掺磷非晶氧化钛负载铂用于高效催化氧化挥发性有机化合物

doi:10.15541/jim20190154

无机材料学报 ›› 2020, Vol. 35 ›› Issue (4): 482-490.DOI: 10.15541/jim20190154

所属专题： 2020年环境材料论文精选(三)有机小分子去除

掺磷非晶氧化钛负载铂用于高效催化氧化挥发性有机化合物

黄谢意^1,²,王鹏^2,³,尹国恒¹,张绍宁¹,赵伟¹,王东¹,毕庆员¹(),黄富强^1,^3,⁴()

1. 中国科学院上海硅酸盐研究所, 高性能陶瓷和超微结构国家重点实验室, 上海 200050
2. 中国科学院大学, 北京 100049
3. 上海科技大学物理科学与技术学院, 上海 200050
4. 北京大学化学与分子工程学院, 稀土材料化学及应用国家重点实验室, 北京 100871

收稿日期:2019-04-12 修回日期:2019-05-24 出版日期:2020-04-20 网络出版日期:2019-06-17
作者简介:黄谢意(1994-), 男, 硕士研究生. E-mail: huangxieyi@student.sic.ac.cn

Removal of Volatile Organic Compounds Driven by Platinum Supported on Amorphous Phosphated Titanium Oxide

HUANG Xieyi^1,²,WANG Peng^2,³,YIN Guoheng¹,ZHANG Shaoning¹,ZHAO Wei¹,WANG Dong¹,BI Qingyuan¹(),HUANG Fuqiang^1,^3,⁴()

1. State Key Laboratory of High Performance Ceramics and Superfine Microstructure, Shanghai Institute of Ceramics, Chinese Academy of Sciences, Shanghai 200050, China
2. University of Chinese Academy of Sciences, Beijing 100049, China
3. School of Physical Science and Technology, ShanghaiTech University, Shanghai 200031, China
4. State Key Laboratory of Rare Earth Materials Chemistry and Applications, College of Chemistry and Molecular Engineering, Peking University, Beijing 100871, China

Received:2019-04-12 Revised:2019-05-24 Published:2020-04-20 Online:2019-06-17
Supported by:
National Key Research and Development Program of China(2016YFB0901600);National Natural Science Foundation of China(21872166);Science & Technology Commission of Shanghai(16ZR1440400);Science & Technology Commission of Shanghai(16JC1401700);The Key Research Program of Chinese Academy of Sciences(QYZDJ-SSW-JSC013);The Key Research Program of Chinese Academy of Sciences(KGZD-EW-T06)

摘要/Abstract

摘要：

高活性催化剂是挥发性有机化合物(VOCs)催化氧化消除的关键因素。本研究通过简单的共沉淀法成功制备了具有高比表面积的非晶介孔磷掺杂氧化钛负载铂催化剂(Pt/ATO-P)。通过P掺杂, 既可获得非晶介孔结构, 又可获得高ATO-P比表面积(可达278.9 m²·g^-1)。非晶介孔Pt/ATO-P催化剂显示出优异的VOCs催化氧化性能和良好的热稳定性。Pt/ATO-P样品在空速为36000 mL·h^-1·g^-1、甲苯浓度为10000 mL·m^-3的反应条件下, 对甲苯催化氧化的T₅₀和T₉₀(实现50%和90%转化率所需的温度)分别为130 ℃和140 ℃, 明显优于无磷催化剂Pt/TiO₂。这些发现可以为拓展非晶介孔磷化材料在环境净化和能源转化等领域的应用提供重要参考。

关键词: 非晶介孔材料, 磷掺杂非晶氧化钛, 铂纳米颗粒, 甲苯催化氧化, VOCs消除

Abstract:

Development of high efficiency catalyst is the key factor to catalytic combustion of volatile organic compounds (VOCs). Herein, amorphous mesoporous phosphated TiO₂ (ATO-P) with high specific surface area supported platinum catalyst was successfully fabricated. P-dopant can increase the surface area (up to 278.9 m²·g^-1) of ATO-P, which is 21 times higher than that of pristine TiO₂, and make the amorphous titanium oxide structure. The supported Pt catalyst with amorphous mesoporous feature shows impressive performance and excellent thermostability for VOCs oxidation. The Pt/ATO-P catalyst exhibits outstanding catalytic efficiency, the T₅₀ and T₉₀ (temperatures required for achieving conversions of 50% and 90%) are respectively 130 ℃ and 140 ℃, for toluene oxidation under high gas hourly space velocity (GHSV) of 36000 mL·h^-1·g^-1 and toluene concentration of 10000 mL·m^-3. The performance is superior to the reference Pt/TiO₂ and comparable with the state-of-the-art catalysts. These findings can make a significant contribution on the new applications of amorphous mesoporous phosphated materials in VOCs removal.

Key words: amorphous mesoporous structure, phosphated TiO₂, Pt nanoparticle, toluene oxidation, VOCs removal

中图分类号:

O782

黄谢意,王鹏,尹国恒,张绍宁,赵伟,王东,毕庆员,黄富强. 掺磷非晶氧化钛负载铂用于高效催化氧化挥发性有机化合物[J]. 无机材料学报, 2020, 35(4): 482-490.

HUANG Xieyi,WANG Peng,YIN Guoheng,ZHANG Shaoning,ZHAO Wei,WANG Dong,BI Qingyuan,HUANG Fuqiang. Removal of Volatile Organic Compounds Driven by Platinum Supported on Amorphous Phosphated Titanium Oxide[J]. Journal of Inorganic Materials, 2020, 35(4): 482-490.

图/表 18

Fig. 1 Structure of amorphous ATO-P prepared via facile co-precipitation

Fig. 2 XRD patterns of TiO2 and ATO-P samples

Fig. 3 TG (solid line) and DSC (dashed line) curves for ATO-P

Fig. 4 SEM (a, b) and HRTEM (c) images, and EDS elemental mapping (d) of ATO-P

Fig. 5 N2 adsorption-desorption isotherms (a) and pore size distributions (b) of ATO-P and TiO2

Table 1 Textural properties and elemental compositions of TiO2 and ATO-P samples

Catalyst	BET surface area /(m²?g^-1)	Pore volume /(cm³?g^-1)	Pore size /nm	Elemental composition /wt%^[a]
Catalyst	BET surface area /(m²?g^-1)	Pore volume /(cm³?g^-1)	Pore size /nm	P	Ti	O
TiO₂	10.9	0.04	15.7	-	60.0	40.0
ATO-P	278.9	0.80	11.4	19.2	32.1	48.7

Fig. 6 FT-IR spectra of TiO2 and ATO-P

Fig. 7 Full XPS spectra (a) of TiO2 and ATO-P; High-resolution XPS P2p (b), Ti2p (c), and O1s (d) of TiO2 and ATO-P

Fig. 8 TEM (a) and HRTEM (b) images of Pt/ATO-P with insert in (a) indicating the particle size distribution of Pt nanoparticles, XRD patterns (c) and XPS Pt4f (d) of Pt/ATO-P

Fig. 9 Toluene conversion (a) of 1wt% Pt/ATO-P with respect to reaction temperature, and thermal stability (b) of Pt/ATO-P at 180 ℃

Fig. 10 Toluene conversion over Pt/ATO-P catalysts with different Pt loadings

Fig. 11 Catalytic activity of Pt/ATO-P for the conversion of benzene (a), ethyl acetate (b), n-hexane (c), and mesitylene (d) with respect to reaction temperature

Fig. S1 SEM (a) and HRTEM (b) images of TiO2

Fig. S2 HRTEM image of Pt/ATO-P

Fig. S3 H2-TPR profiles of Pt/TiO2 and Pt/ATO-P samples

Fig. S4 TEM images of 0.5wt% Pt/ATO-P (a) and 2wt% Pt/ATO-P (b) For the catalyst with low loading of 0.5wt%, there are few Pt nanoparticles in the ATO-P supports. By contract, the Pt particles are larger than that with loading of 1wt% when the loading up to 2wt%

Fig. S5 TEM (a) and HRTEM (b) images of the used Pt/ATO-P catalyst

Fig. S6 XPS Pt 4f spectra of the fresh and the used Pt/ATO-P catalysts

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掺磷非晶氧化钛负载铂用于高效催化氧化挥发性有机化合物

Removal of Volatile Organic Compounds Driven by Platinum Supported on Amorphous Phosphated Titanium Oxide

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