{"department":[{"_id":"MaIb"}],"abstract":[{"lang":"eng","text":"AgSbSe2 is a promising thermoelectric (TE) p-type material for applications in the middle-temperature range. AgSbSe2 is characterized by relatively low thermal conductivities and high Seebeck coefficients, but its main limitation is moderate electrical conductivity. Herein, we detail an efficient and scalable hot-injection synthesis route to produce AgSbSe2 nanocrystals (NCs). To increase the carrier concentration and improve the electrical conductivity, these NCs are doped with Sn2+ on Sb3+ sites. Upon processing, the Sn2+ chemical state is conserved using a reducing NaBH4 solution to displace the organic ligand and anneal the material under a forming gas flow. The TE properties of the dense materials obtained from the consolidation of the NCs using a hot pressing are then characterized. The presence of Sn2+ ions replacing Sb3+ significantly increases the charge carrier concentration and, consequently, the electrical conductivity. Opportunely, the measured Seebeck coefficient varied within a small range upon Sn doping. The excellent performance obtained when Sn2+ ions are prevented from oxidation is rationalized by modeling the system. Calculated band structures disclosed that Sn doping induces convergence of the AgSbSe2 valence bands, accounting for an enhanced electronic effective mass. The dramatically enhanced carrier transport leads to a maximized power factor for AgSb0.98Sn0.02Se2 of 0.63 mW m–1 K–2 at 640 K. Thermally, phonon scattering is significantly enhanced in the NC-based materials, yielding an ultralow thermal conductivity of 0.3 W mK–1 at 666 K. Overall, a record-high figure of merit (zT) is obtained at 666 K for AgSb0.98Sn0.02Se2 at zT = 1.37, well above the values obtained for undoped AgSbSe2, at zT = 0.58 and state-of-art Pb- and Te-free materials, which makes AgSb0.98Sn0.02Se2 an excellent p-type candidate for medium-temperature TE applications."}],"date_published":"2023-06-13T00:00:00Z","publication_status":"published","issue":"12","month":"06","article_processing_charge":"No","date_updated":"2023-08-02T06:29:55Z","pmid":1,"type":"journal_article","day":"13","quality_controlled":"1","title":"Surface chemistry and band engineering in AgSbSe₂: Toward high thermoelectric performance","status":"public","publisher":"American Chemical Society","scopus_import":"1","oa_version":"None","date_created":"2023-07-16T22:01:11Z","user_id":"4359f0d1-fa6c-11eb-b949-802e58b17ae8","_id":"13235","language":[{"iso":"eng"}],"citation":{"mla":"Liu, Yu, et al. “Surface Chemistry and Band Engineering in AgSbSe₂: Toward High Thermoelectric Performance.” <i>ACS Nano</i>, vol. 17, no. 12, American Chemical Society, 2023, pp. 11923–11934, doi:<a href=\"https://doi.org/10.1021/acsnano.3c03541\">10.1021/acsnano.3c03541</a>.","ieee":"Y. Liu <i>et al.</i>, “Surface chemistry and band engineering in AgSbSe₂: Toward high thermoelectric performance,” <i>ACS Nano</i>, vol. 17, no. 12. American Chemical Society, pp. 11923–11934, 2023.","ama":"Liu Y, Li M, Wan S, et al. Surface chemistry and band engineering in AgSbSe₂: Toward high thermoelectric performance. <i>ACS Nano</i>. 2023;17(12):11923–11934. doi:<a href=\"https://doi.org/10.1021/acsnano.3c03541\">10.1021/acsnano.3c03541</a>","apa":"Liu, Y., Li, M., Wan, S., Lim, K. H., Zhang, Y., Li, M., … Cabot, A. (2023). Surface chemistry and band engineering in AgSbSe₂: Toward high thermoelectric performance. <i>ACS Nano</i>. American Chemical Society. <a href=\"https://doi.org/10.1021/acsnano.3c03541\">https://doi.org/10.1021/acsnano.3c03541</a>","chicago":"Liu, Yu, Mingquan Li, Shanhong Wan, Khak Ho Lim, Yu Zhang, Mengyao Li, Junshan Li, Maria Ibáñez, Min Hong, and Andreu Cabot. “Surface Chemistry and Band Engineering in AgSbSe₂: Toward High Thermoelectric Performance.” <i>ACS Nano</i>. American Chemical Society, 2023. <a href=\"https://doi.org/10.1021/acsnano.3c03541\">https://doi.org/10.1021/acsnano.3c03541</a>.","ista":"Liu Y, Li M, Wan S, Lim KH, Zhang Y, Li M, Li J, Ibáñez M, Hong M, Cabot A. 2023. Surface chemistry and band engineering in AgSbSe₂: Toward high thermoelectric performance. ACS Nano. 17(12), 11923–11934.","short":"Y. Liu, M. Li, S. Wan, K.H. Lim, Y. Zhang, M. Li, J. Li, M. Ibáñez, M. Hong, A. Cabot, ACS Nano 17 (2023) 11923–11934."},"article_type":"original","external_id":{"pmid":["37310395"],"isi":["001008564800001"]},"publication_identifier":{"eissn":["1936-086X"],"issn":["1936-0851"]},"publication":"ACS Nano","author":[{"orcid":"0000-0001-7313-6740","full_name":"Liu, Yu","id":"2A70014E-F248-11E8-B48F-1D18A9856A87","first_name":"Yu","last_name":"Liu"},{"full_name":"Li, Mingquan","last_name":"Li","first_name":"Mingquan"},{"full_name":"Wan, Shanhong","last_name":"Wan","first_name":"Shanhong"},{"last_name":"Lim","first_name":"Khak Ho","full_name":"Lim, Khak Ho"},{"first_name":"Yu","last_name":"Zhang","full_name":"Zhang, Yu"},{"last_name":"Li","first_name":"Mengyao","full_name":"Li, Mengyao"},{"full_name":"Li, Junshan","first_name":"Junshan","last_name":"Li"},{"last_name":"Ibáñez","first_name":"Maria","full_name":"Ibáñez, Maria","id":"43C61214-F248-11E8-B48F-1D18A9856A87","orcid":"0000-0001-5013-2843"},{"full_name":"Hong, Min","first_name":"Min","last_name":"Hong"},{"last_name":"Cabot","first_name":"Andreu","full_name":"Cabot, Andreu"}],"doi":"10.1021/acsnano.3c03541","page":"11923–11934","project":[{"_id":"9B8F7476-BA93-11EA-9121-9846C619BF3A","name":"HighTE: The Werner Siemens Laboratory for the High Throughput Discovery of Semiconductors for Waste Heat Recovery"}],"isi":1,"acknowledgement":"Y.L. acknowledges funding from the National Natural Science Foundation of China (NSFC) (Grants No. 22209034), the Innovation and Entrepreneurship Project of Overseas Returnees in Anhui Province (Grant No. 2022LCX002). K.H.L. acknowledges financial support from the National Natural Science Foundation of China (Grant No. 22208293). Y.Z. acknowledges support from the SBIR program NanoOhmics. J.L. is grateful for the project supported by the Natural Science Foundation of Sichuan (2022NSFSC1229). M.I. acknowledges financial support from ISTA and the Werner Siemens Foundation.","year":"2023","intvolume":"        17","volume":17}