Resolving the Reaction Mechanism for H2 Formation from High-Temperature Water-Gas Shift by Chromium-Iron Oxide Catalysts

被引:53
作者
Zhu, Minghui [1 ]
Wachs, Israel E. [1 ]
机构
[1] Lehigh Univ, Operando Mol Spect & Catalysis Lab, Dept Chem & Biomol Engn, Bethlehem, PA 18015 USA
基金
美国国家科学基金会;
关键词
redox mechanism; formate mechanism; associative mechanism; HT-WGS; iron-based catalysts; hydrogen; PROGRAMMED DESORPTION; HYDROGEN-PRODUCTION; FISCHER-TROPSCH; KINETICS; STATIONARY; MAGNETITE; STEAM;
D O I
10.1021/acscatal.6b00659
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 reaction mechanism of the high-temperature water gas shift (HT-WGS) reaction catalyzed by chromium iron oxide catalysts for H-2 production has been studied for 100 years with two reaction mechanisms proposed: redox and associative (involving surface HCOO*). Direct experimental support for either mechanism, however, is still lacking, which hinders a thorough understanding of catalytic roles of each elements and the rational design of Cr-free catalysts. The current study demonstrates, with temperature-programmed surface reaction (TPSR) spectroscopy (CO-TPSR, CO+H2O-TPSR, and HCOOH-TPSR), for the first time that the HT-WGS reaction follows the redox mechanism and that the associative mechanism does not take place.
引用
收藏
页码:2827 / 2830
页数:4
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