Determination of Redox Potential of Sandstone-type Uranium Ore by Potential Drop Methods of Potassium Dichromate and Potassium Permanganate
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摘要:
氧化还原电位是一个体系中所有物质混合氧化还原电位的数量指标，反映了整个体系氧化还原能力的相对强弱，而砂岩型铀矿的氧化还原电位控制着铀等变价元素的地球化学行为，对准确圈出铀富集层位具有重要意义。电位落差法借助于氧化剂溶液测定样品的氧化还原容量，电位差的大小能准确反映出砂岩型铀矿样品所含还原组分的还原能力。本文以重铬酸钾和高锰酸钾作为氧化剂，探讨了应用这两种氧化剂的电位落差法测定砂岩型铀矿氧化还原电位(ΔEh)的特点。系统研究了两种方法溶液介质浓度、氧化剂浓度、平衡电位时间、样品浸泡时间和样品与氧化剂溶液的固液比对ΔEh测定的影响。按照两种方法最优条件测定8个砂岩型铀矿样品，重铬酸钾法ΔEh值在15~118mV之间，相对标准偏差为2.50%~7.44%；高锰酸钾法ΔEh值在45~89mV之间，相对标准偏差为0.89%~1.42%，两种方法在测量8个砂岩型铀矿样品ΔEh的相对水平方面具有一致性，相关系数为0.9882。研究表明重铬酸钾电位落差法的ΔEh更分散跨度更大，能更直观地看出样品间还原能力的差别；高锰酸钾电位落差法的ΔEh稳定性更好。两种电位落差法测量砂岩型铀矿的ΔEh数值可用于其氧化还原分带的划分。
Abstract:BACKGROUND The redox potential is a quantitative indicator of the mixed redox potential of all substances in a system, which reflects the relative strength of the redox capacity of the whole system. It is of great significance to delineate the uranium enrichment horizon. The redox potential of sandstone-type uranium deposits controls the geochemical behavior of uranium and other variable valence elements, and is of great significance for accurately delineating uranium-enriched horizons. The potential difference method is used to measure the redox capacity of the sample by means of the oxidant solution, and the magnitude of the potential difference can accurately reflect the reducing ability of the reducing components in the sandstone-type uranium ore sample.
OBJECTIVES To compare the two methods for the determination of the redox potential (ΔEh) of sandstone-type uranium ores.
METHODS ΔEh of sandstone-type uranium ores was determined by two potential drop methods using potassium dichromate and potassium permanganate as oxidants. The effects of the solution medium concentration, oxidant concentration, equilibrium potential time, sample immersion time, and solid-liquid ratio of sample to oxidant solution on the determination of ΔEh were systematically studied. According to the optimal conditions of the two methods, 8 sandstone-type uranium samples were measured.
RESULTS The ΔEh of the potassium dichromate method was between 15mV and 118mV, and the relative standard deviation was between 2.50% and 7.44%. The ΔEh of the potassium permanganate method was between 45mV and 89mV, with the relative standard deviation of 0.89%-1.42%. The two methods had significant consistency in determining the relative level of ΔEh of 8 sandstone-type uranium ore samples, and the correlation coefficient was 0.9882.
CONCLUSIONS The ΔEh of the potassium dichromate potential drop method is more dispersed with a large range, and the difference in reducing ability between samples can be identified more intuitively. The ΔEh of the potassium permanganate potential drop method is more stable. The ΔEh values of sandstone-type uranium deposits measured by two potential drop methods can be used for the division of redox zoning.
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表 1 不同浓度重铬酸钾条件下重铬酸钾及样品-重铬酸钾浸泡液的电位值
Table 1. Eh values of potassium dichromate and sample-potassium dichromate immersion solution under different concentrations of potassium dichromate
1/6K2Cr2O7溶液浓度(mol/L) 重铬酸钾Eh(mV) 样品-重铬酸钾浸泡液Eh(mV) 落差电位ΔEh(mV) 样品1 样品2 样品3 样品1 样品2 样品3 0.01 892 470 445 727 422 447 165 0.05 940 838 880 861 102 60 79 0.10 982 859 935 879 127 51 107 0.15 990 855 931 879 129 53 105 0.20 983 865 942 886 118 41 97 
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表 2 不同浓度氢氧化钾条件下高锰酸钾及样品-高锰酸钾浸泡液的电位值
Table 2. Eh values of potassium permanganate and sample-potassium permanganate immersion solution under different concentrations of potassium hydroxide
测定溶液 氢氧化钾浓度(×10-3) 0.0 0.5 1.0 1.5 2.0 4.0 6.0 10.0 0.10mol/L 1/3KMnO4Eh(mV) 678 483 482 477 476 476 474 473 砂岩型铀矿浸泡液Eh(mV) 661 442 424 423 421 422 420 418 落差电位ΔEh(mV) 14 41 58 54 55 54 54 55
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表 3 不同平衡电位时间下溶液的电位值
Table 3. Eh values of solution at different equilibrium potential time
测定溶液 Eh(mV) 0min 5min 10min 15min 20min 25min 30min 硫酸亚铁铵-硫酸铁铵标准溶液 402 428 427 430 430 427 430 重铬酸钾溶液 890 936 992 985 990 989 993 砂岩型铀矿重铬酸钾浸泡液 782 810 829 844 845 847 850 高锰酸钾溶液 526 481 481 480 479 481 483 砂岩型铀矿高锰酸钾浸泡液 463 425 424 423 426 428 427
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表 4 不同浸泡时间和固液比下两种方法的ΔEh值
Table 4. Eh values of the two methods under different immersion time and solid-liquid ratio
浸泡时间(min) 重铬酸钾法ΔEh(mV) 高锰酸钾法ΔEh(mV) 样品1 样品2 样品3 样品1 样品2 样品3 30 106 42 88 65 44 87 60 121 50 100 67 42 89 90 125 49 101 69 45 85 120 123 47 103 68 47 86 180 122 52 102 66 44 88 300 128 49 104 64 48 90 固液比(g/mL) 重铬酸钾法ΔEh(mV) 高锰酸钾法ΔEh(mV) 样品1 样品2 样品3 样品1 样品2 样品3 0.5∶50 78 19 47 67 26 51 1.0∶50 96 28 76 87 37 67 1.5∶50 115 40 92 92 39 71 2.0∶50 124 48 104 97 42 75 2.5∶50 136 63 110 101 44 79 3.0∶50 139 85 117 103 45 82 5.0∶50 169 113 136 126 52 92
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表 5 两种方法测量砂岩型铀矿样品的ΔEh值
Table 5. ΔEh values of sandstone-type uranium ore samples with the two methods
样品编号 重铬酸钾法 高锰酸钾法 ΔEh(mV) RSD(%) ΔEh(mV) RSD(%) L002 15 2.94 45 0.96 L003 26 2.50 54 1.12 L004 44 2.75 62 1.32 L005 43 3.56 61 0.97 L006 58 6.60 68 0.89 L007 90 5.38 77 1.08 L008 118 7.44 89 1.27 L009 105 3.32 82 1.42
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表 6 氧化还原环境和高锰酸钾电位落差法氧化还原分带的判断
Table 6. Judgment of redox environment and redox zoning by potassium permanganate potential drop method
样品编号 Fe3+/Fe2+ 氧化还原环境 ΔEh(mV) 氧化还原分带 Q001 2.02 氧化环境 21 氧化岩石带 L003 1.07 弱氧化环境 40 氧化还原过渡带 L006 0.90 弱还原环境 50 还原岩石带 L008 0.27 还原环境 69 强还原带
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