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基于红外光谱的煤炭产地溯源技术研究

林阳 李晶 夏文豪

林阳, 李晶, 夏文豪. 基于红外光谱的煤炭产地溯源技术研究[J]. 地质科技通报, 2022, 41(4): 317-328. doi: 10.19509/j.cnki.dzkq.2022.0124
引用本文: 林阳, 李晶, 夏文豪. 基于红外光谱的煤炭产地溯源技术研究[J]. 地质科技通报, 2022, 41(4): 317-328. doi: 10.19509/j.cnki.dzkq.2022.0124
Lin Yang, Li Jing, Xia Wenhao. Study on coal origin traceability technology based on infrared spectrum[J]. Bulletin of Geological Science and Technology, 2022, 41(4): 317-328. doi: 10.19509/j.cnki.dzkq.2022.0124
Citation: Lin Yang, Li Jing, Xia Wenhao. Study on coal origin traceability technology based on infrared spectrum[J]. Bulletin of Geological Science and Technology, 2022, 41(4): 317-328. doi: 10.19509/j.cnki.dzkq.2022.0124

基于红外光谱的煤炭产地溯源技术研究

doi: 10.19509/j.cnki.dzkq.2022.0124
基金项目: 

国家重点研究计划 2018YFF0215400

国家自然科学基金项目 41972179

详细信息
    作者简介:

    林阳(1998-), 男, 现正攻读矿产普查与勘探专业硕士学位, 主要从事煤地球化学方面的研究工作。E-mail: 819733817@qq.com

    通讯作者:

    李晶(1985-), 女, 副教授, 主要从事煤地质学、煤矿物学、煤地球化学方面的研究工作。E-mail: jingli@cug.edu.cn

  • 中图分类号: O657.33;P618.11

Study on coal origin traceability technology based on infrared spectrum

  • 摘要:

    随着我国煤炭对外依赖程度的不断提高, 煤炭进口掺假、以次充好的问题日益严重, 因此建立准确、快速、便捷、安全、环保的煤炭产地溯源技术的工作势在必行。红外光谱分析技术近年来也已经广泛应用在医药、食品、工业等领域的原产地鉴别工作中。红外光谱中包含丰富的成分与结构信息, 不同国家产出的煤炭, 不同产地的煤炭在组分及分子结构上存在较大的差异, 可以作为产地溯源的特征指示信息。因此, 本研究应用傅里叶红外光谱分析仪对来自5个国家30个进口煤炭样品进行了光谱采集分析, 通过不同产地的煤炭在红外光谱上所表现出的特征性, 以主成分分析和判别分析等化学计量学分析方法创新性地建立了3个国家的基于红外光谱特征信息的煤炭产地溯源模型, 并对模型的准确性进行了验证, 得出的主要认识如下: ①不同国家产出的煤炭, 其测定的红外光谱曲线形状存在差异, 所含有的官能团种类不同, 同种官能团吸收峰的数量、峰位及峰强度也有明显的差异; ②基于3个国家23个煤炭样品的红外光谱测试数据, 建立了官能团的特征信息数据库, 对其进行主成分分析和判别分析等化学计量学方法分析, 建立了俄罗斯、印尼和澳大利亚的煤炭产地溯源模型; ③选取已知产地的煤炭样本对建立的产地溯源模型的准确性进行了验证, 溯源效果准确率达到100%。某一产地的样本量越多, 模型判别分类的准确率更高, 溯源效果也更好。

     

  • 图 1  各国煤样红外谱图

    Figure 1.  Infrared spectrum of coal samples from various countries

    图 2  各国煤样碎石图

    Figure 2.  Coal sample gravel maps from various countries

    图 3  不同国家样本的典则判别函数的散点图

    国别1.俄罗斯;国别2.澳大利亚;国别3.印尼;下同

    Figure 3.  Scatter plots of canonical discriminant function of samples from different countries

    图 4  不同国家组质心和待检测样本的函数坐标散点图

    Figure 4.  Functional coordinatescatter plots ofcentroids and samples to be tested of different countries

    表  1  进口煤炭样品及其基本煤质特征

    Table  1.   Imported coal samples and their basic coal quality characteristics

    煤样 国别 给定品名 镜质体反射率/Ro/% 灰分Ad 水分Mad 挥发分Vdaf
    wB/%
    c1 俄罗斯Vanino 烟煤 0.533 31.88 3.49 46.85
    c2 俄罗斯Shakhtersk 动力煤 0.341 17.53 13.83 48.61
    c3 澳大利亚Newcastle 烟煤 0.707 19.58 5.48 36.73
    c4 印尼adangbay 烟煤 0.394 4.83 33.81 52.36
    c5 印尼Asam Asam 褐煤 0.213 6.78 33.99 54.14
    c7 印尼Balikpapan 褐煤 0.220 7.01 33.16 47.94
    c9 印尼Bunati 褐煤 0.281 5.23 32.72 52.44
    c10 印尼Kaltorang 褐煤 0.261 3.04 31.76 50.55
    c16 印尼Muara Berau 其他煤 0.453 5.43 9.84 40.64
    c39 俄罗斯新西伯利亚新库兹涅茨克欧亚斯煤矿 其他烟煤 0.775 22.15 5.25 38.96
    c40 澳大利亚adelaide 其他烟煤 0.598 20.84 11.07 32.58
    c41 澳大利亚Balmain 其他煤 0.342 7.96 23.36 47.84
    c42 印尼belawan 其他煤 0.338 22.80 12.81 35.61
    c44 澳大利亚bell bay 其他烟煤 0.829 9.36 4.96 34.04
    c45 俄罗斯kuzbass 其他烟煤 0.651 11.70 6.26 40.86
    c46 俄罗斯maly russia 其他烟煤 0.359 2.38 25.07 50.33
    c47 印尼PT adaro Indonesia 褐煤 0.267 4.54 31.13 51.79
    c49 印尼PT bara tabang 其他煤 0.323 7.57 24.12 48.75
    c51 印尼PT bukit asaml(perserd)tbk 其他煤 0.394 6.08 24.29 46.03
    c53 印尼PT mandiri intiperkasa 褐煤 0.301 9.78 34.11 53.49
    c54 印尼PT timuraya tunggal 褐煤 0.279 7.18 33.23 54.05
    c56 印尼PT tunas inti abadi 褐煤 0.313 7.63 28.54 53.14
    c57 印尼PT baba anugrah sejahtera 其他煤 0.395 6.43 20.49 47.15
    c58 印尼PT berau coal 其他烟煤 0.636 12.36 6.22 41.01
    c59 俄罗斯rgakka 褐煤 0.317 7.89 29.32 43.98
    c60 菲律宾semirara mining and power corporation 其他煤 0.353 5.73 28.52 46.39
    c61 马来西亚sibuti 其他烟煤 0.833 10.16 4.76 30.52
    c62 俄罗斯south kuzbass 其他煤 0.256 35.54 26.81 69.32
    c63 菲律宾subac nipa 其他烟煤 0.450 13.85 15.30 47.87
    c64 俄罗斯vladivostok 其他烟煤 0.738 23.59 5.01 35.29
    下载: 导出CSV

    表  2  俄罗斯煤样主成分提取结果

    Table  2.   Principal component extraction results of Russian coal samples

    成分 初始特征值 成分 初始特征值
    特征值 方差百分比/% 累积方差/% 特征值 方差百分比/% 累积方差/%
    1 14.133 32.867 32.867 23 8.25×10-17 1.92×10-16 100
    2 8.036 18.687 51.555 24 7.15×10-17 1.66×10-16 100
    3 6.674 15.52 67.075 25 -3.76×10-19 -8.75×10-19 100
    4 6.266 14.573 81.647 26 -6.73×10-17 -1.57×10-16 100
    5 4.539 10.557 92.204 27 -8.10×10-17 -1.88×10-16 100
    6 3.352 7.796 100 28 -1.11×10-16 -2.58×10-16 100
    7 1.76×10-15 4.09×10-15 100 29 -2.15×10-16 -5.01×10-16 100
    8 1.11×10-15 2.59×10-15 100 30 -2.41×10-16 -5.59×10-16 100
    9 9.99×10-16 2.32×10-15 100 31 -3.09×10-16 -7.19×10-16 100
    10 8.88×10-16 2.07×10-15 100 32 -3.41×10-16 -7.93×10-16 100
    11 7.77×10-16 1.81×10-15 100 33 -3.84×10-16 -8.93×10-16 100
    12 6.50×10-16 1.51×10-15 100 34 -4.73×10-16 -1.10×10-15 100
    13 6.19×10-16 1.44×10-15 100 35 -5.65×10-16 -1.32×10-15 100
    14 5.57×10-16 1.29×10-15 100 36 -5.81×10-16 -1.35×10-15 100
    15 4.98×10-16 1.16×10-15 100 37 -6.21×10-16 -1.44×10-15 100
    16 4.73×10-16 1.10×10-15 100 38 -6.38×10-16 -1.49×10-15 100
    17 3.57×10-16 8.31×10-16 100 39 -8.56×10-16 -1.99×10-15 100
    18 3.51×10-16 8.17×10-16 100 40 -1.08×10-15 -2.51×10-15 100
    19 2.74×10-16 6.38×10-16 100 41 -1.18×10-15 -2.75×10-15 100
    20 2.55×10-16 5.94×10-16 100 42 -1.98×10-15 -4.61×10-15 100
    21 1.96×10-16 4.56×10-16 100 43 -2.87×10-15 -6.68×10-15 100
    22 1.23×10-16 2.87×10-16 100
    下载: 导出CSV

    表  3  印尼煤样主成分提取结果

    Table  3.   Principal component extraction results of Indonesian coal samples

    成分 初始特征值 成分 初始特征值
    特征值 方差百分比/% 累积方差/% 特征值 方差百分比/% 累积方差/%
    1 10.199 24.876 24.876 22 2.46×10-16 5.99×10-16 100
    2 6.657 16.237 41.113 23 2.15×10-16 5.24×10-16 100
    3 5.477 13.358 54.471 24 1.59×10-16 3.88×10-16 100
    4 5.094 12.424 66.894 25 1.28×10-16 3.12×10-16 100
    5 3.563 8.691 75.585 26 -3.60×10-18 -8.78×10-18 100
    6 3.034 7.399 82.984 27 -4.54×10-17 -1.11×10-16 100
    7 2.759 6.730 89.715 28 -1.04×10-16 -2.53×10-16 100
    8 2.043 4.982 94.697 29 -1.35×10-16 -3.29×10-16 100
    9 1.287 3.140 97.837 30 -1.95×10-16 -4.76×10-16 100
    10 0.887 2.163 100 31 -2.68×10-16 -6.54×10-16 100
    11 1.34×10-15 3.26×10-15 100 32 -2.72×10-16 -6.64×10-16 100
    12 1.19×10-15 2.91×10-15 100 33 -3.84×10-16 -9.36×10-16 100
    13 1.03×10-15 2.52×10-15 100 34 -4.29×10-16 -1.05×10-15 100
    14 8.18×10-16 1.99×10-15 100 35 -4.75×10-16 -1.16×10-15 100
    15 7.15×10-16 1.74×10-15 100 36 -5.19×10-16 -1.27×10-15 100
    16 6.65×10-16 1.62×10-15 100 37 -7.33×10-16 -1.79×10-15 100
    17 6.49×10-16 1.58×10-15 100 38 -9.16×10-16 -2.23×10-15 100
    18 5.87×10-16 1.43×10-15 100 39 -1.04×10-15 -2.55×10-15 100
    19 4.93×10-16 1.20×10-15 100 40 -1.62×10-15 -3.96×10-15 100
    20 3.83×10-16 9.35×10-16 100 41 -2.36×10-15 -5.76×10-15 100
    21 3.28×10-16 8.00×10-16 100
    下载: 导出CSV

    表  4  澳大利亚煤样主成分提取结果

    Table  4.   Principal component extraction results of Australian coal samples

    成分 初始特征值 成分 初始特征值
    特征值 方差百分比/% 累积方差/% 特征值 方差百分比/% 累积方差/%
    1 20.332 56.479 56.479 19 8.40×10-17 2.33×10-16 100
    2 10.294 28.596 85.074 20 3.14×10-18 8.72×10-18 100
    3 5.373 14.926 100 21 -5.81×10-17 -1.61×10-16 100
    4 4.84×10-15 1.34×10-14 100 22 -1.13×10-16 -3.14×10-16 100
    5 3.05×10-15 8.46×10-15 100 23 -1.24×10-16 -3.45×10-16 100
    6 1.32×10-15 3.67×10-15 100 24 -1.72×10-16 -4.77×10-16 100
    7 1.19×10-15 3.30×10-15 100 25 -2.19×10-16 -6.08×10-16 100
    8 8.39×10-16 2.33×10-15 100 26 -2.23×10-16 -6.20×10-16 100
    9 6.56×10-16 1.82×10-15 100 27 -2.76×10-16 -7.66×10-16 100
    10 5.62×10-16 1.56×10-15 100 28 -4.01×10-16 -1.11×10-15 100
    11 5.22×10-16 1.45×10-15 100 29 -4.31×10-16 -1.20×10-15 100
    12 4.82×10-16 1.34×10-15 100 30 -5.15×10-16 -1.43×10-15 100
    13 3.94×10-16 1.09×10-15 100 31 -6.00×10-16 -1.67×10-15 100
    14 3.70×10-16 1.03×10-15 100 32 -6.01×10-16 -1.67×10-15 100
    15 3.34×10-16 9.27×10-16 100 33 -8.12×10-16 -2.26×10-15 100
    16 2.57×10-16 7.15×10-16 100 34 -1.16×10-15 -3.22×10-15 100
    17 2.06×10-16 5.71×10-16 100 35 -1.39×10-15 -3.85×10-15 100
    18 1.20×10-16 3.32×10-16 100 36 -3.05×10-15 -8.46×10-15 100
    下载: 导出CSV

    表  5  不同国家的典则判别函数系数

    Table  5.   Coefficient of canonical discriminant function in different countries

    函数系数 函数系数
    1 2 1 2
    芳烃CH链2 0.001 0.012 C-O链1 0.010 0.002
    氢键结合的醇 2.708 -1.069 C-O链2 -0.007 -0.004
    自由缔合的羟基 -9.290 3.126 羟基苯和醚的C-O伸缩振动 0 0.004
    酚、醇的OH 1 1.443 -0.542 C-O链3 0.032 -0.012
    CH链2 0 0.007 C-O链4 0.008 -0.004
    对称CH2伸缩振动 3.870 -5.548 -CH2和-CH3的对称弯曲振动 -0.635 -0.252
    对称RCH3伸缩振动 -0.006 0.007 -CH2和CH3链2 0.286 0.110
    非对称CH2伸缩振动 6.989 -1.928 芳烃CH 3 -0.014 0.006
    CH3的伸缩振动 0.666 2.709 氢键缔合的羰基,-O-取代C=C 1.390 -1.330
    烷烃中甲基(CH3),运动状态为摇摆振动 -15.210 -0.339 羰基 0.111 1.697
    CH3链1 1.560 0.121 CH2组成的长链1 -0.013 0.016
    (常量) -3 291.590 7 693.168 CH2组成的长链2 0.010 -0.001
    下载: 导出CSV

    表  6  组质心处的函数值

    Table  6.   Function value table at group centroid

    组质心处的函数
    国别 函数系数
    1 2
    1 10.442 -5.341
    2 -17.517 -4.856
    3 0.312 5.155
    注:按组平均值进行求值的未标准化典则判别函数
    下载: 导出CSV

    表  7  煤样溯源效果验证表

    Table  7.   Verification table of coal sample traceability effect

    样本编号 国别 Dis_2 Dis1_3 Dis2_3 Dis1_4 Dis2_4 Dis3_4
    CD-44 1 1 10.587 5 -5.688 94 1 0 0
    CD-40 2 2 -17.913 51 -5.685 06 0 1 0
    CD-41 3 3 -0.335 26 4.479 13 0 0 1
    CD-53 3 3 2.548 55 5.245 75 0 0 1
    下载: 导出CSV
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