文献类型：期刊文献

英文题名：Kinetics and Mechanism Study of Low-Temperature Selective Catalytic Reduction of NO with Urea Supported on Pitch-Based Spherical Activated Carbon

作者：Wang, Zhi[1];Wang, Yanli[1];Long, Donghui[1];Mochida, Isao[2];Qiao, Wenming[1];Zhan, Liang[1];Liu, Xiaojun[1];Yoon, Seong-Ho[2];Ling, Licheng[1]

机构：[1]E China Univ Sci & Technol, State Key Lab Chem Engn, Shanghai 200237, Peoples R China;[2]Kyushu Univ, Inst Mat Chem & Engn, Fukuoka 8168580, Japan

年份：2011

卷号：50

期号：10

起止页码：6017

外文期刊名：INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH

收录：;EI(收录号：20112013985570);WOS:【SCI-EXPANDED(收录号:WOS:000290373200017)】；

基金：The authors gratefully acknowledge financial support from the National High-Tech Research and Development Program (No. 2007AA05Z311), the Natural Science Foundation of China (No. 20806024 and No. 20977028), and the Research Fund for the Doctoral Program of Higher Education (No. 200900-74110009).

语种：英文

外文关键词：Temperature - Activated carbon - Activation energy - Kinetics - Oxidation - Metabolism - Selective catalytic reduction - Reaction kinetics - Reduction - Nitrogen oxides

摘要：The kinetics and mechanism of selective catalytic reduction (SCR) of NO with urea supported on pitch-based spherical activated carbons (PSACs) were studied at low temperatures. NO oxidation to NO(2) catalyzed by the 0.5-0.8 nm micropores in PSACs was found to be the rate-limiting step in urea-SCR reaction, which was confirmed by both the apparent activation energy calculations and the kinetics results of urea-SCR reaction and NO oxidation on PSAC. These two reactions gave very similar negative apparent activation energies (-16.5 kJ/mol for urea-SCR reaction and -15.2 kJ/mol for NO oxidation), indicating that the adsorption of reactants on PSAC is of key importance in these two reactions. Moreover, these two reactions were both approximately first-order with respect to NO and one-half order with respect to O(2). It was found that NO(3) from the disproportionation of the produced NO(2) was quickly reduced by supported urea into N(2). After the complete consumption of supported urea, NO(2) started to release, and the carbon surface was gradually oxidized by adsorbed NO(x) species. NO(3) was found to be stably adsorbed on the oxidized carbon surface. On the basis of the results obtained, a reaction mechanism of low-temperature urea-SCR reaction on PSAC was proposed and discussed.