甲醛还原Pt/TiO2催化剂用于温和条件下高效催化氧化甲醛

doi:10.1016/S1872-2067(14)60192-3

催化学报 ›› 2015, Vol. 36 ›› Issue (2): 188-196.DOI: 10.1016/S1872-2067(14)60192-3

甲醛还原Pt/TiO₂催化剂用于温和条件下高效催化氧化甲醛

陈铧耀^a, 芮泽宝^a,b, 纪红兵^a,b

a 中山大学化学与化学工程学院化工系, 广东广州510275;
b 中山大学惠州研究院废气净化与控制研发中心, 广东惠州516081

收稿日期:2014-06-09 修回日期:2014-07-09 出版日期:2015-01-21 发布日期:2015-01-21
通讯作者: 纪红兵
基金资助:
国家自然科学基金(21106189, 21036009); 广东省自然科学基金(S2011040001767); 中央高校基本科研业务费专项资金(12lgpy11).

Titania-supported Pt catalyst reduced with HCHO for HCHO oxidation under mild conditions

Huayao Chen^a, Zebao Rui^a,b, Hongbing Ji^a,b

a Department of Chemical Engineering, School of Chemistry & Chemical Engineering, Sun Yat-Sen University, Guangzhou 510275, Guangdong, China;
b R&D Center of Waste-gas Cleaning & Control, Huizhou Research Institute of Sun Yat-Sen University, Huizhou 516081, Guangdong, China

Received:2014-06-09 Revised:2014-07-09 Online:2015-01-21 Published:2015-01-21
Supported by:
This work was supported by the National Natural Science Foundation of China (21106189 and 21036009), the Natural Science Foundation of Guangdong Province (S2011040001767), and the Fundamental Research Funds for the Central Universities (12lgpy11).

摘要/Abstract

摘要：

通过浸渍法(IM)和沉积-沉淀(DP)法制备了一系列Pt/TiO₂(P25)催化剂, 并分别用甲醛溶液和氢气还原处理催化剂. 利用原位红外监测催化剂表面吸附物种在反应过程中的变化, 探究了催化剂制备和还原条件及Pt负载量对催化剂结构和催化氧化甲醛活性的影响. 结果显示, 用DP法制备并用甲醛还原的Pt/P25催化剂中Pt颗粒分散均匀, 并具有合适的粒径和高浓度的表面活性氧, 显示出良好的甲醛氧化活性. 在空速30 000 ml/(g·h)、反应温度30 ℃和甲醛初始浓度50 mg/m³的条件下, 0.4%Pt/P25(DP-HCHO)上的甲醛转化率达到98%, 并能稳定运行100 h以上. 相比之下, Pt/P25(DP-H₂)由于表面活性氧较少, 不利于甲酸盐氧化, 活性较低. Pt/P25(IM-H₂)虽然具有高浓度的表面活性氧, 却同时具有最大的Pt颗粒粒径, 在甲醛转化为甲酸盐和甲酸盐氧化两步反应中的活性均较差, 因而甲醛氧化活性最差.

关键词: 甲醛, 铂, 二氧化钛, 原位红外光谱, 沉积-沉淀法

Abstract:

A series of Pt/TiO₂(P25) catalysts were prepared by both impregnation (IM) and deposition-precipitation (DP) methods followed by reduction using either a HCHO solution or a H₂ stream. The effects of the preparation and reduction conditions and the Pt loading level on structural properties and performance during HCHO oxidation were then studied based on the assessment of adsorbed species on the catalyst surfaces using in-situ diffuse reflectance infrared Fourier transform spectroscopy (DRIFTS). The results indicated that Pt/P25 prepared by DP and reduced with HCHO exhibited homogeneously dispersed Pt nanoparticles with appropriate particle size in addition to a high concentration of chemisorbed oxygen, and also showed high activity for HCHO oxidation. A HCHO conversion of 98% with stable performance over more than 100 h was achieved over Pt/P25 produced using DP and HCHO reduction at 30 ℃, even with a 0.4% Pt loading. Pt/P25 synthesized using DP with H₂ reduction was less effective at promoting formate decomposition and thus showed less HCHO oxidation activity, likely because of lower levels of chemisorbed oxygen. The Pt/P25 made using IM and H₂ reduction had the highest amount of chemisorbed oxygen but also the largest Pt particles, resulting in the lowest activity for both the formation of formate species and formate decomposition into CO species, and thus showed low HCHO oxidation activity.

Key words: Formaldehyde, Platinum, Titanium, In-situ diffuse reflectance infrared, Fourier transform spectroscopy, Deposition-precipitation

陈铧耀, 芮泽宝, 纪红兵. 甲醛还原Pt/TiO₂催化剂用于温和条件下高效催化氧化甲醛[J]. 催化学报, 2015, 36(2): 188-196.

Huayao Chen, Zebao Rui, Hongbing Ji. Titania-supported Pt catalyst reduced with HCHO for HCHO oxidation under mild conditions[J]. Chinese Journal of Catalysis, 2015, 36(2): 188-196.

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甲醛还原Pt/TiO₂催化剂用于温和条件下高效催化氧化甲醛

Titania-supported Pt catalyst reduced with HCHO for HCHO oxidation under mild conditions

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