276e1d35acd47c1583a7e664f33f0934 Ene_a2023v16n13p5162.pdf 720719e4c7fb4a020d3bb6165440111049e963a1 Ene_a2023v16n13p5162.pdf 641a85fedc5b73c555f7357edef520acb75c30d90a920b96ec5dc750f64e36f1 Ene_a2023v16n13p5162.pdf Title: Improved High Temperature Thermoelectric Properties in Misfit Ca3Co4O9 by Thermal Annealing Subject: Ca3Co4O9, a p-type thermoelectric material based on transition-metal oxides, has garnered significant interest due to its potential in thermoelectric applications. Its unique misfit-layered crystal structure contributes to low thermal conductivity and a high Seebeck coefficient, leading to a thermoelectric figure of merit (zT) of 1 at 1000 K. Conventionally, it has been believed that thermopower reaches its upper limit above 200 K. However, our thermopower measurements on polycrystalline Ca3Co4O9 samples have revealed an unexpected increase in thermopower above 380 K. In this study, we investigate the effects of high oxygen pressure annealing on Ca3Co4O9 and provide an explanation based on the mixed oxide states of cobalt and carrier hopping. Our results demonstrate that annealing induces modifications in the defect chemistry of Ca3Co4O9, leading to a decrease in electron hopping probability and the emergence of a thermal activation-like behavior in thermopower. These findings carry significant implications for the design and optimization of thermoelectric materials based on misfit cobaltates, opening new avenues for enhanced thermoelectric performance. Keywords: Ca3Co4O9; thermoelectricity; heike’s limit; cobaltates Author: Arindom Chatterjee, Alexandros El Sachat, Ananya Banik, Kanishka Biswas, Alejandro Castro-Alvarez, Clivia M. Sotomayor Torres, José Santiso and Emigdio Chávez-Ángel Creator: LaTeX with hyperref Producer: pdfTeX-1.40.21 CreationDate: Tue Jul 4 14:59:42 2023 CEST ModDate: Tue Jul 4 15:02:20 2023 CEST Tagged: no UserProperties: no Suspects: no Form: none JavaScript: no Pages: 13 Encrypted: no Page size: 595.276 x 841.89 pts (A4) Page rot: 0 File size: 4009540 bytes Optimized: no PDF version: 1.7 name type encoding emb sub uni object ID ------------------------------------ ----------------- ---------------- --- --- --- --------- AXFIVA+VnURWPalladioL-Bold Type 1 Custom yes yes no 10 0 RMCKJA+VnURWPalladioL Type 1 Custom yes yes no 15 0 WNXCXB+URWPalladioL-Bold Type 1 Custom yes yes no 19 0 REQTTE+URWPalladioL-Roma Type 1 Custom yes yes no 24 0 HPGZOY+URWPalladioL-Ital Type 1 Custom yes yes no 28 0 JEZHRT+CMSY10 Type 1 Builtin yes yes no 32 0 SOJMCF+PazoMath Type 1 Builtin yes yes no 36 0 FZVQKH+EURM10 Type 1 Builtin yes yes no 40 0 QDIDFO+TimesNewRomanPS-BoldItalicMT Type 1C WinAnsi yes yes no 58 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15:28:37 CET Size: 4009540 Format: PDF Version: 1.7 Status: Well-Formed and valid SignatureMatches: PDF-hul MIMEtype: application/pdf PDFMetadata: Objects: 513 FreeObjects: 1 IncrementalUpdates: 0 DocumentCatalog: PageLayout: SinglePage PageMode: UseNone Outlines: Item: Title: Introduction Destination: edu.harvard.hul.ois.jhove.module.pdf.PdfSimpleObject@4d3167f4 Item: Title: Experimental Methods Destination: edu.harvard.hul.ois.jhove.module.pdf.PdfSimpleObject@ed9d034 Item: Title: Results Destination: edu.harvard.hul.ois.jhove.module.pdf.PdfSimpleObject@6121c9d6 Children: Item: Title: Structural and Elemental Characterizations Destination: edu.harvard.hul.ois.jhove.module.pdf.PdfSimpleObject@87f383f Item: Title: Electronic Transport Properties and Thermoelectric Power Destination: edu.harvard.hul.ois.jhove.module.pdf.PdfSimpleObject@4eb7f003 Item: Title: Conclusions Destination: edu.harvard.hul.ois.jhove.module.pdf.PdfSimpleObject@eafc191 Item: Title: References Destination: edu.harvard.hul.ois.jhove.module.pdf.PdfSimpleObject@612fc6eb Info: Title: Improved High Temperature Thermoelectric Properties in Misfit Ca3Co4O9 by Thermal Annealing Author: Arindom Chatterjee, Alexandros El Sachat, Ananya Banik, Kanishka Biswas, Alejandro Castro-Alvarez, Clivia M. Sotomayor Torres, José Santiso and Emigdio Chávez-Ángel Subject: Ca3Co4O9, a p-type thermoelectric material based on transition-metal oxides, has garnered significant interest due to its potential in thermoelectric applications. Its unique misfit-layered crystal structure contributes to low thermal conductivity and a high Seebeck coefficient, leading to a thermoelectric figure of merit (zT) of 1 at 1000 K. Conventionally, it has been believed that thermopower reaches its upper limit above 200 K. However, our thermopower measurements on polycrystalline Ca3Co4O9 samples have revealed an unexpected increase in thermopower above 380 K. In this study, we investigate the effects of high oxygen pressure annealing on Ca3Co4O9 and provide an explanation based on the mixed oxide states of cobalt and carrier hopping. Our results demonstrate that annealing induces modifications in the defect chemistry of Ca3Co4O9, leading to a decrease in electron hopping probability and the emergence of a thermal activation-like behavior in thermopower. These findings carry significant implications for the design and optimization of thermoelectric materials based on misfit cobaltates, opening new avenues for enhanced thermoelectric performance. 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