Journal of Materiomics
·
2023
·
IF 9.4
Jie Song,Peng Luo,Hailong Sun,Hezhang Li,Chao Wang,Yi Niu,Jing Jiang
Thermoelectric materials are competitive candidates for special cooling applications. Mg 3 Sb 2 -based materials consisting of inexpensive ingredients have profound thermoelectric properties. At present, alloying with Mg 3 Bi 2 is the most effective approach to optimize the thermoelectric properties of Mg 3 Sb 2 -based materials. However, the extremely low abundance of bismuth in the crust contradicts its economic expectation. In this work, the ZrO 2 micro-particles were separated into the Mg 3.2 Sb 1.99 Te 0.01 . The doping effect of Zr atoms at Mg sites increased the electrical conductivity, and the combined secondary phase lowered the lattice thermal conductivity. With acceptable degradation in the Seebeck coefficient, the sample combined with 5% (in mass) ZrO 2 exhibited a dimensionless figure of merit ( zT ) of 0.49 and a power factor of 2.7 mW·m −1 ·K −2 near room temperature. The average zT in the range from 300 K to 500 K reached 0.8, on par with the Mg 3 Sb 2 Mg 3 Bi 2 alloys. Besides, the compressive and bending strengths reach 669 MPa and 269 MPa, respectively, far superior to the common room-temperature thermoelectrics. This secondary phase showed a surprising and uncostly promotion of the Mg 3 Sb 2 -based thermoelectric materials, impelling the realization of its commercial application.
研究领域:
材料科学
·
物理学
✓ 已验证
DOI
高影响因子
Materials Today Physics
·
2020
·
IF 10.443
Juan Li,Shuai Zhang,Fei Jia,Shuqi Zheng,Xiaolei Shi,Daqiang Jiang,Siyu Wang,Guiwu Lu,Liming Wu,Zhi-Gang Chen
Approaching practical thermoelectric devices require high-performance and machinable thermoelectric materials . However, the currently available materials are usually brittle. In this work, Nd-doped Mg 3 Sb 2 -based compounds exhibit not only excellent thermoelectric performance but also superior machinability . Mg 3.2 Nd 0.03 Sb 1.5 Bi 0.5 exhibits a high power factor of 20.6 μW cm −1 K −2 at 725 K and a peak zT of 1.8, which mainly originates from the increased n of ~8 × 10 19 cm −3 by Nd/Mg substitutional defects. Defect calculations predict that other rare earth elements (Sm, Gd, Tb, Dy and Ho) have the same effect as Nd on Mg 3 Sb 2 and the predicted highest achievable electron concentrations at 700 K are ~10 20 cm −3 . The measured hardness, Young's modulus and fracture toughness of Mg 3.2 Nd 0.03 Sb 1.5 Bi 0.5 are 1.1 GPa, 49.8 GPa and 1.4 MPa m 1/2 , respectively. In addition, the sample can be easily machined into the dog-bone shape with external thread at both ends, indicating the excellent machinability of Mg 3 Sb 2 -based materials. This work suggests a bright future of Mg 3 Sb 2 -based thermoelectric materials for practical applications and device fabrication .
研究领域:
材料科学
·
热电材料研究
✓ 已验证
产品关联
DOI
高影响因子
ChemNanoMat
·
2022
·Vol. 9
·期 1
·e202200400
·
IF 3.82
Bo Zhu,Xu Lu,Jiadang Li,Wenhao Xie,Lifei Wang,Qiang Zhang,Jianfeng Fan,Yun Zheng
Graphical The substitution of iso-valent Bi for Sb is adopted to adjust the thermoelectric transport properties of the undoped Mg 3 Sb 2 compound. The improved power factor and figure of merit are obtained accordingly. Bismuth is the most common alloying element for high-performance Mg 3 Sb 2 -based thermoelectric compounds. However, the electrical and thermal transport data is lacking for undoped Mg 3 (Sb, Bi) 2 solid solutions. In this study, theoretical calculation results show that Bi alloying can reduce the band gap of Mg 3 Sb 2 , favoring the regulation of carrier concentration. Both Mg 3 Sb 2 and Mg 3 SbBi compounds present a single band structure on the valence band maximum at Γ of the Brillouin zone. Incorporating the Bi element can slightly increase the density of states (DOS) on the valence band maximum, which is beneficial for the Seebeck coefficient. Mg 3 Sb 2-x Bi x (0≤x≤0.8) compounds were experimentally prepared via ball milling (BM) combined with the spark plasma sintering (SPS) technique. The carrier concentration, electrical conductivity, and power factor of the samples tend to increase with the increasing Bi content. Bismuth alloying significantly reduces the total thermal conductivity in the low-temperature range, with the lowest value of 0.65 Wm −1 K −1 obtained at ∼400 K for the x=0.2 sample. The peak ZT value of 0.077 at 800 K and the average ZT of 0.051 in the temperature range of 450–800 K are obtained for the x=0.2 sample, which is 93% and 219% higher than those of the unalloyed sample, respectively. This work reveals the Bi-alloying induced transport mechanism and provides fundamental thermoelectric data regarding the undoped Mg 3 Sb 2-x Bi x (0≤x≤0.8) solid solutions.
研究领域:
材料科学
·
物理学
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF MATERIALS SCIENCE & TECHNOLOGY
·
2023
·
IF 10.9
Yi-bo Zhang,Ji-Sheng Liang,Chengyan Liu,Qi Zhou,Zhe Xu,Hong-bo Chen,Fu-cong Li,Ying Peng,Lei Miao
P-type Mg 3 Sb 2 -based Zintls have attracted considerable interest in the thermoelectric (TE) field due to their environmental friendliness and low cost. However, compared to their n-type counterparts, they show relatively low TE performance, limiting their application in TE devices. In this work, we simultaneously introduce Bi alloying at Sb sites and Ag doping at Mg sites into the Mg 3 Sb 2 to cooperatively optimize the electrical and thermal properties for the first time, acquiring the highest ZT value of ∼0.85 at 723 K and a high average ZT of 0.39 in the temperature range of 323–723 K in sample Mg 2.94 Ag 0.06 Sb 1.9 Bi 0.1 . The first-principle calculations show that the co-doping of Ag and Bi can shift the Fermi level into the valence band and narrow the band gap, resulting in the increased carrier concentration from 3.50 × 10 17 cm −3 in the reference Mg 3 Sb 0.9 Bi 0.1 to ∼7.88 × 10 19 cm −3 in sample Mg 2.94 Ag 0.06 Sb 0.9 Bi 0.1 . As a result, a remarkable power factor of ∼778.9 µW m − 1 K − 2 at 723 K is achieved in sample Mg 2.94 Ag 0.06 Sb 0.9 Bi 0.1 . Meanwhile, a low lattice thermal conductivity of ∼0.48 W m − 1 K − 1 at 723 K is also obtained with the help of phonon scattering at the distorted lattice, point defects, and nano-precipitates in sample Mg 2.94 Ag 0.06 Sb 0.9 Bi 0.1 . The synergistic effect of using the multi-element co-doping/-alloying to optimize electrical properties in Mg 3 Sb 2 holds promise for further improving the TE performance of Zintl phase materials or even others.
研究领域:
材料科学
·
能源科学
✓ 已验证
DOI
高影响因子
JOURNAL OF MATERIALS SCIENCE
·
2018
·Vol. 53
·期 11
·8039-8048
·
IF 2.993
Lv Feng,Zhang Qiang,Fan Wenhao,Yang Xiaomeng,Fan Jianfeng,Zhang Hua,Chen Shaoping,Wang Wenxian,Tang Xinfeng
Mg 3 Sb 2 compounds were synthesized via low-temperature solid-state reaction (SSR) and ball milling (BM), respectively, followed by spark plasma sintering (SPS) process. The effects of possible sintering pressure-induced orientation in the SPS process have been investigated in terms of the microstructure and thermoelectric transport properties. The results indicate that BM technique causes more severe Mg loss than pure SSR method, leading to distinct Sb phase existing in the product after SPS consolidation process. On the contrary, a single phase of Mg 3 Sb 2 is easily obtained with the combination of SSR and SPS techniques. Besides, these BM–SPS and SSR–SPS samples exhibit the similar microstructure as well as the same electrical and thermal transport properties parallel or perpendicular to the direction of sintering pressure. The study suggests that SSR method embodies the advantages of both the composition control and the orientation elimination in Mg 3 Sb 2 compound as compared to BM method with the specific parameters in the current work. This investigation is quite favorable for this material fabrication and the future application of thermoelectric modules and devices.
研究领域:
材料科学
·
热电材料
✓ 已验证
产品关联
DOI
高影响因子
ACS Applied Materials & Interfaces
·
2020
·
IF 8.758
Jisheng Liang,Hengquan Yang,Chengyan Liu,Lei Miao,Junliang Chen,Sijing Zhu,Zhengchuan Xie,Wenjing Xu,Xiaoyang Wang,Jun Wang,Biaolin Peng,Kunihito Koumoto
Mg3Sb2-based compounds by virtue of nontoxicity and low-cost have become a promising class of candidates for midtemperature thermoelectric power generation. Here, we successfully fabricated n-type Mg3Sb2-based materials using an inexpensive and efficient approach of one-step ball milling and spark plasma sintering, and demonstrate that a complementary and favorable effect of multiple elements coalloying/-doping leads to an excellent thermoelectric performance. The intrinsic p-type conducting behavior for Mg3Sb2 could be changed to n-type through Bi and Se coalloying on Sb sublattices with excess Mg, resulting from the suppression of Mg vacancies and the formation of Mg interstitial. Furthermore, Mn doping on Mg sublattices could soften the chemical bonds, leading to the increase of carrier mobility and concentration simultaneously. Additionally, multielement coalloying/-doping could significantly increase the lattice disorder, which undoubtedly strengthens the phonon scattering and readily results in a suppressed lattice thermal conductivity. As a result, a highest ZT value of 1.6 at 723 K and an average ZT value up to 1.1 were obtained in the temperature range of 323–723 K in the Mg3.18Mn0.02Sb1.5Bi0.49Se0.01 sample, which is one of the highest values among the Te free Mg3Sb2. This work could give guidance for improving the thermoelectric performance of Zintl phase materials or even others using the multielement codoping/-alloying strategy.
研究领域:
材料科学
·
能源工程
✓ 已验证
DOI
PubMed
高影响因子
PHYSICAL CHEMISTRY CHEMICAL PHYSICS
·
2022
·Vol. 24
·期 45
·27812-27818
·
IF 3.945
Juan Li,Fei Jia,Kai Han,Bing Sun,Lianzhen Cao,Yingde Li,Shuai Zhang
Experimental results show an intriguing phenomenon that although Bi and Sb have the same number of valence electrons, Bi/Sb substitution increases the electron concentration of n-type Mg3Sb2-based materials. Using a combination of theoretical calculations and experimental synthesis, this work reveals the physical mechanism of the effect of Bi doping on carrier concentration. The increase in electron concentration mainly originates from the enhanced degree of ionization of donor impurity because of the decrease of conductivity effective mass and increase of dielectric constant caused by the narrowing of bandgap with Bi doping. Based on the collaborative optimization of the electrical and thermal transports, n-type Mg3.175Mn0.025Sb1.48Bi0.48Te0.04 exhibits the best thermoelectric performance with a peak zT of 1.85 at 725 K and an average zT of 1.21. This work demonstrates an effective strategy of bandgap engineering for the optimization of carrier concentration and provides insightful guidance for designing other thermoelectric materials.
研究领域:
材料科学
·
凝聚态物理
✓ 已验证
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2024
·
IF 13.3
Zhe Xu,Xiao-Lei Shi,Yibo Zhang,Jisheng Liang,Meng Li,Chengyan Liu,Lei Miao,Siqi Liu,Shihao Wang,Qi Zhou,Jie Gao,Zhongwei Zhang,Wei-Di Liu,Ying Peng,Jun-Liang Chen,Zhi-Gang Chen
Owing to the non-toxicity and low cost, Mg 3 Sb 2 -based Zintls are promising candidates for mid-temperature thermoelectric applications. However, the thermoelectric performance of p-type Mg 3 Sb 2 is significantly lower than that of n-type ones. Here, we achieve simultaneous optimization of the band structure and enhanced phonon scattering through the combined doping of Na at the cation site and Bi at the anion site, leading to a competitive figure of merit, ZT of 0.73 at 773 K and a maximum theoretical energy conversion efficiency of 6.5 % at a temperature difference of 450 K. First-principles calculations indicate that Na and Bi co-doping effectively narrows the band gap and shifts the Fermi level into the valence band, thereby increasing the hole carrier concentration. This ensures a relatively high Seebeck coefficient and improved electrical conductivity, resulting in an excellent power factor of 7.5 µW cm −1 K −2 . Additionally, by adjusting the amount of Bi nanoprecipitates in the matrix, the heterogeneous interfaces significantly enhance phonon scattering and markedly reduce the lattice thermal conductivity (0.52 W m −1 K −1 ), collectively leading to the high thermoelectric performance. Furthermore, by pairing n-type Mg 3.18 Y 0.02 Sb 1.5 Bi 0.49 Se 0.01 , a double-leg thermoelectric device achieves an energy conversion efficiency of 4.1 % with a temperature difference of 390 K.
研究领域:
材料科学
·
热电材料
✓ 已验证
DOI
高影响因子
PHYSICAL CHEMISTRY CHEMICAL PHYSICS
·
2020
·Vol. 22
·期 13
·7012-7020
·
IF 3.43
Qiang Zhang,Jichong Hou,Jianfeng Fan,Shaoping Chen,Wenhao Fan,Hua Zhang,Wenxian Wang,Yucheng Wu,Bingshe Xu
This work reports the electrical and thermal transport processes in p-type Pb-doped Mg3(1+x)Sb2−yPby (0.02 ≤ x ≤ 0.08; 0 ≤ y ≤ 0.02) compounds. Low-energy electron acceptor defects Mg vacancies are easy to form, which can provide holes and make p-type transport in the Mg3Sb2 matrix. However, with an increase in excess Mg, the transport behavior changes from p type to n type as manifested synergistically by both the Hall coefficient and Seebeck coefficient. This indicates the effective role of Mg in tuning carrier type and concentration for a pristine Mg3Sb2 compound. Upon substitution of Sb by Pb, the hole concentration slightly increases, and mobility is greatly improved by 133% at room temperature. The significant increase in mobility is attributed to the weakening ionized impurity scattering, stemming from the decreasing concentration induced by Pb doping. Thus, the power factor is enhanced with a 146% improvement at room temperature. Consequently, the figure of merit ZT of the Pb-doped sample is 1.8 times larger than the pristine one at around 300 K. Moreover, the non-degenerate transport behavior revealed by electrical properties is simply analyzed regarding the effects of minority carriers on the overall Seebeck coefficient. This study proposes a new strategy of charge compensation for improving mobility and a simple way to guide the prediction about the onset of bipolar conduction for Mg3Sb2-based compounds and other potential thermoelectric materials.
研究领域:
材料科学
·
热电学
✓ 已验证
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2022
·
IF 16.744
Yu Jiang,Marhoun Ferhat,Wenhao Fan,Shaoping Chen,Yachao Wang,Jie Chen,Rasha Abdullah Ahmed Al-Yusufi,Chaochao Dun
Additional cation doping is one of the potential strategies to enhance the thermoelectric (TE) performance of Mg 3 Sb 2 -based materials with precise regulation of interaction between cations and the host. In this work, using Mg 3 Sb 1.5 Bi 0.5 as an example, we confirmed that co-doping rare-earth elements with Y and La is capable to simultaneously improve its power factor and suppress the thermal conductivity : Y is an effective n -type dopant to regulate the optimal carrier concentration, while La doping can modulate the band structure and increase the effective mass that related to the improved Seebeck coefficient . A promising power factor of 18.3 μW cm -1 K -2 is obtained after co-doping. Meanwhile, the lattice thermal conductivity is dramatically reduced to 0.39 W m -1 K -1 at 750 K thanks to the extra defect scattering introduced by Y and La. As a result, a peak figure of merit ( zT ) of 1.76 and a competitive average zT of 1.1 among 300–750 K are achieved in Mg 3.2 Y 0.04 La 0.01 Sb 1.5 Bi 0.5 . The synergistic effect stemming from dual-cations doping provides profound insights for controllable host-dopant design and modulation toward high-efficient n-type TE materials .
研究领域:
材料科学
·
物理学
✓ 已验证
产品关联
DOI
高影响因子
Journal of Materials Chemistry A
·
2021
·Vol. 9
·期 46
·25944-25953
·
IF 12.732
Jingdan Lei,Hexige Wuliji,Kunpeng Zhao,Tian-Ran Wei,Qing Xu,Peng Li,Pengfei Qiu,Xun Shi
Mg3Sb2-based thermoelectric materials have recently received heightened attention due to their diverse merits of high band degeneracy, ultralow lattice thermal conductivity and high carrier mobility. However, the inherently low carrier concentration of pristine Mg3Sb2 seriously hinders the advancement of this material toward high thermoelectric performance. Therefore, searching for proper dopants to optimize the carrier concentration is one of the primary avenues to realize superior thermoelectric performance in Mg3Sb2-based materials. Herein, by considering the electronegativity difference Δχ and mass difference ΔM between the dopant and host elements, we theoretically and experimentally demonstrate lanthanide Gd as an effective dopant to tune the carrier concentration of Mg3Sb1.3Bi0.7 alloys. Owing to its high doping efficiency, a large carrier concentration up to 8.9 × 1019 cm−3 is realized through Gd doping, which is close to the optimal value. Moreover, the coarse grain size commendably mitigates the grain boundary effects and thus ensures high carrier mobility. Combining the greatly suppressed lattice thermal conductivity by point defect scattering, a maximum zT of 1.55 is achieved at 700 K in Mg3.065Sb1.3Bi0.7Gd0.015.
研究领域:
材料科学
·
热电学
·
能量转换
·
固体物理
✓ 已验证
DOI
高影响因子
JOURNAL OF MATERIALS SCIENCE-MATERIALS IN ELECTRONICS
·
2026
·Vol. 37
·期 14
·1093
·
IF 3.2
Ren Peifeng,Gao Xingchen,Fan Wenhao,Zhang Qiang,Chen Shaoping,Fan Jianfeng
Elemental doping plays a crucial role in optimizing carrier concentration and suppressing lattice thermal conductivity in thermoelectric materials. In this study, Cu atoms were doped in both n- and p-type Mg 3 Sb 2 -based thermoelectric compounds. The results indicate that the incorporation of Cu effectively improves the electrical transport properties of Mg 3 Sb 2 -based thermoelectric compounds while simultaneously suppressing their thermal transport, ultimately achieving enhanced thermoelectric properties: (a) For p-type Mg 3 Sb 2 , a small quantity of Cu atoms provides electrons in the lattice interstitial and thus compensates holes, leading to a decreased carrier concentration and electrical conductivity. However, with increasing Cu content, Cu atoms preferentially occupy Mg2 sites, thereby increasing hole concentration, and thus improving electrical conductivity. Further increasing Cu content, an MgCuSb secondary phase forms, which is unfavorable for overall p-type thermoelectric performance of the Mg 3 Sb 2 -based matrix due to the n-type transport of the MgCuSb compound. (b) For n-type Mg 3 Sb 2 , no such secondary phase was observed despite the same Cu-doping content, which involves a distinct doping mechanism from the p-type one. Consequently, the zT values of p-type Mg 3 Sb 2 materials are improved by 17%–33% over the whole temperature range. And regarding the n-type Mg 3 Sb 2 materials, the highest peak zT value of ~1.4 and average zT avg of ~1.04 are achieved. Therefore, the doping of the Cu element proves to be an effective way in optimizing thermoelectric properties of both p-type and n-type Mg 3 Sb 2 -based materials.
✓ 已验证
DOI
高影响因子
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