Abstract
Nanomaterials derived from earth-abundant metal oxides have gained tremendous interest as catalysts; although, water stability remains a challenge. This study examines MgO(111) surfaces for 2-pentanone condensation and their evolution during D2O hydration. Catalyst screening confirmed the high activity of fresh MgO(111) for 2-pentanone condensation relative to conventionally prepared MgO(100). Computational modeling suggests that the (111) surface is readily hydroxylated, and that surface hydroxyls help stabilize the surface and reduce the barrier for 2-pentanone condensation. Vapor-phase D2O hydration after 3 min increased MgO(111) hydroxyls and retained surface area and activity; however, after 1 h, deuteroxide formation reduced the surface area and activity by >30 %. After 24 h, deuteroxide growth slowed down, and surface area and activity remained stable. This suggests MgO(111)-derived hydroxide may be the dominant surface responsible for 2-pentanone condensation following water exposure. Thermal regeneration of the 24-h sample restored 86 % of the surface area and 94 % of the activity.
Original language | English |
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Article number | 120234 |
Journal | Applied Catalysis B: Environmental |
Volume | 294 |
DOIs | |
State | Published - Oct 5 2021 |
Funding
We would like to thank Allyson York, Sarah Shulda, Michael Griffin, Alexander Rein, and Jim Stunkel for their contributions and helpful discussion. This work was authored in part by Alliance for Sustainable Energy, LLC, the manager and operator of the National Renewable Energy Laboratory for the U.S. Department of Energy (DOE) under Contract No. No. DE-AC36-08GO28308. Funding was provided in part by the U.S. Department of Energy Office of Energy Efficiency and Renewable Energy Bioenergy Technologies Office (BETO) . This work was partially performed in collaboration with the Chemical Catalysis for Bioenergy Consortium (ChemCatBio), a member of the Energy Materials Network, and was supported by the DOE Bioenergy Technologies Office under Contract No. DE-AC05-00OR22725 with Oak Ridge National Laboratory and Contract No. DE-AC36-08-GO28308 with NREL. Microscopy was performed in collaboration with the Chemical Catalysis for Bioenergy Consortium under Contract no DE-AC05-00OR22725 with Oak Ridge National Laboratory (ORNL) and through a user project supported by ORNL’s Center for Nanophase Materials Sciences (CNMS), which is sponsored by the Scientific User Facilities Division, Office of Basic Energy Sciences, U.S. Department of Energy. Part of the microscopy research was also supported by the Office of Nuclear Energy, Fuel Cycle R&D Program and the Nuclear Science User Facilities. This research used the NOMAD instrument at the Spallation Neutron Source, a DOE Office of Science User Facility operated by Oak Ridge National Laboratory. The Neutron Scattering research is sponsored by the U.S. Department of Energy (DOE), Office of Energy Efficiency and Renewable Energy, Bioenergy Technologies Office, under contract DE-AC05-00OR22725 with UT-Battelle, LLC. We acknowledge support from the Consortium for Computational Physics and Chemistry by BETO for computational studies. The computing resources are provided by “BEBOP”, a computing cluster operated by the Laboratory Computing Resource Center at Argonne National Laboratory (ANL). This manuscript has been authored in part by UT-Battelle, LLC, under contract DE-AC0500OR22725 with the US Department of Energy (DOE). The US government retains and the publisher, by accepting the article for publication, acknowledges that the US 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 US government purposes. DOE 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 ). The views expressed in the article do not necessarily represent the views of the U.S. Department of Energy or the U.S. Government. The U.S. Government retains and the publisher, by accepting the article for publication, acknowledges that the U.S. Government retains a nonexclusive, paid-up, irrevocable, worldwide license to publish or reproduce the published form of this work, or allow others to do so, for U.S. Government purposes. We would like to thank Allyson York, Sarah Shulda, Michael Griffin, Alexander Rein, and Jim Stunkel for their contributions and helpful discussion. This work was authored in part by Alliance for Sustainable Energy, LLC, the manager and operator of the National Renewable Energy Laboratory for the U.S. Department of Energy (DOE) under Contract No. No. DE-AC36-08GO28308. Funding was provided in part by the U.S. Department of Energy Office of Energy Efficiency and Renewable Energy Bioenergy Technologies Office (BETO). This work was partially performed in collaboration with the Chemical Catalysis for Bioenergy Consortium (ChemCatBio), a member of the Energy Materials Network, and was supported by the DOE Bioenergy Technologies Office under Contract No. DE-AC05-00OR22725 with Oak Ridge National Laboratory and Contract No. DE-AC36-08-GO28308 with NREL. Microscopy was performed in collaboration with the Chemical Catalysis for Bioenergy Consortium under Contract no DE-AC05-00OR22725 with Oak Ridge National Laboratory (ORNL) and through a user project supported by ORNL's Center for Nanophase Materials Sciences (CNMS), which is sponsored by the Scientific User Facilities Division, Office of Basic Energy Sciences, U.S. Department of Energy. Part of the microscopy research was also supported by the Office of Nuclear Energy, Fuel Cycle R&D Program and the Nuclear Science User Facilities. This research used the NOMAD instrument at the Spallation Neutron Source, a DOE Office of Science User Facility operated by Oak Ridge National Laboratory. The Neutron Scattering research is sponsored by the U.S. Department of Energy (DOE), Office of Energy Efficiency and Renewable Energy, Bioenergy Technologies Office, under contract DE-AC05-00OR22725 with UT-Battelle, LLC. We acknowledge support from the Consortium for Computational Physics and Chemistry by BETO for computational studies. The computing resources are provided by “BEBOP”, a computing cluster operated by the Laboratory Computing Resource Center at Argonne National Laboratory (ANL). This manuscript has been authored in part by UT-Battelle, LLC, under contract DE-AC0500OR22725 with the US Department of Energy (DOE). The US government retains and the publisher, by accepting the article for publication, acknowledges that the US 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 US government purposes. DOE 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). The views expressed in the article do not necessarily represent the views of the U.S. Department of Energy or the U.S. Government. The U.S. Government retains and the publisher, by accepting the article for publication, acknowledges that the U.S. Government retains a nonexclusive, paid-up, irrevocable, worldwide license to publish or reproduce the published form of this work, or allow others to do so, for U.S. Government purposes.
Keywords
- Catalyst regeneration
- Metal oxide hydration
- Neutron total scattering