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介孔TiO(B)负载Pt催化剂的甲醛氧化性能增强:羟基的作用

Enhanced Formaldehyde Oxidation Performance of the Mesoporous TiO(B)-Supported Pt Catalyst: The Role of Hydroxyls.

作者信息

Wei Tongtong, Zhao Xuejuan, Li Long, Wang Lei, Lv Shenjie, Gao Lei, Yuan Gaosong, Li Licheng

机构信息

Jiangsu Co-Innovation Center of Efficient Processing and Utilization of Forest Resources, College of Chemical Engineering, Nanjing Forestry University, Nanjing 210037, P. R. China.

School of Materials Science and Engineering, Nanjing Institute of Technology, Nanjing 211167, P. R. China.

出版信息

ACS Omega. 2022 Jul 14;7(29):25491-25501. doi: 10.1021/acsomega.2c02490. eCollection 2022 Jul 26.

Abstract

As one of the crystal phases of titania, TiO(B) was first utilized as a catalyst carrier for the oxidation of formaldehyde (HCHO). The mesoporous TiO(B) loaded with Pt nanoparticles enhanced the HCHO oxidation reaction whose reaction rate was 4.5-8.4 times those of other crystalline TiO-supported Pt catalysts. Simultaneously, Pt/TiO(B) exhibited long-term stable HCHO oxidation performance. The structural characterization results showed that in comparison with Pt/anatase, Pt/TiO(B) had more abundant hydroxyls, facilitating increasing the content of oxygen species. Studies on the role of hydroxyls in HCHO oxidation of Pt/TiO(B) illustrated that synergistic involvement of terminally bound hydroxyls and bridging hydroxyls in HCHO oxidation accelerated the transformation from HCHO to formate via dioxymethylene. Moreover, hydroxyls could avoid the accumulation of excessive formate on Pt/TiO(B) and promote the rapid oxidation of CO. Accordingly, the hydroxyl groups could accelerate each substep of formaldehyde oxidation, which enabled Pt/TiO(B) to exhibit excellent formaldehyde oxidation performance.

摘要

作为二氧化钛的晶相之一,TiO(B)首次被用作甲醛(HCHO)氧化的催化剂载体。负载有铂纳米颗粒的介孔TiO(B)增强了HCHO氧化反应,其反应速率是其他结晶TiO负载的铂催化剂的4.5至8.4倍。同时,Pt/TiO(B)表现出长期稳定的HCHO氧化性能。结构表征结果表明,与Pt/锐钛矿相比,Pt/TiO(B)具有更丰富的羟基,有利于增加氧物种的含量。对Pt/TiO(B)中羟基在HCHO氧化中的作用研究表明,末端结合羟基和桥连羟基在HCHO氧化中的协同参与加速了HCHO通过二氧亚甲基向甲酸盐的转化。此外,羟基可以避免过量甲酸盐在Pt/TiO(B)上的积累,并促进CO的快速氧化。因此,羟基可以加速甲醛氧化的每个子步骤,这使得Pt/TiO(B)表现出优异的甲醛氧化性能。

https://cdn.ncbi.nlm.nih.gov/pmc/blobs/aebd/9330097/d15fdaf447e6/ao2c02490_0002.jpg

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