{"id":{"repo_id":"uiuc","oai_identifier":"oai:www.ideals.illinois.edu:2142/78628"},"canonical_url":"https://search.dev.ndltd.org/etd/uiuc/oai:www.ideals.illinois.edu:2142/78628","repository":{"repo_id":"uiuc","name":"University of Illinois - Urbana-Champaign","base_url":"https://www.ideals.illinois.edu/oai-pmh"},"display":{"title":"Self-healing strategies for lithium-ion battery anodes","abstract":"U of I Only Restriction Lifted for Item 79869 on 2017-07-23T09:15:36Z.","abstract_html":"U of I Only Restriction Lifted for Item 79869 on 2017-07-23T09:15:36Z.","abstract_has_math":false,"creators":["Kang, Sen"],"institution":"University of Illinois at Urbana-Champaign","degree_name":"Ph.D.","degree_level":"Dissertation","degree_discipline":"Materials Science & Engr","degree_department":null,"school":null,"contributors":["Sottos, Nancy R.","White, Scott R.","Braun, Paul V.","Kilian, Kristopher A."],"advisors":[],"committee_chairs":[],"committee_members":[],"year":2015,"date_issued":"2015-07-22T22:33:30Z","date_published":"2015-07-22T22:33:30Z","updated_at":"2026-07-22T22:26:12Z","subjects":["self-healing","conductivity restoration","microelectronics","Li-ion batteries","Si composite anodes","electrical interfaces","carbon black functionalization","microcapsules","polydopamine coating","capsule stability","dynamic bonding","ionic bonding"],"languages":["en"],"rights":["Copyright 2015 Sen Kang"],"rights_urls":[],"identifier_entries":[]},"links":{"outbound_url":"http://hdl.handle.net/2142/78628","outbound_label":"Handle","outbound_source":"dc:identifier"},"metadata_groups":[{"id":"people","label":"People","entries":[{"key":"dc:contributor","label":"Contributor","values":["Sottos, Nancy R.","White, Scott R.","Braun, Paul V.","Kilian, Kristopher A."]},{"key":"dc:creator","label":"Author","values":["Kang, Sen"]}]},{"id":"academic_context","label":"Academic Context","entries":[{"key":"dc:date","label":"Dc Date","values":["2015-07-22T22:33:30Z","2017-07-23T09:15:36Z","2015-05","2015-04-21","2015-5"]},{"key":"dc:type","label":"Dc Type","values":["text"]},{"key":"thesis:degree_discipline","label":"Discipline","values":["Materials Science & Engr"]},{"key":"thesis:degree_level","label":"Degree Level","values":["Dissertation"]},{"key":"thesis:degree_name","label":"Degree Name","values":["Ph.D."]},{"key":"thesis:institution_name","label":"Thesis Institution Name","values":["University of Illinois at Urbana-Champaign"]}]},{"id":"subjects_keywords","label":"Subjects and Keywords","entries":[{"key":"dc:subject","label":"Dc Subject","values":["self-healing","conductivity restoration","microelectronics","Li-ion batteries","Si composite anodes","electrical interfaces","carbon black functionalization","microcapsules","polydopamine coating","capsule stability","dynamic bonding","ionic bonding"]}]},{"id":"language_rights","label":"Language and Rights","entries":[{"key":"dc:language","label":"Dc Language","values":["en"]},{"key":"dc:rights","label":"Dc Rights","values":["Copyright 2015 Sen Kang"]}]},{"id":"identifiers","label":"Identifiers","entries":[{"key":"dc:identifier","label":"Identifier","values":["http://hdl.handle.net/2142/78628"]}]},{"id":"additional","label":"Additional Metadata","entries":[{"key":"dc:description","label":"Description","values":["U of I Only Restriction Lifted for Item 79869 on 2017-07-23T09:15:36Z.","Embargo set by: Seth Robbins for item 79869 Lift date: 2017-07-22T22:34:16Z Reason: Author requested U of Illinois access only (OA after 2yrs) in Vireo ETD system","Thermal-mechanical failure of microelectronic devices often involves in the loss of conductivity of the metal traces and vias, which shortens the lifetime and requires replacement of the entire unit. High-capacity Si composite electrodes in lithium-ion batteries also suffer from the damage of electrical interfaces (particle/binder interfaces) during battery operation, leading to rapid capacity loss. In this dissertation, autonomous restoration of electrical conductivity upon damage is demonstrated in composite battery anodes and a simple electrical circuit via two different approaches. The first approach for conductivity restoration relies on the release of microencapsulated conductive particles to the fracture plane to reconstruct the damaged conductive pathways. In the second approach, dynamic ionic bonds are incorporated at the interface of polymer binder and Si nanoparticles in a composite battery electrode. Robust microcapsules are prepared with carbon black suspensions high in solids loading (up to 0.2 g/mL) for electrical conductivity restoration. Octadecyl groups are covalently functionalized on oxidized carbon black surfaces by two different synthetic routes. Functionalization significantly increases particle hydrophobicity, and improves dispersability and suspension stability in hydrophobic solvents such as o-dichlorobenzene (o-DCB), enabling encapsulation by in situ emulsion polymerization. Upon rupture, microcapsules containing functionalized carbon black (FCB) suspensions exhibit significant particle release relative to microcapsules filled with unfunctionalized carbon black. Two types of core thickeners, epoxy resin or poly 3-hexylthiophene (P3HT), are used to enhance particle release from microcapsules. Microcapsules containing FCB suspensions enable ex-situ conductivity restoration of damaged Si electrodes and an electric circuit. Rupturing of the microcapsules on the line crack of Si electrodes lead to the release of conductive FCB particles to the crack region and eventually full recovery (100 % restoration efficiency) of electrode conductivity. Similarly, partial conductivity restoration is achieved for a damaged electric circuit upon FCB release from microcapsules. A protective polydopamine (PDA) coating is applied to the microcapsule surfaces to enhance the capsule stability in battery electrolytes and other harsh environments. The polymerization of dopamine monomers is initiated by the addition of an oxidant (i.e. ammonium persulfate) in an aqueous solution of neutral pH. The resulting PDA coating is a dense and uniform layer (ca. 50 nm thick). The PDA protective coating significantly increases the capsule stability at elevated temperature (180 oC) as well as in a variety of organic solvents and acidic/basic solutions that otherwise lead to deflation and loss of core content of uncoated microcapsules. Most importantly, the PDA coated microcapsules show significantly reduced core loss in battery electrolyte over 60 days as compared to uncoated microcapsules. Intrinsic conductivity restoration relies on the reversible dissociation and formation of dynamic chemical bonds. Dynamic ionic bonds are incorporated at the interface of Si nanoparticles and polymer binders inside Si composite anodes. The presence of ionic bonds is confirmed by X-ray photoelectron and Raman spectroscopy. The dynamic ionic bonds effectively mitigate the large volume change of Si anodes during lithium intercalation. Si composite anodes with dynamic ionic bonding exhibit excellent cycling stability with a cycle life of 400 cycles and 80 % capacity retention at a current density of 2.1 mA/g.","Submission published under a 24 month embargo labeled 'U of I only', the embargo will last until 2017-05-01","The student, Sen Kang, accepted the attached license on 2015-04-17 at 11:41.","The student, Sen Kang, submitted this Dissertation for approval on 2015-04-17 at 12:01.","This Dissertation was approved for publication on 2015-04-21 at 08:22.","DSpace SAF Submission Ingestion Package generated from Vireo submission #7916 on 2015-07-22 at 14:18:05","Made available in DSpace on 2015-07-22T22:33:30Z (GMT). No. of bitstreams: 2 KANG-DISSERTATION-2015.pdf: 4738553 bytes, checksum: 513048291b102802ace3ee4d781c0ce1 (MD5) LICENSE.txt: 4205 bytes, checksum: 101b8435423e66a2f2c81b9ae2255f4f (MD5) Previous issue date: 2015-04-21"]},{"key":"dc:format","label":"Dc Format","values":["application/pdf"]},{"key":"dc:title","label":"Title","values":["Self-healing strategies for lithium-ion battery anodes"]}]}],"canonical_facts":{"dc:contributor":["Sottos, Nancy R.","White, Scott R.","Braun, Paul V.","Kilian, Kristopher A."],"dc:creator":["Kang, Sen"],"dc:date":["2015-07-22T22:33:30Z","2017-07-23T09:15:36Z","2015-05","2015-04-21","2015-5"],"dc:description":["U of I Only Restriction Lifted for Item 79869 on 2017-07-23T09:15:36Z.","Embargo set by: Seth Robbins for item 79869 Lift date: 2017-07-22T22:34:16Z Reason: Author requested U of Illinois access only (OA after 2yrs) in Vireo ETD system","Thermal-mechanical failure of microelectronic devices often involves in the loss of conductivity of the metal traces and vias, which shortens the lifetime and requires replacement of the entire unit. High-capacity Si composite electrodes in lithium-ion batteries also suffer from the damage of electrical interfaces (particle/binder interfaces) during battery operation, leading to rapid capacity loss. In this dissertation, autonomous restoration of electrical conductivity upon damage is demonstrated in composite battery anodes and a simple electrical circuit via two different approaches. The first approach for conductivity restoration relies on the release of microencapsulated conductive particles to the fracture plane to reconstruct the damaged conductive pathways. In the second approach, dynamic ionic bonds are incorporated at the interface of polymer binder and Si nanoparticles in a composite battery electrode. Robust microcapsules are prepared with carbon black suspensions high in solids loading (up to 0.2 g/mL) for electrical conductivity restoration. Octadecyl groups are covalently functionalized on oxidized carbon black surfaces by two different synthetic routes. Functionalization significantly increases particle hydrophobicity, and improves dispersability and suspension stability in hydrophobic solvents such as o-dichlorobenzene (o-DCB), enabling encapsulation by in situ emulsion polymerization. Upon rupture, microcapsules containing functionalized carbon black (FCB) suspensions exhibit significant particle release relative to microcapsules filled with unfunctionalized carbon black. Two types of core thickeners, epoxy resin or poly 3-hexylthiophene (P3HT), are used to enhance particle release from microcapsules. Microcapsules containing FCB suspensions enable ex-situ conductivity restoration of damaged Si electrodes and an electric circuit. Rupturing of the microcapsules on the line crack of Si electrodes lead to the release of conductive FCB particles to the crack region and eventually full recovery (100 % restoration efficiency) of electrode conductivity. Similarly, partial conductivity restoration is achieved for a damaged electric circuit upon FCB release from microcapsules. A protective polydopamine (PDA) coating is applied to the microcapsule surfaces to enhance the capsule stability in battery electrolytes and other harsh environments. The polymerization of dopamine monomers is initiated by the addition of an oxidant (i.e. ammonium persulfate) in an aqueous solution of neutral pH. The resulting PDA coating is a dense and uniform layer (ca. 50 nm thick). The PDA protective coating significantly increases the capsule stability at elevated temperature (180 oC) as well as in a variety of organic solvents and acidic/basic solutions that otherwise lead to deflation and loss of core content of uncoated microcapsules. Most importantly, the PDA coated microcapsules show significantly reduced core loss in battery electrolyte over 60 days as compared to uncoated microcapsules. Intrinsic conductivity restoration relies on the reversible dissociation and formation of dynamic chemical bonds. Dynamic ionic bonds are incorporated at the interface of Si nanoparticles and polymer binders inside Si composite anodes. The presence of ionic bonds is confirmed by X-ray photoelectron and Raman spectroscopy. The dynamic ionic bonds effectively mitigate the large volume change of Si anodes during lithium intercalation. Si composite anodes with dynamic ionic bonding exhibit excellent cycling stability with a cycle life of 400 cycles and 80 % capacity retention at a current density of 2.1 mA/g.","Submission published under a 24 month embargo labeled 'U of I only', the embargo will last until 2017-05-01","The student, Sen Kang, accepted the attached license on 2015-04-17 at 11:41.","The student, Sen Kang, submitted this Dissertation for approval on 2015-04-17 at 12:01.","This Dissertation was approved for publication on 2015-04-21 at 08:22.","DSpace SAF Submission Ingestion Package generated from Vireo submission #7916 on 2015-07-22 at 14:18:05","Made available in DSpace on 2015-07-22T22:33:30Z (GMT). No. of bitstreams: 2 KANG-DISSERTATION-2015.pdf: 4738553 bytes, checksum: 513048291b102802ace3ee4d781c0ce1 (MD5) LICENSE.txt: 4205 bytes, checksum: 101b8435423e66a2f2c81b9ae2255f4f (MD5) Previous issue date: 2015-04-21"],"dc:format":["application/pdf"],"dc:identifier":["http://hdl.handle.net/2142/78628"],"dc:language":["en"],"dc:rights":["Copyright 2015 Sen Kang"],"dc:subject":["self-healing","conductivity restoration","microelectronics","Li-ion batteries","Si composite anodes","electrical interfaces","carbon black functionalization","microcapsules","polydopamine coating","capsule stability","dynamic bonding","ionic bonding"],"dc:title":["Self-healing strategies for lithium-ion battery anodes"],"dc:type":["text"],"thesis:degree_discipline":["Materials Science & Engr"],"thesis:degree_level":["Dissertation"],"thesis:degree_name":["Ph.D."],"thesis:institution_name":["University of Illinois at Urbana-Champaign"]},"updated_at":"2026-07-22T22:26:12Z"}