直流电弧等离子体制备纳米SiC及其催化特性

doi:10.15541/jim20160371

无机材料学报 ›› 2017, Vol. 32 ›› Issue (4): 351-356.DOI: 10.15541/jim20160371

直流电弧等离子体制备纳米SiC及其催化特性

余洁意¹, 黄昊^1,2, 高见¹, 周雷¹, 高嵩¹, 董星龙¹, 全燮³

(大连理工大学 1. 教育部三束材料改性重点实验室, 材料科学与工程学院; 2. 能源材料及器件实验室, 材料科学与工程学院; 3. 工业生态与环境工程实验室, 环境学院, 大连 116024)

收稿日期:2016-06-13 修回日期:2016-08-03 出版日期:2017-04-20 网络出版日期:2017-03-24
作者简介:余洁意(1984–), 女, 博士研究生. E-mail: yu.jie.yi@hotmail.com
基金资助:
国家自然科学基金(51171033, 51271044);国家中央高校基本科研业务费专项资金(DUT15LAB05, DUT16LAB03)

Synthesis and Catalytic Performances of SiC Nanoparticles by DC Arc-discharge Plasma

YU Jie-Yi¹, HUANG Hao^1,2, GAO Jian¹, ZHOU Lei¹, GAO Song¹, DONG Xing-Long¹, QUAN Xie³

(1. Key Laboratory of Materials Modification by Laser, Ion and Electron Beams (Ministry of Education), School of Materials Science and Engineering, Dalian University of Technology, Dalian 116023, China; 2. Energy Materials & Devices Laboratory, School of Materials Science and Engineering, Dalian University of Technology, Dalian 116023, China; 3. Laboratory of Industrial Ecology and Environmental Engineering (The Ministry of Education, China), School of Environmental Science and Technology, Dalian University of Technology, Dalian 116024, China)

Received:2016-06-13 Revised:2016-08-03 Published:2017-04-20 Online:2017-03-24
About author:YU Jie-Yi. E-mail: yu.jie.yi@hotmail.com
Supported by:
National Natural Science Foundation of China (51171033, 51271044);Fundamental Research Funds for the Central Universities (DUT15LAB05, DUT16LAB03)

摘要/Abstract

摘要：

利用工业块体硅为硅源, CH₄为碳源, 在含有H₂和Ar混合气氛中, 采用直流电弧等离子体法制备SiC纳米粒子。CH₄含量影响SiC纳米粒子的化学组成和形貌。结果显示: 产物中含有3C-SiC和6H-SiC两种物相, 而在CH₄压力为0.005 MPa条件下制备的SiC纳米粒子还含有Si/SiC核壳结构。利用制备的SiC纳米颗粒作为催化剂, 在恒光强下光电催化还原脱除2,4-二氯酚中的Cl原子。结果显示在-1.02 V偏压下光电催化180 min后, 对2,4-二氯酚的去除效率达92.5%, SiC纳米粒子的吸附效率为19.6%。因此, SiC纳米颗粒可取代贵金属, 作为低成本光电催化候选材料用于污水处理。

关键词: 碳化硅, 直流电弧等离子体, 光电催化, 2,4-二氯酚

Abstract:

SiC nanoparticles were synthesized by direct current (DC) arc-discharge plasma method, using bulk Si as silicon source and in a mixed atmosphere of CH₄, H₂ and Ar. The chemical composition and morphology of the SiC nano product were affected by the pressure of CH₄ obviusly. These products were characterized by Transmission electron microscopy (TEM), Raman spectra, Fourier transform infrared (FTIR) spectroscopy, X-ray diffraction (XRD), and X-ray photoelectron spectroscopy (XPS). The results indicate that the product contains the main phases of 3C- and 6H-SiC, while prepared at low CH₄ pressure of 0.005 MPa, which exists few Si/SiC core-shell structures in the product. The SiC nanoparticles, prepared at 0.01 MPa CH₄, were used as the catalyst to remove the Cl atoms in persistent 2,4-dichlorophenol through photoelectric catalytic reduction. The results show that the SiC nanoparticles have good photoelectric catalytic reductive dechlorination ability under ultraviolet illumination at a constant optical intensity of 500 mW/cm². The removal efficiency reaches about 92.5% and the adsorption efficiency is 19.6% at an appropriate bias potential of -1.02 V after 180 min of photoelectric catalysis. Hence, SiC nanoparticles are identified as a kind of low-cost photoelectrocatalysis candidates to replace noble metals in wastewater treatments.

Key words: silicon carbide, DC arc-discharge plasma, photoelectric catalysis, 2,4-dichlorophenol

中图分类号:

X703

余洁意, 黄昊, 高见, 周雷, 高嵩, 董星龙, 全燮. 直流电弧等离子体制备纳米SiC及其催化特性[J]. 无机材料学报, 2017, 32(4): 351-356.

YU Jie-Yi, HUANG Hao, GAO Jian, ZHOU Lei, GAO Song, DONG Xing-Long, QUAN Xie. Synthesis and Catalytic Performances of SiC Nanoparticles by DC Arc-discharge Plasma[J]. Journal of Inorganic Materials, 2017, 32(4): 351-356.

图/表 9

表1 SiC样品制备条件

Table 1 Preparation conditions of SiC samples

Sample	Pressure /MPa			Arc voltage /V	Arc current /A
Sample	H₂	Ar	CH₄	Arc voltage /V	Arc current /A
SiC-0.005	0.01	0.02	0.005	20~40	90
SiC-0.01	0.01	0.02	0.01	20~40	90

图1 (a,b)SiC-0.005和(c,d)SiC-0.01纳米颗粒TEM和高分辨TEM (HR-TEM)照片

Fig. 1 TEM and high resolution (HR-TEM) images of (a,b) SiC-0.005 and (c,d) SiC-0.01 nanoparticles

图2 SiC-0.005和SiC-0.01纳米颗粒Raman光谱图

Fig. 2 Raman spectra of SiC-0.005 and SiC-0.01 nanoparticles

图3 SiC-0.005和SiC-0.01纳米颗粒的XRD图谱

Fig. 3 XRD patterns of SiC-0.005 and SiC-0.01 nanoparticles

图4 SiC-0.005和SiC-0.01纳米颗粒的FTIR图谱

Fig. 4 FTIR spectra of SiC-0.005 and SiC-0.01 nanoparticles

图5 SiC-0.005 (a, b)和SiC-0.01(a’, b’)纳米颗粒XPS图谱

Fig. 5 XPS spectra of SiC-0.005 (a, b) and SiC-0.01 nanoparticles (a, a’) C1s; (b, b’) Si2p

图6 样品SiC-0.005和SiC-0.01紫外-可见吸收光谱图

Fig. 6 UV-visible absorption spectra of SiC-0.005 and SiC-0.01

图7 (a) ITO导电玻璃和SiC-0.01电极分别在黑暗和光照下对2,4-DCP的线性伏安图, (b) SiC-0.01电极分别在有/无2,4-DCP时黑暗和光照下的线性伏安图, 扫描速率为10 mV/s

Fig. 7 Linear voltammograms of (a) ITO and SiC-0.01 electrodes under dark and light with 2,4-DCP;, (b) SiC-0.01 electrodes under dark and light with/without 2,4-DCP, the scanning speed is 10 mV/s

图8 (a) SiC-0.01电极对2,4-DCP吸附曲线、-0.76 V和-1.02 V偏压下的电催化和光电催化去除曲线, (b)降解180 min后还原产物的质谱图

Fig. 8 (a) Adsorption curve, removal curves of electric catalysis and photoelectric catalysis of 2,4-DCP by SiC-0.01 electrodes under bias potentials of -0.76 V and -1.02 V, (b) mass spectrum of reduzate after 180 min of degradation

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直流电弧等离子体制备纳米SiC及其催化特性

Synthesis and Catalytic Performances of SiC Nanoparticles by DC Arc-discharge Plasma

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