Synthesis and thermoelectric properties of Mn-doped AgSbTe₂ compounds

Polycrystalline p-type Ag 0.9 Sb 1.1 x Mn x Te 2.05(x = 0.05,0.10,and 0.20) compounds have been prepared by a combined process of melt-quenching and spark plasma sintering.The sample composition of Ag 0.9 Sb 1.1 x Mn x Te 2.05 has been specially designed in order to achieve the doping effect by replacing part of Sb with Mn and to present the uniformly dispersed Ag 2 Te phase in the matrix by adding insufficient Te,which is beneficial for optimizing the electrical transport properties and enhancing the phonon scattering effect.All the samples have the NaCl-type structure according to our X-ray powder diffraction analysis.After the treatment of spark plasma sintering,only the sample with x = 0.20 has a small amount of MnTe 2 impurities.The thermal analysis indicates that a tiny amount of Ag 2 Te phase exists in all these samples.The presence of the MnTe 2 impurity with high resistance and high thermal conductivity leads to the deteriorative thermoelectric performance of the sample with x = 0.20 due to the decreased electrical transport properties and the increased thermal conductivity.In contrast,the sample with x = 0.10 exhibits enhanced thermoeletric properties due to the Mn-doping effect.A dimensionless thermoelectric figure of merit of 1.2 is attained for the sample with x = 0.10 at 573 K,showing promising thermoelectric properties in the medium temperature range.     

Complex alloying effect on thermoelectric transport properties of Cu_2Ge(Se_(1-x)Te_x)_3

To enhance the thermoelectric performance of Cu_2GeSe_3, a series of Te-alloyed samples Cu_2Ge(Se_(1-x)Te_x)_3 are synthesized and investigated in this work. It is found that the lattice thermal conductivity is reduced drastically for x = 0.1 sample, which may be attributed to the point defects introduced by alloying. However, for samples with x ≥ 0.2, the lattice thermal conductivity increases with increasing x, which is related to a less distorted structure. The structure evolution,together with the change in carrier concentration, also leads to a systemically change in electrical properties. Finally, a z T of 0.55@750 K is obtained for the sample with x = 0.3, about 62% higher than that for the pristine sample.     

Thermoelectric properties of Sr_(0.61)Ba_(0.39)Nb_2O_(6-δ) ceramics in different oxygen-reduction conditions

The thermoelectric properties of Sr0.61Ba0.39Nb2O6-δceramics, reduced in different conditions, are investigated in the temperature range from 323 K to 1073 K. The electrical transport behaviors of the samples are dominated by the thermal-activated polaron hopping in the low temperature range, the Fermi glass behavior in the middle temperature range,and the Anderson localized behavior in the high temperature range. The thermal conductivity presents a plateau at hightemperatures, indicating a glass-like thermal conduction behavior. Both the thermoelectric power factor and the thermal conductivity increase with the increase of the degree of oxygen-reduction. Taking these two factors into account, the oxygen-reduction can still contribute to promoting the thermoelectric figure of merit. The highest ZT value is obtained to be ～0.19 at 1073 K in the heaviest oxygen reduced sample.     

Phase transition and high temperature thermoelectric properties of copper selenide Cu2-x Se （0 ≤ x ≤ 0.25）

With good electrical properties and an inherently complex crystal structure, Cu_2-xSe is a potential “phonon glass electron crystal” thermoelectric material that has previously not attracted much interest. In this study, Cu_2-xSe (0 ≤ x ≤ 0.25) compounds were synthesized by a melting-quenching method, and then sintered by spark plasma sintering to obtain bulk material. The effect of Cu content on the phase transition and thermoelectric properties of Cu_2-xSe were investigated in the temperature range of 300 K—750 K. The results of X-ray diffraction at room temperature show that Cu_2-xSe compounds possess a cubic structure with a space group of Fm3m (#225) when 0.15 < x le 0.25, whereas they adopt a composite of monoclinic and cubic phases when 0 ≤ x ≤ 0.15. The thermoelectric property measurements show that with increasing Cu content, the electrical conductivity decreases, the Seebeck coefficient increases and the thermal conductivity decreases. Due to the relatively good power factor and low thermal conductivity, the nearly stoichiometric Cu₂Se compound achieves the highest ZT of 0.38 at 750 K. It is expected that the thermoelectric performance can be further optimized by doping appropriate elements and/or via a nanostructuring approach.     

Effect of Nb doping on microstructures and thermoelectric properties of SrTiO_3 ceramics

Nb-doped SrTiO_3 thermoelectric ceramics with different niobium concentrations,sintering temperatures and Sr-site vacancies are successfully prepared by high energy ball milling combined with carbon burial sintering.For fully understanding the effect of niobium doping on SrTiO_3,thermoelectric transport properties are systematically investigated in a temperature range from 300 K to 1100 K.The carrier mobility can be significantly enhanced,and the electrical conductivity is quadrupled,when the sintering temperature rises from 1673 K to 1773 K(beyond the eutectic temperature(1713 K) of SrTiO_3–TiO_2).The lattice vibration can be suppressed by the lattice distortion introduced by the doped niobium atoms.However,Sr-site vacancies compensate for the lattice distortion and increase the lattice thermal conductivity more or less.Finally,we achieve a maximum value of figure-of-merit z T of 0.21 at 1100 K for Sr Ti_(0.9)Nb_(0.1)O_3 ceramic sintered at1773 K.     

Anisotropic thermoelectric transport properties in polycrystalline SnSe_2

It is reported that SnSe_2 consisting of the same elements as SnSe, is a new promising thermoelectric material with advantageous layered structure. In this work, the thermoelectric performance of polycrystalline SnSe_2 is improved through introducing SnSe phase and electron doping(Cl doped in Se sites). The anisotropic transport properties of SnSe_2 are investigated. A great reduction of the thermal conductivity is achieved in SnSe_2 through introducing SnSe phase, which mainly results from the strong SnSe_2–SnSe inter-phase scattering. Then the carrier concentration is optimized via Cl doping, leading to a great enhancement of the electrical transport properties, thus an extraordinary power factor of ～5.12 μW·cm~(-1)·K~(-2) is achieved along the direction parallel to the spark plasma sintering(SPS) pressure direction( P). Through the comprehensive consideration on the anisotropic thermoelectric transport properties, an enhanced figure of merit ZT is attained and reaches to ～ 0.6 at 773 K in SnSe_2-2% SnSe after 5% Cl doping along the P direction, which is much higher than ～ 0.13 and ～ 0.09 obtained in SnSe_2-2% SnSe and pristine SnSe_2 samples, respectively.     

Thermoelectric properties of lower concentration K-doped Ca_3Co_4O_9 ceramics

The tuning of electron and phonon by ion doping is an effective method of improving the performances of thermoelectric materials. A series of lower concentration K-doped Ca_(3-x)K_xCo_4O_9(x = 0, 0.05, 0.10, 0.15) polycrystalline ceramic samples are prepared by combining citrate acid sol-gel method with cold-pressing sintering method. The single-phase compositions and plate-like grain morphologies of all samples are confirmed by x-ray diffraction and field emission scanning electron microscope. The effects of lower concentration K doping on the thermoelectric properties of the material are evaluated systematically at high temperatures(300–1026 K). Low concentration K doping causes electrical conductivity to increase up to 23% with little effect on the Seebeck coefficient. Simultaneously, the thermal conductivity of K-doped sample is lower than that of the undoped sample, and the total thermal conductivity reaches a minimum value of approximately1.30 W·m~(-1)·K~(-1), which may be suppressed mainly by the phonon thermal conduction confinement. The dimensionless figure-of-merit ZT of Ca_(2.95)K_(0.05)Co_4O_9 is close to 0.22 at 1026 K, representing an improvement of about 36% compared with that of Ca_3Co_4O_9, suggesting that lower concentration K-doped Ca_3Co_4O_9 series materials are promising thermoelectric oxides for high-temperature applications.     

High Thermoelectric Properties of PbTe Doped with Bi2Te3 and Sb2Te3

The composition-dependent thermoelectric properties of lead telluride (PbTe) doped with bismuth telluride (Bi2Te3), antimony telluride (Sb2Te3) and (BiSb)2Te3 have been studied at room temperature. All the sampies exhibit small thermal conductivity. The figures of merit, 7.63, 1.03 and 8.97 x 10-4, have been obtained in PbTe with these dopants, respectively. These values are several times higher than those of PbTe containing other dopants with small grain sizes. The high thermoelectric performance is explained by electronic topological transition induced by alloying. The results indicate that these dopants are effective to enhance the thermoelectric performance of PbTe.     

Effect of pressure on electronic and thermoelectric properties of magnesium silicide: A density functional theory study

We study the effect of pressure on electronic and thermoelectric properties of Mg_2Si using the density functional theory and Boltzmann transport equations. The variation of lattice constant, band gap, bulk modulus with pressure is also analyzed. Further, the thermoelectric properties(Seebeck coefficient, electrical conductivity, electronic thermal conductivity) have been studied as a function of temperature and pressure up to 1200 K. The results show that Mg_2Si is an n-type semiconductor with a band gap of 0.21 eV. The negative value of the Seebeck coefficient at all pressures indicates that the conduction is due to electrons. With the increase in pressure, the Seebeck coefficient decreases and electrical conductivity increases. It is also seen that, there is practically no effect of pressure on the electronic contribution of thermal conductivity.The paper describes the calculation of the lattice thermal conductivity and figure of merit of Mg_2Si at zero pressure. The maximum value of figure of merit is attained 1.83 × 10~(-3) at 1000 K. The obtained results are in good agreement with the available experimental and theoretical results.     

Composition-Dependent Characterization of Sb2Te3 Thin Films Prepared by Ion Beam Sputtering Deposition

The optimization of ion beam sputtering deposition process for Sb2 Te3 thin films deposited on BK7 glass substrates is reported. The influence of composition ratio on the thermoelectric properties is investigated. X-ray diffraction shows that the major diffraction peaks of the films match with those of Sb2 Te3. Hall effect and Seebeck coefficient measurement reveal that all the samples are of p-type. The Sb2 Te3 thin films exhibit the Seebeck coefficient of 190μVk^-1 and the electrical conductivity of 1.1 × 10^3 Scm^-1 when the atomic ratio of Sb to Te is 0.65. Carrier concentration and motility of the films increase with the increasing atomic ratio of Sb to Te. The Sb2 Tea film with a maximum power factor of 2.26×10^-3 Win^-1K^-2 is achieved when annealed at 400℃. Raman measurement shows that the main peaks are at about 120 cm^-1, 252 cm^-1 and 450 cm^-1, in agreement with those of V-VI compound semiconductors.     

Cu掺杂AgSbTe2化合物的相稳定、晶体结构及热电性能

利用熔融快淬结合放电等离子烧结(SPS), 制备了Cu_xAg_1-xSbTe₂(x= 0---0.3)样品. 粉末X射线衍射(XRD)分析结果显示, SPS处理以前, 含Cu样品形成NaCl型结构的固溶体, 而未加入Cu的样品析出Ag₂Te第二相. 根据热分析和XRD测量结果, Cu的加入能够有效抑制Ag₂Te的析出, 但同时会在快淬样品中产生少量非晶相. 在温度升高到540 K左右时, 非晶相发生晶化, 形成Sb₇Te亚稳相, 并最终转变成Sb₂Te₃稳定相. 对快淬样品进行低温SPS快速处理后, x =0.1样品为面心立方结构的单相化合物, 但是x =0.2, 0.3的样品分别析出第二相Sb₇Te和Sb₂Te₃. 由于析出第二相, x=0.2, 0.3样品的电导率增大, Seebeck系数减小, 热导率相应升高, 综合热电性能降低. x=0.1单相样品的功率因子与文献报道的AgSbTe₂化合物相当. 元素替代的合金化效应 增强了Cu_0.1Ag_0.9SbTe₂化合物的声子散射, 有效降低了样品的热导率. 因此, 单相样品Cu_0.1Ag_0.9SbTe₂表现出较佳的热电性能, 在620 K时热电优值达到1.     

非化学计量比AgSbTe2+x化合物制备及热电性能

采用高纯元素直接熔融、淬火并结合放电等离子烧结方法制备了非化学计量比AgSbTe_2+x(x=0—0.05)系列样品,研究了不同Te含量在300—600 K范围内对样品热电性能的影响规律.结果表明:随着Te含量的增加,Ag⁺离子空位浓度增加,空穴浓度和电导率大幅度提高,Seebeck系数减小.热导率随Te过量程度的增加略有增加,但所有Te过量样品的晶格热导率均介于0.32—0.49 W/mK之间,低于化学计量比样品的值,接近理论最低晶格热导率.AgS 关键词： 2')" href="#">AgSbTe₂ 非化学计量比 热电性能 热导率     

(Bi1-x Agx)2(Te1-ySey)3粉体的机械合金化制备及其放电等离子烧结体的热电输运特性

采用机械合金化制备了n型(Bi_1-xAg_x)₂(Te_1-ySe_y)₃合金粉体,对其进行XRD分析表明Bi,Te,Ag,Se单质粉末,经2h球磨后实现了合金化;SEM分析表明随着机械合金化时间延长粉体颗粒变得均匀、细小,颗粒尺寸在微米至亚微米数量级.采用放电等离子烧结制备了块体样品,研究了合金成分和球磨时间对热电性能的影响.结果表明材料的热电性能与掺杂元素有密切关系,Ag有利于提高功率因子和降低晶格热导率,球磨10h的(Bi_0.99Ag_0.01)₂(Te_0.96Se_0.04)₃合金粉末的烧结块体具有最大的功率因子和最低的晶格热导率,并在323K取得最高ZT值0.52. 关键词： 1-xAg_x)₂(Te_1-ySe_y)₃合金')" href="#">(Bi_1-xAg_x)₂(Te_1-ySe_y)₃合金 机械合金化 放电等离子烧结 热电性能     

熔体旋甩法合成n型(Bi_(0.85)Sb_(0.15))_2(Te_(1-x)Se_x)_3化合物的微结构及热电性能

采用熔体旋甩结合放电等离子烧结(MS-SPS)技术制备了单相n型四元(Bi0.85Sb0.15)2(Te1-xSex)3(x=0.15,0.17,0.19,0.21)化合物,并对所得样品的微结构和热电传输性能进行了系统研究.样品自由断裂面的场发射扫描电子显微镜及抛光面的背散射电子成分分析表明:块体材料晶粒细小,晶粒排列紧密,成分分布均匀且相结构单一,样品中存在大量10—100nm的层状结构.随着Se含量x的增加,样品的电导率和热导率逐渐增加,而Seebeck系数逐渐降低.相比商业应用的区熔材料,MS-SPS方法合成的高Se组成的样品均在425K后表现出更高的ZT值,其中(Bi0.85Sb0.15)2(Te0.83Se0.17)3样品具有最高的ZT值,在360K可达到0.96,并在320—500K均保持较高的ZT值,500K时其ZT值相比区熔材料提高了48%.此外,通过调节Se的含量,可以有效地调控材料的ZT峰值出现的温度段,这对多级或梯度热电器件的制备具有重要意义.     

p型Ag0.5(Pb8－xSnx)In0.5Te10化合物的制备及其热电性能

采用高温熔融缓冷和放电等离子烧结工艺制备了p型Ag_0.5(Pb_8-xSn_x)In_0.5Te₁₀五元化合物.研究了Sn含量对化合物载流子传输特性及热电性能的影响规律.结果表明：在Ag_0.5(Pb_8-xSn_x)In_0.5Te₁₀(x 关键词： 0.5(Pb_8-xSn_x)In_0.5Te₁₀')" href="#">Ag_0.5(Pb_8-xSn_x)In_0.5Te₁₀ 合成 载流子 热电性能     

Effect of thermal treatment on the thermoelectric properties of Sb<Subscript>0.9</Subscript>Bi<Subscript>1.1</Subscript>Te<Subscript>2.9</Subscript>Se<Subscript>0.1</Subscript> solid solution thin films

The effect thermal treatment in a vacuum has on the thermoelectric properties of Sb_0.9Bi_1.1Te_2.9Se_0.1 solid solution thin films obtained via ion-beam sputtering in an argon atmosphere is considered. It is established that the specific resistance and thermopower are determined by the type and concentration of intrinsic point defects of the Sb_0.9Bi_1.1Te_2.9Se_0.1 solid solution. The power factor values are found to be comparable to those of nanostructured materials based on (Bi,Sb)₂(Te,Se)₃ solid solutions.     

Sb2Te3 纳米结构的制备与表征

以室温热电性能优异的传统热电材料Sb₂Te₃为研究对象,利用化学气相沉积法制备Sb₂Te₃单晶纳米结构,并研究其生长机理.实验结果表明,不加催化剂时Sb₂Te₃易生长成六方纳米盘,在金催化剂条件下定向生长成纳米线.Sb₂Te₃的形貌与其晶体结构和生长机理有关.Sb₂Te₃为三角结构,Sb和     

Evaluation of Thermoelectric Properties of Ag0.366Sb0.558Te

Ternary AgSbTe₂ materials are frequently reported to show a promising thermoelectric performance, due to the intrinsically low lattice thermal conductivity and complex valence band structure. However, stoichiometric AgSbTe₂ is found to be thermodynamically unstable and would partially decompose into Ag₂Te and Sb₂Te₃ during thermal cycling. Instead, Ag_0.366Sb_0.558Te is the composition for stabilizing the single-phase according to the Ag₂Te-Sb₂Te₃ phase diagram, while the thermoelectric transport properties have rarely been reported and are the focus of this work. Sn/Sb substitution is found to effectively increase not only the carrier concentration from ≈5 × 10¹⁹ cm⁻³ to ≈4 × 10²¹ cm⁻³, but also the density-of-states effective mass, leading to an enhanced Seebeck coefficient along with a decreased carrier mobility. Single parabolic band (SPB) model with acoustic phonon scattering enables a good understanding on the charge transport. The increased carrier concentration effectively suppresses the bipolar effect at high temperatures. As a result, a peak zT of ≈1.3 and an average of ≈0.9 are achieved.     

Thermoelectric properties in p-type nanostructured Ge-doped Sb100GeTe150 alloy

Ge-doped Sb₁₀₀GeTe₁₅₀ alloy were prepared using spark plasma sintering technique, and its thermoelectric properties were evaluated over the temperature range 318–492 K. Through XRD analysis, we observed the same single phase as Sb₂Te₃ and weakened diffraction peaks. Rietveld refinement reveals that there is 0.96 at.% Ge that occupies in the Sb sites, leading to the lattice distortion in the Sb–Te crystal. High-resolution TEM images show that there are many nanodomains randomly distributed in the matrix with a large amount of amorphous phase adjoined. Measurements indicated that the Seebeck coefficients (α) increase and the electrical and thermal conductivities decrease with temperature in the entire temperature range. The maximum α value reaches 135 μV/K at 492 K, and the thermal conductivities are about 0.3 W/mK lower than those of present Sb₂Te₃ for the corresponding temperatures. The highest thermoelectric figure of merit ZT for the nanostructured alloy Sb₁₀₀GeTe₁₅₀ is 0.84 at 492 K, whereas that of the currently prepared Sb₂Te₃ is 0.74 at the corresponding temperature.