• 综述 •
曾毅, 任永生, 马文会, 陈辉, 詹曙, 曹静. 冶金法生产太阳能级硅的除硼方法、技术及工艺[J]. 化学进展, 2022, 34(4): 926-949.
Yi Zeng, Yongsheng Ren, Wenhui Ma, Hui Chen, Shu Zhan, Jing Cao. Boron Removal Method, Technology and Process for Producing Solar Grade Silicon by Metallurgical Method[J]. Progress in Chemistry, 2022, 34(4): 926-949.
太阳能作为一种绿色可再生能源受到了广泛关注,而杂质去除是从冶金级硅中获得太阳能级硅所需的纯化过程,对硅基太阳能电池的制备至关重要。冶金法制备太阳能级多晶硅新工艺技术由于其能耗低、成本低和污染少等优点,成为研究开发的热点,但如何有效地去除硼是我们面临的最严峻的挑战之一。本文综述了硼的热力学和动力学性质(溶解度、扩散率、扩散系数、传质系数和活度系数)以及近年来除硼的相关课题研究(吹气、炉渣处理、等离子体处理、酸浸和溶剂精炼)。研究发现,溶剂精炼是一种很有前途的获取高纯硅的方法,硅的富集率以及硼的去除率均可达到90%以上,而添加剂能够加强硼化物的形成和析出来改进除硼工艺,且后续几乎可被完全消除,不会对精炼硅造成污染,这将更加有效除硼并增加工艺实用性。最后本文对几种除硼工艺进行了比较分析,并对冶金法的应用前景进行了展望。
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Slags (mass fraction) | D Si | DS | βSi | βS | δSi | δS | Temp. | ref |
---|---|---|---|---|---|---|---|---|
Unit | 10-8 m2·s-1 | 10-9 m2·s-1 | 10-6 m·s-1 | 10-7 m·s-1 | mm | mm | K | - |
- | 2.4±0.7 | 1687 | Kodera[ | |||||
- | 1.2 | 1687 | Garander[ | |||||
0.63Na2O-0.37SiO2 | 3.66 | 1973 | Fang et al.[ | |||||
0.4CaO-0.4SiO2-0.2MgO | 43 | 1923 | Krystad et al.[ | |||||
0.2CaO-0.6SiO2-0.1CaF2-0.1Al2O3 | 6.85 | 1.01 | 2073 | Zhang et al.[ | ||||
- | 2.1 | 1687 | Tang et al.[ | |||||
0.5CaO-0.5SiO2 | 1.46 | 170 | 31.6 | 0.086 | 1823 | Wu et al.[ | ||
0.4CaO-0.4SiO2-0.2K2CO3 | 243 | 1823 | Wu et al.[ | |||||
0.55CaO-0.45SiO2 | 14 | 1823 | Nishimoto et al.[ | |||||
0.20CaO-0.17SiO2-0.63CaCl2 | 8.46 | 250 | 0.34 | 1723 | Wang et al.[ | |||
0.37CaO-0.63SiO2 | 5.24 | 62 | 0.85 | 1723 | Wang et al.[ |
Interaction coefficients | Results | ref |
---|---|---|
240(1723 K),80±20(1723 K),73±1(1773 K) | Noguchi et al.[ | |
-0.38±0.84(1723 K) | Inoue et al.[ | |
370±140(1273 K), 120±40(1373 K), 67±20(1473 K) | Yoshikawa et al.[ | |
1313(1173 K), 970(1273 K), 610(1373 K), 400(1473 K) | Yoshikawa et al.[ | |
2506±143(1173 K) | Xu et al.[ | |
-159±45(1483 K), -111±28(1533 K), -96±12(1583 K); -164±8(1723 K), -105±8(1733 K) | Khajavi et al.[ |
Alloys | Results | ref |
---|---|---|
Si | 0.8 | Hall[ |
Si-Al | 0.22(1273 K),0.32(1373 K), 0.49(1473 K) | Yoshikawa et al.[ |
Si-17 wt% Fe | 0.07(1480 K) | Esfahani et al.[ |
Si-Sn | 0.038(1500 K, calculated) | Zhao et al.[ |
Si-34 wt% Ni | 20~65 | Yin et al.[ |
Si-20 wt% Fe Si-50 at% Cu Si-50 at% Cu+Zr | 0.33(1483 K),0.41(1533 K), 0.49(1583 K) 0.29(1345 K) 0.21(1345 K) | Khajavi et al.[ Ren et al.[ Ren et al.[ |
Authors and ref | Alloy system | B removal efficiency | P removal efficiency | Si separation method |
---|---|---|---|---|
Yoshikawa and Morita et al.[ | Si-54 wt% Al | 56→0.81 ppmw (98.6%) | 35.8→0.93 ppmw (97.4%) | Electromagnetic separation |
Obinata and Komatsu et al.[ | Si-Al | 120→20 ppmw (83.3%) | Electrolysis separation | |
Yoshikawa et al.[ | Si-54 wt% Al + Ti | 65.4→0.42 ppmw (99.4%) | - | Electromagnetic separation |
Gumaste et al.[ | Si-Al | 6→6 ppmw | 45→15 ppmw (98.6%) | Pouring+acid leaching |
Gu et al.[ | Si-Al | 8→1.55 ppmw (80.6%) | 13→0.41 ppmw(96.8%) | Pouring the residual alloy+ |
Acid leaching | ||||
Li et al.[ | 35 wt% Si-Al | 8.33→5.25 ppmw (37.0%) | 33.65→13.5 ppmw (60.0%) | Super gravity separation |
Hu et al.[ | Si-Sn | 12.1→3.3 ppmw (Si-Sn alloy) | 242.6→44.5 ppmw (Si-Sn alloy) | Super gravity separation |
Si-Al | →0.28 ppmw (Si-Al alloy) | →0.46 ppmw (Si-Al alloy) | ||
Jie et al.[ | 30 wt% Si-Al | 65→3.1 ppmw (93.4%) | 68→10.8 ppmw (81.4%) | Electromagnetic separation |
Li et al.[ | 22.8 wt% Si-Al | 14.8→3.8 ppmw (74.3%) | - | Acid leaching |
Li et al.[ | Si-63.8 wt% Al | 14.8→1.4 ppmw (90.5%) | - | Acid leaching |
Ma and Lei et al.[ | 45 wt% Si-Al | 27.9→10.8 ppmw (61.3%) | 104.9→2.5 ppmw (97.6%) | Electromagnetic separation |
+Directional solidification | ||||
Si-54 wt% Al + Zr | 65.4→0.42 ppmw (99.4%) | - | Electromagnetic separation | |
Al-46 wt% Si + Hf | 58.9→1.04 ppmw (98.2%) | - | Electromagnetic separation | |
Al-46 wt% Si + Ti | 58.9→0.46 ppmw (99.2%) | - | Electromagnetic separation | |
Esfahani et al.[ | Si-17 wt% Fe | 27→2 ppmw (92.6%) | 68→29 ppmw (57.4%) | Heavy medium |
Khajavi et al.[ | Si-Fe | (70%, at 1583 K; 65%, at 1483 K) | - | Acid leaching |
Wu et al.[ | Si-Fe | - | 378.5→17.2 ppmw (95.5%) | Acid leaching |
Luo and Huang et al.[ | Si-Cu | 3.12→1.29 ppmw (58.7%) | 17.14→9.9 ppmw (42.2%) | Acid leaching |
Si-50 wt% Cu + | 3.12→0.35 ppmw (88.8%) | 17.14→7.27 ppmw (57.8%) | Acid leaching | |
slag treatment | ||||
Si-Cu | 36→27 ppmw (25%) | 25→18 ppmw (28%) | Directional solidification | |
Li et al.[ | 30 wt% Si-Cu | 15→1 ppmw (93.3%) | 20→1 ppmw (95%) | Acid leaching |
Zhang et al.[ | Si-Sn | - | 16.1→3.77 ppmw (85.51%) | Zone melting directional |
solidification method | ||||
Li et al.[ | Si-Sn+ | 12.92→0.79 ppmw (93.9%) | - | Acid leaching |
slag treatment | ||||
Ma et al.[ | Si-Sn | 33→11.6 ppmw (64.8%) | 37→9.7 ppmw (73.8%) | Directional solidification method |
Sn-84.4 wt% Si + | 33→9.2 ppmw (75.1%) | 36.2→9.6 ppmw (73.5%) | Directional solidification method | |
slag treatment | ||||
Sn-26.2 wt% Si + | 33→0.3 ppmw (99.1%) | - | Electromagnetic separation | |
slag treatment | ||||
Hu et al.[ | Si-Sn + Ca | 10.3→3.12 ppmw (69.71%) | 108.5→28.9 ppmw (73.36%) | Super gravity separation |
Li et al.[ | Si-Al-Sn | 14.8→3.8 ppmw (74.3%) | - | Electromagnetic separation |
Si-Al-Zn | 14.8→3.8 ppmw(74.3%) | - | Acid leaching | |
Zhao et al.[ | 6 wt% Si-Sn | 15→0.1 ppmw (99.3%) | - | Acid leaching |
Lei et al.[ | Si-5wt% Zr | 52→35 ppmw (32.7%) | 51→12 ppmw (76.5%) | Acid leaching |
Morito et al.[ | Si-Na | - | 73→3.4 ppmw (95.3%) | Acid leaching |
Lai et al.[ | Si-Ca | 8.6→3 ppmw (65.1%) | 35→4 ppmw (88.6%) | Acid leaching |
Ren et al.[ | Si-50 at% Sn + Zr | 120→31.2 ppmw (73.6%) | - | Directional solidification+ Acid leaching |
Ren et al.[ | Si-50 at% Cu + Zr | 80→5.3 ppmw (93.4%) | - | Directional solidification + Acid leaching |
Chen et al.[ | Al-35at% Si + V | 73.6→35.5 ppma (76.8%) | - | Directional solidification + Acid leaching |
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