TY - JOUR
AU - Wang, Wenju
AB - Abstract Coal is the dominant composition of fossil fuel but, with the accompanying gaseous products, causes environmental pollution. Here, we report a methodology to improve C conversion in co-gasification. The steam gasification and chemical looping gasification (CLG) of lignite and rice husk with oxygen uncoupling over 5% NiO/CuO oxygen carrier were conducted by non-isothermal kinetics method in a fixed-bed reactor. The gasification results showed that the yields of gas products in CLG of lignite or rice husk are higher than that in steam gasification. The yields of gases in chemical looping co-gasification (CLCG) are higher than that in steam co-gasification. In the co-gasification, the complementation of reactivity between fuels facilitated the C conversion rate, so the yields in co-gasification were higher than in individual gasification. The C conversion in CLCG of lignite and rice husk is 14.51% higher than that in steam co-gasification. 1. INTRODUCTION Nowadays, coal is still a dominant traditional fossil fuel [1, 2] and the traditional application of coal is combustion; the accompanying gaseous products such as SO2, NOx and COx can cause environmental pollution [3–5]. Therefore, searching an efficient and clean utilization method for coal is of great significance to the harmonious development between human and environment. Gasification is exactly an efficient way of coal utilization because of the usefulness of derived chemical products [6, 7]. The chemical looping gasification (CLG) plays a key role in syngas generation. In the process of CLG, heat was transferred to solid fuel by oxygen carriers and the pure oxygen is replaced by the lattice oxygen of oxygen carrier [8–11]. Compared with the traditional gasification method, the gasification efficiency is higher in CLG; moreover, the demand of heat from outside and the cost of pure oxygen production are all saved. Table 1 Proximate and ultimate analyses of lignite and rice husk. . Proximate analysis (wt%, ad) . Ultimate analysis (wt%, daf) . . Mad . Vad . Aad . FCad . C . H . O . N . S . Lignite 9.90 46.80 17.60 25.70 78.22 3.74 15.19 1.63 1.22 Rice husk 7.40 73.78 11.01 7.81 23.40 10.26 64.13 0.77 1.44 . Proximate analysis (wt%, ad) . Ultimate analysis (wt%, daf) . . Mad . Vad . Aad . FCad . C . H . O . N . S . Lignite 9.90 46.80 17.60 25.70 78.22 3.74 15.19 1.63 1.22 Rice husk 7.40 73.78 11.01 7.81 23.40 10.26 64.13 0.77 1.44 ad indicates on air-dry basis; daf, on dry-ash-free basis. Open in new tab Table 1 Proximate and ultimate analyses of lignite and rice husk. . Proximate analysis (wt%, ad) . Ultimate analysis (wt%, daf) . . Mad . Vad . Aad . FCad . C . H . O . N . S . Lignite 9.90 46.80 17.60 25.70 78.22 3.74 15.19 1.63 1.22 Rice husk 7.40 73.78 11.01 7.81 23.40 10.26 64.13 0.77 1.44 . Proximate analysis (wt%, ad) . Ultimate analysis (wt%, daf) . . Mad . Vad . Aad . FCad . C . H . O . N . S . Lignite 9.90 46.80 17.60 25.70 78.22 3.74 15.19 1.63 1.22 Rice husk 7.40 73.78 11.01 7.81 23.40 10.26 64.13 0.77 1.44 ad indicates on air-dry basis; daf, on dry-ash-free basis. Open in new tab Biomass is a renewable and promising alternative energy source, and it is considered carbon-neutral during the utilization process [12]. Co-gasification of coal and biomass, considered as a bridge between energy productions based on fossil fuels and energy production based on renewable fuels, has been paid much attention in recent years [13–15]. In view of the high volatile content of biomass and the good reactivity of fixation carbon, co-gasification of them will make a big difference. The co-gasification promotes the temperature of gasification and the decomposition of tar and C conversion, and the utilization efficiency of fuel has been improved. In addition, the synergy in co-gasification improves the efficiency of gasification. The synergy is explained as the catalysis of alkali metal in biomass. Researchers found that biomass could promote the efficiency of coal gasification and enhance the syngas [16–18]. The synergy between biomass and coal is formed by the transformation, deactivation and catalytic effect of K in biomass as well as the process of transferring H radicals and active OH from biomass to coal [19]. Lignite is a kind of coal with the lowest degree of coalification, the highest porosity and the highest reactivity [20, 21]. The direct combustion of lignite brings serious air pollution; hence, it is important to improve the utilization of lignite to make up the disadvantages of low-grade coal. In addition, rice husk is a typical biomass resource, whose yields are ~148 million tons each year. If we cannot take full advantage of these rice hush, it is not only a waste of resources but also a pollution of the environment. Pyrolysis shows great potential to transform biomass rice husk into biofuels [22]; the rice husk coke was obtained after pyrolysis at 800°C for 5 h in N2. So, lignite and rice husk coke were selected as the coal and the biomass, respectively. It is important to select an efficient oxygen carrier in chemical looping co-gasification (CLCG) of coal and biomass. The thermodynamic characters, reactive properties, cost, physical strength, melting temperature and impacts on the environment of oxygen carriers are all needed to be considered while selecting the suitable catalysts [23]. In recent years, the performances of Ni-, Cu-, Fe-, Mn- and Co-based oxygen carriers have been regarded as possible candidates in CLG. Cu-based oxygen carriers have more lattice oxygen, better resistance to sintering and better oxygen decoupling capacity compared with other oxygen carriers [24, 25]. All these characters make CuO become a promising oxygen carrier. However, CuO oxygen carriers have a major drawback of low melting point, which is frequently not within the CLC operating temperature range [24]. In addition, NiO has a high melting point of 2228 K and it often works at high temperatures [26]. Based on that, CuO/NiO bimetal oxide has been proposed to as a better oxygen carrier. Chang et al. [27] reported that the CuO/NiO oxygen carrier possesses a high reactivity in the five-cycle CLC test. Adánez et al. [28] used Ni-Cu oxygen carriers to reduce or avoid CO and H2 emissions during a CLC process working at high temperatures. However, few studies have been done in CLCG of coal and biomass with Ni-Cu oxygen carrier. In this work, 5% NiO/CuO oxygen carrier was synthesized by using a sol–gel method and its performance was tested in CLCG of coal and biomass on a fixed-bed system by non-isothermal methods. 2. EXPERIMENTAL 2.1. Material preparation The oxygen carrier was prepared by a sol–gel method. Ni(NO3)2·6H2O and Cu(NO3)2·3H2O (1,20) were added into deionized water to prepare mixed solution. A 0.3-M citric acid solution was then added into the mixed solution. The molar ratio of metal to citric acid was 2:1. The mixed solution was evaporated to dryness with vigorous stirring at 80°C. The obtained solid was then put in an oven at 120°C to become xerogel. Finally, the xerogel was heated to 800°C with a heating rate of 10°C/min, calcined at 800°C for 1 h. Finally, triturated into powder, the composite oxygen carrier (5% NiO/CuO) was prepared. The proximate analysis and ultimate analysis of samples are listed in Table 1. The average sample size of lignite and rice husk has been screened to 380–830 and 180 μm, respectively. 2.2. Tests of oxygen uncoupling performances The schematic diagram shown in Figure 1 was to investigate the development of NiO/CuO oxygen carriers for O2 uncoupling performance. As the relative low heating rate in the test, a non-isothermal Coats−Redfern method is usually adopted to meet the single heating rate in pyrolysis [29]. A 100-mg catalyst was heated from room temperature to 1000°C to release O2 directly. The released oxygen concentration was recorded by a zirconia oxygen analyzer. Figure 1 Open in new tabDownload slide Schematic diagram of fixed-bed experimental system for oxygen uncoupling. Figure 1 Open in new tabDownload slide Schematic diagram of fixed-bed experimental system for oxygen uncoupling. 2.3. Gasification experiments The steam gasification and CLG were performed on a fixed-bed system heated by an electric tube furnace, and the schematic layout of the laboratory setup was shown in Figure 2. In each run, the mixture (fuel/catalyst = 1:1) that was thoroughly mixed with agate mortar and pestle was heated in a quartz bowl from ambient temperature to 900°C with a ramp of 20°C/min in Ar at a flow rate of 50 ml/min. The temperature of sample was then maintained isothermally for 2 h. In order to sweep away the residual air, pure Ar was introduced to the reactor for 30 min before the test. It is worth noting that the distilled water was not pumped into the reactor until the reaction temperature reached to 300°C. Deionized water is introduced into the reactor with a liquid hourly space velocity of 3 h−1. After being treated with cooling and drying processes, the produced gases were detected by a gas chromatography finally. Figure 2 Open in new tabDownload slide Schematic diagram of gasification experiment system for tests of oxygen carrier performance. Figure 2 Open in new tabDownload slide Schematic diagram of gasification experiment system for tests of oxygen carrier performance. Figure 3 Open in new tabDownload slide The oxygen uncoupling curves of oxygen carriers. Figure 3 Open in new tabDownload slide The oxygen uncoupling curves of oxygen carriers. 3. RESULTS AND DISCUSSION 3.1. Oxygen uncoupling performance on Cu-based oxygen carrier The O2 emission behavior of both CuO and 5%NiO/CuO were investigated under Ar, and the results were shown in Figure 3. CuO is prone to release lattice oxygen in high temperature. It can be observed that CuO began to release oxygen at ~760°C [30, 31], and oxygen uncoupling continued until the reaction temperature reached to 1000°C. In this case, the amount of oxygen releasing reached 10%, which is similar to the result of Zhang et al. [32]. The initial decomposition temperature of combined 5% NiO/CuO oxygen carrier was 700°C, and the oxygen is released until the temperature rose to 920°C. Since the lower content of NiO, the mass loss of 5% NiO/CuO was the same as that of CuO. The initial temperature of 5% NiO/CuO oxygen carriers was lower, which was attributed to the synergy between CuO and NiO. 3.2. CLG of lignite The outlet gases including H2, CO, CO2 and CH4 were analyzed by an online gas chromatography. The effect of 5%NiO/CuO on the gasification of lignite char was illustrated in Figure 4. The yields of H2, CO, CO2 and CH4 in steam gasification of lignite reached maximums of 0.034, 0.014, 0.023 and 0.01 mol/g, respectively. The yield of H2 over lignite-5% NiO/CuO is 0.037 mol/g, which is 8.82% higher than that in steam gasification of lignite. The process of chemical looping is exothermic, and the heat released during the CLG facilitated the water gas shift reaction (CO + H2O → CO2 + H2). Furthermore, the theory of Le Chatelier showed that the higher temperature is conducive to the gasification of lignite (C + H2O → H2 + CO). As a result, the yield of H2 is higher. The CO yield in CLG of lignite is 0.017 mol/g, and it was 21.4% higher than that in steam gasification. The higher yield of CO was due to the reduction reaction of C with 5% NiO/CuO and water. Only a very small amount of CH4 (2.45% of total amount of available gas in CLG) was observed. It generated mainly by methanation reaction and a small amount produced by the scission and reuniting of the organic functional groups [31], which accounted for the earlier generation of CH4. CO2 generates slowly in the early stage of reaction and it was mainly produced by water–gas shift reaction. It was reported that the ash, even for the washed ash, had catalytic effect on the gasification of coal [33]. The 5% NiO/CuO can be regarded as the higher contents of ash in lignite, which caused the increase of gas yields. Figure 4 Open in new tabDownload slide Yield of produced gas in CLG of lignite. (a:H2, b:CO, c: CH4, d: CO2) Figure 4 Open in new tabDownload slide Yield of produced gas in CLG of lignite. (a:H2, b:CO, c: CH4, d: CO2) 3.3. CLG of rice husk NiO/CuO was used as oxygen carrier in the CLG of rice husk experiments, the mass of rice husk and oxygen carrier were fixed 0.5 g and the results were shown in Figure 5. The H2 yield in the CLG of rice husk is shown in Figure 5a (0.013 mol/g). It is 12.89% higher than that in steam gasification of rice husk. The production of hydrogen is the same as the reason in the Section 3.1, but beyond that, the secondary cracking of rice husk coke was also beneficial to the yield of H2. The yields of CO and CO2 in CLG of rice husk are 4.16 × 10−3 and 8.81 × 10−3 mol/g, which are 34.37% and 5.26% higher than those in steam gasification, respectively. The increases of CO2 and CO yields were by the reasons of the conversion of semi-coke fixed carbon to COx [34] and the oxidation of CO to CO2 by hydroxyl group formed by water molecules [35]. The ratio of CO to H2 in CLG (32.50%) was higher than that in steam gasification (27.43%).The proportion of CH4 in CLG is 1.43%, and it is 1.10% in steam gasification. Figure 5 Open in new tabDownload slide Yield of produced gas in the CLG of rice husk. (a:H2, b:CO, c: CH4, d: CO2) Figure 5 Open in new tabDownload slide Yield of produced gas in the CLG of rice husk. (a:H2, b:CO, c: CH4, d: CO2) 3.4. Steam co-gasification and CLCG of lignite and rice husk In the steam co-gasification experiments, the mass of lignite and rice husk were both 0.25 g and the results were illustrated in Figure 6. There is a delay in the production of H2 because of the delayed heat transfer between samples and device. The pyrolysis of rice husk char need a high temperature, so the rate of gas formation achieves a maximum at about 25 min when the residual volatiles were released [36]. The yield of H2 in co-gasification is 78.16% of that in 0.5-g lignite gasification, 237% of that in rice husk gasification. Similar result was found Arifin et al. [37] that co-gasification promotes the hydrogen yield if the carbon is ~50% by mass. The yield of H2 was the largest among four gas products, and the increase of hydrogen production in co-gasification is also the most. It has been discovered that the behaviors of co-gasification of coal and biomass are better than those of coal gasification [38–40]. Tursun et al. [38] found that the carbon conversion and gas yield increase with the increase of biomass blending ratio. Li et al. [40] discovered that the reactivity index of blend char of sawdust and coal achieves the maximum when the biomass/coal ratio is 80:20. Figure 6 Open in new tabDownload slide Gas yield in co-gasification and gasification of lignite and rice husk. (a: H2, b: CO, c: CH4, d: CO2) Figure 6 Open in new tabDownload slide Gas yield in co-gasification and gasification of lignite and rice husk. (a: H2, b: CO, c: CH4, d: CO2) The results of CLCG experiments were shown in Figure 7, in which the results of CLG were added in for comparison. The mass ratio of fuel to oxygen carrier was 1:1(0.5 g) and the mass ratio of lignite to rice husk was also 1:1(0.25 g). For gas products (H2, CO, CO2 and CH4), the yields in CLCG were all higher than in individual CLG. The higher yields were due to the synergetic effect caused by the transferring of active OH and H radicals from the biomass to the coal. Figure 7 Open in new tabDownload slide Gas yield in CLG and CLCG of lignite and rice husk. Figure 7 Open in new tabDownload slide Gas yield in CLG and CLCG of lignite and rice husk. Figure 8 Open in new tabDownload slide C conversion in different gasification experiments. (a:H2, b:CO, c: CH4, d: CO2) Figure 8 Open in new tabDownload slide C conversion in different gasification experiments. (a:H2, b:CO, c: CH4, d: CO2) 3.5. The carbon conversion in all gasification experiments The gasification of rice husk is mainly based on the break of weak ether bond (R-O-R) in lignin and cellulose [41]. Hence, the activation energy in rice husk gasification is high. In the gasification of lignite, the reactions are mainly based on the break of C=C bond in polycyclic aromatic hydrocarbons [42]. Therefore, the activation energy in coal gasification is low. However, compared with coal, rice husk has higher volatile content, higher H/C ratio and O/C ratio. These features make rice husk show good thermal reactivity. So, as shown in Figure 8, the C conversions of lignite and rice husk in steam gasification are 58.75% and 60.05%, respectively. In CLG process, the C conversion of lignite-5% NiO/CuO is 66.94%, the C conversion of rice husk-5% NiO/CuO is 68.49%. In the co-gasification, the complementation of reactivity between fuels increases the C conversion rate. Therefore, C conversion in co-gasification is higher than that in individual feed gasification. Furthermore, the C conversion in the steam co-gasification of lignite and rice husk is 62.43%, and in CLCG process, the C conversion of lignite and rice husk is 71.49%, which is 14.51% higher than that in steam co-gasification. It was due to the catalysis of 5% NiO/CuO. There are some evidences to support the strong catalysis of Cu-Ni oxygen carriers. Li et al. [43] reported that the Cu-Ni alloy could promote the gasification of carbonaceous species. Othman and Bosrooh [44] found that the presence of Ni promotes the carbon conversion and the production of hydrocarbons in coal gasification. Nishiyama [45] reported that Ni improves the reactivity of coal char and the carbon conversion in gasification. Tomita et al. [46] discovered that the Ni catalysts have great catalytic activity and the process of coal gasification with Ni is rapid. 4. CONCLUSIONS In this work, A NiO-modified Cu-based oxygen carrier was prepared by the sol–gel method. The reactivity of rice husk char and lignite with the oxygen carrier were investigated using a fixed-bed reactor equipped with an online gas chromatography. In addition, the oxygen uncoupling performance of 5% NiO/CuO oxygen carrier was tested by a zirconia oxygen analyzer. It showed that CuO began to release oxygen at ~760°C, and the initial decomposition temperature of 5% NiO/CuO oxygen carrier was 700°C; the reduction of decomposition temperature was attributed to the synergy between CuO and NiO. H2 was mainly produced by the water gas shift reaction (CO + H2O → CO2 + H2) and the gasification of lignite (C + H2O → H2 + CO). The process of chemical looping is exothermic, and the heat released during the CLG facilitated the production of H2. The increases of CO2 and CO yields were by the reasons of the conversion of semi-coke fixed carbon to COx and the oxidation of CO to CO2 by hydroxyl group formed by water molecules. CH4 generated mainly by methanation reaction, and a small amount produced by the scission and reuniting of the organic functional groups. Due to the catalysis of alkali metal in rice husk, there is a synergy between lignite and rice husk. The synergy improved the efficiency of gasification. It was found that the yields of gaseous products in CLG of lignite or rice husk are higher than that of steam gasification. The yields of gases (H2, CO, CO2 and CH4) in CLCG are higher than that in steam co-gasification. Rice husk has higher volatile content, higher H/C ratio and O/C ratio. These features make rice husk show good thermal reactivity, so the C conversion of rice husk was higher than that of lignite. In the co-gasification, the complementation of reactivity between fuels facilitated the C conversion rate, so the yields in co-gasification were higher than in individual gasification. 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TI - Study of chemical looping co-gasification of lignite and rice husk with Cu-Ni oxygen carrier
JF - International Journal of Low-Carbon Technologies
DO - 10.1093/ijlct/ctab037
DA - 2021-05-05
UR - https://www.deepdyve.com/lp/oxford-university-press/study-of-chemical-looping-co-gasification-of-lignite-and-rice-husk-QemMmTxTam
SP - 1
EP - 1
VL - Advance Article
IS - 
DP - DeepDyve
ER -