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摘要: 回顧了我國微生物浸出技術發展的歷史進程, 總結了我國開展生物浸銅技術的探索與應用進程, 介紹了紫金山銅礦、德興銅礦兩個典型的生物浸銅案例; 探討了浸礦細菌分離、鑒定與富集, 生物浸出機理與界面反應, 浸出體系多級滲流行為, 孔隙結構重構與定量化, 浸出體系多場耦合與過程模擬, 電子廢棄物中的銅金屬回收領域的主要進展.最后, 結合生物浸銅技術的當前進展, 闡述了生物浸銅技術面臨的環保、安全等方面的挑戰與未來發展趨勢, 為今后該領域的研究提供良好借鑒.Abstract: Mineral resources are the mainstay industries supporting the development of the national economy. Due to its excellent ductility, electrical and thermal conductivity, copper is widely used in construction, power, transportation, and manufacturing as an important strategic metal resource. According to statistics, in terms of output and consumption of ten kinds of non-ferrous metals such as copper, aluminum, and zinc, China has ranked first in the world for more than ten consecutive years. China's copper resources are poorly endowed, being low grade, highly ore-deficient, and of poor ore floatability; the use of conventional separation methods has been costly and caused serious environmental pollution due to difficulties with residue disposal. Bioleaching is a special mining technology that leaches and yields valuable metal elements from inside ores using leaching bacteria. Copper metal resources inside low-grade ores, waste ores, and boundary ores are recycled efficiently using bioleaching technology, which is efficient, and both environmentally-friendly and economical. Currently, more than a quarter of the world's copper production depends on this technology. However, the microbial copper leaching process has always been regarded as a "black box", being difficult to effectively monitor and regulate. This paper reviews the history of bioleaching technology in China, reviews those copper mines that have carried out exploration into or application of bioleaching technology, and introduces two typical copper bioleaching industrial cases, the Zijinshan and Dexing Copper Mines. This paper explores (a) the main process of isolation, identification and enrichment of leaching bacteria, (b) the bioleaching mechanism and interface reaction, (c) the multistage seepage behavior of leaching systems, (d) the reconstruction and quantification of pore structures, (e) the multi-field coupling and process simulation of leaching systems, and (f) copper metal recycling from waste printed circuit boards. Finally, along with the current status of copper bioleaching, major challenges such as environmental protection, security, and future trends in copper bioleaching are discussed as a basis for further research.
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Key words:
- solution mining /
- bioleaching /
- ore heap leaching /
- solution seepage /
- pore evolution
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圖 3 低品位銅礦微生物浸出的工業化流程(以堆浸為例)
Figure 3. Industrial process of low-grade copper bioleaching (heap leaching)
圖 5 浸礦過程中的界面反應與吸附菌的原子力顯微圖像[84-85]. (a) 浸礦系統中細菌-礦物相互作用; (b) 基于原子力顯微鏡的礦物與細菌微觀形貌
Figure 5. Interface reaction and AFM micro images of attached bacteria during leaching process[84-85]: (a) interaction effect of bacteria-mineral inside ore leaching system; (b) micro morphology of minerals and bacterial based on atomic force microscope
圖 6 云南某氧化銅礦浸堆嚴重的板結及鈍化現象. (a) 礦堆低滲透性；(b) 礦堆板結及鈍化現象
Figure 6. Severe curing and passivation phenomena in heaps of copper oxide ores, Yunnan Province: (a) low perimiability of ore heap; (b) heap compaction and passivation phenomenon
圖 8 基于COMSOL Multiphysics的雙重孔隙結構內優先流路徑模擬[108]. (a) 單孔隙度模型; (b) 微孔網絡滲透率5.18×10-11 mm2; (c) 微孔網絡滲透率8.54×10-10 mm2
Figure 8. Simulation of preferential flow pathways inside dual pore structures using COMSOL Multiphysics[108]: (a) single macro porosity model; (b) micro-pore network permeability is 5.18×10-11 mm2; (c) micro-pore network permeability is 8.54×10-10 mm2
表 1 我國低品位銅礦微生物浸出技術的主要探索與應用(不完全統計)
Table 1. Exploration and successful industrial cases of low-grade copper bioleaching in China (incomplete statistics)
礦山名稱 地點 礦物特征 主要特點 德興銅礦[34] 江西，德興 Cu 0.30%(質量分數，下同)，原生硫化銅為主 始建于1965年，自1979年開始使用生物浸出技術，1997年建成生物廢石浸出廠，銅浸出率30%，年產陰極銅2000 t 羊拉銅礦[35] 云南，迪慶 Cu 1.01% (氧化銅為主，孔雀石0.36%, 硅孔雀石0.29%, 輝銅礦0.29%) 利用Providencia sp. JAT-1開展堿性細菌浸礦研究; 初始pH值8，初始溫度為30 ℃，浸礦156 h后銅浸出率達54.5% 紫金山銅礦[36-37] 福建，上杭 低品位硫化銅礦為主，Cu 0.38% 采用萃取-電積生物堆浸技術，2006年，建成年產銅礦20000 t堆浸廠 官房銅礦[38] 云南，臨滄 次生硫化銅礦為主，Cu 0.9% 2003年建成生物堆浸廠，處置原生及次生硫化銅礦 中條山銅礦[39] 山西，運城 次生硫化銅59.1%，自由氧化銅37.4%，Cu 0.65% 地下原位破碎浸出，生物浸出與酸浸結合，2000年年產銅500 t 銅官山銅礦[40] 安徽，銅陵 Cu 0.9% 自1965年實驗地下生物浸出，1980年銅回收率達95%，2003年停產 大寶山銅礦[41] 廣東，韶關 Cu 1.06% (原生及次生硫化銅占總質量90%)，Fe 26.8%; 利用大寶山銅礦分離出的T.f菌，進行生物廢石堆浸 玉龍銅礦[42] 西藏，江達 Cu 2.75% (次生硫化銅礦28.95%, 原生硫化銅35%) 氧化銅礦及硫化礦的萃取-電積生物堆浸廠，地處西藏高海拔地區(4569~5118 m); 其中，硫化礦中的銅回收率超過80% 阿舍勒銅礦[43] 新疆，哈巴河 Cu 2.43% 2004年7月，生物堆浸廠建成并使用，銅浸出率達80% 永平銅礦[44] 江西，上饒 Cu 0.32% (原生硫化銅65.6%) 我國第二大露天礦，始建于1984年，自上世紀90年代，利用生物浸出回收低品位銅礦和廢石 賽什塘銅礦[45] 青海，興海 Cu 0.83% (硫化銅礦與氧化銅為主) 地處青藏高原的高海拔地區(3450 m); 開展高寒-低氧含量環境下的生物浸出實驗 東川銅礦[46] 云南，東川 Cu 0.9%~1.5% (硫化銅礦33%，氧化銅礦41%) 始建于上世紀60年代，順利開展了工業級的生物浸出實驗 冬瓜山銅礦[47] 安徽，銅陵 Cu 0.94%~1.06% (黃銅礦為主), 主要浸礦細菌為A.f (CUMT-1 & ZJJN-3) 利用Acidithiobacillus ferrooxidans和Acidithiobacillus thiooxidans開展黃銅礦浸出實驗 金川銅鎳礦[48] 甘肅，金川 Cu 0.44% (原生硫化銅69.8%, 自由氧化銅20.6%，次生硫化銅8% 生物浸出探索自2006至2009年運行，鎳銅鈷多金屬聯合浸出，40 d后銅浸出率達93.48% 東鄉銅礦[49] 江西，福州 Cu 1.34% (黃銅礦1.01%, 輝銅礦0.33%), 黃鐵礦11.48%, Fe 30.05% 采用原生硫化銅地下破碎原位浸出技術，高硫、高鐵礦石 云浮銅鎳礦[50] 江西，梅州 我國第一大FeS2礦山 多細菌聯合浸出探索，Betaproteobacteria 47.75%, Gammaproteobacteria 37.84%為主 薩熱克銅礦[51] 新疆，烏恰 Cu 1.34%，次生硫化銅礦(黃銅礦，輝銅礦等) 開展生物浸出工業級實驗，經155 d后，銅浸出率達93.77% 多寶山銅礦[52] 黑龍江，嫩江 Cu 0.51%，原生硫化銅(黃銅礦為主) 開展浸出實驗，經326 d后，銅浸出率僅為15.5%，大量CaSO4導致板結鈍化現象嚴重 大冶鐵礦[53] 湖北，大冶 Cu 0.35%，硫化銅32.3%，自由氧化銅26.3% 低品位廢石堆浸，高氧化性，高泥，經80 d浸出試驗，銅浸出率達83.97% 中衛銅礦[54] 寧夏，中衛 Cu 0.32%，次生硫化銅59.38%，原生硫化銅37.5% 開展工業試驗，經315 d后銅浸出率達83.03%，板結嚴重，產生大量CaSO4 哈密銅鎳礦[55] 新疆，哈密 Cu 3%, 硫化銅礦為主 含錳低品位硫化銅礦，開展銅鎳生物浸出實驗，銅浸出率達32.6% 
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表 2 世界范圍內已分離獲得的浸銅細菌(不完全統計)[59]
Table 2. Leaching bacteria after being isolated and identified around the world (incomplete statistics)[59]
細菌種類 NCBI編號 菌種采樣位置及國家 Acidithiobacillus ferrivorans CF27 CCCS000000000 某銅鈷礦的酸性礦坑水，美國 Acidiplasma sp.MBA-1 JYHS00000000 某銅礦浸出反應器，俄羅斯 Acidiplasma cupricumulans BH2 LKBH00000000 某硫化銅礦，緬甸 Ferrovum sp. JA12 LJWX00000000 某硫化銅礦礦坑水，德國 Ferrovum sp.Z-31 LRRD00000000 某銅礦酸性礦坑水，德國 Acidithiobacillus thiooxidans Licanantay JMEB00000000 某銅礦，智利 "Ferrovum myxofaciens" P3GT JPOQ00000000 某銅礦礦坑水，英國 "Acidibacillus ferrooxidans" DSM 5130T LPVJ00000000 某低品位黃銅礦礦坑水，巴西 Ferrimicrobium acidiphilum DSM 19497T JQKF00000000 某銅礦礦坑水，英國 Leptospirillum sp.Sp-Cl LGSH00000000 某銅礦，智利 Sulfobacillus thermosulfidooxidans Cutipay ALWJ00000000 某銅礦滲濾液，智利 Acidithiobacillus ferrooxidans (4664533.3)# 德興銅礦，中國 Sulfobacillus thermosulfidooxidans DSM 9293T (2506210005)* 某自熱礦床，哈薩克斯坦 Acidithiobacillus ferrooxidans ATCC 53993 NC_011206 某銅礦，亞美尼亞 Acidithiobacillus caldus SM-1 NC_015850 微生物資源前期開發國家重點實驗室，中國
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