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二维共价键子结构Zintl相热电材料研究及进展

袁珉慧 乐文凯 谈小建 帅晶

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二维共价键子结构Zintl相热电材料研究及进展

袁珉慧, 乐文凯, 谈小建, 帅晶

Research progress of two-dimensional covalent bond substructure Zintl phase thermoelectric materials

Yuan Min-Hui, Le Wen-Kai, Tan Xiao-Jian, Shuai Jing
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  • 热电材料可以实现热能和电能间的直接相互转换, 在半导体制冷和热能回收方面有着重要应用. Zintl相热电材料由电负性差异较大的阴阳离子组成, 其输运特征符合“声子玻璃, 电子晶体”的概念, 因此受到了广泛的研究, 特别是具有二维共价键子结构Zintl相热电材料凭借优异的电性能更是被寄予厚望. 本文综述了具有二维共价键子结构的典型Zintl相热电材料, 梳理了研究最广且性能突出的CaAl2Si2结构1-2-2型、原胞内原子较多本征低热导率的9–4+x–9型、具有天然空位而本征热导率极低的2-1-2型、以及电性能相对较好的ZrBeSi结构1-1-1型Zintl相的研究进展; 其中还特别总结了性能优异的Mg3Sb2基n型Zintl材料的研究发展. 本文概括总结了每种体系近年来的研究进展及性能调控方法, 讨论了进一步优化其热电性能的可能策略, 并对其未来发展进行了展望.
    Thermoelectric materials can realize the direct conversion between thermal energy and electrical energy, and thus having important applications in semiconductor refrigeration and heat recovery. Zintl phase is composed of highly electronegative cations and anions, which accords with the concept of “phonon glass, electron crystal” (PGEC). Thermoelectric properties of Zintl phase have attracted extensive interest, among which the two-dimensional (2D) covalent bond structure featured Zintl phases have received more attention for their outstanding electrical properties. In this review, Zintl phase materials with two-dimensional covalent bond substructures are reviewed, including 1-2-2-type, 9–4+x–9-type, 2-1-2-type and 1-1-1-type Zintl phase. The 1-2-2-type Zintl phase is currently the most widely studied and best-performing Zintl material. It is worth mentioning that the maximum ZT value for the Mg3Sb2-based n-type Zintl material with the CaAl2Si2 structure has been reported to reach 1.85, and the average ZT value near room temperature area also reaches 1.4. The 9–4+x–9-type Zintl material with a mass of atoms in unit cell contributes to lower thermal conductivity thus relatively high ZT value. The 2-1-2-type Zintl material has extremely low thermal conductivity due to the intrinsic vacancies, which has been developing in recent years. The 1-1-1-type Zintl material with the same ZrBeSi structure as the 2-1-2-type Zintl material, shows better electrical transport performance. In sum, this review summarizes the recent progress and optimization methods of those typical Zintl phases above. Meanwhile, the future optimization and development of Zintl phase with two-dimensional covalent bond substructures are also prospected.
      通信作者: 谈小建, tanxiaojian@nimte.ac.cn ; 帅晶, shuaij3@mail.sysu.edu.cn
    • 基金项目: 国家自然科学基金 (批准号: 52002413, 21875273)、广东省自然科学基金(批准号: 2021A1515010612)、浙江省自然科学基金杰出青年项目(批准号: LR21E020002)和中国科学院青年创新促进会(批准号: 2019298)资助的课题.
      Corresponding author: Tan Xiao-Jian, tanxiaojian@nimte.ac.cn ; Shuai Jing, shuaij3@mail.sysu.edu.cn
    • Funds: Project supported by the National Natural Science Foundation of China (Grant Nos. 52002413, 21875273), the Natural Science Foundation of Guangdong Province, China (Grant No. 2021A1515010612), the Natural Science Foundation of Zhejiang Province, China (Grant No. LR21E020002), and Youth Innovation Promotion Association CAS (Grant No. 2019298).
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  • 图 1  (a) 各类型结构中典型Zintl相ZT值对比图[8,10-12,14,18,21,24,25,28,32-35]; (b) 2D典型Zintl相最大ZT值随时间变化总结图

    Fig. 1.  (a) ZT values of typical Zintl phases with 2D covalent bond substructures [8,10-12,14,18,21,24,25,28,32-35]; (b) summary diagram of the maximum ZT value of some representative 2D Zintl phase over time.

    图 2  AB2X2型Zintl材料 (a) 晶体结构; (b) 单胞扩展键; (c) 单胞不扩展键晶体结构示意图; (d) Sb基AB2X2型Zintl相ZT值对比图; (e) Bi基AB2X2型Zintl相ZT值对比图[8,21,34,36-45]

    Fig. 2.  (a) Crystal structure of AB2X2-type Zintl material; (b), (c) unit cell. Temperature-dependent ZT values of (d) Sb-based AB2X2-type Zintl phases; (e) Bi-based AB2X2-type Zintl phases[8,21,34,36-45].

    图 3  Mg3Sb2 Zintl材料 (a) 晶体结构; (b) c轴方向晶体结构; (c) a轴方向晶体结构示意图; (d) Mg3Sb2结构由传统认为的层状结构到三维结构示意图; (e) 近年Mg3Sb2基Zintl相主要工作ZT值随温度变化图[9,10,22,23,48,66,69,76-78]; (f) 突出Mg3Sb2相300—500 K及300—773 K温区下平均ZT值对比图[9-12,69,73,75,78-82]

    Fig. 3.  (a) Crystal structure of Mg3Sb2; (b) crystal structure along the c axis; (c) crystal structure along the a axis; (d) Mg3Sb2 structure with traditional layered covalent bonds compared to the 3D covalent bonds; (e) temperature-dependent ZT values of Mg3Sb2-based Zintl phases[9,10,22,23,48,66,69,76-78]; (f) average ZT values of Mg3Sb2-based Zintl phases at 300−500 K and 300−773 K[9-12,69,73,75,78-82].

    图 4  Ca9Zn4Sb9相 (a) 晶体结构图; (b) a轴晶体结构图; 9–4+x–9型Zintl相近年来典型结构(c)ZT值随温度变化图; (d) 泽贝克系数随温度变化图; (e) 电阻率随温度变化图; (f) 热导率及晶格热导率随温度变化图[27,28,87-90]

    Fig. 4.  (a) Crystal structure of Ca9Zn4Sb9; (b) crystal structure of Ca9Zn4Sb9 along a axis. Temperature-dependent (c) ZT values; (d) Seebeck coefficient; (e) electrical resistivity; (f) thermal conductivity of 9–4+x–9 type Zintl phases [27,28,87-90].

    图 5  (a) EuZn2Sb2单胞晶体结构图; (b) Eu2ZnSb2相与EuZn2Sb2相结构对比图[25]; (c) Eu2ZnSb2a轴方向晶体结构图; (d) Eu2ZnSb2c轴方向晶体结构示意图; (e) Eu2ZnSb2相扩胞后晶体结构示意图; (f) Eu2ZnSb2相扩胞后a轴方向晶体结构示意图; (g) 2-1-2型Zintl相近年来典型结构ZT值随温度变化图; (h) S随温度变化图; (i) 电阻率随温度变化图; (j) 2-1-2型Zintl相与9–4+x–9, 1-2-2型典型Zintl相晶格热导率随温度变化对比图[8,24,25,27,90,92]

    Fig. 5.  (a) Unit cell of EuZn2Sb2; (b) unit cell of Eu2ZnSb2 ; (c) unit cell of Eu2ZnSb2 along the a axis;(d) crystal structure along the c axis; (e) crystal structure of Eu2ZnSb2; (f) in the a axis direction after cell expansion. Temperature-dependent (g) ZT values; (h) Seebeck coefficient; (i) electrical resistivity of 2-1-2 type Zintl phases; (j) lattice thermal conductivity of 2-1-2, 9–4+x–9 and 1-2-2type Zintl phases [8,24,25,27,90,92].

    图 6  SrAgSbZintl相 (a) 晶体结构示意图; (b)延c轴方向晶体结构示意图. 1-1-1型Zintl相近年来典型结构 (c) ZT值随温度变化图; (d) 电阻率随温度变化图; (e) 热导率随温度变化图; (f) 1-1-1型Zintl相功率因子较同结构1-2-2型Zintl相随温度变化对比图[24-26,106]

    Fig. 6.  (a) Crystal structure of SrAgSb; (b) crystal structure of SrAgSb along the c axis. Temperature-dependent (c) ZT values; (d) power factors (compared with 2-1-2 Zintl phases); (e) electric resistivity; (f) thermal conductivity of typical 1-1-1 Zintl phases[24-26,106].

    表 1  1-2-2型层状Zintl材料热电性能汇总表

    Table 1.  Summary of thermoelectric properties of 1-2-2 type layered Zintl materials.

    时间材料Ρ/(mΩ·cm)S/(μV·K–1)κ/(W·m–1·K–1)ZTT/KZTRT
    2005Ca0.25Yb0.75Zn2Sb2[36]3.71701.40.567730.08
    2007BaZn2Sb2[38]6.11851.250.336730.05
    2008YbZn1.9Mn0.1Sb2[57]1.51501.60.657260.05
    2008EuZn2Sb2[58]1.81801.450.97130.16
    2009YbCd1.6Zn0.4Sb2[46]1.661801.11.26500.2
    2010Yb0.6Ca0.4Cd2Sb2[37]4.42400.90.967000.14
    2010Yb0.75Eu0.25Cd2Sb2[59]424010.976500.18
    2010EuZn1.8Cd0.2Sb2[47]22001.41.066500.18
    2011YbCd1.85Mn0.15Sb2[60]5.72450.61.146500.17
    2012YbMg2Bi2[39]51801.80.446500.07
    2014Yb0.99Zn2Sb2[61]1.31601.70.858000.05
    2016YbCd1.9Mg0.1Sb2[40]3.32301.021.086500.2
    2016Ca0.5Yb0.5Mg2Bi2[49]2.81871.0818730.1
    2016Ca0.995Na0.005Mg2Bi1.98[54]32001.250.98730.05
    2016Eu0.2Yb0.2Ca0.6Mg2Bi2[8]3.52150.921.38750.25
    2018YbCd1.5Zn0.5Sb2[34]1.71721.21.267000.18
    2018Yb0.96Ba0.04Cd1.5Zn0.5Sb2[34]21850.941.37000.18
    2019Ba0.7975Yb0.2Na0.0025Cd2Sb2[41]4.12100.810.937000.1
    2019EuCd1.4Zn0.6Sb2[42]3.522010.967000.18
    2020Ca0.65Yb0.35Mg1.9Zn0.1Bi1.98[43]2.631851.0417730.2
    2020YbMg2Bi1.58Sb0.4[44]4.121911.058730.14
    2020Sm0.25Yb0.375Eu0.375Mg2Bi1.99[45]3.71970.90.97730.18
    2020(Yb0.9Mg0.1)Mg0.8Zn1.198Ag0.002Sb2[21]4.752570.741.57730.28
    下载: 导出CSV

    表 2  Mg3Sb2基Zintl材料热电性能汇总表

    Table 2.  Summary of thermoelectric properties of Mg3Sb2-based layered Zintl materials.

    时间材料ρ/(mΩ·cm)S/(μV·K–1)κ/(W·m–1·K–1)ZTT/KZTRT
    2006Mg3Sb2[83]292881.20.218750.001
    2013Mg3Bi0.2Sb1.8[76]404000.580.67500.01
    2014Mg3Pb0.2Sb1.8[48]28.62800.280.847730.03
    2015Mg2.9875Na0.0125Sb2[66]5.42000.950.67730.03
    2017Mg2.985Ag0.015Sb2[22]92050.650.517250.08
    2016Mg3.2Sb1.5Bi0.49Te0.01[67]5–2860.791.517160.2
    2016Mg3Sb1.48Bi0.48Te0.04[53]10–2050.731.67500.6
    2017Mg3.05Nb0.15Sb1.5Bi0.49Te0.01[9]4.35–2770.841.577000.31
    2017Mg3.1Co0.1Sb1.5Bi0.49Te0.01[69]5.1–2950.781.77730.4
    2018Mg3.15Mn0.05Sb1.5Bi0.49Te0.01[10]4.5–3020.791.857230.42
    2019Mg3+δSb1.5Bi0.49Te0.01:Mn0.01[78]4.5–2900.91.67730.65
    2019Mg3.05SbBi0.97Te0.03[74]1.7–2020.921.315000.71
    2019Mg3.02Y0.02Sb1.5Bi0.5[11]4.2–2700.761.87730.2
    2020Mg3.2Sb1.99Te0.01+GNP[23]6.4–3200.741.77500.18
    2021Mg3.17B0.03Sb1.5Bi0.49Te0.01[12]5.4–2960.691.817730.62
    下载: 导出CSV

    表 3  9–4+x–9型层状Zintl材料热电性能汇总表

    Table 3.  Summary of thermoelectric properties of 9–4+x–9 type layered Zintl materials.

    时间材料ρ/(mΩ·cm)S/(μV·K–1)κ/(W·m–1·K–1)ZTT/KZTRT
    2014Yb9Mn4.2Sb9[87]7.91850.580.79500.035
    2015Eu9Cd3.75Ag1.42Sb9[91]2.0851.00.327500.03
    2016Ca9Zn4.35Cu0.15Sb9[89]3.01400.80.728730.1
    2017Ca9Zn4.6Sb9[27]11.02700.481.18730.1
    2019Ca6.75Eu2.25Zn4.7Sb9[28]5.552000.531.057730.21
    2021Sr9Mg4.45Bi9[90]3.751350.650.577730.14 (323 K)
    下载: 导出CSV

    表 4  2-1-2型层状Zintl材料热电性能汇总表

    Table 4.  Summary of thermoelectric properties of 2-1-2 type layered Zintl materials.

    时间材料ρ/(mΩ·cm)S/(μV·K–1)κ/(W·m–1·K–1)ZTT/KZTRT
    2017Yb2CdSb2[92]51550.520.25230.23
    2017Yb1.64Eu0.36CdSb2[92]3.51700.60.75230.26
    2018Eu2ZnSb2[25]24.42900.420.67230.14
    2018Eu2Zn0.98Sb2[25]82200.4818230.22
    2020Eu2Zn0.97Ag0.06Sb2[24]102200.430.938230.2
    2020Eu2Zn0.95Ag0.06Sb2[24]5.31940.51.18230.2
    下载: 导出CSV

    表 5  1-1-1型层状Zintl材料热电性能汇总表

    Table 5.  Summary of thermoelectric properties of 1-1-1 type layered Zintl materials.

    时间材料ρ/(mΩ·cm)S/(μV·K–1)κ/(W·m-1·K–1)ZTT/KZTRT
    2018Ca0.85La0.15Ag0.89Sb[106]1.851201.30.528600.07
    2018Ca0.55Sr0.3La0.15Ag0.89Sb[106]1.61251.00.78230.1
    2020SrAgSb[26]0.951142.20.57730.07
    2020Sr1.01AgSb[26]1.271251.70.587730.1
    2020EuCuSb[26]0.64832.90.37730.03
    2020EuAgSb[26]0.74902.40.357730.05
    下载: 导出CSV
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出版历程
  • 收稿日期:  2021-05-28
  • 修回日期:  2021-06-19
  • 上网日期:  2021-08-15
  • 刊出日期:  2021-10-20

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