Understanding Active Sites in the Water–Gas Shift Reaction for Pt–Re Catalysts on Titania

ACS Catalysis ◽  
2017 ◽  
Vol 7 (4) ◽  
pp. 2597-2606 ◽  
Author(s):  
Audrey S. Duke ◽  
Kangmin Xie ◽  
Amy J. Brandt ◽  
Thathsara D. Maddumapatabandi ◽  
Salai C. Ammal ◽  
...  
2016 ◽  
Vol 25 (6) ◽  
pp. 1051-1057 ◽  
Author(s):  
Xiaodong Chen ◽  
Xiong Su ◽  
Binglian Liang ◽  
Xiaoli Yang ◽  
Xinyi Ren ◽  
...  

2012 ◽  
Vol 286 ◽  
pp. 279-286 ◽  
Author(s):  
Jorge H. Pazmiño ◽  
Mayank Shekhar ◽  
W. Damion Williams ◽  
M. Cem Akatay ◽  
Jeffrey T. Miller ◽  
...  

Author(s):  
Lingling Zhang ◽  
Qi Song ◽  
Yimeng Xing ◽  
Zhichun Si ◽  
Yuxiang Liu ◽  
...  

Reverse water gas shift reaction (RWGS) is an important process which plays a vital role in many CO2 utilization related reactions. Noble metals are the most active catalysts in RWGS, but the high price and low reserve strangled their applications. In the present work, we reported a non-transition-metal MgAl2O4 catalyst which showed outstanding activity and stability at high temperatures in the RWGS reaction and improved performance after doping of single atomic Nin+. The catalyst can obtain 46% of CO2 conversion in durability test of 75 h at 800 °C under high weight hourly space velocities (225 000 ml g-1 h-1). The adsorption sites, possible reaction route, and effects of Nin+ single atoms on the (111) surface of MgAl2O4 for RWGS were investigated by in situ DRIFTS and DFT calculations. The results indicated that the rate determining reaction step of RWGS on MgAl2O4 and Ni (SA)/MgAl2O4 were both the reaction of OH* + H* → H2O* + *, but the energy barrier was significantly reduced after introducing single atomic Nin+. Nin+ atoms can increase the hydroxyl coverage on the surface of catalyst and Al3+ sites near the Nin+ ion are considered as the predominant active sites for RWGS reactions.


2021 ◽  
Author(s):  
Jian Zhang ◽  
Pan Yin ◽  
Ming Xu ◽  
Guoqing Cui ◽  
Jun Yu ◽  
...  

Abstract In the heterogeneous field, modulation over strong metal-support interactions (SMSI) plays a crucial role in boosting catalytic performance toward interface-sensitive reactions (e.g., water gas shift reaction, WGSR). Herein, a CuZnTi ternary catalyst was prepared via in situ structural topological transformation from CuZnTi-layered double hydroxides precursor (CuZnTi-LDHs). The resulting catalyst Cu/ZnTi-MMO(H350) exhibits an extraordinarily high catalytic activity toward low temperature-WGSR with a reaction rate of 19.7 μmolCO gcat-1 s-1 at 250 °C, among the highest level in Cu-based catalysts. Advanced electron microscope and in situ spectroscopy characterizations verify that Cu nanoparticles (particle size: 7~10 nm) are modified by ZnTi-mixed metal oxides with abundant Cuδ+−Ov−Ti3+ (0<δ<1) interfacial sites. Incorporation of Ti element facilitates the reduction of ZnO to stabilize Cuδ+ species at the interface, which enhances the chemisorption of CO molecule. Simultaneously, neighboring Ov−Ti3+ species significantly promotes the dissociation of H2O molecule. The structure-activity correlation studies based on quasi-in situ XPS, in situ DRIFTS, in situ and operando EXAFS reveal that the interfacial sites (Cuδ+−Ov−Ti3+) serve as the intrinsic active sites of WGS reaction. A combination of in situ characterization techniques and DFT calculations further substantiate that associative mechanism is the predominant reactive path below 200 °C whilst redox mechanism is overwhelming above 250 °C in the presence of Cu/ZnTi-MMO catalyst. This work demonstrates a facile modulation on metal-support interfacial structure via LDHs approach, which paves a way for rational design and preparation of heterogeneous catalysts.


2010 ◽  
Vol 273 (1) ◽  
pp. 18-28 ◽  
Author(s):  
Ching-Shiun Chen ◽  
Tzu-Wen Lai ◽  
Chen-Chih Chen

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