Jie Zhao, Ruixue Bao, Ruru Sun, Xiaolong Zhang, Tao Zhang, Chuanyi Wang
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引用次数: 0
Abstract
The reverse water–gas shift reaction (RWGS) has been regarded as an important route for CO2 utilization. Because the RWGS reaction is a mildly endothermic and competitive reaction with CO2 methanation, it is necessary to explore catalysts with high activity and selectivity at low reaction temperatures. Herein, we investigate the catalytic characteristic of silica-supported Pt-In alloy for RWGS reaction by comparing it with silica-supported Pt and In2O3-modified Pt. It is found that Pt-In/SiO2 exhibits significantly higher activity than Pt/SiO2 at reaction temperatures from 140 to 200 °C, and equivalent activities appear at 240 °C. Further raising the temperatures, the activity of Pt/SiO2 increases rapidly. CO selectivity over Pt-In/SiO2 is close to 100 % and higher than Pt/SiO2 (∼95 %) under dynamic reaction mode, being attributed to the effective expelling of CO away from the Pt-In surface by CO2 molecules and the decreased atomic hydrogen supply. Moreover, the formate and the redox pathways were followed over Pt-In/SiO2 and Pt/SiO2, respectively. Except for higher activity and selectivity to CO, In2O3-modified Pt exhibits the same catalytic pathways as Pt/SiO2. The present work supplied a guide to explore efficient catalysts for RWGS reaction at low reaction temperatures.
水气倒转反应（RWGS）已被认为是二氧化碳利用的重要途径。由于RWGS反应是一个温和的吸热和与CO2甲烷化竞争的反应，因此有必要探索在低反应温度下具有高活性和选择性的催化剂。本文通过对比二氧化硅负载Pt和in2o3修饰Pt对RWGS反应的催化性能，研究了二氧化硅负载Pt- in合金对RWGS反应的催化性能。结果表明，在反应温度为140 ~ 200℃时，Pt- in /SiO2表现出明显高于Pt/SiO2的活性，在反应温度为240℃时表现出相当的活性。温度进一步升高，Pt/SiO2的活性迅速提高。在动态反应模式下，Pt- in /SiO2的CO选择性接近100%，高于Pt/SiO2(~ 95%)，这是由于CO2分子有效地将CO从Pt- in表面排出和原子氢供应减少所致。此外，Pt- in /SiO2和Pt/SiO2上分别发生甲酸和氧化还原反应。除了对CO具有更高的活性和选择性外，in2o3修饰的Pt表现出与Pt/SiO2相同的催化途径。本研究为探索低反应温度下RWGS反应的高效催化剂提供了指导。
期刊介绍：
Molecular Catalysis publishes full papers that are original, rigorous, and scholarly contributions examining the molecular and atomic aspects of catalytic activation and reaction mechanisms. The fields covered are:
Heterogeneous catalysis including immobilized molecular catalysts
Homogeneous catalysis including organocatalysis, organometallic catalysis and biocatalysis
Photo- and electrochemistry
Theoretical aspects of catalysis analyzed by computational methods
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