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Hydrothermal Carbonization of Municipal Waste Streams

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Hydrothermal Carbonization of Municipal Waste Streams ARTICLE pubs.acs.org/est Hydrothermal Carbonization of Municipal Waste Streams ,† ‡ § † || Nicole D. Berge,*^ Kyoung S. Ro, Jingdong Mao, Joseph R. V. Flora, Mark A. Chappell, and Sunyoung Bae † Department of Civil and Environmental Engineering, University of South Carolina, 300 Main Street, Columbia, South Carolina 29208, United States ‡ USDA-ARS Coastal Plains Soil, Water, and Plant Research Center, 2611 West Lucas Street, Florence, South Carolina 29501, United States §Department of Chemistry and Biochemistry, Old Dominion University, 4541 Hampton Boulevard, Norfolk, Virginia 23529, United States Environmental) Laboratory, U.S. Army Corps of Engineers, 3909 Halls Ferry Road, Vicksburg, Mississippi 39180, United States ^ Department of Chemistry, Seoul Women’s University, 139-774 126 Gongreung-Dong, Nowon-Gu, Seoul, Korea bS Supporting Information ABSTRACT: Hydrothermal carbonization (HTC) is a novel thermal conver- sion process that can be used to convert municipal waste streams into sterilized, value-added hydrochar. HTC has been mostly applied and studied on a limited number of feedstocks, ranging from pure substances to slightly more complex biomass such as wood, with an emphasis on nanostructure generation. There has been little work exploring the carbonization of complex waste streams or of utilizing HTC as a sustainable waste management technique. The objectives of this study were to evaluate the environmental implications associated with the carbonization of representative municipal waste streams (including gas and liquid products), to evaluate the physical, chemical, and thermal properties of the produced hydrochar, and to determine carbonization energetics associated with each waste stream. Results from batch carbonization experiments indicate 49À75% of the initially present carbon is retained within the char, while 20À37% and 2À11% of the carbon is transferred to the liquid- and gas-phases, respectively. The composition of the produced hydrochar suggests both dehydration and decarboxylation occur during carbonization, resulting in structures with high aromaticities. Process energetics suggest feedstock carbonization is exothermic. ’ INTRODUCTION promoted, ultimately enhancing hydrolysis.4 Because hydrolysis Hydrothermal carbonization (HTC) is a novel thermal con- exhibits a lower activation energy than many dry thermochemical version process that can be a viable means for treating/stabilizing conversion reactions, lower temperature HTC reactions can proceed with the same level of conversion efficiency as higher waste streams while minimizing greenhouse gas production and 1,4 producing residual material with intrinsic value. HTC is a wet, temperature processes. relatively low temperature (180À350 °C) process that, under To date, HTC has been mostly applied and studied on a limited number of feedstocks (Table SIÀS3), ranging from pure autogenous pressures, has been reported as a method to convert 1 carbohydrates into a carbonaceous residue referred to as hydro- substances to slightly more complex biomass such as wood. char. HTC was first experimentally explored as a means to Recent motivations for utilizing this technique have concentrated produce coal from cellulose in 1913 by Bergius.1,2 This process on creating novel low-cost carbon-based nanomaterials/nano- À 12,13 has been shown to be exothermic in nature for pure compounds2 4 structures from carbohydrates, rather than on exploring the use of HTC as a sustainable waste management technique.1 Results and energetically more advantageous than dry carbonization fi processes (e.g., pyrolysis) for feedstocks containing moisture.1,5 from previous studies indicate a signi cant fraction of carbon Titirici et al.6 Sevilla and Fuertes,7,8 and Funke and Zeigler 4 remains within the hydrochar during the HTC process, suggesting carbonization of waste streams may mitigate greenhouse gas report that char formation results from a series of hydrolysis, 1,2,4,6À8 condensation, decarboxylation, and dehydration reactions. emissions. Reported percentages of carbon bound within Water is a necessary and key ingredient of HTC.2,4 As tempera- tures increase, the physical and chemical properties of water Received: February 8, 2011 À change significantly, mimicking that of organic solvents.9 11 Accepted: May 24, 2011 Consequently, saturation concentrations of dissolved inorganic Revised: April 17, 2011 and organic components increase greatly and ionic reactions are Published: June 14, 2011 r 2011 American Chemical Society 5696 dx.doi.org/10.1021/es2004528 | Environ. Sci. Technol. 2011, 45, 5696–5703 Environmental Science & Technology ARTICLE I Table 1. Proximate and Ultimate Analysis of Initial Feedstocks and Produced Hydrochar initial feedstock hydrochar parameters paper food mixed MSW AD waste (dried) paper food mixed MSW AD waste proximate analysesa moisture (%) 7.6 12.6 6.3 8.1 3.2 5.7 5.9 3.3 b volatile matter (%db) 79.6 77.6 62.0 55.9 52.8 53.4 33.6 34.5 fi xed C (%db) 9.6 14.8 9.6 8.2 19.8 29.7 14.6 6.4 a ash (%db) 10.9 7.5 28.4 35.9 24.2 11.2 46.0 55.8 HHV (MJ/kgdb) 14.0 18.1 16.5 15.5 23.9 29.1 20.0 13.7 ultimate analysesc H(%db) 5.0 5.8 3.8 4.8 4.6 5.8 2.7 3.9 C(%db) 36.0 42.5 28.5 32.6 57.4 67.6 33.5 27.8 O(%db) 48.1 40.8 38.7 20.3 12.8 9.9 14.2 7.8 N(%db) 0.04 3.2 0.56 5.5 0.07 4.6 0.63 2.0 S(%db) 0.02 0.22 0.05 0.92 0.05 0.22 0.05 0.77 d ( ( ( ( av hydrochar yield (%db) 29.2 0.24 43.8 3.2 63.2 5.0 47.1 13 e av hydrochar yield (%daf) 34.1 45.6 83.8 25.6 fixed carbon yield (%)f 8.5 15.8 23.9 10.6 energetic retention efficiency (%)g 49.8 70.3 76.8 41.5 energy densificationh 2.2 1.82 1.73 1.5 a b c d e f fi ASTM D3172. ASTM D3175-07. ASTM D3176-02. (Mdb,char/Mdb,feedstock)*100. Mdaf,char/Mdaf,feedstock. % char yield*(% xed carbondaf,char/ fi g h I (100-%ashfeedstock)), as de ned by ref 31. (Mchar*HHVchar)/(Mfeedstock*HHVfeedstock). HHVchar/HHVfeedstock. db = dry basis; daf = dry ash free basis. the hydrochar (20À100%) vary significantly with feedstock and were chosen for evaluation: paper (33% (wt.) of waste discarded reaction conditions (Table SIÀS3). Titirici et al.2 report changes in landfills), food waste, mixed municipal solid waste (MSW), in feedstock composition influences degradation pathways and and anaerobic digestion (AD) waste. Discarded office paper was hydrochar’s physical and chemical structure. as the paper feedstock; it was shredded (2 Â 10-mm rectangles) The potential to use the carbonized wastes (i.e., hydrochar) prior to use. Rabbit food was used to simulate food wastes for environmental- and energy-related applications adds to the discarded in landfills (following ref 20) and was crushed prior to attractiveness of this approach. The char produced via HTC use. Mixed MSW was simulated using representative waste contains attractive surface functionalization patterns2,6,8,14 that materials and mixed to achieve distributions typically landfilled.21 make the char amendable to beneficial end-use applications such Composition of the mixed MSW (wt. basis) is as follows: 45.5% as an adsorbent for harmful pollutants,15 feedstock for carbon paper (shredded discarded office paper), 9.6% glass (crushed glass fuel cells,16,17 and a soil amendment (similar to char from bottles), 16.4% plastic (shredded discarded plastic bottles), 17.6% pyrolysis/gasification, e.g., ref 18). Liu et al.15 demonstrated that food (crushed rabbit food), and 10.9% metal (shredded discarded hydrochar had a much higher capacity for copper removal (e.g., ion aluminum cans). AD waste (sludge) was chosen to represent human exchange) than that of char produced via pyrolysis. In addition, municipal waste and was acquired from an anaerobic digester at a HTC of waste materials may require less solids processing/ local wastewater treatment facility. Table 1 contains the physical and treatment (such as mechanical dewatering of biosolids1,19)and chemical characteristics associated with these feedstocks. handling (hydrochar is sterilized). Carbonization may also ther- Carbonization Experiments. HTC of the waste streams was mally degrade or transform emerging compounds, such as phar- conducted in 160-mL stainless steel tubular reactors rated to maceuticals, personal care products, and endocrine disrupting withstand anticipated temperatures and pressures. Carboniza- compounds, which currently pose significant environmental con- tion of the feedstocks was conducted by loading each reactor with cerns/treatment challenges in waste streams.1 dry solids and DI water to obtain a solids concentration of 20% The purpose of this study was to determine the feasibility of (wt.). The AD waste was received as a wet waste stream, hydrothermally carbonizing model municipal waste streams. The consisting of approximately 3.0% (wt.) solids. The total mass specific objectives of this study were to (1) evaluate the environ- of AD waste added to each reactor was equivalent to the total mental implications associated with the carbonization of representa- mass of that added to reactors containing the dry feedstock. All tive municipal waste streams (municipal solid waste and human liquid reactors were heated to 250 °C in a laboratory oven for 20 h. The wastes), including the gas and liquid products; (2) evaluate the reactors were removed from the oven and subsequently placed in physical, chemical, and thermal properties of the hydrochar; and (3) a cold water bath to quench the reaction. After the reactors were determine carbonization energetics associated with each waste stream. cooled, samples from the solid (proximate and ultimate analysis, energy content, 13C solid-state NMR), liquid (total organic ’ MATERIALS AND METHODS carbon (TOC), pH, chemical oxygen demand (COD), biochem- ical oxygen demand (BOD)), and gas phases (gas volume and Feedstocks.
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