本文選題：超臨界水　切入點(diǎn)：水熱氣化　出處：《華東師范大學(xué)》2017年碩士論文

【摘要】：隨著世界人口的快速增長(zhǎng)以及經(jīng)濟(jì)的高速發(fā)展,化石能源的開發(fā)程度和消費(fèi)水平迅速增加。但化石能源不可再生,且其儲(chǔ)量十分有限。因此,轉(zhuǎn)變能源結(jié)構(gòu),研究利用新一代可再生、環(huán)境友好型能源是人類可持續(xù)發(fā)展所面臨的緊迫任務(wù)。生物質(zhì)能源由于原料豐富、來源廣泛、生產(chǎn)操作工藝安全等特點(diǎn),近年來被普遍認(rèn)為是化石燃料的主要替代能源。脂質(zhì)作為生物質(zhì)中重要的組成部分,因其所占比例高、分布廣泛、熱值高,是目前新型生物質(zhì)能源的研究熱點(diǎn)。相較于傳統(tǒng)的生物質(zhì)工業(yè)轉(zhuǎn)化途徑(酶降解和熱裂解),通過水熱氣化法將其轉(zhuǎn)化為燃?xì)馐且粭l方便快捷的路徑,不需要進(jìn)行干燥、萃取等大量耗能且會(huì)導(dǎo)致污染的額外處理,綠色環(huán)保,獲得的燃?xì)鉄嶂递^高,具有良好的應(yīng)用前景。本論文根據(jù)脂質(zhì)在超臨界水中水解后的主要成分脂肪酸,選取了一系列模型化合物,采用自制的石英釜式生物質(zhì)超臨界水氣化反應(yīng)實(shí)驗(yàn)裝置考察其超臨界水熱氣化過程,以期為脂質(zhì)生物質(zhì)的超臨界水熱氣化研究提供實(shí)驗(yàn)數(shù)據(jù)參考及理論依據(jù)。本文的主要研究?jī)?nèi)如下:1.非催化條件下長(zhǎng)鏈脂肪酸的超臨界水熱氣化反應(yīng)研究以正十五酸為主要研究對(duì)象,正十四酸和油酸作為驗(yàn)證。在不添加催化劑的情況下,各實(shí)驗(yàn)因素對(duì)脂肪酸SCWG的影響順序?yàn)?反應(yīng)溫度反應(yīng)保留時(shí)間反應(yīng)物質(zhì)量分?jǐn)?shù)。反應(yīng)溫度的提升會(huì)生成更多的氣體組分,元素回收率及HHV也隨之上升;在一定的反應(yīng)溫度和壓力下,反應(yīng)保留時(shí)間的增加在絕大多數(shù)條件下使氣體產(chǎn)率、元素回收率和HHV隨之增加,但隨著保留時(shí)間的進(jìn)一步增加,氣體產(chǎn)率、元素回收率和HHV增長(zhǎng)幅度降低。隨著反應(yīng)物質(zhì)量分?jǐn)?shù)的增加,脂肪酸超臨界水熱氣化(SCWG)的氣體產(chǎn)率、元素回收率和HHV有一定降低。C元素回收率在400-450 ℃較高,在所測(cè)整體溫度區(qū)間最高值為16.8%;H元素回收率在500-550℃較高,最高值為57.1%;HHV最高可達(dá)16.8kJ·kg-1,大約相當(dāng)于標(biāo)準(zhǔn)煤熱值的57%。液相產(chǎn)物除了殘留未反應(yīng)的脂肪酸以脂肪酸外以脫羧后的直鏈烴為主,同時(shí)含有部分芳香烴和高聚物。將氣體產(chǎn)物分布數(shù)據(jù)和液相產(chǎn)物的表征相結(jié)合,根據(jù)脂肪酸實(shí)際分解情況,探究了脂肪酸非催化超臨界水氣化四種重要中間反應(yīng)受各反應(yīng)因素的作用及其對(duì)反應(yīng)結(jié)果的影響。2.催化條件下長(zhǎng)鏈脂肪酸的超臨界水熱氣化反應(yīng)研究考察了Pd/C、Pt/C、Rh/C和Ru/C四種催化劑對(duì)脂肪酸SCWG反應(yīng)過程的影響,通過研究SCWG氣體產(chǎn)物的分布,發(fā)現(xiàn)Ru/C對(duì)脂肪酸催化SCWG反應(yīng)的催化效果最佳,C元素回收率可達(dá)95.67%,H元素回收率可達(dá)135.73%;HHV最高可達(dá)36.38 kJ·g-1,大約相當(dāng)于標(biāo)準(zhǔn)煤熱值的124%。實(shí)驗(yàn)結(jié)果表明,四種催化劑催化的SCWG氣體總產(chǎn)率和C元素回收率均有上升;H元素回收率在Pd/C催化下基本不變,在其他三種催化劑下有較大程度的提升;HHV在Pd/C催化下略有下降,在其他三種催化劑的作用下有較大程度的提升。催化SCWG反應(yīng)的脂肪酸基本完全轉(zhuǎn)化,只有極少量的殘留,直鏈飽和烴類為液相產(chǎn)物的主要成分;芳香烴和其他不飽和烴種類、濃度都有大幅降低。將氣體產(chǎn)物分布數(shù)據(jù)和液相產(chǎn)物的表征相結(jié)合,分析了催化劑對(duì)各產(chǎn)物含量變化的影響及可能的催化機(jī)理。
[Abstract]:With the rapid development of the rapid growth of the world's population and economy, fossil energy development and consumption level is increasing rapidly. But the fossil energy is non renewable, and its reserves are very limited. Therefore, change the energy structure, research on the use of a new generation of renewable, environmentally friendly energy source is the urgent task for the biomass of human sustainable development. Because of the energy rich raw materials, a wide range of sources, production operation process safety, in recent years is generally considered to be the main alternative to fossil fuels. As an important lipid in biomass components, because of its high proportion, wide distribution, high calorific value, is the focus of new biomass energy compared to the traditional way. Industrial conversion of biomass (enzymatic degradation and pyrolysis), transformed into gas is a convenient path through the water steaming method, without the need for drying, extraction etc. Additional, a lot of energy and can cause pollution, high calorific value of fuel gas is obtained, which has good application prospects. This paper is based on the main components of lipid hydrolysis in supercritical water after fatty acid, a series of model compounds were selected, using the self-made silica kettle type biomass gasification in supercritical water reaction experiment apparatus to investigate the supercritical hydrothermal gasification process, provide experimental data and theoretical basis for supercritical hydrothermal gasification of biomass in order to lipid. The main research work of this paper are as follows: 1. under the condition of non catalytic supercritical hydrothermal gasification of long chain fatty acids react with acid as the main research object is fifteen, is fourteen and acid verify. Without the addition of oleic acid as catalyst under the order of the effects of experimental factors on fatty acid SCWG as the reaction temperature and the reaction time of the reactant mass fraction of retained temperature. Ascension will generate more gas component elements, recovery and HHV also increased; in certain reaction temperature and pressure, increase the retention time of the reaction gas yield in most conditions, recovery rates and HHV increased, but with the further increase of retention time, gas yield, recovery rate and elements the growth rate of HHV decreased. With the increase of the mass fraction of the reactants, fatty acids in supercritical hydrothermal gasification (SCWG) gas yield, recovery rates and HHV have lower.C recovery rates at 400-450 degrees higher in the measured temperature range the highest value is 16.8%; the recovery rate of H elements in 500-550 degrees higher and the maximum value is 57.1%; HHV reached 16.8kJ / kg-1, roughly equivalent to standard coal calorific value of 57%. liquid products in addition to straight chain fatty acid residues of unreacted fatty acid by decarboxylation after, also contain some aromatic Characterization of hydrocarbons and polymers. The gas distribution data products and liquid products combined, according to the actual situation of the decomposition of fatty acids, fatty acid non catalytic supercritical water gasification of four kinds of important intermediate reaction by various reaction factors and its influence on the reaction results of long chain fatty acid catalyzed by.2. under the condition of supercritical hydrothermal gasification reaction of Pd/C, Pt/C, Rh/C and Ru/C of four kinds of catalysts on the fatty acids of SCWG process, the distribution of SCWG gas products, found that the catalytic effect of Ru/C on the catalytic reaction of fatty acid SCWG, C element recovery was 95.67%, H element recovery rate can reach up to 135.73% HHV; 36.38 kJ - g-1, roughly equivalent to standard coal calorific value of 124%.. The experimental results show that the total yield of SCWG gas and C four catalyst element recovery rate increased; H element recovery rate under the catalysis of Pd/C basic Change, have greatly improved in the other three kinds of catalyst; HHV decreased in the presence of Pd/C has greatly improved in the other three kinds of catalyst. Fatty acid catalyzed SCWG reaction of the basic conversion, only a very small amount of residues, straight chain saturated hydrocarbons as the main composition of the liquid products; aromatic hydrocarbons and other unsaturated hydrocarbon types, concentrations were significantly reduced. The characterization of product gas and liquid product distribution data combined with the analysis of the effect of catalyst on the content changes of each product and the possible mechanism of catalysis.

【學(xué)位授予單位】：華東師范大學(xué)
【學(xué)位級(jí)別】：碩士
【學(xué)位授予年份】：2017
【分類號(hào)】：TK6;TQ645.6

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