| Pd-Fe/α-Al_2O_3催化CO偶联制草酸二乙酯催化剂临氢失活研究 |
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| 引用本文： | 房金刚,李振花,许根慧,王保伟,宋瑛.Pd-Fe/α-Al_2O_3催化CO偶联制草酸二乙酯催化剂临氢失活研究[J].石油化工,2003,32(12):1021-1023. |
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| 作者姓名： | 房金刚 李振花 许根慧 王保伟 宋瑛 |
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| 作者单位： | 天津大学化,工学院一碳化学与化工国家重点实验室,天津,300072 |
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| 基金项目： | 国家九五科技攻关项目(96-539-01-01)。 |
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| 摘 要： | 一氧化碳常压气相催化偶联制草酸二乙酯的反应中,由于氢的引入致使偶联反应催化剂Pd-Fe/α-Al2O3失活。研究了不同氢含量条件下催化剂失活以及失活催化剂再生规律,发现催化剂的失活为可逆的,且失活速率随原料气中氢含量的增加而加快。应用X射线光电子能谱、程序升温还原等方法对催化剂中Pd的形态变化进行了分析,发现临氢失活催化剂比反应后催化剂的Pd2+含量要低得多。结果表明,原料气中氢的存在抑制了二价钯的烷氧基中间体Pd(OC2H5)2在催化剂上的产生,从而抑制了草酸二乙酯的生成,导致了催化剂的失活。
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| 关 键 词： | 氢 钯 失活 草酸二乙酯 CO偶联 催化剂 |
| 文章编号： | 1000-8144(2003)12-1021-03 |
| 修稿时间： | 2003年6月10日 |
Study on Deactivation of Pd-Fe/α-Al2O3 Catalyst with Hydrogen in CO Coupling to Diethyl Oxalate |
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| FANG Jin-gang,LI Zhen-hua,XU Gen-hui,WANG Bao-wei,SONG Ying ing,Tianjin University,Tianjin ,China.Study on Deactivation of Pd-Fe/α-Al2O3 Catalyst with Hydrogen in CO Coupling to Diethyl Oxalate[J].Petrochemical Technology,2003,32(12):1021-1023. |
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| Authors: | FANG Jin-gang LI Zhen-hua XU Gen-hui WANG Bao-wei SONG Ying ing Tianjin University Tianjin China |
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| Affiliation: | FANG Jin-gang,LI Zhen-hua,XU Gen-hui,WANG Bao-wei,SONG Ying ing,Tianjin University,Tianjin 300072,China) |
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| Abstract: | Pd-Fe/α-Al_2O_3 catalyst was deactivated with introduction of H_2 to gaseous phase reaction of CO coupling to diethyl oxalate(DEO).Study on effect of different H_2 concentration showed that deactivation of catalyst was reversible and rate of deactivation was correspondent to concentration of H_2.XPS and TPR showed that after CO reaction,Pd on catalyst would be partially oxidized to Pd~(2+),but the amount of Pd~(2+) was much less than that in deactivated catalyst.Due formation of Pd~(2+)(OC_2H_5)_2,an intermediate to DEO,was inhibited by H_2,leading to catalyst deactivation. |
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| Keywords: | H_2 Pd deactivation diethyl oxalate CO coupling catalyst |
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