自然科学版
陕西师范大学学报(自然科学版)
合成气定向催化转化科学与技术专题
N掺杂对TiO2负载Cu基催化剂甲醛乙炔化性能的影响
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王志鹏, 牛珠珠, 班丽君, 郝全爱, 张鸿喜, 李海涛*, 赵永祥*
(山西大学 化学化工学院 精细化学品教育部工程研究中心, 山西 太原 030006)
李海涛,男,副教授,硕士生导师,主要从事多相催化研究。E-mail: htli@sxu.edu.cn 赵永祥,男,教授,博士生导师,主要从事多相催化研究。E-mail: yxzhao@sxu.edu.cn
摘要:
以TiO2及N掺杂的TiO2为载体、CuCl2·2H2O为铜源、NaOH为沉淀剂,采用沉积沉淀法制备了Cu含量(质量分数,下同)为30%的CuO/TiO2及CuO/N-TiO2催化剂。结合N2物理吸附、XRD、XPS、H2-TPR、CO-IR等表征,研究了N掺杂对TiO2负载CuO催化剂结构及甲醛乙炔化性能的影响。结果表明,经N掺杂的TiO2呈现出较多的Ti3+物种及氧空位,增加了CuO与载体间的相互作用,有利于CuO物种的分散。在炔化反应过程中,CuO原位转变为高分散的Cu+活性中心,催化剂表现出高的催化活性与使用稳定性。
关键词:
甲醛乙炔化;CuO/N-TiO2催化剂;Cu+活性中心;Ti3+物种;氧空位
收稿日期:
2018-10-31
中图分类号:
TP391.42
文献标识码:
A
文章编号:
1672-4291(2019)01-0101-08
基金项目:
国家自然科学基金(U1710221, 21503124);山西省国际科技合作项目(201703D421034)
Doi:
The influence of N doping on TiO2 supported Cu-based catalyst for formaldehyde ethynylation
WANG Zhipeng, NIU Zhuzhu, BAN Lijun, HAO Quan′ai, ZHANG Hongxi, LI Haitao*, ZHAO Yongxiang*
(School of Chemistry and Chemical Engineering, Engineering Research Center of Ministry of Education for Fine Chemicals, Shanxi University, Taiyuan 030006, Shanxi, China)
Abstract:
CuO/TiO2 and CuO/N-TiO2 catalysts with 30% Cu loading were prepared by deposition-precipitation method using copper chloride as copper source, sodium hydroxide as precipitant, and TiO2 and N-TiO2 as supports. Combined with the characterization of N2 physical adsorption-desorption, X-ray diffraction(XRD), H2-temperature programmed reduction(H2-TPR), X-ray photoelectron spectroscopy (XPS) , CO Fourier transform infrared spectroscopy (CO-IR), and etc, the effects of N doping on the structure of TiO2 supported CuO catalyst and the catalytic performance of formaldehyde ethynylation were studied. The results show that N-doped TiO2 presented more Ti3+ species and oxygen vacant sites, which increased the interaction between CuO and the carrier and was conducive to the dispersion of CuO species. In the process of ethynylation, CuO is transformed into highly dispersed Cu+ active species in situ, and the catalyst shows high catalytic activity and stability.
KeyWords:
formaldehyde ethynylation; CuO/N-TiO2 catalyst; Cu+ active species; Ti3+ species ; oxygen vacant sites