生物炭的加氢催化应用及生物炭浸出液的毒性评估
发布时间：2018-11-26 15:13
【摘要】：生物质指由绿色植物直接或间接利用太阳能进行光合作用而形成的有机物质,是一种重要的可再生资源。由于世界范围的能源危机以及相关的环境污染日益加重,木质生物质能源的可再生性和环境友好性引起了人们的广泛关注。生物质能通过加氢裂解、热解、气化、液化以及直接燃烧等方式转化为能源。木质生物质通常可在高温下进行催化加氢,得到含苯环的小分子物质,可用于化学品、石油类产品等的制备。而热解生物质产生生物油是生物质能源转化的另一种方式,得到的副产物生物炭是一种具有多孔结构的坚固的碳框架,常被用以进行土壤修复以及碳封存。但是其对于土壤性质及土壤生物的影响一直存在争议,近年来,许多研究关注生物炭材料的其它应用。例如将生物炭进行修饰改性后,可用于有机污染物和重金属吸附；而将生物炭作为基底材料负载金属纳米颗粒,则可用于催化有机物转化等。本文主要研究利用快速热解方式制备负载金属的催化剂,并且研究其在木质素加氢反应中的催化作用。此外,我们研究了将不同来源的生物炭应用于土壤修复时可能发生的生物毒性影响,主要的研究内容及结论如下：1.利用快速热解装置一步热解浸渍镍盐和钼盐的锯末,得到负载纳米金属镍和碳化钼的生物炭催化剂Ni-Mo2C/C。将其应用于木质素加氢催化,得到的液体产物通过GC-MS分析产物类型及产率,结果表明添加催化剂反应组中,产物相比对照组明显增多且选择性增加。2.利用传统化学还原法将镍盐和钼盐还原于同样条件制备的生物炭上,得到催化剂材料(Ni-MoO2/C)应用于木质素加氢催化,并没有得到与Ni-Mo2C/C类似的良好效果,证明一步热解方法具有显著的优越性。结合TEM, XRD, XPS等表征以及GC-MS产物分布推测可能的反应机理,纳米镍和碳化钼颗粒能有效进攻碳氧双键,且石墨化的碳基底结构能帮助催化剂上电子转移。3.利用不同生物质材料(稻壳、锯末、蒲草)在相同条件下通过快速热解得到生物炭材料,并且研究其提取液对于植物(小麦)、动物(秀丽杆隐线虫)、微生物(铜绿假单胞菌)的生长影响。结果表明,稻壳、锯末类生物炭浸出液对生物生长影响较小,而蒲草类生物质浸出液严重抑制生物生长,特别是对秀丽杆隐线虫具有剧烈毒性。
[Abstract]:Biomass, which is an important renewable resource, refers to the organic matter formed by the direct or indirect use of solar energy for photosynthesis by green plants. Due to the worldwide energy crisis and the increasing environmental pollution, the regeneration and environmental friendliness of wood biomass energy have attracted wide attention. Biomass energy is converted into energy by hydrocracking, pyrolysis, gasification, liquefaction and direct combustion. Wood biomass can be hydrogenated at high temperature to obtain small molecular substances containing benzene ring, which can be used in the preparation of chemicals, petroleum products and so on. Pyrolysis biomass to produce bio-oil is another way of biomass energy conversion. The by-product biochar is a porous structure of a solid carbon framework, often used for soil remediation and carbon sequestration. However, its influence on soil properties and soil organisms has been controversial. In recent years, many researches have focused on other applications of biochar materials. For example, modified biochar can be used to adsorb organic pollutants and heavy metals, while biochar can be used as substrate material to support metal nanoparticles, which can be used to catalyze organic conversion and so on. In this paper, the catalyst supported on metal was prepared by rapid pyrolysis, and its catalytic effect in hydrogenation of lignin was studied. In addition, we studied the possible toxic effects of biochar from different sources on soil remediation. The main contents and conclusions are as follows: 1. Using a rapid pyrolysis device, the sawdust of nickel salt and molybdenum salt was pyrolyzed in one step, and the biocarbon catalyst Ni-Mo2C/C. supported on nano-nickel and molybdenum carbide was obtained. The liquid product was analyzed by GC-MS for the type and yield of lignin hydrogenation. The results showed that the products in the reaction group increased significantly and selectivity was increased compared with the control group. The nickel salt and molybdenum salt were reduced to biochar under the same conditions by the traditional chemical reduction method. The catalyst material (Ni-MoO2/C) was applied to the hydrogenation of lignin, and the effect was not similar to that of Ni-Mo2C/C. It is proved that the one-step pyrolysis method has obvious advantages. Combined with the TEM, XRD, XPS characterization and the possible reaction mechanism of GC-MS products distribution, the nickel and molybdenum carbide nanoparticles can effectively attack the carbon-oxygen double bond, and the graphitized carbon substrate structure can help the electron transfer on the catalyst. Using different biomass materials (rice husk, sawdust, cattlegrass) under the same conditions, the biochar materials were obtained by rapid pyrolysis, and the extracts of biochar were studied for plants (wheat) and animals (Cryptonematodes elegans). Effects of microorganisms (Pseudomonas aeruginosa) on growth. The results showed that rice husks and sawdust biochar leachate had little effect on biological growth, while the biomass extract of Cattlegrass seriously inhibited biological growth, especially to Cryptonematodes elegans.
【学位授予单位】：中国科学技术大学
【学位级别】：硕士
【学位授予年份】：2016
【分类号】：O643.36
本文编号：2358911
[Abstract]:Biomass, which is an important renewable resource, refers to the organic matter formed by the direct or indirect use of solar energy for photosynthesis by green plants. Due to the worldwide energy crisis and the increasing environmental pollution, the regeneration and environmental friendliness of wood biomass energy have attracted wide attention. Biomass energy is converted into energy by hydrocracking, pyrolysis, gasification, liquefaction and direct combustion. Wood biomass can be hydrogenated at high temperature to obtain small molecular substances containing benzene ring, which can be used in the preparation of chemicals, petroleum products and so on. Pyrolysis biomass to produce bio-oil is another way of biomass energy conversion. The by-product biochar is a porous structure of a solid carbon framework, often used for soil remediation and carbon sequestration. However, its influence on soil properties and soil organisms has been controversial. In recent years, many researches have focused on other applications of biochar materials. For example, modified biochar can be used to adsorb organic pollutants and heavy metals, while biochar can be used as substrate material to support metal nanoparticles, which can be used to catalyze organic conversion and so on. In this paper, the catalyst supported on metal was prepared by rapid pyrolysis, and its catalytic effect in hydrogenation of lignin was studied. In addition, we studied the possible toxic effects of biochar from different sources on soil remediation. The main contents and conclusions are as follows: 1. Using a rapid pyrolysis device, the sawdust of nickel salt and molybdenum salt was pyrolyzed in one step, and the biocarbon catalyst Ni-Mo2C/C. supported on nano-nickel and molybdenum carbide was obtained. The liquid product was analyzed by GC-MS for the type and yield of lignin hydrogenation. The results showed that the products in the reaction group increased significantly and selectivity was increased compared with the control group. The nickel salt and molybdenum salt were reduced to biochar under the same conditions by the traditional chemical reduction method. The catalyst material (Ni-MoO2/C) was applied to the hydrogenation of lignin, and the effect was not similar to that of Ni-Mo2C/C. It is proved that the one-step pyrolysis method has obvious advantages. Combined with the TEM, XRD, XPS characterization and the possible reaction mechanism of GC-MS products distribution, the nickel and molybdenum carbide nanoparticles can effectively attack the carbon-oxygen double bond, and the graphitized carbon substrate structure can help the electron transfer on the catalyst. Using different biomass materials (rice husk, sawdust, cattlegrass) under the same conditions, the biochar materials were obtained by rapid pyrolysis, and the extracts of biochar were studied for plants (wheat) and animals (Cryptonematodes elegans). Effects of microorganisms (Pseudomonas aeruginosa) on growth. The results showed that rice husks and sawdust biochar leachate had little effect on biological growth, while the biomass extract of Cattlegrass seriously inhibited biological growth, especially to Cryptonematodes elegans.
【学位授予单位】：中国科学技术大学
【学位级别】：硕士
【学位授予年份】：2016
【分类号】：O643.36
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