning electron microscopy, transmission electron microscopy, X-ray photoelectron spectroscopy, X-ray diffraction, and ultraviolet-visible spectroscopy. Compared with that of a pure Na₂Ti₆O₁₃ membrane, the Au-Cu(I)@Na₂Ti₆O₁₃ membrane displayed much higher photocatalytic activity for the decomposition of acetaldehyde, a typical volatile organic compound, under visible light illumination. It was found that the photocatalytic activity of the Au-Cu(I)@Na₂Ti₆O₁₃ membrane increased as the amount of Au was increased. The membrane loaded with 2.85 wt% Au showed the highest photocatalytic activity in the decomposition of acetaldehyde of the investigated materials. We found that in the photocatalyst membrane, Na₂Ti₆O₁₃ acted as a support material, Au displayed plasmonic absorption, and Cu(I) behaved as a co-catalyst. The present membrane materials can avoid the self-aggregation typically observed during the course of photocatalytic reactions. As a result, they can be easily separated, recycled, and reactivated after their practical application, making these functional materials attractive for use in air cleaning applications.

Key words: Na₂Ti₆O₁₃, Au modification, Cu(I) nanocluster modification, Synergistic effect, Photocatalysis

杨静静, 刘保顺, 赵修建. 一种可见光活性的等离子体纳米Au-Cu(I)@Na₂Ti₆O₁₃光催化滤膜的制备和对乙醛的降解[J]. 催化学报, 2017, 38(12): 2048-2055.

Jingjing Yang, Baoshun Liu, Xiujian Zhao. A visible-light-active Au-Cu(I)@Na₂Ti₆O₁₃ nanostructured hybrid pasmonic photocatalytic membrane for acetaldehyde elimination[J]. Chinese Journal of Catalysis, 2017, 38(12): 2048-2055.

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一种可见光活性的等离子体纳米Au-Cu(I)@Na₂Ti₆O₁₃光催化滤膜的制备和对乙醛的降解

A visible-light-active Au-Cu(I)@Na₂Ti₆O₁₃ nanostructured hybrid pasmonic photocatalytic membrane for acetaldehyde elimination

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