壁载氨氧化催化剂X/TiO2(X=Pt、Pd、Au)制备与反应机理

doi:10.16085/j.issn.1000-6613.2017-0435

化工进展 ›› 2017, Vol. 36 ›› Issue (11): 4093-4098.DOI: 10.16085/j.issn.1000-6613.2017-0435

壁载氨氧化催化剂X/TiO₂(X=Pt、Pd、Au)制备与反应机理

邱伟, 陶阳, 蒋炜, 梁斌

四川大学化学工程学院, 四川成都 610065

收稿日期:2017-03-16 修回日期:2017-05-23 出版日期:2017-11-05 发布日期:2017-11-05
通讯作者: 蒋炜,教授,从事微反应器应用于氨氧化问题研究。
作者简介:邱伟(1991-),男,硕士研究生。
基金资助:
国家自然科学基金项目（21476146，21176157）。

Preparation of wall-loaded X/TiO₂ (X=Pt,Pd,Au) catalysts for ammonia oxidation process and the reaction mechanism

QIU Wei, TAO Yang, JIANG Wei, LIANG Bin

School of Chemical Engineering, Sichuan University, Chengdu 610065, Sichuan, China

Received:2017-03-16 Revised:2017-05-23 Online:2017-11-05 Published:2017-11-05

摘要/Abstract

摘要： 催化剂壁载化是在微通道反应器内负载催化剂的有效方法，适用于氨氧化过程这一强放热气固反应体系，但不同的催化剂壁载化后其催化性能还有待研究。本研究通过将Pt、Pd、Au 3种贵金属通过光催化沉积方法负载于TiO₂纳米管上并组装入微通道反应器内，考察了其催化氨氧化过程性能，并通过密度泛函方法解释了其性能差异。结果证实，TiO₂载体对催化过程无明显影响，3种催化剂催化活性顺序为Pt/TiO₂ > Pd/TiO₂ > Au/TiO₂，其中Pt/TiO₂氨转化率在280℃下即可达100%，NO选择性380℃即达99%。TPD检测及模拟证实，NH₃及O₂在催化剂表面吸附能大小顺序为Pt > Pd > Au，与催化活性顺序一致。

关键词: 催化剂, 化学反应, 数值模拟, 微反应器, 吸附

Abstract: Wall-loading is an effective method to load catalyst inside microchannel reactor,which can be applied to highly exothermic gas-solid reactions such as ammonia oxidation. However,the catalytic performance of different wall-loaded catalysts needs to be further studied. In this research,three metals Pt,Pd,and Au,were loaded on TiO₂ nanotubes by photocatalytic deposition,and then assembled in a microchannel reactor to evaluate their catalytic performance for ammonia oxidation. The performance difference was discussed based on the density functional method. Results confirmed that no significant catalytic activity of bare TiO₂ nanotubes had been observed. The determined activity sequence of three catalysts is Pt/TiO₂ > Pd/TiO₂ > Au/TiO₂. Ammonia conversion by Pt/TiO₂ reached 100% at 280℃,and NO selectivity was up to 99% at 380℃. TPD analysis and simulation confirmed the adsorption energy of NH₃ and O₂ on the catalyst surface was in the order of Pt > Pd > Au,which was consistent with that of their catalytic activity.

Key words: catalyst, chemical reaction, numerical simulation, microreactor, adsorption

中图分类号:

TQ11

邱伟, 陶阳, 蒋炜, 梁斌. 壁载氨氧化催化剂X/TiO₂(X=Pt、Pd、Au)制备与反应机理[J]. 化工进展, 2017, 36(11): 4093-4098.

QIU Wei, TAO Yang, JIANG Wei, LIANG Bin. Preparation of wall-loaded X/TiO₂ (X=Pt,Pd,Au) catalysts for ammonia oxidation process and the reaction mechanism[J]. Chemical Industry and Engineering Progress, 2017, 36(11): 4093-4098.

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壁载氨氧化催化剂X/TiO₂(X=Pt、Pd、Au)制备与反应机理

Preparation of wall-loaded X/TiO₂ (X=Pt,Pd,Au) catalysts for ammonia oxidation process and the reaction mechanism

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