Quality Control of Different Types of Honey and Propolis Collected from Romanian Accredited Beekeepers and Consumer’s Risk Assessment
Abstract
:1. Introduction
2. Materials and Methods
2.1. Sample Collection
2.2. Heavy Metals and Pesticides Detection
2.2.1. Heavy Metals Analysis
2.2.2. Pesticides Analysis
2.3. Risk Characterisation for Consumer’s Health
2.3.1. Bioconcentration Factor
2.3.2. Estimated Daily Intake (EDI)
2.3.3. Hazard Quotient (HQ)
2.4. Statistical Analysis
3. Results
3.1. The Concentration of Heavy Metals in Investigated Samples
3.2. The Concentration of Pesticides in Investigated Samples
3.3. Heavy Metal and Pesticide Accumulation from Soil to Bees’ Products
3.4. Estimated Risk to Consumers through Honey Consumption
4. Discussion
5. Conclusions
Author Contributions
Funding
Institutional Review Board Statement
Informed Consent Statement
Data Availability Statement
Conflicts of Interest
References
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Element | R2 | LOD (mg/kg) | LOQ (mg/kg) |
---|---|---|---|
Cadmium | 0.992 | 1.8 × 10−3 | 19 × 10−3 |
Copper | 0.998 | 50 × 10−3 | 153 × 10−3 |
Zinc | 0.988 | 61 × 10−3 | 238 × 10−3 |
Chromium | 0.995 | 52 × 10−3 | 165 × 10−3 |
Lead | 1.000 | 49 × 10−3 | 166 × 10−3 |
Nickel | 0.999 | 54 × 10−3 | 184 × 10−3 |
Manganese | 0.984 | 58 × 10−3 | 202 × 10−3 |
Element | R2 | LOD (mg/kg) | LOQ (mg/kg) |
---|---|---|---|
p, p′-DDT | 0.994 | 1.95 × 10−3 | 12.38 × 10−3 |
o, p′-DDT | 1.000 | 2.21 × 10−3 | 14.35 × 10−3 |
p, p′-DDE | 0.998 | 2.48 × 10−3 | 17.44 × 10−3 |
Sample | Cd | Cu | Zn | Cr | Pb | Ni | Mn |
---|---|---|---|---|---|---|---|
Black locust honey | 0.047 ± 0.009 | 2.132 ± 0.066 | 3.502 ± 0.052 | 1.729 ± 0.059 | 0.213 ± 0.073 | 0.828 ± 0.058 | 1.518 ± 0.075 |
Linden honey | 0.028 ± 0.006 | 1.599 ± 0.052 | 3.793 ± 0.056 | 1.507 ± 0.083 | 0.294 ± 0.055 | 0.698 ± 0.062 | 1.107 ± 0.047 |
Multifloral honey | 0.030 ± 0.006 | 1.134 ± 0.065 | 3.886 ± 0.062 | 1.869 ± 0.068 | 0.539 ± 0.054 | 0.485 ± 0.070 | 1.838 ± 0.069 |
Rapeseed honey | 0.063 ± 0.007 | 2.422 ± 0.064 | 3.188 ± 0.068 | 1.272 ± 0.051 | 0.274 ± 0.058 | 0.858 ± 0.074 | 1.662 ± 0.075 |
Propolis | 0.080 ± 0.006 | 3.203 ± 0.052 | 4.195 ± 0.067 | 2.344 ± 0.074 | 0.651 ± 0.063 | 1.146 ± 0.061 | 2.184 ± 0.067 |
Soil | 3.599 ± 0.061 | 25.056 ± 0.092 | 135.012 ± 0.089 | 34.078 ± 0.090 | 51.979 ± 0.121 | 26.931 ± 0.096 | 425.983 ± 0.121 |
MAL * mg/kg in honey [55,56,57] | 0.02 | 0.50 | 1.00 | - | 0.2 | - | |
MAL * mg/kg dry soil [54] | 3 | 100 | 300 | 100 | 50 | 50 | 1500 |
Sample | Cd | Cu | Zn | Cr | Pb | Ni | Mn |
---|---|---|---|---|---|---|---|
Black locust honey | 0.014 ± 0.004 | 0.216 ± 0.062 | 0.807 ± 0.052 | 1.408 ± 0.067 | 0.141 ± 0.048 | 0.623 ± 0.064 | 0.724 ± 0.080 |
Linden honey | 0.016 ± 0.003 | 0.290 ± 0.055 | 0.885 ± 0.060 | 1.498 ± 0.065 | 0.138 ± 0.047 | 0.488 ± 0.067 | 0.877 ± 0.062 |
Multifloral honey | 0.013 ± 0.005 | 0.384 ± 0.057 | 0.882 ± 0.062 | 1.332 ± 0.067 | 0.120 ± 0.048 | 0.663 ± 0.093 | 0.841 ± 0.068 |
Rapeseed honey | 0.012 ± 0.004 | 0.399 ± 0.055 | 0.774 ± 0.072 | 1.702 ± 0.067 | 0.134 ± 0.042 | 0.564 ± 0.079 | 0.738 ± 0.085 |
Propolis | 0.016 ± 0.004 | 0.402 ± 0.059 | 0.947 ± 0.090 | 1.868 ± 0.065 | 0.160 ± 0.044 | 0.876 ± 0.082 | 1.026 ± 0.086 |
Soil | 1.649 ± 0.091 | 20.049 ± 0.093 | 98.01 ± 0.095 | 27.148 ± 0.063 | 19.579 ± 0.069 | 18.881 ± 0.070 | 412.976 ± 0.124 |
MAL * mg/kg in honey [55,56,57] | 0.02 | 0.50 | 1.00 | - | 0.2 | - | |
MAL * mg/kg dry soil [54] | 3 | 100 | 300 | 100 | 50 | 50 | 1500 |
Sample | p, p′-DDT | o, p′-DDT | p, p′-DDE |
---|---|---|---|
A1 Area | |||
Black locust honey | 0.0261 ± 0.0044 | 0.0200 ± 0.0063 | 0.0201 ± 0.0042 |
Linden honey | 0.0179 ± 0.0045 | 0.0163 ± 0.0094 | 0.0150 ± 0.0026 |
Multifloral honey | 0.0311 ± 0.0042 | 0.0166 ± 0.0057 | 0.0297 ± 0.0067 |
Rapeseed honey | 0.0266 ± 0.0045 | 0.0217 ± 0.0061 | 0.0210 ± 0.0044 |
Propolis | 0.0320 ± 0.0062 | 0.0247 ± 0.0044 | 0.0300 ± 0.0052 |
Soil | 0.0485 ± 0.0080 | 0.0422 ± 0.0063 | 0.0535 ± 0.0075 |
A2 Area | |||
Black locust honey | 0.0066 ± 0.0036 | 0.0118 ± 0.0035 | 0.0101 ± 0.0048 |
Linden honey | 0.0055 ± 0.0037 | 0.0067 ± 0.0047 | 0.0058 ± 0.0037 |
Multifloral honey | 0.0138 ± 0.0046 | 0.0068 ± 0.0041 | 0.0123 ± 0.0051 |
Rapeseed honey | 0.0137 ± 0.0048 | 0.0105 ± 0.0052 | 0.0095 ± 0.0052 |
Propolis | 0.0127 ± 0.0052 | 0.0115 ± 0.0044 | 0.0149 ± 0.0044 |
Soil | 0.0132 ± 0.0043 | 0.0156 ± 0.0054 | 0.0177 ± 0.0063 |
MAL * mg/kg honey [61] | Total DDT 0.05 | ||
MAL * mg/kg dry soil [54] | 0.25 | 0.25 | 0.25 |
Sample | Area | Mean Value | Standard Deviation | Standard Error | Minimal Value | Maximal Value |
---|---|---|---|---|---|---|
Black locust honey | A1 | 0.013 | 0.002 | 0.001 | 0.009 | 0.016 |
A2 | 0.008 | 0.003 | 0.001 | 0.004 | 0.013 | |
Linden honey | A1 | 0.008 | 0.002 | 0.0002 | 0.006 | 0.011 |
A2 | 0.009 | 0.002 | 0.001 | 0.007 | 0.013 | |
Multifloral honey | A1 | 0.008 | 0.002 | 0.0002 | 0.006 | 0.011 |
A2 | 0.008 | 0.003 | 0.001 | 0.002 | 0.013 | |
Rapeseed honey | A1 | 0.018 | 0.002 | 0.001 | 0.014 | 0.021 |
A2 | 0.008 | 0.003 | 0.001 | 0.002 | 0.012 | |
Propolis | A1 | 0.022 | 0.002 | 0.0005 | 0.019 | 0.024 |
A2 | 0.010 | 0.002 | 0.001 | 0.007 | 0.013 |
Sample | Area | Mean Value | Standard Deviation | Standard Error | Minimal Value | Maximal Value |
---|---|---|---|---|---|---|
Black locust honey | A1 | 0.085 | 0.003 | 0.001 | 0.081 | 0.089 |
A2 | 0.011 | 0.003 | 0.001 | 0.006 | 0.015 | |
Linden honey | A1 | 0.064 | 0.002 | 0.001 | 0.059 | 0.067 |
A2 | 0.014 | 0.003 | 0.001 | 0.01 | 0.018 | |
Multifloral honey | A1 | 0.045 | 0.003 | 0.001 | 0.041 | 0.049 |
A2 | 0.019 | 0.003 | 0.001 | 0.014 | 0.023 | |
Rapeseed honey | A1 | 0.097 | 0.003 | 0.001 | 0.093 | 0.101 |
A2 | 0.020 | 0.003 | 0.001 | 0.015 | 0.024 | |
Propolis | A1 | 0.128 | 0.002 | 0.001 | 0.125 | 0.131 |
A2 | 0.020 | 0.003 | 0.001 | 0.016 | 0.024 |
Sample | Area | Mean Value | Standard Deviation | Standard Error | Minimal Value | Maximal Value |
---|---|---|---|---|---|---|
Black locust honey | A1 | 0.026 | 0.0002 | 0.001 | 0.025 | 0.027 |
A2 | 0.008 | 0.001 | 0.002 | 0.007 | 0.009 | |
Linden honey | A1 | 0.028 | 0.0002 | 0.001 | 0.027 | 0.029 |
A2 | 0.009 | 0.001 | 0.002 | 0.008 | 0.010 | |
Multifloral honey | A1 | 0.029 | 0.0002 | 0.001 | 0.028 | 0.030 |
A2 | 0.009 | 0.001 | 0.002 | 0.008 | 0.010 | |
Rapeseed honey | A1 | 0.024 | 0.001 | 0.002 | 0.023 | 0.025 |
A2 | 0.008 | 0.001 | 0.003 | 0.007 | 0.009 | |
Propolis | A1 | 0.031 | 0.0002 | 0.001 | 0.030 | 0.032 |
A2 | 0.010 | 0.001 | 0.003 | 0.008 | 0.011 |
Sample | Area | Mean Value | Standard Deviation | Standard Error | Minimal Value | Maximal Value |
---|---|---|---|---|---|---|
Black locust honey | A1 | 0.051 | 0.002 | 0.001 | 0.048 | 0.053 |
A2 | 0.052 | 0.002 | 0.001 | 0.048 | 0.056 | |
Linden honey | A1 | 0.044 | 0.002 | 0.001 | 0.041 | 0.048 |
A2 | 0.055 | 0.002 | 0.001 | 0.052 | 0.059 | |
Multifloral honey | A1 | 0.055 | 0.002 | 0.001 | 0.052 | 0.057 |
A2 | 0.049 | 0.002 | 0.001 | 0.045 | 0.053 | |
Rapeseed honey | A1 | 0.037 | 0.002 | 0.0006 | 0.035 | 0.040 |
A2 | 0.063 | 0.002 | 0.001 | 0.059 | 0.066 | |
Propolis | A1 | 0.069 | 0.002 | 0.001 | 0.065 | 0.072 |
A2 | 0.069 | 0.002 | 0.001 | 0.065 | 0.072 |
Sample | Area | Mean Value | Standard Deviation | Standard Error | Minimal Value | Maximal Value |
---|---|---|---|---|---|---|
Black locust honey | A1 | 0.004 | 0.001 | 0.0002 | 0.002 | 0.006 |
A2 | 0.007 | 0.002 | 0.001 | 0.003 | 0.011 | |
Linden honey | A1 | 0.006 | 0.001 | 0.0003 | 0.004 | 0.008 |
A2 | 0.007 | 0.002 | 0.001 | 0.003 | 0.010 | |
Multifloral honey | A1 | 0.010 | 0.001 | 0.0002 | 0.009 | 0.012 |
A2 | 0.006 | 0.002 | 0.001 | 0.002 | 0.010 | |
Rapeseed honey | A1 | 0.005 | 0.001 | 0.0001 | 0.003 | 0.007 |
A2 | 0.007 | 0.002 | 0.001 | 0.004 | 0.010 | |
Propolis | A1 | 0.013 | 0.001 | 0.0004 | 0.011 | 0.014 |
A2 | 0.008 | 0.002 | 0.001 | 0.004 | 0.011 |
Sample | Area | Mean Value | Standard Deviation | Standard Error | Minimal Value | Maximal Value |
---|---|---|---|---|---|---|
Black locust honey | A1 | 0.031 | 0.002 | 0.001 | 0.028 | 0.034 |
A2 | 0.033 | 0.003 | 0.001 | 0.028 | 0.039 | |
Linden honey | A1 | 0.026 | 0.002 | 0.001 | 0.022 | 0.029 |
A2 | 0.026 | 0.004 | 0.001 | 0.021 | 0.031 | |
Multifloral honey | A1 | 0.018 | 0.003 | 0.001 | 0.014 | 0.022 |
A2 | 0.035 | 0.005 | 0.001 | 0.028 | 0.042 | |
Rapeseed honey | A1 | 0.032 | 0.003 | 0.001 | 0.027 | 0.036 |
A2 | 0.030 | 0.004 | 0.001 | 0.024 | 0.036 | |
Propolis | A1 | 0.043 | 0.002 | 0.001 | 0.039 | 0.046 |
A2 | 0.046 | 0.004 | 0.001 | 0.039 | 0.052 |
Sample | Area | Mean Value | Standard Deviation | Standard Error | Minimal Value | Maximal Value |
---|---|---|---|---|---|---|
Black locust honey | A1 | 0.00356 | 0.00018 | 0.00005 | 0.00333 | 0.00385 |
A2 | 0.00175 | 0.00019 | 0.00006 | 0.00148 | 0.00203 | |
Linden honey | A1 | 0.0026 | 0.00011 | 0.00003 | 0.00244 | 0.00279 |
A2 | 0.00212 | 0.00015 | 0.00004 | 0.00191 | 0.00237 | |
Multifloral honey | A1 | 0.00432 | 0.00016 | 0.00005 | 0.00406 | 0.00455 |
A2 | 0.00204 | 0.00017 | 0.00005 | 0.00182 | 0.0023 | |
Rapeseed honey | A1 | 0.0039 | 0.00018 | 0.00005 | 0.00362 | 0.00418 |
A2 | 0.00179 | 0.00021 | 0.00006 | 0.0015 | 0.00211 | |
Propolis | A1 | 0.00513 | 0.00016 | 0.00005 | 0.00486 | 0.00535 |
A2 | 0.00248 | 0.00021 | 0.00006 | 0.0022 | 0.00281 |
Sample | Area | Mean Value | Standard Deviation | Standard Error | Minimal Value | Maximal Value |
---|---|---|---|---|---|---|
Black locust honey | A1 | 0.545 | 0.094 | 0.027 | 0.396 | 0.708 |
A2 | 0.513 | 0.283 | 0.082 | 0.077 | 0.923 | |
Linden honey | A1 | 0.373 | 0.094 | 0.027 | 0.229 | 0.542 |
A2 | 0.423 | 0.291 | 0.084 | 0.077 | 0.923 | |
Multifloral honey | A1 | 0.649 | 0.088 | 0.025 | 0.500 | 0.771 |
A2 | 0.064 | 0.355 | 0.102 | 0.385 | 1.538 | |
Rapeseed honey | A1 | 0.556 | 0.094 | 0.027 | 0.396 | 0.708 |
A2 | 0.058 | 0.373 | 0.108 | 0.462 | 1.615 | |
Propolis | A1 | 0.668 | 0.129 | 0.037 | 0.458 | 0.854 |
A2 | 0.981 | 0.403 | 0.116 | 0.308 | 1.615 |
Sample | Area | Mean Value | Standard Deviation | Standard Error | Minimal Value | Maximal Value |
---|---|---|---|---|---|---|
Black locust honey | A1 | 0.476 | 0.151 | 0.044 | 0.286 | 0.762 |
A2 | 0.789 | 0.238 | 0.069 | 0.4 | 1.2 | |
Linden honey | A1 | 0.389 | 0.224 | 0.065 | 0.119 | 0.762 |
A2 | 0.450 | 0.314 | 0.091 | 0.067 | 1.067 | |
Multifloral honey | A1 | 0.397 | 0.136 | 0.039 | 0.167 | 0.619 |
A2 | 0.456 | 0.274 | 0.079 | 0.067 | 0.933 | |
Rapeseed honey | A1 | 0.518 | 0.145 | 0.042 | 0.286 | 0.762 |
A2 | 0.700 | 0.350 | 0.101 | 0.133 | 1.267 | |
Propolis | A1 | 0.589 | 0.107 | 0.031 | 0.429 | 0.762 |
A2 | 0.767 | 0.293 | 0.085 | 0.333 | 1.333 |
Sample | Area | Mean Value | Standard Deviation | Standard Error | Minimal Value | Maximal Value |
---|---|---|---|---|---|---|
Black locust honey | A1 | 0.381 | 0.080 | 0.080 | 0.283 | 0.509 |
A2 | 0.598 | 0.287 | 0.287 | 0.176 | 1 | |
Linden honey | A1 | 0.285 | 0.049 | 0.049 | 0.208 | 0.358 |
A2 | 0.343 | 0.223 | 0.223 | 0.059 | 0.706 | |
Multifloral honey | A1 | 0.561 | 0.126 | 0.126 | 0.358 | 0.736 |
A2 | 0.725 | 0.304 | 0.304 | 0.176 | 1.118 | |
Rapeseed honey | A1 | 0.398 | 0.085 | 0.085 | 0.415 | 0.736 |
A2 | 0.559 | 0.309 | 0.309 | 0.471 | 1.294 | |
Propolis | A1 | 0.568 | 0.099 | 0.099 | 0.283 | 0.509 |
A2 | 0.877 | 0.260 | 0.260 | 0.059 | 1 |
Contaminant | EDI * | HQ | RfD [46] (mg/kg bw) | ||
---|---|---|---|---|---|
A1 | A2 | A1 | A2 | ||
Cd | 1.75 × 10−6 | 0.56 × 10−6 | 1.75 × 10−3 | 0.56 × 10−3 | 0.001 |
Cu | 7.60 × 10−5 | 1.30 × 10−5 | 1.52 × 10−4 | 0.26 × 10−4 | 0.5 |
Zn | 9.00 × 10−3 | 2.10 × 10−3 | 1.50 × 10−4 | 0.35 × 10−4 | 1 |
Mn | 6.40 × 10−5 | 3.30 × 10−5 | 4.30 × 10−5 | 2.20 × 10−5 | 1.5 |
Pb | 1.40 × 10−5 | 0.50 × 10−5 | 4.00 × 10−3 | 1.40 × 10−3 | 0.0035 |
Ni | 3.00 × 10−5 | 2.40 × 10−5 | 2.40 × 10−3 | 1.50 × 10−3 | 0.02 |
Cr | 6.60 × 10−5 | 6.20 × 10−5 | 4.70 × 10−4 | 4.40 × 10−4 | 0.14 |
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Mititelu, M.; Udeanu, D.I.; Nedelescu, M.; Neacsu, S.M.; Nicoara, A.C.; Oprea, E.; Ghica, M. Quality Control of Different Types of Honey and Propolis Collected from Romanian Accredited Beekeepers and Consumer’s Risk Assessment. Crystals 2022, 12, 87. https://doi.org/10.3390/cryst12010087
Mititelu M, Udeanu DI, Nedelescu M, Neacsu SM, Nicoara AC, Oprea E, Ghica M. Quality Control of Different Types of Honey and Propolis Collected from Romanian Accredited Beekeepers and Consumer’s Risk Assessment. Crystals. 2022; 12(1):87. https://doi.org/10.3390/cryst12010087
Chicago/Turabian StyleMititelu, Magdalena, Denisa Ioana Udeanu, Mirela Nedelescu, Sorinel Marius Neacsu, Anca Cecilia Nicoara, Eliza Oprea, and Manuela Ghica. 2022. "Quality Control of Different Types of Honey and Propolis Collected from Romanian Accredited Beekeepers and Consumer’s Risk Assessment" Crystals 12, no. 1: 87. https://doi.org/10.3390/cryst12010087
APA StyleMititelu, M., Udeanu, D. I., Nedelescu, M., Neacsu, S. M., Nicoara, A. C., Oprea, E., & Ghica, M. (2022). Quality Control of Different Types of Honey and Propolis Collected from Romanian Accredited Beekeepers and Consumer’s Risk Assessment. Crystals, 12(1), 87. https://doi.org/10.3390/cryst12010087