TY - JOUR
T1 - Submonolayer Is Enough
T2 - Switching Reaction Channels on Pt/SiO2by Atomic Layer Deposition
AU - Tang, Xin
AU - Liu, Chao
AU - Long, Edmund A.
AU - Lin, Wei
AU - Hackler, Ryan A.
AU - Wang, Xiang
AU - Marks, Laurence D.
AU - Notestein, Justin M.
AU - Stair, Peter C.
N1 - Funding Information:
This material is based upon work supported by the Institute for Catalysis in Energy Processes (ICEP) at Northwestern University under U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences Award DOE DE-FG02-03-ER15457.
Publisher Copyright:
© 2021 American Chemical Society.
PY - 2021/9/2
Y1 - 2021/9/2
N2 - The reaction mechanism of CO2 with H2 is studied on platinum nanoparticles supported on fumed silica. It is found that platinum nanoparticle size, reaction temperature, and metal oxide promoters play important roles in determining the reaction rate and the mechanism of forming surface carbonyl species. Metal oxide promoters consist of submonolayer titanium oxide or aluminum oxide overcoated onto the catalysts by atomic layer deposition (ALD). These alter the CO formation rate, influence the adsorption and desorption behavior, and switch the surface reaction channel from the Eley-Rideal to Langmuir-Hinshelwood mechanism due to an enhancement of CO2 affinity to the metal-metal oxide interface. At the temperatures relevant for catalytic turnover, ALD overcoating significantly increases catalytic activity in CO2 hydrogenation to CH4 and CO, while the identity of the oxide overcoat helps control product selectivity.
AB - The reaction mechanism of CO2 with H2 is studied on platinum nanoparticles supported on fumed silica. It is found that platinum nanoparticle size, reaction temperature, and metal oxide promoters play important roles in determining the reaction rate and the mechanism of forming surface carbonyl species. Metal oxide promoters consist of submonolayer titanium oxide or aluminum oxide overcoated onto the catalysts by atomic layer deposition (ALD). These alter the CO formation rate, influence the adsorption and desorption behavior, and switch the surface reaction channel from the Eley-Rideal to Langmuir-Hinshelwood mechanism due to an enhancement of CO2 affinity to the metal-metal oxide interface. At the temperatures relevant for catalytic turnover, ALD overcoating significantly increases catalytic activity in CO2 hydrogenation to CH4 and CO, while the identity of the oxide overcoat helps control product selectivity.
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U2 - 10.1021/acs.jpcc.1c04972
DO - 10.1021/acs.jpcc.1c04972
M3 - Article
AN - SCOPUS:85114596095
VL - 125
SP - 18725
EP - 18733
JO - Journal of Physical Chemistry C
JF - Journal of Physical Chemistry C
SN - 1932-7447
IS - 34
ER -