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柠檬酸络合法制备Ba促进ZrO_2负载Ru催化剂上氨合成反应性能
引用本文:林建新,王自庆,张留明,倪军,王榕,魏可镁.柠檬酸络合法制备Ba促进ZrO_2负载Ru催化剂上氨合成反应性能[J].催化学报,2012,33(7):1075-1079.
作者姓名:林建新  王自庆  张留明  倪军  王榕  魏可镁
作者单位:福州大学化肥催化剂国家工程研究中心,福建 福州,350002
基金项目:中国石油科技创新基金(2010D-5006-0502);国家科技支撑计划(2007BAE08B02);福建省教育厅科技项目(JK2011005)~~
摘    要:采用柠檬酸络合法制备了一系列不同含量Ba掺杂的ZrO2,再用浸渍法制备了K-Ru/Ba-ZrO2催化剂并将其用于氨合成反应.采用X射线衍射和CO2程序升温脱附技术考察了Ba含量对催化剂结构与性能的影响.结果表明,Ba掺入ZrO2后形成的BaZrO3有助于其负载的Ru催化剂氨合成活性的显著提高.在5.0MPa,10000h–1,425oC时,Ru/Ba-ZrO2(Ba:Zr摩尔比为1:1)催化剂活性最高,出口氨浓度和反应速率分别达9.24%和29.77mmol/(g·h).这主要归因于载体的强电子传导性能和碱性提高.

关 键 词:  二氧化锆    氨合成  电子作用

Ammonia Synthesis over Ruthenium Catalysts using Barium-Doped Zirconia as Supports Prepared by Citric Acid Method
LIN Jianxin , WANG Ziqing , ZHANG Liuming , NI Jun , WANG Rong , WEI Kemei.Ammonia Synthesis over Ruthenium Catalysts using Barium-Doped Zirconia as Supports Prepared by Citric Acid Method[J].Chinese Journal of Catalysis,2012,33(7):1075-1079.
Authors:LIN Jianxin  WANG Ziqing  ZHANG Liuming  NI Jun  WANG Rong  WEI Kemei
Institution:National Engineering Research Center of Chemical Fertilizer Catalyst, Fuzhou University, Fuzhou 350002, Fujian, China
Abstract:Barium-promoted zirconia (Ba-ZrO2) was synthesized by the citric acid method and used as supports for Ru/Ba-ZrO2 catalysts, which were prepared by incipient wetness impregnation with K2RuO4 as precursor. The obtained Ba-ZrO2 and catalysts were characterized by X-ray diffraction and CO2 temperature-programmed desorption. The effect of Ba content on the structure and catalytic activity of K-Ru/Ba-ZrO2 catalysts is discussed. The formation of BaZrO3 can improve significantly the catalytic activity of Ru/Ba-ZrO2 for ammonia synthesis. The ammonia concentration and rate of ammonia synthesis of the K-Ru/Ba-ZrO2 catalyst (molar ratio of Ba:Zr is 1:1) were 9.24% and 29.77 mmol/(g·h), respectively, at 425 °C, 5.0 MPa, and 10000 h–1. Improvements in electron conductivity and the basic nature of the catalyst may be the main reasons for such high catalytic activity in ammonia synthesis.
Keywords:barium  zircona  ruthenium  ammonia synthesis  electronic conductivity
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