Crops ›› 2023, Vol. 39 ›› Issue (3): 66-74.doi: 10.16035/j.issn.1001-7283.2023.03.009

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Study on Geographical Origin of Buckwheat Based on Mineral Element Fingerprint

Zhang Yufen1(), Qi Jingkai1(), Wang Guiling2, Zhao Baoping3, Zhou Lei4   

  1. 1Life Science College of Inner Mongolia Minzu University, Tongliao 028043, Inner Mongolia, China
    2Zhalantun Green Industry Development Center, Zhalantun 162650, Inner Mongolia, China
    3Agriculture College of Inner Mongolia Agricultural University, Hohhot 010019, Inner Mongolia, China
    4Agriculture College of Inner Mongolia Minzu University, Tongliao 028043, Inner Mongolia, China
  • Received:2021-08-31 Revised:2022-01-15 Online:2023-06-15 Published:2023-06-16

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Abstract:

The contents of 20 elements including Na, Mg, K, Ca, V, Cr, Mn, Fe, Co, Ni, Cu, Zn, Se, Sr, Rb, Cs, Ba, As, Cd and Pb in buckwheats produced from eight regions were determined by microwave digestion inductively coupled plasma mass spectrometry (ICP-MS). The main mineral elements affecting buckwheat producing areas were selected by correlation analysis, significance analysis and principal component analysis. Buckwheat from different producing areas were classified by cluster analysis and discriminant analysis. The results showed that there were significant differences of different producing areas from other elements, except V and Cs, buckwheat from different producing areas had its unique mineral element fingerprint information. The five elements, Rb, Sr, Co, Ba and Cr, were screened out by stepwise discriminant analysis, the overall discriminant rates of buckwheat producing areas were 93.3% and 98.3%, respectively, by cross validation test and original test. Therefore, mineral element fingerprint combined with chemometrics could identify buckwheat from different producing areas, which provided technical support for the study of geographical origin of buckwheat.

Key words: Buckwheat, Mineral element fingerprint, ICP-MS, Chemometrics, Origin identification

Table 1

Regression equation, correlation coefficient, the average recovery rates, RSD, LOD and LOQ of 20 elements"

元素
Element		 方程
Regression equation		 相关系数
r		 平均回收率
Average recovery rate (%)		 相对标准偏差
RSD (%)		 检出限
LOD (ng/L)		 定量限
LOQ (ng/L)
Na y=2.3434×10-2x+1.7451×10-3 0.9998 104.03 3.58 0.02 0.06
Mg y=1.4054×10-2x+6.1057×10-3 0.9994 99.36 2.25 0.23 0.69
K y=9.4088×10-3x+1.3102×10-3 0.9999 103.44 3.51 0.27 0.81
Ca y=2.7369×10-2x+2.7185×10-3 0.9995 103.15 2.38 0.27 0.81
V y=26595x-2315 0.9999 97.66 1.03 0.12 0.36
Cr y=21732x+16741 0.9999 96.43 1.29 0.14 0.42
Mn y=29948x+24815 0.9999 100.32 1.35 0.17 0.52
Fe y=638.2x+30613 0.9991 100.22 1.26 0.49 1.47
Co y=1167.32x+53559.43 0.9997 98.64 1.81 0.04 0.12
Ni y=5929x+3726 0.9998 97.85 0.81 0.43 1.30
Cu y=12482x+14115 0.9999 99.94 0.65 0.06 0.18
Zn y=3735x+16733 0.9995 102.67 1.39 0.63 1.89
As y=3657x+5919 0.9998 97.25 0.54 0.48 1.45
Se y=409x-154 0.9998 99.11 0.83 1.25 3.75
Rb y=29523x+4150 0.9999 99.84 1.24 1.01 3.03
Sr y=38416x+15168 0.9995 95.37 3.14 0.03 0.09
Cd y=3297x+1346 0.9999 99.84 1.43 0.08 0.24
Cs y=33083x+1099 0.9999 98.22 1.36 0.11 0.33
Ba y=27186x+42380 0.9996 96.43 1.67 0.06 0.18
Pb y=10495x+1280 0.9998 101.28 1.62 0.07 0.21

Table 2

Contents of mineral elements in buckwheat"

元素
Element		 含量
Content (mg/kg)		 最小值
Minimum		 最大值
Maximum		 偏度
Skewness		 峰度
Kurtosis		 P 变异系数
CV (%)
Na 80.11(68.66, 105.54) 27.45 179.29 0.61 -0.70 0.04 44.37
Mg 2344.10±227.74 1800.93 2672.05 -0.47 -0.11 0.44 9.72
K 4456.92±972.21 2368.55 6807.71 0.11 0.60 0.96 21.81
Ca 103.54±48.85 33.52 212.50 0.28 -0.79 0.27 47.18
Fe 28.38±7.46 18.37 47.07 0.61 -0.12 0.15 26.29
Mn 31.95±8.23 18.86 48.07 0.42 -0.39 0.36 25.76
Cu 8.07(13.49, 28.28) 6.23 60.55 2.87 8.52 0.00 58.39
Zn 16.97±5.18 8.07 29.01 -0.49 -0.35 0.90 30.52
Se 0.04(0.04, 0.09) 0.00 0.19 1.64 1.46 0.00 72.64
Ni 5.29±1.09 3.69 8.06 0.85 0.36 0.11 20.60
Cr 0.84(0.66, 1.10) 0.17 2.20 1.11 0.91 0.03 53.01
Co 0.56(0.39, 0.73) 0.09 1.87 1.70 3.35 0.00 102.27
V 0.11(0.04, 0.18) 0.01 0.82 3.44 13.83 0.00 105.59
Rb 20.76±10.45 4.70 41.22 0.43 -0.88 0.25 50.34
Sr 3.87±1.99 1.05 9.75 0.85 1.29 0.20 51.42
Cs 0.14(0.05, 0.23) 0.01 1.06 3.87 16.99 0.00 78.09
Ba 2.93(2.87, 14.29) 0.58 14.29 1.31 0.76 0.00 69.89
Pb 0.08(0.12, 0.53) 0.02 1.99 1.98 3.56 0.00 176.52
Cd 0.09(0.09, 0.35) 0.00 1.29 2.05 3.79 0.00 118.14
As 0.27(0.24, 0.61) 0.00 1.70 1.51 1.51 0.00 108.24

Table 3

Correlation analysis of different elements in buckwheat"

元素
Element		 Na Mg K Ca Fe Mn Cu Zn Se Ni Cr Co V Rb Sr Cs Ba Pb Cd As
Na 1
Mg 0.31 1
K 0.60** 0.48* 1
Ca 0.09 0.34 -0.03 1
Fe -0.11 0.03 0.17 -0.03 1
Mn 0.05 -0.03 0.13 -0.14 0.67** 1
Cu -0.21 0.14 -0.23 0.20 0.11 0.14 1
Zn 0.51** 0.27 0.15 0.19 0.12 0.24 -0.08 1
Se 0.58** -0.13 0.10 -0.20 -0.11 0.04 -0.11 0.39* 1
Ni 0.42* 0.18 0.29 0.17 -0.18 -0.33 -0.30 0.21 0.28 1
Cr 0.07 0.14 -0.04 0.17 -0.42* -0.20 -0.23 0.11 -0.11 0.34 1
Co -0.15 -0.10 0.10 0.13 0.47* 0.43* -0.06 0.18 -0.05 -0.27 -0.32 1
V -0.16 0.22 -0.04 0.19 -0.40* -0.30 -0.02 -0.12 -0.31 -0.02 0.42* -0.27 1
Rb 0.65** 0.21 0.26 0.05 -0.47* -0.39* -0.25 0.22 0.54** 0.60** 0.16 -0.26 0.05 1
Sr 0.10 0.22 -0.06 0.06 -0.30 -0.11 -0.06 0.13 -0.04 -0.06 0.43* -0.19 0.55** 0.20 1
Cs 0.13 -0.04 0.32 -0.17 -0.13 -0.29 -0.22 0.00 0.11 0.58** -0.08 -0.04 0.01 0.35 -0.23 1
Ba -0.15 0.24 0.21 -0.01 -0.15 -0.30 0.02 -0.13 -0.25 -0.01 0.10 -0.25 0.49** -0.03 0.41* 0.19 1
Pb -0.26 0.03 0.00 0.31 0.49** 0.19 -0.09 0.21 -0.21 0.02 0.01 0.76** -0.14 -0.32 -0.15 0.05 -0.17 1
Cd 0.01 0.47* 0.11 0.31 0.20 0.16 0.40* 0.33 -0.29 -0.38* -0.21 0.17 0.23 -0.35 0.26 -0.22 0.22 0.22 1
As -0.05 0.27 -0.13 0.25 0.23 0.32 0.39* 0.51** -0.02 -0.37 -0.08 0.43* 0.18 -0.29 0.27 -0.27 -0.07 0.47* 0.76** 1

Table 4

Difference analysis of mineral elements in buckwheat from different producing areas mg/kg"

元素
Element		 吉林
Jilin		 内蒙古东部
Eastern
Inner Mongolia		 内蒙古西部
Western
Inner Mongolia		 陕西
Shaanxi		 甘肃
Gansu		 四川
Sichuan		 贵州
Guizhou		 云南
Yunnan
Na 32.08±6.29f 169.48±10.43a 76.28±3.26d 61.82±22.91de 51.02±7.02ef 39.03±11.51ef 108.04±11.99c 145.23±22.20b
Mg 2054.64±219.72c 2274.96±24.09bc 2702.97±59.96a 2346.78±83.67b 2295.52±166.07b 2272.45±90.12bc 2419.67±101.76b 2307.16±59.44b
K 3686.75±1147.08cd 5233.55±133.97b 3433.51±77.75d 4634.96±203.06bc 4383.46±820.83bcd 4169.54±520.79bcd 5159.61±649.51b 6401.06±353.27a
Ca 64.98±7.27d 56.20±5.36d 76.73±15.39cd 95.40±8.66c 178.09±31.23a 135.60±4.74b 145.89±21.93b 144.73±10.61b
Fe 32.96±5.39b 26.93±1.91bc 22.08±2.57c 21.34±3.46c 26.01±5.34bc 29.90±0.33bc 43.67±4.52a 27.64±9.42bc
Mn 28.79±2.57c 27.55±2.82c 25.97±5.58cd 20.05±1.52d 47.65±5.58a 35.93±6.64b 35.92±4.03b 34.67±2.51b
Cu 14.31±11.87cd 6.76±0.47d 40.16±1.59b 7.14±0.34d 23.51±11.46c 15.11±2.25cd 53.45±7.81a 7.32±0.37d
Zn 17.32±3.35b 21.24±1.84b 16.41±4.19bc 18.10±3.05b 13.96±6.19c 18.49±3.79b 28.07±1.01a 18.13±3.51b
Se 0.06±0.02bc 0.17±0.02a 0.04±0.02bc 0.04±0.03bc 0.03±0.01c 0.04±0.01bc 0.03±0.02c 0.10±0.08b
Ni 4.61±0.69b 5.19±1.60b 4.98±0.86b 5.23±0.48b 11.01±1.07a 5.66±1.80b 4.64±0.41b 5.47±0.85b
Cr 0.51±0.05bc 0.58±0.29bc 0.84±0.11bc 1.11±0.16b 1.08±0.79b 2.13±0.04a 0.21±0.04c 0.94±0.38bc
Co 1.61±0.33a 0.33±0.05cd 0.42±0.32bcd 0.29±0.03d 0.50±0.25bcd 0.79±0.37b 0.71±0.18bc 0.51±0.11bcd
V 0.06±0.04a 0.03±0.03a 0.09±0.12a 0.31±0.44a 0.13±0.16a 0.13±0.18a 0.08±0.09a 0.08±0.09a
Rb 26.96±5.24bc
 37.07±5.25a 25.06±8.12bc 23.60±5.23bc 15.27±5.93cd 11.28±2.21d 15.07±3.25cd 13.75±4.59d
Sr 3.25±0.62bc 3.25±0.81bc 4.07±1.84b 7.62±1.82a 1.28±0.29c 3.50±2.35bc 4.82±0.43b 3.14±0.67bc
Cs 0.05±0.03a 0.23±0.04a 0.12±0.08a 0.14±0.04a 0.33±0.51a 0.04±0.01a 0.05±0.02a 0.17±0.13a
Ba 2.19±1.35d 2.39±0.86d 2.84±1.14d 13.31±1.28a 7.03±3.37b 1.21±0.23d 5.61±0.92c 2.87±0.28d
Pb 0.05±0.03b 0.04±0.04b 0.12±0.16b 0.08±0.02b 0.37±0.48b 1.41±0.82a 1.05±0.26a 0.12±0.08b
Cd 0.15±0.18b 0.07±0.02b 0.15±0.19b 0.45±0.45b 0.05±0.06b 0.12±0.01b 0.92±0.34a 0.06±0.04b
As 0.03±0.04c 0.26±0.04b 0.31±0.20b 0.52±0.77ab 0.43±0.7ab 0.62±0.18ab 1.18±0.46a 0.16±0.07c

Table 5

Principal component analysis of mineral elements in buckwheat"

变量
Variable		 主成分Principal component
PC1 PC2 PC3 PC4 PC5 PC6
Na -0.18 0.85 0.30 0.17 0.15 -0.14
Mg 0.19 0.02 0.39 0.01 -0.43 -0.59
K -0.09 0.49 0.29 0.56 0.36 0.10
Ca 0.16 -0.44 0.18 0.74 0.29 -0.11
Fe 0.63 0.33 -0.30 0.45 -0.15 0.26
Mn 0.33 0.23 -0.42 0.10 0.62 0.09
Cu 0.59 -0.16 0.15 0.19 -0.60 -0.19
Zn 0.67 0.63 0.08 0.02 -0.02 -0.06
Se -0.45 0.75 -0.01 0.06 -0.01 -0.08
Ni -0.45 -0.49 0.16 0.59 -0.03 0.01
Cr 0.08 -0.39 -0.09 -0.29 0.58 -0.52
Co 0.26 -0.02 -0.66 -0.09 -0.15 0.52
Rb -0.59 0.57 0.38 -0.13 -0.06 -0.08
Sr 0.28 0.14 0.58 -0.55 0.16 0.28
Ba -0.05 -0.37 0.71 0.10 -0.04 0.34
Pb 0.76 -0.07 -0.05 0.26 0.21 -0.28
Cd 0.73 0.09 0.46 0.04 -0.16 0.27
As 0.81 0.11 0.31 -0.04 0.19 -0.08
特征值Eigenvalue 5.25 3.16 2.43 2.01 1.54 1.14
方差贡献率Variance contribution rate (%) 26.27 15.80 12.14 10.05 7.72 5.70
累积方差贡献率Cumulative variance contribution rate (%) 26.27 42.06 54.20 64.25 71.98 77.67

Fig.1

PCA of mineral element content of buckwheat from different producing areas"

Fig.2

Fisher discriminant function of buckwheat from different producing areas"

Table 6

Validation results of stepwise discriminant analysis of buckwheat from different producing areas"

检验类型
Test type		 产地
Producing area		 预测组Prediction group 总数
Total
内蒙古东部
Eastern Inner
Mongolia		 吉林
Jilin		 内蒙古西部
Western
Inner Mongolia		 甘肃
Gansu		 陕西
Shaanxi		 四川
Sichuan		 云南
Yunnan		 贵州
Guizhou
回代检验
Original test		 内蒙古东部 10 0 0 0 0 0 0 0 10
吉林 0 8 0 0 0 0 0 0 8
内蒙古西部 0 0 10 0 0 0 0 0 10
甘肃 0 0 0 8 0 0 0 0 8
陕西 0 0 0 1 7 0 0 0 8
四川 0 0 0 0 0 5 0 0 5
云南 0 0 0 0 0 0 5 0 5
贵州 0 0 0 0 0 0 0 6 6
正确判别率 (%) 100.0 100.0 100.0 100.0 87.5 100.0 100.0 100.0 98.3
交叉验证
Cross validation		 内蒙古东部 10 0 0 0 0 0 0 0 10
吉林 0 8 0 0 0 0 0 0 8
内蒙古西部 0 0 10 0 0 0 0 0 10
甘肃 0 0 0 7 1 0 0 0 8
陕西 0 0 0 0 8 0 0 0 8
四川 0 0 0 0 0 4 1 0 5
云南 0 0 0 0 0 1 3 1 5
贵州 0 0 0 0 0 0 0 6 6
正确判别率 (%) 100.0 100.0 100.0 87.5 100.0 80.0 60.0 100.0 93.3

Fig.3

Systematic cluster analysis of mineral elements in buckwheat from different producing areas"

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