{"id":{"repo_id":"must-thes","oai_identifier":"oai:scholarsmine.mst.edu:doctoral_dissertations-3837"},"canonical_url":"https://search.dev.ndltd.org/etd/must-thes/oai:scholarsmine.mst.edu:doctoral_dissertations-3837","repository":{"repo_id":"must-thes","name":"Missouri University of Science and Technology","base_url":"https://scholarsmine.mst.edu/do/oai/"},"display":{"title":"Deep understanding of degradation in lithium ion batteries through experimental and first-principles study","abstract":"\"The growing interests in Lithium-ion Batteries (LIBs) have significantly accelerated the development of active materials. However, the key challenge is that electrode materials suffer from degradation, which include transition metal dissolution, solid electrolyte interphase (SEI) layer formation, and mechanical fracture. To address these issues, applying an ultrathin coating onto active materials via Atomic Layer Deposition (ALD) is an efficient way. Although numerious works have been done for active material performance improvement via ALD technology, the fundamental enhancement mechanisms of ALD coating on battery performance improvement are not yet known. Therefore, this dissertation consists of four papers, which focused on the ALD coating impact on Li intercalation, metal dissolution, Li ion diffusivity and interfacial property of SEI layer via first-principles study. Paper I explained why CeO<sub>2</sub> coating has better performance than Al<sub>2</sub>O<sub>3</sub> coating material via faster Li diffusion, facile intercalation, and less mechanical damage of coating. Paper II discovered an unexpected metal dissolution that ultrathin CeO<sub>2</sub> coating intensifies the Mn dissolution of LMO and it was confirmed in several ways, including ICP-OES measurement, Mn vacancy formation energy calculation, COOP analysis, PDOS analysis, and cell level performance. Paper III revealed that the ALD CeO<sub>2</sub> coating thickness impact on Li ion diffusivity in coated LMO is related to surface and bulk diffusion domination and phase transition of coating layers. Paper IV demonstrated that the fracture strength of inorganic components of SEI layer was higher than organic component, implying that the inorganic-organic interface can effectively block electron transport from electrolyte to anode particles to prevent futher oxidation of active materials\"--Abstract, page iv.","abstract_html":"&quot;The growing interests in Lithium-ion Batteries (LIBs) have significantly accelerated the development of active materials. However, the key challenge is that electrode materials suffer from degradation, which include transition metal dissolution, solid electrolyte interphase (SEI) layer formation, and mechanical fracture. To address these issues, applying an ultrathin coating onto active materials via Atomic Layer Deposition (ALD) is an efficient way. Although numerious works have been done for active material performance improvement via ALD technology, the fundamental enhancement mechanisms of ALD coating on battery performance improvement are not yet known. Therefore, this dissertation consists of four papers, which focused on the ALD coating impact on Li intercalation, metal dissolution, Li ion diffusivity and interfacial property of SEI layer via first-principles study. Paper I explained why CeO&lt;sub&gt;2&lt;/sub&gt; coating has better performance than Al&lt;sub&gt;2&lt;/sub&gt;O&lt;sub&gt;3&lt;/sub&gt; coating material via faster Li diffusion, facile intercalation, and less mechanical damage of coating. Paper II discovered an unexpected metal dissolution that ultrathin CeO&lt;sub&gt;2&lt;/sub&gt; coating intensifies the Mn dissolution of LMO and it was confirmed in several ways, including ICP-OES measurement, Mn vacancy formation energy calculation, COOP analysis, PDOS analysis, and cell level performance. Paper III revealed that the ALD CeO&lt;sub&gt;2&lt;/sub&gt; coating thickness impact on Li ion diffusivity in coated LMO is related to surface and bulk diffusion domination and phase transition of coating layers. Paper IV demonstrated that the fracture strength of inorganic components of SEI layer was higher than organic component, implying that the inorganic-organic interface can effectively block electron transport from electrolyte to anode particles to prevent futher oxidation of active materials&quot;--Abstract, page iv.","abstract_has_math":false,"creators":["He, Yufang"],"institution":"Missouri University of Science and Technology","degree_name":"Ph. D. in Mechanical Engineering","degree_level":null,"degree_discipline":null,"degree_department":null,"school":null,"contributors":[],"advisors":[],"committee_chairs":[],"committee_members":[],"year":null,"date_issued":"","date_published":null,"updated_at":"2026-07-24T03:18:34Z","subjects":["Energy Systems","Mechanical Engineering"],"languages":[],"rights":[],"rights_urls":[],"identifier_entries":[]},"links":{"outbound_url":"https://scholarsmine.mst.edu/doctoral_dissertations/2832","outbound_label":"Repository record","outbound_source":"dc:identifier"},"metadata_groups":[{"id":"people","label":"People","entries":[{"key":"dc:creator","label":"Author","values":["He, Yufang"]}]},{"id":"academic_context","label":"Academic Context","entries":[{"key":"dc:type","label":"Dc Type","values":["Dissertation - Open Access"]},{"key":"thesis:degree_name","label":"Degree Name","values":["Ph. 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To address these issues, applying an ultrathin coating onto active materials via Atomic Layer Deposition (ALD) is an efficient way. Although numerious works have been done for active material performance improvement via ALD technology, the fundamental enhancement mechanisms of ALD coating on battery performance improvement are not yet known. Therefore, this dissertation consists of four papers, which focused on the ALD coating impact on Li intercalation, metal dissolution, Li ion diffusivity and interfacial property of SEI layer via first-principles study. Paper I explained why CeO<sub>2</sub> coating has better performance than Al<sub>2</sub>O<sub>3</sub> coating material via faster Li diffusion, facile intercalation, and less mechanical damage of coating. Paper II discovered an unexpected metal dissolution that ultrathin CeO<sub>2</sub> coating intensifies the Mn dissolution of LMO and it was confirmed in several ways, including ICP-OES measurement, Mn vacancy formation energy calculation, COOP analysis, PDOS analysis, and cell level performance. Paper III revealed that the ALD CeO<sub>2</sub> coating thickness impact on Li ion diffusivity in coated LMO is related to surface and bulk diffusion domination and phase transition of coating layers. Paper IV demonstrated that the fracture strength of inorganic components of SEI layer was higher than organic component, implying that the inorganic-organic interface can effectively block electron transport from electrolyte to anode particles to prevent futher oxidation of active materials\"--Abstract, page iv."]},{"key":"dc:title","label":"Title","values":["Deep understanding of degradation in lithium ion batteries through experimental and first-principles study"]}]}],"canonical_facts":{"dc:creator":["He, Yufang"],"dc:description.abstract":["\"The growing interests in Lithium-ion Batteries (LIBs) have significantly accelerated the development of active materials. However, the key challenge is that electrode materials suffer from degradation, which include transition metal dissolution, solid electrolyte interphase (SEI) layer formation, and mechanical fracture. To address these issues, applying an ultrathin coating onto active materials via Atomic Layer Deposition (ALD) is an efficient way. Although numerious works have been done for active material performance improvement via ALD technology, the fundamental enhancement mechanisms of ALD coating on battery performance improvement are not yet known. Therefore, this dissertation consists of four papers, which focused on the ALD coating impact on Li intercalation, metal dissolution, Li ion diffusivity and interfacial property of SEI layer via first-principles study. Paper I explained why CeO<sub>2</sub> coating has better performance than Al<sub>2</sub>O<sub>3</sub> coating material via faster Li diffusion, facile intercalation, and less mechanical damage of coating. Paper II discovered an unexpected metal dissolution that ultrathin CeO<sub>2</sub> coating intensifies the Mn dissolution of LMO and it was confirmed in several ways, including ICP-OES measurement, Mn vacancy formation energy calculation, COOP analysis, PDOS analysis, and cell level performance. Paper III revealed that the ALD CeO<sub>2</sub> coating thickness impact on Li ion diffusivity in coated LMO is related to surface and bulk diffusion domination and phase transition of coating layers. Paper IV demonstrated that the fracture strength of inorganic components of SEI layer was higher than organic component, implying that the inorganic-organic interface can effectively block electron transport from electrolyte to anode particles to prevent futher oxidation of active materials\"--Abstract, page iv."],"dc:identifier":["https://scholarsmine.mst.edu/doctoral_dissertations/2832"],"dc:subject":["Energy Systems","Mechanical Engineering"],"dc:title":["Deep understanding of degradation in lithium ion batteries through experimental and first-principles study"],"dc:type":["Dissertation - Open Access"],"thesis:degree_name":["Ph. D. in Mechanical Engineering"],"thesis:institution_name":["Missouri University of Science and Technology"]},"updated_at":"2026-07-24T03:18:34Z"}