Carbon intermediates during CO2 reforming of methane over Ni-CaO-ZrO2 catalysts: A temperature-programmed surface reaction study

被引:31
|
作者
Wang, Changzhen [1 ]
Sun, Nannan [2 ]
Wei, Wei [2 ]
Zhao, Yongxiang [1 ]
机构
[1] Shanxi Univ, Minist Educ, Engn Res Ctr Fine Chem, Taiyuan 030006, Peoples R China
[2] Chinese Acad Sci, Shanghai Adv Res Inst, CAS Key Lab Low Carbon Convers Sci & Engn, Shanghai 201203, Peoples R China
基金
中国国家自然科学基金;
关键词
Temperature-programmed surface reaction; CO2; reforming; Methane; Carbon intermediate; Coking mechanism; SOLID-SOLUTION CATALYSTS; SYNTHESIS GAS; HYDROGEN-PRODUCTION; NOBLE-METALS; DIOXIDE; NI; CH4; NICKEL; COKE; DEACTIVATION;
D O I
10.1016/j.ijhydene.2016.08.128
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
The carbon intermediates for dry reforming of methane over Ni-CaO-ZrO2, catalysts during the initial reaction period were studied by temperature-programmed surface reaction (TPSR) techniques, including temperature-programmed hydrogenation (TPH), temperature-programmed CO2 reaction (TPRn CO2) and temperature-programmed oxidation (TPO). Three carbon species were detected on the catalysts surface during dry reforming, namely C alpha, C beta and C gamma. However, due to the different redox properties of Ni-CaO-ZrO2 catalysts, the individual carbon intermediate amount and interaction with the catalyst surface was distinct, which in turn led to the different reaction performance of both catalysts. The TPH-TPO and TPRn CO2-TPO tests showed that H-2 and CO2 had weaker elimination ability than O-2 and their elimination ability was lied on the carbon intermediate properties and the interaction with the support. According to the TPSR results, a possible mechanism of coking for dry reforming over Ni-CaO-ZrO2 catalysts was proposed, based on which the carbon intermediates might convert to the others or dissolve on the metal sites forming carbon deposits. (C) 2016 Hydrogen Energy Publications LLC. Published by Elsevier Ltd. All rights reserved.
引用
收藏
页码:19014 / 19024
页数:11
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