酸性助剂对V2O5/TiO2催化剂甲醇选择氧化为甲缩醛的影响

doi:10.1016/S1872-2067(12)60690-1

催化学报 ›› 2013, Vol. 34 ›› Issue (11): 2110-2117.DOI: 10.1016/S1872-2067(12)60690-1

酸性助剂对V₂O₅/TiO₂催化剂甲醇选择氧化为甲缩醛的影响

蔡景轩, 傅玉川, 孙清, 贾敏慧, 沈俭一

南京大学化学化工学院介观化学教育部重点实验室, 江苏南京210093

收稿日期:2013-07-07 修回日期:2013-08-16 出版日期:2013-10-18 发布日期:2013-10-18
通讯作者: Yuchuan Fu,Jianyi Shen
基金资助:
国家自然科学基金(21073088);高等学校博士学科点专项科研基金(200802841038);国家重点基础研究发展计划(973计划,2005CB221400);中央高校基本科研业务费专项基金.

Effect of acidic promoters on the titania-nanotubes supported V₂O₅ catalysts for the selective oxidation of methanol to dimethoxymethane

Jingxuan Cai, Yuchuan Fu, Qing Sun, Minhui Jia, Jianyi Shen

Laboratory of Mesoscopic Chemistry, School of Chemistry and Chemical Engineering, Nanjing University, Nanjing 210093, Jiangsu, China

Received:2013-07-07 Revised:2013-08-16 Online:2013-10-18 Published:2013-10-18
Contact: Yuchuan Fu,Jianyi Shen
Supported by:
This work was supported by the National Natural Science Foundation of China (21073088), the Specialized Research Fund for the Doctoral Program of Higher Education (200802841038), the National Basic Research Program of China (2005CB221400), and the Fundamental Research Funds for the Central Universities.

摘要/Abstract

摘要：

研究了酸性助剂对TiO₂纳米管(TNT)负载的V₂O₅催化剂(V₂O₅/TNT)性能的影响, 发现经硫酸、磷酸或磷钨酸处理后, TNT的结构稳定, 但表面酸性和氧化-还原性发生了变化, 从而改变了甲醇选择氧化为甲缩醛的催化性能. 实验结果表明, V₂O₅/TNT催化剂经硫酸修饰和673 K焙烧, 其甲缩醛选择性显著提高, 且维持了较高的甲醇转化率. 催化剂表征表明, 高温焙烧促进了硫酸根与钒物种之间的强相互作用, 从而提高了催化剂的表面酸性而没有降低钒的氧化-还原性. 磷酸和磷钨酸修饰虽然也提高了V₂O₅/TNT催化剂的表面酸性, 但降低了其中钒氧化物的氧化-还原能力, 反而降低了催化剂的活性.

关键词: 甲醇选择氧化, 甲缩醛, 酸性助剂, 表面酸性, 表面氧化-还原性

Abstract:

The effect of acidic promoters on the titania-nanotubes (TNT) supported V₂O₅ catalysts (VTNT) was investigated. The structure of TNT was quite stable after the treatment with sulfuric, phosphoric, and phosphotungstic acids, respectively. The acid-modified VTNT catalysts were tested for the selective oxidation of methanol to dimethoxymethane (DMM). It was found that only the VTNT modified with sulfuric acid followed by calcination at 673 K exhibited the significantly enhanced selectivity to DMM with high methanol conversions. The calcination created some sulfate groups strongly interacted with vanadium species, which enhanced the strengths of surface acidity without weakening the redox ability of vanadium sites. The addition of phosphoric and phosphotungstic acids might enhance the surface acidity of V₂O₅/TiO₂, but weakened its redox ability, and therefore had the negative effect for the target reaction.

Key words: Selective oxidation of methanol, Dimethoxymethane, Acidic additive, Surface acidity, Surface redox property

蔡景轩, 傅玉川, 孙清, 贾敏慧, 沈俭一. 酸性助剂对V₂O₅/TiO₂催化剂甲醇选择氧化为甲缩醛的影响[J]. 催化学报, 2013, 34(11): 2110-2117.

Jingxuan Cai, Yuchuan Fu, Qing Sun, Minhui Jia, Jianyi Shen. Effect of acidic promoters on the titania-nanotubes supported V₂O₅ catalysts for the selective oxidation of methanol to dimethoxymethane[J]. Chinese Journal of Catalysis, 2013, 34(11): 2110-2117.

×
扫码分享

导出引用管理器 EndNote|Ris|BibTeX

链接本文: https://www.cjcatal.com/CN/10.1016/S1872-2067(12)60690-1

https://www.cjcatal.com/CN/Y2013/V34/I11/2110

参考文献

[1] Yu K P, Yu W Y, Ku M C, Liou Y C, Chien S H. Appl Catal B, 2008, 84: 112
[2] Vijayan B, Dimitrijevic N M, Rajh T, Gray K. J Phys Chem C, 2010, 114: 12994
[3] Liu J W, Fu Y C, Sun Q, Shen J Y. Microporous Mesoporous Mater, 2008, 116: 614
[4] Jiang G D, Lin Z F, Zhu L H, Ding Y B, Tang H Q. Carbon, 2010, 48: 3369
[5] Cummings F R, Le Roux L J, Mathe M K, Knoesen D. Mater Chem Phys, 2010, 124: 234
[6] Torrente-Murciano L, Lapkin A A, Bavykin D V, Walsh F C, Wilson K. J Catal, 2007, 245: 272
[7] Sato Y, Koizumi M, Miyao T, Naito S. Catal Today, 2006, 111: 164
[8] Idakiev V, Yuan Z Y, Tabakova T, Su B L. Appl Catal A, 2005, 281: 149
[9] Fu Y C, Shen J Y. Chem Commun, 2007: 2172
[10] Zhao H Y, Bennici S, Shen J Y, Auroux A. J Catal, 2010, 272: 176
[11] Guo H Q, Li D B, Jiang D, Li W H, Sun Y H. Catal Commun, 2010, 11: 396
[12] Mizuno N, Misono M. Chem Rev, 1998, 98: 199
[13] Bond G C. Appl Catal A, 1997, 157: 91
[14] Sun Q, Fu Y C, Liu J W, Auroux A, Shen J Y. Appl Catal A, 2008, 334: 26
[15] Chen J P, Yang R T. J Catal, 1993, 139: 277
[16] Samantaray S K, Parida K. J Mol Catal A, 2001, 176: 151
[17] Blanco J, Avila P, Barthelemy C, Bahamonde A, Odriozola J A, De LaBanda J F G, Heinemann H. Appl Catal, 1989, 55: 151
[18] Stanger U L, Orel B, Regis A, Colomban P. J Sol-Gel Sci Technol, 1997, 8: 965
[19] Deo G, Wachs I E, Haber J. Crit Rev Surf Chem, 1994, 4: 141
[20] Dunn J P, Jehng J M, Kim D S, Briand L E, Stenger H G, Wachs I E. J Phys Chem B, 1998, 102: 6212
[21] Besselmann S, Freitag C, Hinrichsen O, Muhler M. Phys Chem Chem Phys, 2001, 3: 4633
[22] Lin C H, Chien S H, Chao J H, Sheu C Y, Cheng Y C, Huang Y J, Tsai C H. Catal Lett, 2002, 80: 153
[23] Bavykin D V, Friedrich J M, Walsh F C. Adv Mater, 2006, 18: 2807
[24] Avila P, Blanco J, Bahamonde A, Palacios J M, Barthelemy C. J Mater Sci, 1993, 28: 4113
[25] Liu H C, Bayat N, Iglesia E. Angew Chem Int Ed, 2003, 42: 5072
[26] Tatibouet J M. Appl Catal A, 1997, 148: 213

酸性助剂对V₂O₅/TiO₂催化剂甲醇选择氧化为甲缩醛的影响

Effect of acidic promoters on the titania-nanotubes supported V₂O₅ catalysts for the selective oxidation of methanol to dimethoxymethane

PDF

可视化

摘要/Abstract

引用本文

使用本文

扫码分享

参考文献

相关文章 15

编辑推荐

Metrics

[1]	贾爱平, 张云尚, 宋通洋, 胡一鸣, 郑万彬, 罗孟飞, 鲁继青, 黄伟新. TiO₂晶面依赖的Ir-TiO_x相互作用对Ir/TiO₂催化剂巴豆醛选择性加氢性能的影响[J]. 催化学报, 2021, 42(10): 1742-1754.
[2]	廖文敏, 赵培培, 岑丙横, 贾爱平, 鲁继青, 罗孟飞. Co-Cr-O复合氧化物上丙烷低温完全氧化:结构效应、反应动力学和原位光谱研究[J]. 催化学报, 2020, 41(3): 442-453.
[3]	李露露, 李佩晓, 谭伟, 马凯莉, 邹伟欣, 汤常金, 董林. 表面Mo修饰提高CeTiO_x催化剂低温脱硝性能[J]. 催化学报, 2020, 41(2): 364-373.
[4]	姚小江, 曹俊, 陈丽, 亢科科, 陈阳, 田密, 杨复沫. MnO_x/CeO₂纳米棒催化剂在低温NH₃-SCR反应中的阳离子(Zr⁴⁺,Al³⁺,Si⁴⁺)掺杂效应[J]. 催化学报, 2019, 40(5): 733-743.
[5]	马占玲, 马现刚, 刘红超, 朱文良, 郭新闻, 刘中民. Cs/ZSM-35分子筛催化甲缩醛和乙酸甲酯发生一步法羟醛缩合反应[J]. 催化学报, 2018, 39(6): 1129-1137.
[6]	常化振, 史传宁, 李明冠, 张涛, 王驰中, 江莉龙, 王秀云. 不同阳离子(NH₄⁺,Na⁺,K⁺,Ca²⁺)溴化物对商用SCR催化剂化学中毒影响机制研究[J]. 催化学报, 2018, 39(4): 710-717.
[7]	陈磊, 翁鼎, 汪家道, 翁端, 曹丽. WO₃改性CeO₂-TiO₂催化剂的低温NH₃-NO/NO₂ SCR活性和机理研究[J]. 催化学报, 2018, 39(11): 1804-1813.
[8]	姚小江, 陈丽, 孔婷婷, 丁世敏, 罗琼, 杨复沫. 负载型铈基催化剂在NH₃-SCR反应中的载体效应[J]. 催化学报, 2017, 38(8): 1423-1430.
[9]	姚小江, 马凯莉, 邹伟欣, 何圣贵, 安继斌, 杨复沫, 董林. 制备方法对MnO_x-CeO₂催化剂理化性质及低温NH₃-SCR脱硝性能的影响[J]. 催化学报, 2017, 38(1): 146-159.
[10]	邓澄浩, 冷莉, 周静红, 周兴贵, 袁渭康. 预处理温度对甘油氢解双金属Ir-Re催化剂性能的影响[J]. 催化学报, 2015, 36(10): 1750-1758.
[11]	赵鹬, 王俊恩, 陈慧, 张晓艳, 傅玉川, 沈俭一. 高表面积复合氧化物Co-O-Si的制备及其催化1-己烯骨架异构和噻吩加氢脱硫活性[J]. 催化学报, 2014, 35(8): 1402-1409.
[12]	杨琦, 张海涛, 孔猛, 包秀秀, 费金华, 郑小明. 多级孔ZSM-5分子筛的合成及其在甲醇脱水制二甲醚反应中的应用[J]. 催化学报, 2013, 34(8): 1576-1582.
[13]	傅玉川;孙清;沈俭一. 甲缩醛的合成与重整制氢[J]. 催化学报, 2009, 30(8): 791-800.
[14]	郭岱石;马紫峰;蒋淇忠;叶伟东;李春波. SO2-4/SiO2表面酸性的红外光谱和密度泛函理论研究[J]. 催化学报, 2007, 28(7): 627-634.
[15]	张清德;谭猗生;杨彩虹;柳玉琴;韩怡卓. MnCl2-H4SiW12O40/SiO2催化氧化二甲醚制取甲缩醛[J]. 催化学报, 2006, 27(10): 916-920.