Low Temperature Water–Gas Shift/Methanol Steam Reforming: Alkali Doping to Facilitate the Scission of Formate and Methoxy C–H Bonds over Pt/ceria Catalyst

2007 ◽  
Vol 122 (1-2) ◽  
pp. 9-19 ◽  
Author(s):  
Harold N. Evin ◽  
Gary Jacobs ◽  
Javier Ruiz-Martinez ◽  
Uschi M. Graham ◽  
Alan Dozier ◽  
...  
2007 ◽  
Vol 328 (1) ◽  
pp. 14-26 ◽  
Author(s):  
John M. Pigos ◽  
Christopher J. Brooks ◽  
Gary Jacobs ◽  
Burtron H. Davis

2007 ◽  
Vol 120 (3-4) ◽  
pp. 166-178 ◽  
Author(s):  
Harold N. Evin ◽  
Gary Jacobs ◽  
Javier Ruiz-Martinez ◽  
Gerald A. Thomas ◽  
Burtron H. Davis

Catalysts ◽  
2021 ◽  
Vol 11 (2) ◽  
pp. 210
Author(s):  
Caleb Daniel Watson ◽  
Michela Martinelli ◽  
Donald Charles Cronauer ◽  
A. Jeremy Kropf ◽  
Gary Jacobs

Recent studies have shown that appropriate levels of alkali promotion can significantly improve the rate of low-temperature water gas shift (LT-WGS) on a range of catalysts. At sufficient loadings, the alkali metal can weaken the formate C–H bond and promote formate dehydrogenation, which is the proposed rate determining step in the formate associative mechanism. In a continuation of these studies, the effect of Rb promotion on Pt/ZrO2 is examined herein. Pt/ZrO2 catalysts were prepared with several different Rb loadings and characterized using temperature programmed reduction mass spectrometry (TPR-MS), temperature programmed desorption (TPD), diffuse reflectance infrared Fourier transform spectroscopy (DRIFTS), an X-ray absorption near edge spectroscopy (XANES) difference procedure, extended X-ray absorption fine structure spectroscopy (EXAFS) fitting, TPR-EXAFS/XANES, and reactor testing. At loadings of 2.79% Rb or higher, a significant shift was seen in the formate ν(CH) band. The results showed that a Rb loading of 4.65%, significantly improves the rate of formate decomposition in the presence of steam via weakening the formate C–H bond. However, excessive rubidium loading led to the increase in stability of a second intermediate, carbonate and inhibited hydrogen transfer reactions on Pt through surface blocking and accelerated agglomeration during catalyst activation. Optimal catalytic performance was achieved with loadings in the range of 0.55–0.93% Rb, where the catalyst maintained high activity and exhibited higher stability in comparison with the unpromoted catalyst.


2004 ◽  
Vol 267 (1-2) ◽  
pp. 27-33 ◽  
Author(s):  
Gary Jacobs ◽  
Adam Crawford ◽  
Leann Williams ◽  
Patricia M Patterson ◽  
Burtron H Davis

2004 ◽  
Vol 269 (1-2) ◽  
pp. 63-73 ◽  
Author(s):  
Gary Jacobs ◽  
Patricia M. Patterson ◽  
Uschi M. Graham ◽  
Dennis E. Sparks ◽  
Burtron H. Davis

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