NaZn_(13)型和Ce6_Ni_2Si_3型稀土-过渡族化合物的磁性和磁热效应
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摘要
本文研究了NaZn_(13)型La(Fe, M)_(13) ( M=Si,Al )基化合物和Ce6Ni2Si3型(Tb_(1-x)Dy_x)_6Co_(1.67)Si_3化合物的磁性和磁熵变,得到的主要结果有:
1、利用磁测量和中子衍射的方法研究了La_(0.6)Pr_(0.4)Fe_(11.5)Si_(1.5)化合物的结构、磁性和磁热效应。结果表明,由于La_(0.6)Pr_(0.4)Fe_(11.5)Si_(1.5)化合物在居里温度附近存在~1.1 K的两相共存区,导致利用Maxwell关系计算所得磁熵变出现明显的尖峰。在居里温度以上发生磁场诱导的从顺磁态到铁磁态的变磁转变,变磁转变的临界磁场随温度的升高而升高。
2、研究了La_(0.5)Pr_(0.5)Fe_(11.5-x)Co_xSi_(1.5)C_(0.2) (x=0, 0.2, 0.4, 0.6和0.8)化合物的磁性和磁熵变。结果表明,Co对Fe的替代可使居里温度明显升高,消除了磁滞后,但磁熵变明显降低。
3、研究了La_(0.5)Pr_(0.5)Fe_(11.4)Si_(1.6)H_x(x=0, 0.9, 1.6)间隙化合物的结构、磁性和磁熵变。结果表明,氢原子的引入可调节居里温度至室温附近,可使变磁转变减弱,热滞后和磁滞后均明显减小,保持了大磁熵变和高制冷能力的特性。
4、利用固-固反应和气-固反应制备了La_(0.7)Pr_(0.3)Fe_(11.5)Si_(1.5)C_(0.2)H_x间隙化合物。研究了该化合物的磁性、磁滞后、磁熵变和制冷能力。结果表明,少量间隙碳的引入使磁滞损耗明显降低,磁熵变略有降低。间隙氢原子的引入可以调节居里温度至~320 K,基本消除热滞后和磁滞后,且保持了大磁熵变的特性。此外,少量碳的引入有利于间隙氢化物的制备,提高了氢化物的机械性能和热稳定性。
5、利用气-固反应制备了LaFe_(11.5)Al_(1.5)H_x和LaFe_(11.5)Al_(1.5_C_(0.2)H_x间隙氢化物,研究了它们的磁性和磁熵变。结果表明,当x=1.3时,LaFe_(11.5)Al_(1.5)H_x化合物的居里温度达到295K,具有明显的二级相变特征,在0-5T磁场变化下,最大磁熵变和制冷能力分别达到12.3 J·kg~(-1) K~(-1)和387 J·kg~(-1)。LaFe_(11.5)Al_(1.5)C_(0.2)H_(1.0)化合物在0-5 T磁场变化下的最大磁熵变为_(13).8 J·kg~(-1)·K~(-1),比金属Gd高出~ 40%,并在623 K以下仍能保持良好的热稳定性。
6、合成了(Tb_(1-x)Dy-x)_6Co_(1.67)Si_3(x=0, 0.2, 0.4, 0.6, 0.8)化合物,分析了Dy替代Tb对磁性和磁熵变的影响。结果表明,(Tb_(1-x)Dy_x)_6Co_(1.67)Si_3化合物存在多个相变(TC、TSR、T1和T2),随着Dy含量的增加,居里温度线性降低,磁熵变略有减小。替代前后,均具有很高的制冷能力,具有很大的应用潜力。
The structure, magnetism, magnetic transition, magnetic entropy change, magnetic hysteresis, and refrigeration capacity of La(Fe,M)_(13) (M=Si,Al) and (Tb_(1-x)Dy_x_6Co_(1.67)Si_3 compounds, were systematically studied in present paper. The main results are as follows:
1. The structure, magnetism, and magnetic entropy change of La_(0.6)Pr_(0.4)Fe_(11.5)Si_(1.5) compound were studied utilizing magnetic measurement and neutron diffraction method. It is found that the coexistent phase area about 1.1K for Pr_(0.4)La_(0.6)Fe_(11.5)Si_(1.5), measured with temperature cooling or heating, results in the false peak of magnetic entropy. The magnetic field induced metamagnetic transition takes place above Curie temperature. And the critical field grows up with increasing temperature.
2. The substitution of Co for Fe strengthens the exchange interaction among T-T in La_(0.5)Pr_(0.5)Fe_(11.5-x)Co_xSi_(1.5)C_(0.2) compounds, and leads to the Curie temperature increasing obviously. Large magnetic entropy and efficient refrigeration capacity are retained. A little bit of Co can eliminate the magnetic hysteresis and drive the magnetic phase transition from first-order to second-order.
3. Magnetic properties and magnetic entropy changes have been investigated in La_(0.5)Pr_(0.5)Fe_(11.4)Si_(1.6)H_x (x=0, 0.9, 1.6) hydrides. It is found that the Curie temperature can be tuned to room temperature by adjusting hydrogen content. It is attractive that both thermal and magnetic hysteresis are remarkably reduced because of the weakness of the itinerant-electron metamagnetic transition after hydrogenation, while the large magnetic entropy change and considerable RC are retained.
4. La_(0.7)Pr_(0.3)Fe_(11.5)Si_(1.5)C_(0.2)H_x (x=0, 0.6, 1.2) compounds were successfully prepared by solid-solid and gas-solid phase reactions. The structure, magnetism, magnetic entropy change, magnetic hysteresis, and refrigeration capacity of La_(0.7)Pr_(0.3)Fe_(11.5_Si_(1.5)C_(0.2)H_x were studied. It is found that small content carbon introducing can not sacrifice the large magnetic entropy, while the maximal hysteresis loss at TC decreases remarkably. The Curie temperature TC can be tuned to ~320 K by the following introduction of interstitial hydrogen. It is attractive that both thermal and magnetic hysteresis are eliminated after hydrogenation,while the large magnetic entropy change is retained. Moreover, the introduction of a small content of carbon is benefit to the following preparation of hydride and improved the mechanical performance and the thermostability.
5. The LaFe_(11.5)Al_(1.5)H_x and LaFe_(11.5)Al_(1.5)C_(0.2)H_x compounds were prepared by gas-solid phase reaction, and the magnetism and magnetic entropy change were well studied. The Curie temperature TC can be tuned to 295 K for LaFe_(11.5)Al_(1.5)H_x compounds by the introduction of interstitial hydrogen (x=1.3). It is obvious that LaFe_(11.5)Al_(1.5)H_(1.3) compound shows the second-order transition feature. The maximal values of -ΔS for LaFe_(11.5)Al_(1.5)H_(1.3) compound is 12.3 J·kg~(-1) K~(-1) at TC for a field change of 0-5 T. The maximal values of -ΔS for LaFe_(11.5)Al_(1.5)C_(0.2)H_(1.0) compound is _(13).8 J·kg~(-1) K~(-1) at TC for a field change of 0-5 T, which is ~ 40% higher than that of Gd. Moreover, the LaFe_(11.5)Al_(1.5)C_(0.2)H_(1.0) compound is stable even at 623 K.
6. The magnetic and magnetocaloric properties of (Tb_(1-x)Dy_x)_6Co_(1.67)Si_3 (x=0, 0.2, 0.4, 0.6, and 0.8) have been experimentally investigated. The compounds undergo multiple second-order magnetic transitions. The Curie temperature decreases linearly as the content of Dy grows from 0 to 0.8. The maximal magnetic entropy change slightly decreases when Dy is introduced. Large refrigeration capacity (RC) value are achieved for (Tb_(1-x)Dy_x)_6Co_(1.67)Si_3 (x=0, 0.2, 0.4, 0.6, 0.8) compounds under a field change of 0-5 T, which is benefit for application.
1、利用磁测量和中子衍射的方法研究了La_(0.6)Pr_(0.4)Fe_(11.5)Si_(1.5)化合物的结构、磁性和磁热效应。结果表明,由于La_(0.6)Pr_(0.4)Fe_(11.5)Si_(1.5)化合物在居里温度附近存在~1.1 K的两相共存区,导致利用Maxwell关系计算所得磁熵变出现明显的尖峰。在居里温度以上发生磁场诱导的从顺磁态到铁磁态的变磁转变,变磁转变的临界磁场随温度的升高而升高。
2、研究了La_(0.5)Pr_(0.5)Fe_(11.5-x)Co_xSi_(1.5)C_(0.2) (x=0, 0.2, 0.4, 0.6和0.8)化合物的磁性和磁熵变。结果表明,Co对Fe的替代可使居里温度明显升高,消除了磁滞后,但磁熵变明显降低。
3、研究了La_(0.5)Pr_(0.5)Fe_(11.4)Si_(1.6)H_x(x=0, 0.9, 1.6)间隙化合物的结构、磁性和磁熵变。结果表明,氢原子的引入可调节居里温度至室温附近,可使变磁转变减弱,热滞后和磁滞后均明显减小,保持了大磁熵变和高制冷能力的特性。
4、利用固-固反应和气-固反应制备了La_(0.7)Pr_(0.3)Fe_(11.5)Si_(1.5)C_(0.2)H_x间隙化合物。研究了该化合物的磁性、磁滞后、磁熵变和制冷能力。结果表明,少量间隙碳的引入使磁滞损耗明显降低,磁熵变略有降低。间隙氢原子的引入可以调节居里温度至~320 K,基本消除热滞后和磁滞后,且保持了大磁熵变的特性。此外,少量碳的引入有利于间隙氢化物的制备,提高了氢化物的机械性能和热稳定性。
5、利用气-固反应制备了LaFe_(11.5)Al_(1.5)H_x和LaFe_(11.5)Al_(1.5_C_(0.2)H_x间隙氢化物,研究了它们的磁性和磁熵变。结果表明,当x=1.3时,LaFe_(11.5)Al_(1.5)H_x化合物的居里温度达到295K,具有明显的二级相变特征,在0-5T磁场变化下,最大磁熵变和制冷能力分别达到12.3 J·kg~(-1) K~(-1)和387 J·kg~(-1)。LaFe_(11.5)Al_(1.5)C_(0.2)H_(1.0)化合物在0-5 T磁场变化下的最大磁熵变为_(13).8 J·kg~(-1)·K~(-1),比金属Gd高出~ 40%,并在623 K以下仍能保持良好的热稳定性。
6、合成了(Tb_(1-x)Dy-x)_6Co_(1.67)Si_3(x=0, 0.2, 0.4, 0.6, 0.8)化合物,分析了Dy替代Tb对磁性和磁熵变的影响。结果表明,(Tb_(1-x)Dy_x)_6Co_(1.67)Si_3化合物存在多个相变(TC、TSR、T1和T2),随着Dy含量的增加,居里温度线性降低,磁熵变略有减小。替代前后,均具有很高的制冷能力,具有很大的应用潜力。
The structure, magnetism, magnetic transition, magnetic entropy change, magnetic hysteresis, and refrigeration capacity of La(Fe,M)_(13) (M=Si,Al) and (Tb_(1-x)Dy_x_6Co_(1.67)Si_3 compounds, were systematically studied in present paper. The main results are as follows:
1. The structure, magnetism, and magnetic entropy change of La_(0.6)Pr_(0.4)Fe_(11.5)Si_(1.5) compound were studied utilizing magnetic measurement and neutron diffraction method. It is found that the coexistent phase area about 1.1K for Pr_(0.4)La_(0.6)Fe_(11.5)Si_(1.5), measured with temperature cooling or heating, results in the false peak of magnetic entropy. The magnetic field induced metamagnetic transition takes place above Curie temperature. And the critical field grows up with increasing temperature.
2. The substitution of Co for Fe strengthens the exchange interaction among T-T in La_(0.5)Pr_(0.5)Fe_(11.5-x)Co_xSi_(1.5)C_(0.2) compounds, and leads to the Curie temperature increasing obviously. Large magnetic entropy and efficient refrigeration capacity are retained. A little bit of Co can eliminate the magnetic hysteresis and drive the magnetic phase transition from first-order to second-order.
3. Magnetic properties and magnetic entropy changes have been investigated in La_(0.5)Pr_(0.5)Fe_(11.4)Si_(1.6)H_x (x=0, 0.9, 1.6) hydrides. It is found that the Curie temperature can be tuned to room temperature by adjusting hydrogen content. It is attractive that both thermal and magnetic hysteresis are remarkably reduced because of the weakness of the itinerant-electron metamagnetic transition after hydrogenation, while the large magnetic entropy change and considerable RC are retained.
4. La_(0.7)Pr_(0.3)Fe_(11.5)Si_(1.5)C_(0.2)H_x (x=0, 0.6, 1.2) compounds were successfully prepared by solid-solid and gas-solid phase reactions. The structure, magnetism, magnetic entropy change, magnetic hysteresis, and refrigeration capacity of La_(0.7)Pr_(0.3)Fe_(11.5_Si_(1.5)C_(0.2)H_x were studied. It is found that small content carbon introducing can not sacrifice the large magnetic entropy, while the maximal hysteresis loss at TC decreases remarkably. The Curie temperature TC can be tuned to ~320 K by the following introduction of interstitial hydrogen. It is attractive that both thermal and magnetic hysteresis are eliminated after hydrogenation,while the large magnetic entropy change is retained. Moreover, the introduction of a small content of carbon is benefit to the following preparation of hydride and improved the mechanical performance and the thermostability.
5. The LaFe_(11.5)Al_(1.5)H_x and LaFe_(11.5)Al_(1.5)C_(0.2)H_x compounds were prepared by gas-solid phase reaction, and the magnetism and magnetic entropy change were well studied. The Curie temperature TC can be tuned to 295 K for LaFe_(11.5)Al_(1.5)H_x compounds by the introduction of interstitial hydrogen (x=1.3). It is obvious that LaFe_(11.5)Al_(1.5)H_(1.3) compound shows the second-order transition feature. The maximal values of -ΔS for LaFe_(11.5)Al_(1.5)H_(1.3) compound is 12.3 J·kg~(-1) K~(-1) at TC for a field change of 0-5 T. The maximal values of -ΔS for LaFe_(11.5)Al_(1.5)C_(0.2)H_(1.0) compound is _(13).8 J·kg~(-1) K~(-1) at TC for a field change of 0-5 T, which is ~ 40% higher than that of Gd. Moreover, the LaFe_(11.5)Al_(1.5)C_(0.2)H_(1.0) compound is stable even at 623 K.
6. The magnetic and magnetocaloric properties of (Tb_(1-x)Dy_x)_6Co_(1.67)Si_3 (x=0, 0.2, 0.4, 0.6, and 0.8) have been experimentally investigated. The compounds undergo multiple second-order magnetic transitions. The Curie temperature decreases linearly as the content of Dy grows from 0 to 0.8. The maximal magnetic entropy change slightly decreases when Dy is introduced. Large refrigeration capacity (RC) value are achieved for (Tb_(1-x)Dy_x)_6Co_(1.67)Si_3 (x=0, 0.2, 0.4, 0.6, 0.8) compounds under a field change of 0-5 T, which is benefit for application.
引文
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