Academic Journal

A Tunable Structural Family with Ultralow Thermal Conductivity: Copper-Deficient Cu 1– x □ x Pb 1– x Bi 1+ x S 3

التفاصيل البيبلوغرافية
العنوان: A Tunable Structural Family with Ultralow Thermal Conductivity: Copper-Deficient Cu 1– x □ x Pb 1– x Bi 1+ x S 3
المؤلفون: Krishnendu Maji (4015358), Pierric Lemoine (4027778), Adèle Renaud (2127709), Bin Zhang (64682), Xiaoyuan Zhou (1604638), Virginia Carnevali (11558361), Christophe Candolfi (1507195), Bernard Raveau (2623870), Rabih Al Rahal Al Orabi (1728118), Marco Fornari (1441531), Paz Vaqueiro (1587727), Mathieu Pasturel (1518838), Carmelo Prestipino (2043814), Emmanuel Guilmeau (3929957)
سنة النشر: 2022
المجموعة: Smithsonian Institution: Digital Repository
مصطلحات موضوعية: Biophysics, Biochemistry, Biotechnology, Inorganic Chemistry, Chemical Sciences not elsewhere classified, Physical Sciences not elsewhere classified, Information Systems not elsewhere classified, ultralow thermal conductivity, tunable structural family, thermal barrier applications, substantial anharmonic effects, obtained upon cl, low energy hints, lattice dynamics calculations, interesting structural prototype, enhance phonon scattering, connects heat transport, ultralow κ values, ultralow κ value, highly pure materials, 9 , 3 , type sulfide cupbbi, type thermoelectric sulfides, type thermoelectric compounds, partial pb replacement, chemical formula cu, 6 – 0, 5 , type sulfide
الوصف: Understanding the mechanism that connects heat transport with crystal structures and order/disorder phenomena is crucial to develop materials with ultralow thermal conductivity (κ), for thermoelectric and thermal barrier applications, and requires the study of highly pure materials. We synthesized the n-type sulfide CuPbBi 5 S 9 with an ultralow κ value of 0.6–0.4 W m –1 K –1 in the temperature range 300–700 K. In contrast to prior studies, we show that this synthetic sulfide does not exhibit the ordered gladite mineral structure but instead forms a copper-deficient disordered aikinite structure with partial Pb replacement by Bi, according to the chemical formula Cu 1/3 □ 2/3 Pb 1/3 Bi 5/3 S 3 . By combining experiments and lattice dynamics calculations, we elucidated that the ultralow κ value of this compound is due to very low energy optical modes associated with Pb and Bi ions and, to a smaller extent, Cu. This vibrational complexity at low energy hints at substantial anharmonic effects that contribute to enhance phonon scattering. Importantly, we show that this aikinite-type sulfide, despite being a poor semiconductor, is a potential matrix for designing novel, efficient n-type thermoelectric compounds with ultralow κ values. A drastic improvement in the carrier concentration and thermoelectric figure of merit have been obtained upon Cl for S and Bi for Pb substitution. The Cu 1– x □ x Pb 1– x Bi 1+ x S 3 series provides a new, interesting structural prototype for engineering n-type thermoelectric sulfides by controlling disorder and optimizing doping.
نوع الوثيقة: article in journal/newspaper
اللغة: unknown
Relation: https://figshare.com/articles/journal_contribution/A_Tunable_Structural_Family_with_Ultralow_Thermal_Conductivity_Copper-Deficient_Cu_sub_1_i_x_i_sub_sub_i_x_i_sub_Pb_sub_1_i_x_i_sub_Bi_sub_1_i_x_i_sub_S_sub_3_sub_/18614020
DOI: 10.1021/jacs.1c11998.s001
الاتاحة: https://doi.org/10.1021/jacs.1c11998.s001
Rights: CC BY-NC 4.0
رقم الانضمام: edsbas.C992F359
قاعدة البيانات: BASE
الوصف
DOI:10.1021/jacs.1c11998.s001