Abstract
Methane conversion has received renewed interest due to the rapid growth in production of shale gas. Methane combustion for power generation and transportation is one of the alternatives for methane utilization. However, complete conversion of methane is critical to minimize negative environmental effects from unburned methane, whose noxious effect is 25 times greater than that of CO2. Although perovskite catalysts have high thermal stability, their low activities for methane combustion prevent them from being utilized on a commercial basis. In this work, we show the impact from reconstruction of surface and subsurface monolayers of perovskite catalysts on methane combustion, using SrTiO3 (STO) as a model perovskite. Several STO samples obtained through different synthetic methods and subjected to different postsynthetic treatments were tested for methane combustion. Through top surface characterization, kinetic experiments (including isotope labeling experiments) and density functional theory calculations, it is shown that both surface segregation of Sr and creation of step surfaces of STO can impact the rate of methane combustion over an order of magnitude. This work highlights the role of surface reconstruction in tuning perovskite catalysts for methane activation.
| Original language | English |
|---|---|
| Pages (from-to) | 10306-10315 |
| Number of pages | 10 |
| Journal | ACS Catalysis |
| Volume | 8 |
| Issue number | 11 |
| DOIs | |
| State | Published - Nov 2 2018 |
Funding
We thank Henry Luftman (Lehigh University) for performing LEIS analysis. This research was sponsored by the U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences, Chemical Sciences, Geosciences, and Biosciences Division. Parts of the work including electron microscopy (X.L. and M.C.), DRIFTS, BET, and kinetic measurement were conducted at the Center for Nanophase Materials Sciences (CNMS), which is a DOE Office of Science User Facility. This research used resources of the National Energy Research Scientific Computing Center, a DOE Office of Science User Facility supported by the Office of Science of the U.S. Department of Energy under Contract DE-AC02-05CH11231. This manuscript has been authored by UT-Battelle, LLC, under Contract DE-AC05-00OR22725 with the U.S. Department of Energy. The United States Government retains and the publisher, by accepting the article for publication, acknowledges that the United States Government retains a nonexclusive, paid-up, irrevocable, worldwide license to publish or reproduce the published form of this manuscript, or allow others to do so, for United States Government purposes. The Department of Energy will provide public access to these results of federally sponsored research in accordance with the DOE Public Access Plan (http://energy. gov/downloads/doe-public-access-plan) We thank Henry Luftman (Lehigh University) for performing LEIS analysis. This research was sponsored by the U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences, Chemical Sciences, Geosciences, and Biosciences Division. Parts of the work including electron microscopy (X.L. and M.C.), DRIFTS, BET, and kinetic measurement were conducted at the Center for Nanophase Materials Sciences (CNMS), which is a DOE Office of Science User Facility. This research used resources of the National Energy Research Scientific Computing Center, a DOE Office of Science User Facility supported by the Office of Science of the U.S. Department of Energy under Contract DE-AC02-05CH11231. This manuscript has been authored by UT-Battelle, LLC, under Contract DE-AC05-00OR22725 with the U.S. Department of Energy.
| Funders | Funder number |
|---|---|
| BET | |
| DOE Office of Science | DE-AC05-00OR22725, DE-AC02-05CH11231 |
| DRIFTS | |
| Office of Basic Energy Sciences | |
| U.S. Department of Energy | |
| Office of Science | |
| Chemical Sciences, Geosciences, and Biosciences Division |