Structure-dependent activity and stability of Al2O3 supported Rh catalysts for the steam reforming of n-dodecane

被引：14
作者：
Ao, Jingyan [1 ]
Wang, Ting [1 ]
Zhang, Bofeng [1 ]
Liu, Sibao [1 ]
Liu, Guozhu [1 ,2 ,3 ]
机构：
[1] Tianjin Univ, Sch Chem Engn & Technol, Key Lab Green Chem Technol, Minist Educ, Tianjin 300072, Peoples R China
[2] Haihe Lab Sustainable Chem Transformat, Tianjin 300072, Peoples R China
[3] Tianjin Univ, Zhejiang Inst, Ningbo 315201, Zhejiang, Peoples R China
来源：
INTERNATIONAL JOURNAL OF HYDROGEN ENERGY | 2022年 / 47卷 / 61期
基金：
中国国家自然科学基金;
关键词：
Alumina morphology; Rhodium catalyst; Steam reforming; Hydrogen; METHANE PARTIAL OXIDATION; RH/AL2O3 MODEL CATALYST; RICH GAS-PRODUCTION; HYDROGEN-PRODUCTION; ALUMINA CATALYSTS; TAR REMOVAL; PERFORMANCE; RHODIUM; SURFACE; FUEL;
D O I：
10.1016/j.ijhydene.2022.05.286
中图分类号：
O64 [物理化学（理论化学）、化学物理学];
学科分类号：
070304 ; 081704 ;
摘要：
Steam reforming of liquid hydrocarbon fuels is an appealing way for the production of hydrogen. In this work, the Rh/Al2O3 catalysts with nanorod (NR), nanofiber (NF) and sponge-shaped (SP) alumina supports were successfully designed for the steam reforming of n-dodecane as a surrogate compound for diesel/jet fuels. The catalysts before and after reaction were well characterized by using ICP, XRD, N-2 adsorption, TEM, HAADF-STEM, H-2- TPR, CO chemisorption, NH3-TPD, CO2-TPD, XPS, Al-27 NMR and TG. The results confirmed that the dispersion and surface structure of Rh species is quite dependent on the enclosed various morphologies. Rh/Al2O3-NR possesses highly dispersed, uniform and accessible Rh particles with the highest percentage of surface electron deficient Rh-0 active species, which due to the unique properties of Al2O3 nanorod including high crystallinity, relatively large alumina particle size, thermal stability, and large pore volume and size. As a consequent, Rh/Al2O3-NR catalyst exhibited superior catalytic activity towards steam reforming re-actions and hydrogen production rate over other two catalysts. Especially, Rh/Al2O3-NR catalyst showed the highest hydrogen production rate of 87,600 mmol gfuel-1 gRh-1min-1 among any Rh-based catalysts and other noble metal-based catalysts to date. After long-term reaction, a significant deactivation occurred on Rh/Al2O3-NF and Rh/Al2O3-SP cata-lysts, due to aggregation and sintering of Rh metal particles, coke deposition and poor hydrothermal stability of nanofibrous structure. In contrast, the Rh/Al2O3-NR catalyst shows excellent reforming stability with negligible coke formation. No significantly sin-tering and aggregation of the Rh particles is observed after long-term reaction. Such great catalyst stability can be explained by the role of hydrothermal stable nanorod alumina support, which not only provides a unique environment for the stabilization of uniform and small-size Rh particles but also affords strong surface basic sites. (c) 2022 Hydrogen Energy Publications LLC. Published by Elsevier Ltd. All rights reserved.
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收藏
页码：25471 / 25485
页数：15
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