催化学报

催化学报 ›› 2010, Vol. 31 ›› Issue (10): 1247-1252.DOI: 10.3724/SP.J.1088.2010.00327

• 研究论文 • 上一篇    下一篇

Pt/CexZr1-xO2 催化剂在含硫合成气中催化水煤气变换反应活性

刘冰 1,2, 李文钊 1, 徐恒泳 1   

  1. 1 中国科学院大连化学物理研究所, 辽宁大连 116023; 2 中国科学院研究生院, 北京 100049
  • 收稿日期:2010-10-25 出版日期:2010-10-25 发布日期:2014-03-04

Water Gas Shift Activity of Pt/CexZr1-xO2 Catalysts in Sulfur-Containing Syngas

LIU Bing1,2, LI Wenzhao1, XU Hengyong1,*   

  1. 1Dalian Institute of Chemical Physics, Chinese Academy of Sciences, Dalian 116023, Liaoning, China; 2Graduate University of Chinese Academy of Sciences, Beijing 100049, China
  • Received:2010-10-25 Online:2010-10-25 Published:2014-03-04

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摘要： 采用浸渍法制备了 Pt/CexZr1-xO2 催化剂, 通过 X 射线衍射和程序升温还原等方法对催化剂进行了表征, 并在固定床反应器中评价了催化剂在合成气和含硫合成气中的水煤气变换活性. 结果表明, 铈锆固溶体的氧化还原能力强于 CeO2, Zr 的掺杂明显改善了 CeO2 的孔道结构, 其担载的 Pt 催化剂具有更高的金属分散度, 因而活性更高. 两种催化剂在含硫合成气中的催化活性较无硫合成气中的均有所降低, 且 H2S 浓度越大, 催化剂活性下降越多, 但这种因吸附硫而引起的失活是可逆的, 即催化剂重新暴露在无 H2S 重整气的还原性气氛下活性能基本恢复.

关键词: 水煤气变换, 铈, 锆, 固溶体, 氧化还原能力, 铂, 硫化氢, 可逆中毒

Abstract: A series of Pt/CexZr1-xO2 catalysts were prepared by the wet-impregnation method, characterized by X-ray diffraction and tem-perature-programmed reduction, and tested in the water gas shift (WGS) reaction. The results show that the CexZr1-xO2 solid solution has higher redox ability, and doping ceria with zirconium apparently changes the pore structure. The Pt catalysts supported on CexZr1-xO2 has higher Pt dispersion and WGS activity in pure reforming syngas. The WGS activity dropped in sulfur-containing syngas over the Pt/CexZr1-xO2 catalysts. The loss of activity increases with the increase of H2S content, but the deactivation of the catalyst due to H2S adsorp-tion is reversible and can be readily reversed in the reducing atmosphere of the WGS mixture without H2S.

Key words: water gas shift, cerium, zirconium, solid solution, redox ability, platinum, hydrogen sulfide, reversible poisoning