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具有高NH-SCO活性和热稳定性的Pt/SiO-AlO的优化设计方法

Optimized Design Method for Pt/SiO-AlO with High NH-SCO Activity and Thermal Stability.

作者信息

Sun Mengmeng, Zhou Shuo, Wang Suning, Song Chang

机构信息

College of Science, Sichuan Agricultural University, Xin Kang Road, Yucheng District, Ya'an 625014, China.

Guangxi Key Laboratory of Optical and Electronic Materials and Devices, College of Materials Science and Engineering, Guilin University of Technology, Guilin 541004, China.

出版信息

ACS Omega. 2022 Jan 21;7(4):3177-3184. doi: 10.1021/acsomega.1c03780. eCollection 2022 Feb 1.

Abstract

Pt/SiO-AlO catalysts were prepared by the traditional impregnation method (IM) and the strong electrostatic adsorption (SEA) process. Differences in particle size, surface chemical state, Pt adsorption site, ammonia oxidation activity, and thermal stability of Pt species were studied systematically. For the fresh catalyst of Pt/SiO-AlO-IM (Pt/SiO-AlO-IM-fresh), Pt species were dispersed unselectively on SiO-AlO, and the large average size (6.6 nm) of Pt species could be observed in a bimodal distribution (ranges of 5.5-6.5 and 8.5-9.5 nm). After the hydrothermal treatment, the Pt size of the aged catalyst (Pt/SiO-AlO-IM-aged) increased significantly, especially Pt particles on SiO showed obvious agglomeration and some even increased to 40 nm. Conversely, for the catalyst prepared through the SEA process, Pt species of Pt/SiO-AlO-SEA-fresh were selectively absorbed on AlO, the Pt particle size was in the range of 1.5-6.0 nm, and the average particle size was only 2.7 nm. After hydrothermal aging, Pt species did not show obvious agglomeration (the average particle size was 3.2 nm). Above all, Pt/SiO-AlO-SEA presented better catalytic activity and thermal stability than Pt/SiO-AlO-IM, i.e., the temperatures of 50% NH conversion for the fresh and aged Pt/SiO-AlO-SEA catalysts were 216 and 223 °C, respectively, much lower than those for Pt/SiO-AlO-IM-fresh (228 °C) and Pt/SiO-AlO-IM-aged (250 °C).

摘要

采用传统浸渍法(IM)和强静电吸附(SEA)工艺制备了Pt/SiO-AlO催化剂。系统研究了Pt物种的粒径、表面化学状态、Pt吸附位点、氨氧化活性和热稳定性的差异。对于新鲜的Pt/SiO-AlO-IM催化剂(Pt/SiO-AlO-IM-新鲜),Pt物种无选择性地分散在SiO-AlO上,在双峰分布(5.5-6.5和8.5-9.5 nm范围)中可观察到较大的Pt物种平均粒径(6.6 nm)。水热处理后,老化催化剂(Pt/SiO-AlO-IM-老化)的Pt粒径显著增加,尤其是SiO上的Pt颗粒出现明显团聚,部分甚至增大到40 nm。相反,对于通过SEA工艺制备的催化剂,Pt/SiO-AlO-SEA-新鲜的Pt物种选择性吸附在AlO上,Pt粒径在1.5-6.0 nm范围内,平均粒径仅为2.7 nm。水热老化后,Pt物种未出现明显团聚(平均粒径为3.2 nm)。综上所述,Pt/SiO-AlO-SEA比Pt/SiO-AlO-IM表现出更好的催化活性和热稳定性,即新鲜和老化的Pt/SiO-AlO-SEA催化剂50% NH转化率的温度分别为216和223 °C,远低于Pt/SiO-AlO-IM-新鲜(228 °C)和Pt/SiO-AlO-IM-老化(250 °C)的温度。

https://cdn.ncbi.nlm.nih.gov/pmc/blobs/7f6a/8811775/6bc3f443f465/ao1c03780_0002.jpg

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