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1. Zintl Phase Compounds Mg3Sb2−xBix (x = 0, 1, and 2) Monolayers: Electronic, Phonon and Thermoelectric Properties From ab Initio Calculations

   https://doi.org/10.3389/fmech.2022.876655  

   Chang, Zheng ; Ma, Jing ; Yuan, Kunpeng ; Zheng, Jiongzhi ; Wei, Bin ; Al-Fahdi, Mohammed ; Gao, Yufei ; Zhang, Xiaoliang ; Shao, Hezhu ; Hu, Ming ; et al ( April 2022 , Frontiers in Mechanical Engineering)

   The Mg 3 Sb 2− x Bi x family has emerged as the potential candidates for thermoelectric applications due to their ultra-low lattice thermal conductivity ( κ L ) at room temperature (RT) and structural complexity. Here, using ab initio calculations of the electron-phonon averaged (EPA) approximation coupled with Boltzmann transport equation (BTE), we have studied electronic, phonon and thermoelectric properties of Mg 3 Sb 2− x Bi x (x = 0, 1, and 2) monolayers. In violation of common mass-trend expectations, increasing Bi element content with heavier Zintl phase compounds yields an abnormal change in κ L in two-dimensional Mg 3 Sb 2− x Bi x crystals at RT (∼0.51, 1.86, and 0.25 W/mK for Mg 3 Sb 2 , Mg 3 SbBi, and Mg 3 Bi 2 ). The κ L trend was detailedly analyzed via the phonon heat capacity, group velocity and lifetime parameters. Based on quantitative electronic band structures, the electronic bonding through the crystal orbital Hamilton population (COHP) and electron local function analysis we reveal the underlying mechanism for the semiconductor-semimetallic transition of Mg 3 Sb 2-− x Bi x compounds, and these electronic transport properties (Seebeck coefficient, electrical conductivity, and electronic thermal conductivity) were calculated.more »We demonstrate that the highest dimensionless figure of merit ZT of Mg 3 Sb 2− x Bi x compounds with increasing Bi content can reach ∼1.6, 0.2, and 0.6 at 700 K, respectively. Our results can indicate that replacing heavier anion element in Zintl phase Mg 3 Sb 2− x Bi x materials go beyond common expectations (a heavier atom always lead to a lower κ L from Slack’s theory), which provide a novel insight for regulating thermoelectric performance without restricting conventional heavy atomic mass approach.« less
2. Experimental validation of high thermoelectric performance in RECuZnP ₂ predicted by high-throughput DFT calculations

   https://doi.org/10.1039/D0MH01112F  

   Pöhls, Jan-Hendrik ; Chanakian, Sevan ; Park, Junsoo ; Ganose, Alex M. ; Dunn, Alexander ; Friesen, Nick ; Bhattacharya, Amit ; Hogan, Brea ; Bux, Sabah ; Jain, Anubhav ; et al ( January 2021 , Materials Horizons)

   Accurate density functional theory calculations of the interrelated properties of thermoelectric materials entail high computational cost, especially as crystal structures increase in complexity and size. New methods involving ab initio scattering and transport (AMSET) and compressive sensing lattice dynamics are used to compute the transport properties of quaternary CaAl 2 Si 2 -type rare-earth phosphides RECuZnP 2 (RE = Pr, Nd, Er), which were identified to be promising thermoelectrics from high-throughput screening of 20 000 disordered compounds. Experimental measurements of the transport properties agree well with the computed values. Compounds with stiff bulk moduli (>80 GPa) and high speeds of sound (>3500 m s −1 ) such as RECuZnP 2 are typically dismissed as thermoelectric materials because they are expected to exhibit high lattice thermal conductivity. However, RECuZnP 2 exhibits not only low electrical resistivity, but also low lattice thermal conductivity (∼1 W m −1 K −1 ). Contrary to prior assumptions, polar-optical phonon scattering was revealed by AMSET to be the primary mechanism limiting the electronic mobility of these compounds, raising questions about existing assumptions of scattering mechanisms in this class of thermoelectric materials. The resulting thermoelectric performance ( zT of 0.5 for ErCuZnP 2 at 800 K) is amongmore »the best observed in phosphides and can likely be improved with further optimization.« less
3. The impact of site selectivity and disorder on the thermoelectric properties of Yb ₂₁ Mn ₄ Sb ₁₈ solid solutions: Yb ₂₁ Mn _4−x Cd _x Sb ₁₈ and Yb _21−y Ca _y Mn ₄ Sb ₁₈

   https://doi.org/10.1039/d1ma00497b  

   He, Allan ; Cerretti, Giacomo ; Kauzlarich, Susan M. ( August 2021 , Materials Advances)

   Thermoelectric materials can convert heat into electricity. They are used to generate electricity when other power sources are not available or to increase energy efficiency by recycling waste heat. The Yb 21 Mn 4 Sb 18 phase was previously shown to have good thermoelectric performance due to its large Seebeck coefficient (∼290 μV K −1 ) and low thermal conductivity (0.4 W m −1 K −1 ). These characteristics stem respectively from the unique [Mn 4 Sb 10 ] 22− subunit and the large unit cell/site disorder inherent in this phase. The solid solutions, Yb 21 Mn 4− x Cd x Sb 18 ( x = 0, 0.5, 1.0, 1.5) and Yb 21− y Ca y Mn 4 Sb 18 ( y = 3, 6, 9, 10.5) have been prepared, their structures characterized and thermoelectric properties from room temperature to 800 K measured. A detailed look into the structural disorder for the Cd and Ca solid solutions was performed using synchrotron powder X-ray diffraction and pair distribution function methods and shows that these are highly disordered structures. The substitution of Cd gives rise to more metallic behavior whereas Ca substitution results in high resistivity. As both Cd and Ca aremore »isoelectronic substitutions, the changes in properties are attributed to changes in the electronic structure. Both solid solutions show that the thermal conductivities remain extremely low (∼0.4 W m −1 K −1 ) and that the Seebeck coefficients remain high (>200 μV K −1 ). The temperature dependence of the carrier mobility with increased Ca substitution, changing from approximately T −1 to T −0.5 , suggests that another scattering mechanism is being introduced. As the bonding changes from polar covalent with Yb to ionic for Ca, polar optical phonon scattering becomes the dominant mechanism. Experimental studies of the Cd solid solutions result in a max zT of ∼1 at 800 K and, more importantly for application purposes, a ZT avg ∼ 0.6 from 300 K to 800 K.« less
4. The intrinsic thermal transport properties of the biphenylene network and the influence of hydrogenation: a first-principles study

   https://doi.org/10.1039/D1TC04154A  

   Zhang, Pei ; Ouyang, Tao ; Tang, Chao ; He, Chaoyu ; Li, Jin ; Zhang, Chunxiao ; Hu, Ming ; Zhong, Jianxin ( December 2021 , Journal of Materials Chemistry C)

   Utilizing first-principles calculations combined with phonon Boltzmann transport theory up to fourth-order anharmonicity, we systematically investigate the thermal transport properties of the biphenylene network [BPN, recently synthesized experimentally by Fan et al. , Science , 2021, 372 , 852–856] and hydrogenated BPN (HBPN). The calculations show that four-phonon scattering significantly affects the lattice thermal conductivity ( κ ) of BPN. At room temperature, the κ of BPN is reduced from 582.32 (1257.07) W m −1 K −1 to 309.56 (539.88) W m −1 K −1 along the x ( y ) direction after considering the four-phonon scattering. Moreover, our results demonstrate that the thermal transport in BPN could also be greatly suppressed by hydrogenation, where the κ of HBPN along the x ( y ) direction is merely 16.62% (10.14%) of that of pristine BPN at 300 K. The mechanism causing such an obvious decrease of κ of HBPN is identified to be due to the enhanced phonon scattering rate and reduced group velocity, which is further revealed by the increased scattering phase space and weakened C–C bond. The results presented in this work shed light on the intrinsic thermal transport features of BPN and HBPN, which will help usmore »to understand the phonon transport processes and pave the way for their future developments in the thermal field.« less
5. Ultralow lattice thermal conductivity of chalcogenide perovskite CaZrSe3 contributes to high thermoelectric figure of merit

   https://doi.org/10.1038/s41524-019-0253-5  

   Osei-Agyemang, Eric ; Adu, Challen Enninful ; Balasubramanian, Ganesh ( December 2019 , npj Computational Materials)

   An emerging chalcogenide perovskite, CaZrSe₃, holds promise for energy conversion applications given its notable optical and electrical properties. However, knowledge of its thermal properties is extremely important, e.g. for potential thermoelectric applications, and has not been previously reported in detail. In this work, we examine and explain the lattice thermal transport mechanisms in CaZrSe₃using density functional theory and Boltzmann transport calculations. We find the mean relaxation time to be extremely short corroborating an enhanced phonon–phonon scattering that annihilates phonon modes, and lowers thermal conductivity. In addition, strong anharmonicity in the perovskite crystal represented by the Grüneisen parameter predictions, and low phonon number density for the acoustic modes, results in the lattice thermal conductivity to be limited to 1.17 W m⁻¹ K⁻¹. The average phonon mean free path in the bulk CaZrSe₃sample (N → ∞) is 138.1 nm and nanostructuring CaZrSe₃sample to ~10 nm diminishes the thermal conductivity to 0.23 W m⁻¹ K⁻¹. We also find that p-type doping yields higher predictions of thermoelectric figure of merit than n-type doping, and values ofZT~0.95–1 are found for hole concentrations in the range 10¹⁶–10¹⁷ cm⁻³and temperature between 600 and 700 K.