Synergistic tuning of carrier mobility, effective mass, and point defects scattering triggered high thermoelectric performance in n-type Ge-doped PbTe

Synergistic tuning of carrier mobility, effective mass, and point defects scattering triggered high thermoelectric performance in n-type Ge-doped PbTe
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载流子迁移率、有效质量和点缺陷散射的协同调节引发了 n 型 Ge 掺杂 PbTe 的高热电性能

DOI:
10.1063/1.5084083
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发表时间:
2019-02
影响因子:
3.2
通讯作者:
Ang Ran
Ang Ran
中科院分区:
物理与天体物理3区
文献类型:
--
作者:
Wang Zhengshang;He Huan;Cui Xudong;Liu Hangtian;Qiu Wenbin;Chen Longqing;Zhou Binqiang;Tang Jun;Ang Ran

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在中温p型碲化铅材料中,取得了显著热电性能的研究成果。然而,n型PbTe表现出相对较差的品质因数ZT,迫切期望其被增强并与p型对应物兼容。在这里,我们报告,过量的Pb的引入可以有效地消除n型Pb 1 + x Te − 0.4% I中的阳离子空位,导致载流子迁移率μ的显著提高。此外,进一步的Ge掺杂诱导了热电性能的大幅增强,这是由于n型Pb 1.01 Te − 0.4% I − y % Ge中改善的电输运性能和增加的声子散射的综合效应。Ge的掺杂不仅由于有效质量m的增加而导致Seebeck系数的增加,而且由于点缺陷散射的加强而导致晶格热导率的急剧下降。结果,Pb 1.01 Te − 0.4% I − 3% Ge在723 K时的ZT值大幅提高,达到1.31。在323 ~ 823 K的宽温度范围内,Ge掺杂的平均ZTave值为10.87,计算的转换效率为13.5%。通过对载流子迁移率、有效质量和点缺陷的协同调控,我们发现n型Pb1.01 Te − 0.4% I − y % Ge具有很大的潜力,而在中温p型PbTe中,已经取得了显著的热电性能。然而,n型PbTe表现出相对较差的品质因数ZT,迫切期望其被增强并与p型对应物兼容。在这里,我们报告,过量的Pb的引入可以有效地消除n型Pb 1 + x Te − 0.4% I中的阳离子空位,导致载流子迁移率μ的显著提高。此外,进一步的Ge掺杂诱导了热电性能的大幅增强,这是由于n型Pb 1.01 Te − 0.4% I − y % Ge中改善的电输运性能和增加的声子散射的综合效应。Ge的掺杂不仅由于有效质量m的增加而导致Seebeck系数的增加,而且由于点缺陷散射的加强而导致晶格热导率的急剧下降。因此,ZT的巨大增强...
Most achievements on remarkable thermoelectric performance have been made in the intermediate-temperature p-type PbTe. However, the n-type PbTe exhibits a relatively poor figure of merit ZT, which is urgently expected to be enhanced and compatible with the p-type counterpart. Here, we report that the introduction of excessive Pb can effectively eliminate cation vacancies in the n-type Pb 1 + x Te − 0.4 % I, leading to a considerable improvement of carrier mobility μ. Moreover, further Ge doping induces a large enhancement of thermoelectric properties due to the combined effect of improved electrical transport properties and increased phonon scattering in the n-type Pb 1.01 Te − 0.4 % I − y % Ge. The Ge doping not only contributes to the increase of the Seebeck coefficient owing to the increased effective mass m ∗, but also gives rise to the dramatic decrease of lattice thermal conductivity due to the strengthened point defects scattering. As a result, a tremendous enhancement of the ZT value at 723 K reaches ∼ 1.31 of Pb 1.01 Te − 0.4 % I − 3 % Ge. Particularly, the average Z T a v e value of ∼ 0.87 and calculated conversion efficiency η ∼ 13.5 % is achieved by Ge doping in a wide temperature range from 323 to 823 K. The present findings demonstrate the great potential in the n-type Pb 1.01 Te − 0.4 % I − y % Ge through a synergistic tuning of carrier mobility, effective mass, and point defects engineering strategy.Most achievements on remarkable thermoelectric performance have been made in the intermediate-temperature p-type PbTe. However, the n-type PbTe exhibits a relatively poor figure of merit ZT, which is urgently expected to be enhanced and compatible with the p-type counterpart. Here, we report that the introduction of excessive Pb can effectively eliminate cation vacancies in the n-type Pb 1 + x Te − 0.4 % I, leading to a considerable improvement of carrier mobility μ. Moreover, further Ge doping induces a large enhancement of thermoelectric properties due to the combined effect of improved electrical transport properties and increased phonon scattering in the n-type Pb 1.01 Te − 0.4 % I − y % Ge. The Ge doping not only contributes to the increase of the Seebeck coefficient owing to the increased effective mass m ∗, but also gives rise to the dramatic decrease of lattice thermal conductivity due to the strengthened point defects scattering. As a result, a tremendous enhancement of the ZT...
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