Production of aluminum alloys in electrolysis cells based on Hall-Héroult process: a review
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摘要: 現代霍爾-埃魯特(H-H)法鋁電解槽規模大、工藝成熟, 利用該法電解制備鋁基合金具有明顯技術和經濟優勢. 目前國內外研究主要是在現有氟化物熔鹽體系中添加多種合金元素氧化物, 合理調節電解質成分和工藝參數, 借助共電沉積和欠電位機制, 成功制備出多種鋁基合金, 工業化試驗亦有初步成果. 本文綜合分析了上述進展及發展前景, 并指出在實現合金組成精準調控、合金產品成分均勻化、電解槽高電流效率運行等方面存在的問題, 旨在為相關研究提供參考.Abstract: Modern large-scale Hall-Héroult (H-H) aluminum electrolysis cells have super high amperage and a well-developed process technology; thus, they present great technical and economic advantages for the production of Al-based alloys. Compared with the traditional alloy production methods, H-H-based processes have a great potential in improving product quality, simplifying production process, and reducing energy consumption. In this review, the major achievements in the production of various common aluminum alloys, such as Al-RE (rare earth metals), Al-Mg, and Al-Si/Ti alloys using H-H-based processes, were summarized from the domestic and international literature. The main properties of cryolite-based electrolyte systems that determine whether the alloy production can proceed smoothly by H-H process were first discussed based on previous research results. Studies on the electrolyte structure, melting point, and conductivity of the cryolite-based electrolytes with varying compositions were described in details. For producing Al-based alloys, the conventional fluorides electrolytes can be modified by adding various oxides of alloying metals. The electrolysis mechanisms of cathode co-deposition and underpotential deposition are usually utilized with the addition of multiple metals oxides, and the electrolyte composition and processing parameters are appropriately adjusted in H-H-based processes. Moreover, the potential distribution in the interfacial reaction processes during electrolysis for the alloying process in electrolyte is proposed based on the existing electrochemical data. In addition, some industrial trials showed promising results for the future development. At present, these trials, especially for Al-Si and Al-Ti alloys, indicate that the contents of alloying elements can be stabilized within a certain range by adjusting electrolyte compositions, current density, feeding cycle, and other parameters. There are, however, problems associated with the accurate control of alloy compositions, the homogenous quality in bulk alloy products, and the electrolysis cell operation with high current efficiency. Further research is needed to address these problems.
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圖 2 熔鹽電解鋁合金界面電化學反應過程及電勢分布示意圖
Figure 2. Schematic of the potentials in the interfacial reaction process of molten salt electrolysis for aluminum alloys
圖 3 部分合金元素氧化物以及冰晶石電解質成分的熱力學分解電壓數值與溫度的關系
Figure 3. Theoretical decomposition voltages of alloying metal oxides and cryolitic components with varying temperature
圖 4 Al-Sc合金掃描電鏡圖.(a)Sc質量分數為0.75%;(b)Sc質量分數為0.94%[18]
Figure 4. SEM micrographs of Al-Sc alloys: (a) 0.75% Sc; (b) 0.94% Sc
表 1 部分合金元素金屬氧化物在冰晶石基熔鹽體系中的溶解度
Table 1. Solubility of selected oxides of alloying metals in cryolitic melts
合金元素氧化物 冰晶石基電解質組成(質量分數/%) 溫度/℃ 溶解度/% 參考文獻 MgO 90NaF-NaCl 850 1.2 [22] NaCl-80Na3AlF6 850 1.9 [22] 17.5NaCl-NaF-40Na3AlF6 850 2.1 [22] Nd2O3 LiF-NdF3-BaF2 800~900 7~10 [23] Sc2O3 7LiF-3Al2O3-Na3AlF6(CR=2.2) 900~980 3~5 [24] (3~9)ScF3-Na3AlF6(CR=2.1) 950~990 4.01~5.68 [25] (CR=2.4~2.8)Na3AlF6-3MgF2-3CaF2-(1.5~4.5)Al2O3 960~980 1.95~4.75 [26] CeO2 5Al2O3-Na3AlF6(CR=2.7) 1040 1.65 [27] Ce2O3 6Al2O3-Na3AlF6(CR=2.7) 1000 13.6 [27] La2O3 5Al2O3-Na3AlF6(CR=2.7) 1000 14.3 [27] TiO2 3.5Al2O3-Na3AlF6 1020 5.2 [28] SiO2 Na3AlF6 1010 5 [29] CuO (1~9)Al2O3-Na3AlF6 1020 0.13~0.75 [30] Cu2O (0.4~10)Al2O3-Na3AlF6 1020 0.2~0.28 [30] 
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表 2 Al-RE金屬間化合物標準吉布斯自由能、偏摩爾吉布斯自由能以及欠沉積電位實驗值
Table 2. Experimental values of standard Gibbs free energies, partial molar Gibbs free energies of RE, and underpotential of Al-RE IMC
金屬間化合物 T/K ΔGf?/ (kJ·mol-1) $ \Delta {{\tilde G}_{{\rm{RE}}}}/\left( {{\rm{kJ}} \cdot {\rm{mo}}{{\rm{l}}^{ - 1}}} \right) $ ΔEUPD/V 參考文獻 Al3Sc 723 -150.7 -150.7 0.521 [40] 773 -145.1 -145.5 0.501 Al2Sc 723 -133.3.5 -98.4 0.340 [40] 773 -127.5 -92.4 0.319 AlSc 723 -93.2 -52.9 0.183 [40] 773 -84.1 -40.7 0.141 AlSc2 723 -108.4 -15.3 0.053 [40] 773 -105.0 -21.6 0.075 PrAl11/3 693 -180.65 -180.65 0.624 [49] 723 -179.92 -179.92 0.622 773 -177.66 -177.66 0.614 823 -174.86 -174.86 0.604 Al3Ho 673 -157.6 -157.6 0.544 [50] 723 -155.4 -155.4 0.537 773 -152.8 -152.8 0.528
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中文字幕在线观看表 3 H-H法制備鋁基合金工業化實驗數據
Table 3. Industrial experimental data of Al-based alloys prepared by Hall-Héroult based process
合金體系 電解質組成/% 溫度/℃ 電流強度/kA 槽電壓/V 合金元素質量分數/% 電流效率/% 參考文獻 Al-Ce (1~3)Ce2CO3-Al2O3-Na3AlF6(CR= 2.35~2.45) 940~950 150 4.25~4.28 5.0~5.5 — [56] Al-Mn Al2O3-Na3AlF6(CR=2.9)-MnO2 958 24 5.1 1.0~1.8 82.9 [79] Al2O3-Na3AlF6(CR=2.8~2.9)-MnO2 950 30 4.5~4.6 2.5~2.7 85 [80] Al-Ti Al2O3-Na3AlF6-(0.2~0.5)TiO2 945~955 42 4.48~4.63 0.17~0.52 72~88 [74] Al2O3-Na3AlF6-(0.23~0.25)TiO2 959~963 — 4.13 0.22~0.27 92~93 [10] Al-Si (2~2.5)Al2O3-Na3AlF6-(0.1~0.5)SiO2 960 200 4.03~4.08 ＜4.38 — [77] Al-Si-Ti Al2O3-Na3AlF6-CaF2-MgF2-(0.87~ 1.47)SiO2-(0.075~0.15)TiO2 — 60 4.5 (4~10)Si- (0.39~0.91)Ti 73.86 [81]
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