{"id":{"repo_id":"uiuc","oai_identifier":"oai:www.ideals.illinois.edu:2142/113326"},"canonical_url":"https://search.dev.ndltd.org/etd/uiuc/oai:www.ideals.illinois.edu:2142/113326","repository":{"repo_id":"uiuc","name":"University of Illinois - Urbana-Champaign","base_url":"https://www.ideals.illinois.edu/oai-pmh"},"display":{"title":"Structural and mechanistic identification of heterogeneous catalysts","abstract":"Due to their importance and widespread use in the chemical and energy industries, understanding and improving heterogeneous catalysts is essential to advance their development and enable more sustainable processes. Atomically disperse or single atom catalysts have shown particular promise for their ability to exceed nanoparticle catalysts with regards to activity, stability and selectivity for a growing number of chemical reactions. Understanding key properties of these materials, such as structure-property relationships, structural dynamics and reaction-driven restructuring, is, however, often complicated by issues including low weight loadings, strong metal-support interactions and heterogeneity in active component speciations. The following work details how these challenges may be addressed through a review of how a multimodal approach including scanning transmission electron microscopy, diffuse reflectance infrared Fourier transform spectroscopy, X-ray photoelectron spectroscopy and X-ray absorption spectroscopy may be employed to identify the catalytically relevant properties (charge state, electronic structure, atomic configuration, bonding interaction). Furthermore, this approach is demonstrated through its application to Pt-Ni bimetallic nanoparticles on mesoporous silica, single atom Pt on CeO2, nanoparticle Pt on CeO2 and single atom Pt on Gd-doped CeO2.","abstract_html":"Due to their importance and widespread use in the chemical and energy industries, understanding and improving heterogeneous catalysts is essential to advance their development and enable more sustainable processes. Atomically disperse or single atom catalysts have shown particular promise for their ability to exceed nanoparticle catalysts with regards to activity, stability and selectivity for a growing number of chemical reactions. Understanding key properties of these materials, such as structure-property relationships, structural dynamics and reaction-driven restructuring, is, however, often complicated by issues including low weight loadings, strong metal-support interactions and heterogeneity in active component speciations. The following work details how these challenges may be addressed through a review of how a multimodal approach including scanning transmission electron microscopy, diffuse reflectance infrared Fourier transform spectroscopy, X-ray photoelectron spectroscopy and X-ray absorption spectroscopy may be employed to identify the catalytically relevant properties (charge state, electronic structure, atomic configuration, bonding interaction). Furthermore, this approach is demonstrated through its application to Pt-Ni bimetallic nanoparticles on mesoporous silica, single atom Pt on CeO2, nanoparticle Pt on CeO2 and single atom Pt on Gd-doped CeO2.","abstract_has_math":false,"creators":["Kottwitz, Matthew"],"institution":"University of Illinois at Urbana-Champaign","degree_name":"Ph.D.","degree_level":"Dissertation","degree_discipline":"Chemistry","degree_department":null,"school":null,"contributors":["Nuzzo, Ralph G.","Gewirth, Andrew A.","Kenis, Paul J. A.","Murphy, Catherine J."],"advisors":[],"committee_chairs":[],"committee_members":[],"year":2022,"date_issued":"2022-01-12T22:56:10Z","date_published":"2022-01-12T22:56:10Z","updated_at":"2026-07-22T22:24:53Z","subjects":["single atom","catalysis","heterogeneous"],"languages":["en"],"rights":["Copyright 2021 Matthew Kottwitz"],"rights_urls":[],"identifier_entries":[]},"links":{"outbound_url":"http://hdl.handle.net/2142/113326","outbound_label":"Handle","outbound_source":"dc:identifier"},"metadata_groups":[{"id":"people","label":"People","entries":[{"key":"dc:contributor","label":"Contributor","values":["Nuzzo, Ralph G.","Gewirth, Andrew A.","Kenis, Paul J. 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Atomically disperse or single atom catalysts have shown particular promise for their ability to exceed nanoparticle catalysts with regards to activity, stability and selectivity for a growing number of chemical reactions. Understanding key properties of these materials, such as structure-property relationships, structural dynamics and reaction-driven restructuring, is, however, often complicated by issues including low weight loadings, strong metal-support interactions and heterogeneity in active component speciations. The following work details how these challenges may be addressed through a review of how a multimodal approach including scanning transmission electron microscopy, diffuse reflectance infrared Fourier transform spectroscopy, X-ray photoelectron spectroscopy and X-ray absorption spectroscopy may be employed to identify the catalytically relevant properties (charge state, electronic structure, atomic configuration, bonding interaction). Furthermore, this approach is demonstrated through its application to Pt-Ni bimetallic nanoparticles on mesoporous silica, single atom Pt on CeO2, nanoparticle Pt on CeO2 and single atom Pt on Gd-doped CeO2.","Submission published under a 24 month embargo labeled 'Closed Access', the embargo will last until 2023-08-01","The student, Matthew Kottwitz, accepted the attached license on 2021-07-15 at 14:43.","The student, Matthew Kottwitz, submitted this Dissertation for approval on 2021-07-15 at 14:54.","This Dissertation was approved for publication on 2021-07-16 at 09:35.","DSpace SAF Submission Ingestion Package generated from Vireo submission #16964 on 2022-01-12 at 13:05:06","Made available in DSpace on 2022-01-12T22:56:10Z (GMT). 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The following work details how these challenges may be addressed through a review of how a multimodal approach including scanning transmission electron microscopy, diffuse reflectance infrared Fourier transform spectroscopy, X-ray photoelectron spectroscopy and X-ray absorption spectroscopy may be employed to identify the catalytically relevant properties (charge state, electronic structure, atomic configuration, bonding interaction). Furthermore, this approach is demonstrated through its application to Pt-Ni bimetallic nanoparticles on mesoporous silica, single atom Pt on CeO2, nanoparticle Pt on CeO2 and single atom Pt on Gd-doped CeO2.","Submission published under a 24 month embargo labeled 'Closed Access', the embargo will last until 2023-08-01","The student, Matthew Kottwitz, accepted the attached license on 2021-07-15 at 14:43.","The student, Matthew Kottwitz, submitted this Dissertation for approval on 2021-07-15 at 14:54.","This Dissertation was approved for publication on 2021-07-16 at 09:35.","DSpace SAF Submission Ingestion Package generated from Vireo submission #16964 on 2022-01-12 at 13:05:06","Made available in DSpace on 2022-01-12T22:56:10Z (GMT). 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