生物质催化热解和气化的应用基础研究
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摘要
随着能源形势日益严峻,环境污染问题日趋严重,合理开发和利用新型可再生的洁净能源已成为当前紧迫的研究课题。生物质能作为唯一可储存和运输的可再生能源,其高效转换和洁净利用日益受到全世界的关注。生物质热转化技术是实现其能量转换的最有效途径,尤其是将其转化为气体燃料或气化发电。而限制其气化应用的瓶颈和主要障碍是气体中焦油的存在,催化热解气化被认为是去除焦油和提高气化效率最有效的方法。本文依托华中科技大学环境学院和新加坡南洋理工大学环境科学与工程研究院国际交流合作项目,对生物质(油棕废弃物和锯屑)的催化热解和气化技术展开了系统的研究,主要研究内容及成果如下:
锯屑和油棕废弃物分别是木材加工业和东南亚油棕种植地区的主要固体废弃物。在实际应用和实验室研究中,必需预先经过干燥、破碎和筛分,得到不同粒径范围的实验原料。其理化特性分析显示:油棕废弃物和锯屑都含有较高的挥发份,相对较低的固定碳含量;它们的低位热值约为20MJ/kg,与烟煤和褐煤的热值相当。同时,原料中有害元素N和S含量极低,灰分含量小于5%,所以油棕废弃物和锯屑都是环境友好的生物质资源。
催化剂的研制是本课题的重要工作之一。本文开发和制备了负载型纳米镍基催化剂,以纳米氧化镍为活性成分,将其负载到γ-Al2O3或自制的赤泥粉煤灰载体上,评价了它在生物质催化热解和气化过程中的催化活性。
纳米氧化镍粉体的制备采用均匀沉淀法,并利用FTIR、TGA、XRD、TEM等手段对所得纳米NiO颗粒及其前驱体进行了表征和分析。同时探讨了制备纳米氧化镍的最佳工艺条件;并利用热重分析仪初步评价了纳米氧化镍对生物质三种主要成分热解的催化活性,而且与微米NiO的催化性能进行了比较。结果表明:纳米NiO能显著地降低反应的活化能,导致生物质热分解发生在更低的温度,显示出比微米NiO更好的催化活性。在此基础上,以γ-Al2O3为载体,利用沉淀——沉积的方法制备了负载型Nano-NiO/γ-Al2O3催化剂,催化剂中NiO负载量达12wt%以上,负载的NiO粒径在12-18nm之间,其表面积高于商业镍基催化剂。此外,为节省催化剂制备成本和减少环境污染,本文利用工业固废——赤泥和粉煤灰等为原料,制备了催化剂载体,探讨了载体的焙烧工艺和最佳配方。载体的性能测试表明,所制备的催化剂载体符合工业要求,达到了废物资源化的目的。随后,参照Nano-NiO/γ-Al2O3催化剂的制备方法和条件,制备了负载型Nano-NiO/赤泥粉煤灰催化剂,其NiO负载量约10wt%,表面积甚至高于Nano-NiO/γ-Al2O3催化剂。
利用逆流上吸式固定床对油棕废弃物的热解进行了详细研究,重点探讨了两个主要的热解运行条件(温度和气体停留时间)对油棕废弃物热解产物特性的影响,并采用各种分析手段对热解产物进行了全面的分析,尤其是建立了热解焦油的系统分析方法。实验证明:温度对生物质热解产物的分布和特性起着重要的作用。随着热解温度升高,固体残余焦炭和液体焦油的产量显著降低,气体产量快速增加,气体中H2、CO和CH4的含量随之升高,而CO2含量急剧减小。热解温度升高也使焦油中含氧化合物种类和含量减少,而芳香化合物含量升高,焦油成分随温度而变化。气体停留时间对生物质的热解也有很重要的影响,本实验条件下,停留时间为15s时,气体产量最大。同时,采用HSC模拟软件对油棕废弃物的热解进行了热力学平衡模拟计算,计算结果与生物质热解实验中的产物特性和变化趋势相符。此外,还以苯甲醚为焦油模型化合物,对其热解机理进行了初步的探讨,提出了自由基反应机理,较好地解释了热解实验中焦油的变化趋势。
在双床石英反应器系统上对油棕废弃物的催化热解进行了对比研究,并评价了各种催化剂的催化性能,测试了纳米镍基催化剂的寿命和再生的方法。实验结果表明:焦炭对生物质热解有一定的催化作用,能提高气体成分中CO的含量,但催化过程中,焦炭被逐渐消耗。白云石能有效地去除热解气中的焦油,提高气体产率,但对甲烷的重整和转化没有催化效果。本文开发的负载型Nano-NiO/γ-Al2O3催化剂和Nano -NiO/赤泥粉煤灰催化剂的催化活性相当,这两种镍基催化剂都能高效去除生物质热解过程中产生的焦油,并显著提高气体产率,调整气体成分,其催化效果明显优于白云石和焦炭。特别地,纳米镍基催化剂的抗失活能力强,失活速率缓慢,并可通水蒸汽和二氧化碳混合气使之再生。
利用本实验室自行设计的双床不锈钢反应器系统,在连续进料方式下,对锯屑水蒸气催化气化进行了系统的试验研究,探讨和分析了各工艺参数对锯屑催化气化的影响。研究结果表明:生物质气化过程中引入水蒸气和升高温度均能显著提高产气量和H2产率,水蒸气的最佳通入量为1.33(S/B)。催化剂的影响也很大,本文所开发的Nano-NiO/γ-Al2O3催化剂的催化效果明显优于白云石和焦炭催化剂,具有极大的应用价值。相对于生物质催化热解,水蒸气催化气化的产气量、H2产率和焦油去除效率更高,残余焦炭量更少,因而更适合产气或制H2。
为了开拓生物质热转化产物的利用途径,本文探讨了生物质气作为燃料电池燃料的可行性,研究了生物质气组成对其发电效率的影响;同时,考察了生物质热转化后的残余焦炭对工业废水中铜离子的吸附性能。结果显示,其吸附效率达86%以上。这些开拓性研究将有助于生物质热转化技术的进一步开发和利用。
In view of the severe lack of energy and increasing environmental pollution worldwide, to explore clean energy technologies has become an important and timely research topic. Biomass, as the only reproducible energy that can be stored and transported, is taking great attentions of worldwide researchers with its high effect and cleanness. Biomass pyrolysis/gasification is one of the most efficient processes for converting biomass to energy, especially for gas fuel and power production. However, tar is generally formed in the process, which inhibits the further development and commercialization of biomass gasification. The catalytic pyrolysis is considered as the most potent technique to remove tar, thus to improve gasifying effect and the quality of produced gas. Under the scheme of the research cooperation between Huazhong University of Science and Technology (HUST) and Institute of Environmental Science and Engineering (IESE), Nanyang Technological University (Singapore), the PhD candidate has spent two years of research in IESE on his project entitled“Developing novel catalysts for advanced biomass pyrolysis and gasification”, aiming to develop an advanced biomass gasification technique to convert efficiently palm oil wastes and sawdust into bioenergy. The main findings of this study are summarized as follows:
Sawdust and palm oil wastes are the main solid wastes coming respectively from wood process and palm oil plants in ASEAN countries. In the practical application and lab work, the wastes were dried, crashed, and sieved in order to get raw materials in different particle sizes. The physicochemical property of these materials showed that palm oil waste and sawdust both contained more volatiles and lower fixed carbon comparing to coal, and their low heat values are ~ 20 MJ/kg, which are similar with that of soft coal and lignite coal. In addition, the baneful elements N and S are of very low contents in raw materials, which are less than 5%. Therefore, palm oil wastes and sawdust are both environment-friendly biomass sources.
A main task of the thesis research is to develop catalysts suitable for biomass catalytic pyrolysis and gasification. Based on the knowledge obtained on the latest development of nanotechnology, the supported Nano-NiO/γ-Al2O3 catalysts were developed in this study, involving Nano-NiO particles as an active component loaded on carriers such as commercialγ-Al2O3 and the carriers produced in this study. Meantime, the catalytic activity of the developed Nano-NiO/Al2O3 catalysts in biomass pyrolysis/gasification was evaluated systematically using several reactors.
Nano-NiO particles were prepared by homogeneous precipitation method. Different approaches such as FTIR, TGA, XRD and TEM were used to characterize and analysis the NiO nanoparticles and their precursors. Meanwhile, the optimum conditions for preparing NiO nanoparticles were screened. The catalytic activity of NiO nanoparticles in pyrolyzing three main biomass components was evaluated by TGA, and the catalytic performance was compared with that of Micro-NiO. The results indicated that nano-NiO could reduce markedly the activation energy in reaction, leading to biomass pyrolysis at lower temperature. Compared with micro-NiO, nano-NiO had a better catalytic activity over micro-NiO. From the above successful work, the supported nano-NiO/γ-Al2O3 catalysts were further developed involvingγ-Al2O3 as carrier through deposition-precipitation (DP) Method. The loaded capacity of NiO was more than 12 wt%, the sizes of NiO particles were found between 12 and 18 nm, and its surface area was larger than commercial Nickel-based catalysts. Furthermore, in view of saving cost and protecting environment, industrial solid wastes, i.e. red putty and fly ash were used as raw materials of carriers in this study. The influence of calcinations conditions on preparing the carrier and the optimum proportion of raw materials were investigated. It’s the performance test showed that the prepared carrier met the industrial standards. Following that, the supported catalyst, with nano-NiO coated on putty-fly ash carrier, was prepared following the same method as preparing nano-NiO/γ-Al2O3. The loading capacity of NiO in the supported catalyst was over 10 wt%, and its specific surface area showed larger than nano-NiO/γ-Al2O3.
A countercurrent fixed bed reactor was used for detailed investigation of palm oil waste pyrolysis. The study focused on the influence of two important pyrolysis conditions such as temperature and gas residence time on the distribution of pyrolysis products. Meanwhile, various analytical means were utilized to characterize the obtained products. In particular, the full screening method of tar in different fractions was established. It demonstrated that temperature played an important role in biomass pyrolysis. As the pyrolysis temperature increased, the gas yield enhanced while that of tar and char reduced. Meanwhile, the amount of H2, CO, and CH4 in product gas increased with the increasing temperature; contrarily, that of CO2 in gas dropped significantly. Furthermore, the proportion of oxygenated compounds in tar declined with temperature increasing, while that of the aromatic hydrocarbons and PAHs showed a marked increase, and the changing trend of oil components versus temperature could be concluded. Gas residence time also demonstrated a big effect on pyrolysis process. When the residence time was 15 s, the yield of gas products reached the biggest. At the same time, HSC software was used to simulate thermodynamically the process and products generated in biomass pyrolysis. The simulation results were consistent with those derived from experimental investigation. Besides, anisole was utilized as a tar model component to explore the mechanism and pathway of tar pyrolysis, and a radical reaction mechanism was put forward to explain preferably the changing trend of the tar components derived from biomass pyrolysis.
On a double-bed system equipped quartz reactor, the catalytic pyrolysis of palm oil wastes was conducted to evaluate the performance of various catalysts, and to test the lifetime and potential regeneration of nano-nickel catalysts. The results indicated that the char had certain catalytic activity on biomass pyrolysis, especially in upgrading CO amount in gas products, in a price of itself consumption. Dolomite could remove effectively tar in gas, and increased the yield of gas, but it had almost no impact in methane reforming and transforming. The two nano-nickel catalysts developed in this study showed a similar catalytic activity, and they both reduced sharply the yield of tar in biomass pyrolysis whilst increased markedly the gas production and improved significantly the quality of the produced gas. Both the developed nano-nickel catalysts were superior to dolomite and char in removing tar during biomass pyrolysis. In particular, nano-nickel catalysts had strong anti-deactivation and slow deactivation rate, and they could possibly be regenerated by adding H2O and CO2.
A home designed double-fixed bed system equipped steel reactor with continuous feeding was used to investigate systematically the catalytic gasification of sawdust with adding stream vapor. The influence of various technical parameters on sawdust catalytic gasification was analyzed experimentally. It was found that the higher temperature and adding vapor were favorable for increasing the gas yield and upgrading H2 gas, and the optimum quantity of adding vapor is 1.33 (S/B) in biomass gasification. The developed nano-NiO/γ-Al2O3 catalyst was proven to have a better performance over dolomite and char for catalytic gasification of biomass. Compared with catalytic pyrolysis, biomass gasification with the presence of vapor was more beneficial owing to the higher gas yield and larger proportion of the valuable H2, the higher efficiency for tar removal, as well as lower residue yields.
To further develop and utilize the products derived from biomass thermochemical conversion, the feasibility of using bio-gas generated from this study as the fuel of solid oxide fuel cell was explored, and the influence of gas composition on the efficiency of power production was investigated. Meanwhile, the absorption performance of residual char on Cu2+ in industrial wastes water was tested. The results revealed that the absorption efficiency of char on Cu2+ was over 86%. These explorations and preliminary studies would facilitate the further development and advances of biomass thermochemical conversion technology.
锯屑和油棕废弃物分别是木材加工业和东南亚油棕种植地区的主要固体废弃物。在实际应用和实验室研究中,必需预先经过干燥、破碎和筛分,得到不同粒径范围的实验原料。其理化特性分析显示:油棕废弃物和锯屑都含有较高的挥发份,相对较低的固定碳含量;它们的低位热值约为20MJ/kg,与烟煤和褐煤的热值相当。同时,原料中有害元素N和S含量极低,灰分含量小于5%,所以油棕废弃物和锯屑都是环境友好的生物质资源。
催化剂的研制是本课题的重要工作之一。本文开发和制备了负载型纳米镍基催化剂,以纳米氧化镍为活性成分,将其负载到γ-Al2O3或自制的赤泥粉煤灰载体上,评价了它在生物质催化热解和气化过程中的催化活性。
纳米氧化镍粉体的制备采用均匀沉淀法,并利用FTIR、TGA、XRD、TEM等手段对所得纳米NiO颗粒及其前驱体进行了表征和分析。同时探讨了制备纳米氧化镍的最佳工艺条件;并利用热重分析仪初步评价了纳米氧化镍对生物质三种主要成分热解的催化活性,而且与微米NiO的催化性能进行了比较。结果表明:纳米NiO能显著地降低反应的活化能,导致生物质热分解发生在更低的温度,显示出比微米NiO更好的催化活性。在此基础上,以γ-Al2O3为载体,利用沉淀——沉积的方法制备了负载型Nano-NiO/γ-Al2O3催化剂,催化剂中NiO负载量达12wt%以上,负载的NiO粒径在12-18nm之间,其表面积高于商业镍基催化剂。此外,为节省催化剂制备成本和减少环境污染,本文利用工业固废——赤泥和粉煤灰等为原料,制备了催化剂载体,探讨了载体的焙烧工艺和最佳配方。载体的性能测试表明,所制备的催化剂载体符合工业要求,达到了废物资源化的目的。随后,参照Nano-NiO/γ-Al2O3催化剂的制备方法和条件,制备了负载型Nano-NiO/赤泥粉煤灰催化剂,其NiO负载量约10wt%,表面积甚至高于Nano-NiO/γ-Al2O3催化剂。
利用逆流上吸式固定床对油棕废弃物的热解进行了详细研究,重点探讨了两个主要的热解运行条件(温度和气体停留时间)对油棕废弃物热解产物特性的影响,并采用各种分析手段对热解产物进行了全面的分析,尤其是建立了热解焦油的系统分析方法。实验证明:温度对生物质热解产物的分布和特性起着重要的作用。随着热解温度升高,固体残余焦炭和液体焦油的产量显著降低,气体产量快速增加,气体中H2、CO和CH4的含量随之升高,而CO2含量急剧减小。热解温度升高也使焦油中含氧化合物种类和含量减少,而芳香化合物含量升高,焦油成分随温度而变化。气体停留时间对生物质的热解也有很重要的影响,本实验条件下,停留时间为15s时,气体产量最大。同时,采用HSC模拟软件对油棕废弃物的热解进行了热力学平衡模拟计算,计算结果与生物质热解实验中的产物特性和变化趋势相符。此外,还以苯甲醚为焦油模型化合物,对其热解机理进行了初步的探讨,提出了自由基反应机理,较好地解释了热解实验中焦油的变化趋势。
在双床石英反应器系统上对油棕废弃物的催化热解进行了对比研究,并评价了各种催化剂的催化性能,测试了纳米镍基催化剂的寿命和再生的方法。实验结果表明:焦炭对生物质热解有一定的催化作用,能提高气体成分中CO的含量,但催化过程中,焦炭被逐渐消耗。白云石能有效地去除热解气中的焦油,提高气体产率,但对甲烷的重整和转化没有催化效果。本文开发的负载型Nano-NiO/γ-Al2O3催化剂和Nano -NiO/赤泥粉煤灰催化剂的催化活性相当,这两种镍基催化剂都能高效去除生物质热解过程中产生的焦油,并显著提高气体产率,调整气体成分,其催化效果明显优于白云石和焦炭。特别地,纳米镍基催化剂的抗失活能力强,失活速率缓慢,并可通水蒸汽和二氧化碳混合气使之再生。
利用本实验室自行设计的双床不锈钢反应器系统,在连续进料方式下,对锯屑水蒸气催化气化进行了系统的试验研究,探讨和分析了各工艺参数对锯屑催化气化的影响。研究结果表明:生物质气化过程中引入水蒸气和升高温度均能显著提高产气量和H2产率,水蒸气的最佳通入量为1.33(S/B)。催化剂的影响也很大,本文所开发的Nano-NiO/γ-Al2O3催化剂的催化效果明显优于白云石和焦炭催化剂,具有极大的应用价值。相对于生物质催化热解,水蒸气催化气化的产气量、H2产率和焦油去除效率更高,残余焦炭量更少,因而更适合产气或制H2。
为了开拓生物质热转化产物的利用途径,本文探讨了生物质气作为燃料电池燃料的可行性,研究了生物质气组成对其发电效率的影响;同时,考察了生物质热转化后的残余焦炭对工业废水中铜离子的吸附性能。结果显示,其吸附效率达86%以上。这些开拓性研究将有助于生物质热转化技术的进一步开发和利用。
In view of the severe lack of energy and increasing environmental pollution worldwide, to explore clean energy technologies has become an important and timely research topic. Biomass, as the only reproducible energy that can be stored and transported, is taking great attentions of worldwide researchers with its high effect and cleanness. Biomass pyrolysis/gasification is one of the most efficient processes for converting biomass to energy, especially for gas fuel and power production. However, tar is generally formed in the process, which inhibits the further development and commercialization of biomass gasification. The catalytic pyrolysis is considered as the most potent technique to remove tar, thus to improve gasifying effect and the quality of produced gas. Under the scheme of the research cooperation between Huazhong University of Science and Technology (HUST) and Institute of Environmental Science and Engineering (IESE), Nanyang Technological University (Singapore), the PhD candidate has spent two years of research in IESE on his project entitled“Developing novel catalysts for advanced biomass pyrolysis and gasification”, aiming to develop an advanced biomass gasification technique to convert efficiently palm oil wastes and sawdust into bioenergy. The main findings of this study are summarized as follows:
Sawdust and palm oil wastes are the main solid wastes coming respectively from wood process and palm oil plants in ASEAN countries. In the practical application and lab work, the wastes were dried, crashed, and sieved in order to get raw materials in different particle sizes. The physicochemical property of these materials showed that palm oil waste and sawdust both contained more volatiles and lower fixed carbon comparing to coal, and their low heat values are ~ 20 MJ/kg, which are similar with that of soft coal and lignite coal. In addition, the baneful elements N and S are of very low contents in raw materials, which are less than 5%. Therefore, palm oil wastes and sawdust are both environment-friendly biomass sources.
A main task of the thesis research is to develop catalysts suitable for biomass catalytic pyrolysis and gasification. Based on the knowledge obtained on the latest development of nanotechnology, the supported Nano-NiO/γ-Al2O3 catalysts were developed in this study, involving Nano-NiO particles as an active component loaded on carriers such as commercialγ-Al2O3 and the carriers produced in this study. Meantime, the catalytic activity of the developed Nano-NiO/Al2O3 catalysts in biomass pyrolysis/gasification was evaluated systematically using several reactors.
Nano-NiO particles were prepared by homogeneous precipitation method. Different approaches such as FTIR, TGA, XRD and TEM were used to characterize and analysis the NiO nanoparticles and their precursors. Meanwhile, the optimum conditions for preparing NiO nanoparticles were screened. The catalytic activity of NiO nanoparticles in pyrolyzing three main biomass components was evaluated by TGA, and the catalytic performance was compared with that of Micro-NiO. The results indicated that nano-NiO could reduce markedly the activation energy in reaction, leading to biomass pyrolysis at lower temperature. Compared with micro-NiO, nano-NiO had a better catalytic activity over micro-NiO. From the above successful work, the supported nano-NiO/γ-Al2O3 catalysts were further developed involvingγ-Al2O3 as carrier through deposition-precipitation (DP) Method. The loaded capacity of NiO was more than 12 wt%, the sizes of NiO particles were found between 12 and 18 nm, and its surface area was larger than commercial Nickel-based catalysts. Furthermore, in view of saving cost and protecting environment, industrial solid wastes, i.e. red putty and fly ash were used as raw materials of carriers in this study. The influence of calcinations conditions on preparing the carrier and the optimum proportion of raw materials were investigated. It’s the performance test showed that the prepared carrier met the industrial standards. Following that, the supported catalyst, with nano-NiO coated on putty-fly ash carrier, was prepared following the same method as preparing nano-NiO/γ-Al2O3. The loading capacity of NiO in the supported catalyst was over 10 wt%, and its specific surface area showed larger than nano-NiO/γ-Al2O3.
A countercurrent fixed bed reactor was used for detailed investigation of palm oil waste pyrolysis. The study focused on the influence of two important pyrolysis conditions such as temperature and gas residence time on the distribution of pyrolysis products. Meanwhile, various analytical means were utilized to characterize the obtained products. In particular, the full screening method of tar in different fractions was established. It demonstrated that temperature played an important role in biomass pyrolysis. As the pyrolysis temperature increased, the gas yield enhanced while that of tar and char reduced. Meanwhile, the amount of H2, CO, and CH4 in product gas increased with the increasing temperature; contrarily, that of CO2 in gas dropped significantly. Furthermore, the proportion of oxygenated compounds in tar declined with temperature increasing, while that of the aromatic hydrocarbons and PAHs showed a marked increase, and the changing trend of oil components versus temperature could be concluded. Gas residence time also demonstrated a big effect on pyrolysis process. When the residence time was 15 s, the yield of gas products reached the biggest. At the same time, HSC software was used to simulate thermodynamically the process and products generated in biomass pyrolysis. The simulation results were consistent with those derived from experimental investigation. Besides, anisole was utilized as a tar model component to explore the mechanism and pathway of tar pyrolysis, and a radical reaction mechanism was put forward to explain preferably the changing trend of the tar components derived from biomass pyrolysis.
On a double-bed system equipped quartz reactor, the catalytic pyrolysis of palm oil wastes was conducted to evaluate the performance of various catalysts, and to test the lifetime and potential regeneration of nano-nickel catalysts. The results indicated that the char had certain catalytic activity on biomass pyrolysis, especially in upgrading CO amount in gas products, in a price of itself consumption. Dolomite could remove effectively tar in gas, and increased the yield of gas, but it had almost no impact in methane reforming and transforming. The two nano-nickel catalysts developed in this study showed a similar catalytic activity, and they both reduced sharply the yield of tar in biomass pyrolysis whilst increased markedly the gas production and improved significantly the quality of the produced gas. Both the developed nano-nickel catalysts were superior to dolomite and char in removing tar during biomass pyrolysis. In particular, nano-nickel catalysts had strong anti-deactivation and slow deactivation rate, and they could possibly be regenerated by adding H2O and CO2.
A home designed double-fixed bed system equipped steel reactor with continuous feeding was used to investigate systematically the catalytic gasification of sawdust with adding stream vapor. The influence of various technical parameters on sawdust catalytic gasification was analyzed experimentally. It was found that the higher temperature and adding vapor were favorable for increasing the gas yield and upgrading H2 gas, and the optimum quantity of adding vapor is 1.33 (S/B) in biomass gasification. The developed nano-NiO/γ-Al2O3 catalyst was proven to have a better performance over dolomite and char for catalytic gasification of biomass. Compared with catalytic pyrolysis, biomass gasification with the presence of vapor was more beneficial owing to the higher gas yield and larger proportion of the valuable H2, the higher efficiency for tar removal, as well as lower residue yields.
To further develop and utilize the products derived from biomass thermochemical conversion, the feasibility of using bio-gas generated from this study as the fuel of solid oxide fuel cell was explored, and the influence of gas composition on the efficiency of power production was investigated. Meanwhile, the absorption performance of residual char on Cu2+ in industrial wastes water was tested. The results revealed that the absorption efficiency of char on Cu2+ was over 86%. These explorations and preliminary studies would facilitate the further development and advances of biomass thermochemical conversion technology.
引文
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