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Frontiers of Agricultural Science and Engineering

ISSN 2095-7505

ISSN 2095-977X(Online)

CN 10-1204/S

Postal Subscription Code 80-906

Front. Agr. Sci. Eng.    2023, Vol. 10 Issue (3) : 437-447    https://doi.org/10.15302/J-FASE-2023507
RESEARCH ARTICLE
ASSESSMENT OF HEAVY METALS IN HYDROCHAR PRODUCED BY HYDROTHERMAL CARBONIZATION OF DAIRY MANURE
B. Brian HE1(), Zheting BI2, Lide CHEN3
1. Chemical & Biological Engineering, College of Engineering, University of Idaho, 875 Perimeter Drive MS 0904, Moscow, ID 83844, USA
2. Shape Therapeutics, 700 Dexter Avenue North, SL15, Seattle, WA 98109, USA
3. Soil and Water Systems, Twin Falls Research and Extension Center, University of Idaho, 315 Falls Ave., Twin Falls, ID 83303, USA
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Abstract

● Content of heavy metals in hydrochar varies considerably, from 50% to 100%.

● Concentrations of heavy metals in hydrochar can be higher than those in the dairy manure.

● Concentrations of heavy metals in hydrochar are far below the regulatory level.

Hydrochar produced from dairy manure is a regulated biosolid if being promoted for agricultural applications thus must have the properties that comply with all environmental standards and government regulations, including the levels of heavy metals (HMs). In this study, systematic research was conducted on HM levels in hydrochar from dairy manure and on the effects of processing conditions, including processing temperature (180–255 °C), holding time (30120 min) and solid content of manure slurry (2%15%), through a central composite design and statistical analyses. It was found that HMs can be retained in hydrochar, ranging from 40% to 100%. The processing temperature and solid content in the feed were the most influential process parameters that affected HMs retention in hydrochar. Statistical analysis showed that there was no single optimal point to minimize HMs retained in hydrochar, but there were minimization points at given processing time and solid content. Most HMs concentrations were higher in hydrochar than those initially in dairy manure but were greatly below the thresholds as set by the US government regulations. Thus, hydrochar is feasible for use as a phosphorus-enriched organic fertilizer and/or soil amendment for agricultural applications without serious concerns about HMs it might contain.

Keywords heavy metals      dairy manure      hydrochar      hydrothermal carbonization      waste management     
Corresponding Author(s): B. Brian HE   
Just Accepted Date: 26 May 2023   Online First Date: 28 June 2023    Issue Date: 20 September 2023
 Cite this article:   
B. Brian HE,Zheting BI,Lide CHEN. ASSESSMENT OF HEAVY METALS IN HYDROCHAR PRODUCED BY HYDROTHERMAL CARBONIZATION OF DAIRY MANURE[J]. Front. Agr. Sci. Eng. , 2023, 10(3): 437-447.
 URL:  
https://academic.hep.com.cn/fase/EN/10.15302/J-FASE-2023507
https://academic.hep.com.cn/fase/EN/Y2023/V10/I3/437
Heavy metal Ceiling concentration (mg·kg−1) Cumulative loading rate (kg·ha−1) Monthly average concentration (mg·kg−1) Annual loading rate (kg·ha−1·yr−1)
Arsenic* 75 41 41 2
Cadmium* 85 39 39 1.9
Chromium* 3000 3000 1200 150
Copper 4300 1500 1500 75
Lead* 840 300 300 15
Mercury* 57 17 17 0.85
Molybdenum 75
Nickel 420 420 420 21
Selenium* 100 100 36 5
Zinc 7500 2800 2800 140
Tab.1  US Environmental Protection Agency regulatory determination and pollutant limits for land applied sewage sludge§
Heavy metal* Manure sample§ Analytical detection limit (mg·kg−1)
Oven-dried (mg·kg−1) Air-dried (mg·kg−1)
Arsenic nd nd 40
Barium 50.3 ± 3.5 47.3 ± 3.2 0.8
Cadmium nd nd 0.8
Chromium 15.0 ± 1.0 18.3 ± 1.5 2
Copper 94.0 ± 4.4 88.3 ± 58.0 4
Lead nd nd 10
Molybdenum nd nd 10
Nickel 6.3 ± 0.2 6.1 ± 0.3 2
Zinc 267 ± 11.5 250 ± 10.0 2
Tab.2  Heavy metal contents in the dairy manure used for this study
Run no. Process variables Cr retention rate§ (%)
Temperature (A) (°C) Time (B) (min) Solid content (C) (%, m/m) Average SD
1 195 30 5 26.33 4.16
2 195 30 15 20.33 0.58
3 195 90 5 26.00 2.65
4 195 90 15 21.00 1.00
5 235 30 5 32.67 5.51
6 235 30 15 21.67 0.58
7 235 90 5 34.00 1.00
8 235 90 15 17.67 11.85
9 215 60 10 25.33 0.58
10 195 60 10 23.33 0.58
11 235 60 10 27.00 1.00
12 215 30 10 23.00 0.00
13 215 90 10 25.00 1.00
14 215 60 5 25.33 1.53
15 215 60 15 21.67 2.08
Tab.3  Process parameters in CCD and experimental results on Cr retention in hydrochar
Fig.1  Processing temperature effect on (a) concentrations and (b) retention rates of heavy metals in manure and hydrochar samples. Experiments were conducted in triplicate at 60 min of processing holding time and 10% of solid content.
Fig.2  Effect of processing holding time on (a) concentrations and (b) retention rates of heavy metals in manure and hydrochar samples. Experiments were conducted in triplicate at 215 °C and 10% of solid content.
Fig.3  Effect of solid content on (a) concentrations and (b) retention rates of heavy metals in manure and hydrochar samples. Experiments were conducted in triplicate at 215 °C and 60 min of processing holding time.
Source SS df MS F P Concentration (%)
Processing temperature (A) 85.5 2 42.8 1.84 0.1871 7.1
Holding time (B) 0.2 2 0.1 0.0049 0.9951 0.0
Solid content (C) 530.7 2 265.3 11.4 0.0006 43.8
A × B 12.5 4 3.1 0.134 0.9676 1.0
A × C 144.6 4 36.2 1.56 0.2283 11.9
B × C 8.7 4 2.2 0.0941 0.9831 0.7
A × B × C 17.3 8 2.2 0.0932 0.9990 1.4
Error/Residual 417.7 18 23.2 34.5
Total 1211.6 44
Tab.4  ANOVA of process parameters on Cr retention rates in hydrochar
Source Coeff.§ P (2 tails)
Constant 24.28 0.000
Processing temperature (A) 1.600 0.024
Holding time (B) –0.033 0.961
Solid content (C) –4.200 0.000
A × B –0.375 0.624
A × C –2.042 0.011
B × C –0.542 0.480
A × B × C –0.792 0.304
R2 0.6128
F 5.382
Tab.5  Y-hat model regression*
Fig.4  Multiple plots of process parameters and interactions on Cr retention rates.
Fig.5  Y-hat interaction plots showing the effects of (a) process parameters of processing temperature, holding time and solid content and (b) processing temperature and time at a constant solid content of 10%.
Heavy metal Concentration in hydrochar* (mg·kg–1)
Arsenic < 40
Barium 44–60
Cadmium < 0.8
Chromium 21–30
Copper 130–183
Lead < 10
Mercury nt
Molybdenum < 10
Nickel 19–49
Selenium nt
Zinc 373–473
Tab.6  Summary of heavy metals in hydrochar produced from dairy manure under various processing condition
1 S M, Heilmann J S, Molde J G, Timler B M, Wood A L, Mikula G V, Vozhdayev E C, Colosky K A, Spokas K J Valentas . Phosphorus reclamation through hydrothermal carbonization of animal manures. Environmental Science & Technology, 2014, 48(17): 10323–10329
https://doi.org/10.1021/es501872k
2 B B, He L Chen . Hydrochar as a vehicle for phosphorus cycling from dairy manure to cropland. Global Journal of Engineerring Sciences, 2021, 7(5): GJES.MS.ID.000672
3 F, Zhang Y, Li M, Yang W Li . Content of heavy metals in animal feeds and manures from farms of different scales in northeast China. International Journal of Environmental Research and Public Health, 2012, 9(8): 2658–2668
https://doi.org/10.3390/ijerph9082658
4 F A, Nicholson B J, Chambers J R, Williams R J Unwin . Heavy metal contents of livestock feeds and animal manures in England and Wales. Bioresource Technology, 1999, 70(1): 23–31
https://doi.org/10.1016/S0960-8524(99)00017-6
5 M, Irshad A H, Malik S, Shaukat S, Mushtaq M Ashraf . Characterization of heavy metals in livestock manures. Polish Journal of Environmental Studies, 2013, 22(4): 1257–1262
6 L, Bouwman K K, Goldewijk Der Hoek K W, Van A H W, Beusen Vuuren D P, Van J, Willems M C, Rufino E Stehfest . Exploring global changes in nitrogen and phosphorus cycles in agriculture induced by livestock production over the 1900–2050 period. Proceedings of the National Academy of Sciences of the United States of America, 2013, 110(52): 20882–20887
https://doi.org/10.1073/pnas.1012878108
7 E Brands . Siting restrictions and proximity of Concentrated Animal Feeding Operations to surface water. Environmental Science & Policy, 2014, 38: 245–253
https://doi.org/10.1016/j.envsci.2014.01.006
8 P A, Vadas J M Powell . Monitoring nutrient loss in runoff from dairy cattle lots. Agriculture, Ecosystems & Environment, 2013, 181: 127–133
https://doi.org/10.1016/j.agee.2013.09.025
9 R, Liu J, Wang J, Shi Y, Chen C, Sun P, Zhang Z Shen . Runoff characteristics and nutrient loss mechanism from plain farmland under simulated rainfall conditions. Science of the Total Environment, 2014, 468–469: 1069–1077
10 Q, Lang M, Chen Y, Guo Z, Liu C Gai . Effect of hydrothermal carbonization on heavy metals in swine manure: speciation, bioavailability and environmental risk. Journal of Environmental Management, 2019, 234: 97–103
https://doi.org/10.1016/j.jenvman.2018.12.073
11 R, Anjum E, Grohmann N Krakat . Anaerobic digestion of nitrogen rich poultry manure: impact of thermophilic biogas process on metal release and microbial resistances. Chemosphere, 2017, 168: 1637–1647
https://doi.org/10.1016/j.chemosphere.2016.11.132
12 Q, Lang Y, Guo Q, Zheng Z, Liu C Gai . Co-hydrothermal carbonization of lignocellulosic biomass and swine manure: hydrochar properties and heavy metal transformation behavior. Bioresource Technology, 2018, 266: 242–248
https://doi.org/10.1016/j.biortech.2018.06.084
13 States Environmental Protection Agency (US EPA) United . A Plain English Guide to the EPA Part 503 Biosolids Rule. US EPA, 1994. Available at US EPA website on May 11, 2023
14 M, Rajkumar Y, Ma H Freitas . Improvement of Ni phytostabilization by inoculation of Ni resistant Bacillus megaterium SR28C. Journal of Environmental Management, 2013, 128: 973–980
https://doi.org/10.1016/j.jenvman.2013.07.001
15 J, Lehmann S Joseph . Biochar for Environmental Management—Science, Technology and Implementation. 2nd ed. New York: Routledge, Taylro & Grancis Group, 2015
16 Z, Liu A, Quek Hoekman S, Kent M P, Srinivasan R Balasubramanian . Thermogravimetric investigation of hydrochar-lignite co-combustion. Bioresource Technology, 2012, 123: 646–652
https://doi.org/10.1016/j.biortech.2012.06.063
17 L Githinji . Effect of biochar application rate on soil physical and hydraulic properties of a sandy loam. Archives of Agronomy and Soil Science, 2014, 60(4): 457–470
https://doi.org/10.1080/03650340.2013.821698
18 X, Cao L, Ma Y, Liang B, Gao W Harris . Simultaneous immobilization of lead and atrazine in contaminated soils using dairy-manure biochar. Environmental Science & Technology, 2011, 45(11): 4884–4889
https://doi.org/10.1021/es103752u
19 J W, Lee B, Hawkins D M, Day D C Reicosky . Sustainability: the capacity of smokeless biomass pyrolysis for energy production, global carbon capture and sequestration. Energy & Environmental Science, 2010, 3(11): 1695–1705
https://doi.org/10.1039/c004561f
20 States Environmental Protection Agency (US EPA) United . Use of Composting for Biosolids Management. US EPA, 2022. Available at US EPA website on May 11, 2023
21 M T, Reza J G, Lynam M H, Uddin C J Coronella . Hydrothermal carbonization: fate of inorganics. Biomass and Bioenergy, 2013, 49: 86–94
https://doi.org/10.1016/j.biombioe.2012.12.004
22 X, Wang C, Li B, Zhang J, Lin Q, Chi Y Wang . Migration and risk assessment of heavy metals in sewage sludge during hydrothermal treatment combined with pyrolysis. Bioresource Technology, 2016, 221: 560–567
https://doi.org/10.1016/j.biortech.2016.09.069
23 X, Xu E Jiang . Treatment of urban sludge by hydrothermal carbonization. Bioresource Technology, 2017, 238: 182–187
https://doi.org/10.1016/j.biortech.2017.03.174
24 H, Fu B, Wang H, Wang H, Liu H, Xie L, Han N, Wang L, Sun Y, Feng L Xue . Assessment of livestock manure-derived hydrochar as cleaner products: insights into basic properties, nutrient composition, and heavy metal content. Journal of Cleaner Production, 2022, 330: 129820
https://doi.org/10.1016/j.jclepro.2021.129820
25 C, Song W, Yuan S, Shan Q, Ma H, Zhang X, Wang N K, Niazi H Wang . Changes of nutrients and potentially toxic elements during hydrothermal carbonization of pig manure. Chemosphere, 2020, 243: 125331
https://doi.org/10.1016/j.chemosphere.2019.125331
26 G, Chen J, Wang F, Yu X, Wang H, Xiao B, Yan X Cui . A review on the production of P-enriched hydro/bio-char from solid waste: transformation of P and applications of hydro/bio-char. Chemosphere, 2022, 301: 134646
https://doi.org/10.1016/j.chemosphere.2022.134646
27 H, Wang Z, Yang X, Li Y Liu . Distribution and transformation behaviors of heavy metals and phosphorus during hydrothermal carbonization of sewage sludge. Environmental Science and Pollution Research International, 2020, 27(14): 17109–17122
https://doi.org/10.1007/s11356-020-08098-4
28 Congress US . Resource Conservation and Recovery Act. Public Law 94–580. US Congress, 1976. Available at US government information website on May 11, 2023
29 Society of Agricultural and Biological Engineers (ASABE) American . ANSI/ASAE S358.3 MAY2012 (R2021). Moisture measurement—Forages. St. Joseph, Ml: ASABE, 2021
30 K, Anderson G, Farwell P, Gibson B Ricks . Total recoverable elements in biological, plant, and animal tissue and feed samples. Standard Methods SMM.57.070.04. Moscow: Analytical Sciences Laboratory, University of Idaho, 2017
31 B B He . Batch process operational effects on phosphorus attainment in hydrochar produced by hydrothermal carbonization of dairy manure. Journal of the American Society of Agricultural and Biological Engineers, 2023, 66(1): 141–148
https://doi.org/10.13031/ja.15194
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