本文關(guān)鍵詞：超臨界水體系下Ni基雙金屬催化劑對(duì)苯酚的催化氣化研究　出處：《昆明理工大學(xué)》2017年碩士論文　論文類型：學(xué)位論文

  更多相關(guān)文章： 超臨界水沉積 雙金屬納米顆粒 苯酚 生物質(zhì) 超臨界水氣化

【摘要】：隨著化石燃料的枯竭、環(huán)境污染的惡化,以生物質(zhì)為原料生產(chǎn)生物燃油或生物燃?xì)獾姆椒ū徽J(rèn)為是緩解這些問(wèn)題最有效的方法之一。本論文是以環(huán)境污染物苯酚作為生物質(zhì)的模型化合物,負(fù)載型鎳基雙金屬納米顆粒為催化劑在超臨界水中催化氣化苯酚,通過(guò)分析其反應(yīng)產(chǎn)物,探究生物質(zhì)在超臨界水中的氣化情況。用浸漬法制備的一系列xNi-yRu/Ce02雙金屬催化劑在超臨界水中氣化苯酚的研究結(jié)果表明雙金屬納米催化劑比單金屬納米催化劑有更好的催化效果。其中10Ni-1Ru/CeO2催化劑對(duì)苯酚的氣化效果最好,將該雙金屬催化劑在500℃下催化氣化苯酚時(shí),反應(yīng)達(dá)到平衡后苯酚的碳?xì)饣蔬_(dá)到了 90%。GC-MS的結(jié)果顯示,在氣化過(guò)程中,10Ni-lRu/CeO2催化劑能夠有效的抑制二聚體如二苯并呋喃以及多環(huán)芳香烴的生成。建立動(dòng)力學(xué)模型對(duì)超臨界水催化氣化苯酚過(guò)程進(jìn)行模擬顯示氣體生成反應(yīng)過(guò)程的活化能為110 ± 17 kJ/mol及頻率因子為16.7 ± 2.6,而結(jié)焦過(guò)程的活化能和頻率因子分別為38 ± 5 kJ/mol以及3.9 ± 0.8。對(duì)10Ni-1Ru/CeO2催化劑進(jìn)行回收再利用顯示其在500℃的超臨界水體系中具有良好的穩(wěn)定性。綜合來(lái)看,利用10Ni-1Ru/CeO2雙金屬催化劑在超臨界水體系下催化氣化苯酚可以成為苯酚處理的一個(gè)有效方法,并為生物質(zhì)的氣化提供理論基礎(chǔ)。在制備催化劑過(guò)程中,本研究開發(fā)了用超臨界水沉積制備雙金屬納米催化劑的新方法,并通過(guò)超臨界水同時(shí)沉積法和連續(xù)沉積法成功的制備了以鎳鈷為例的雙金屬納米催化劑。在超臨界水催化氣化苯酚實(shí)驗(yàn)中同時(shí)沉積和分步沉積法形成的納米催化劑的催化活性都有所不同,其中Co-Ni/AC催化劑催化效果最好,在500℃時(shí),反應(yīng)達(dá)到平衡后苯酚的碳?xì)饣蔬_(dá)到了 95%。對(duì)催化劑進(jìn)行回收使用,Ni-Co/AC催化劑和Mix/AC催化劑的活性都有一定程度的下降,而Co-Ni/AC催化劑碳?xì)饣蕸](méi)發(fā)生改變,說(shuō)明該方法合成的Co-Ni/AC催化劑可用于苯酚的有效處理。
[Abstract]:With the depletion of fossil fuels, worsening environmental pollution, one method of using biomass as raw material for the production of bio fuel or method of biological gas is considered to be the most effective to alleviate these problems. This paper is based on the environmental pollutants phenol as model compounds of biomass, the supported nickel bimetallic nanoparticles as catalyst in supercritical water catalytic gasification phenol, through the analysis of the reaction products, explore the biomass in supercritical water gasification. A series of xNi-yRu/Ce02 prepared by impregnation of the double metal catalyst in supercritical water gasification research results show that the catalytic effect of phenol Nanobimetallic catalyst is better than single nano metal catalyst. The effect of 10Ni-1Ru/CeO2 catalyst on gasification phenol best the double metal catalyst, catalytic gasification of phenol under the temperature of 500 DEG C, the reaction reached balance after the carbon gasification rate of phenol. At 90%.GC-MS shows that in the gasification process, 10Ni-lRu/CeO2 catalyst can inhibit two dimers such as two benzofuran and polycyclic aromatic hydrocarbon generation effectively. Establishing the dynamic model to simulate the gas generation process is activated for 110 + 17 kJ/mol and the frequency factor is 16.7 + 2.6 of phenol in supercritical water gasification the catalytic process, then show good stability in supercritical water system of 500 DEG C in the coking process of activation energy and frequency factor were 38 + 5 and 3.9 + kJ/mol 0.8. on 10Ni-1Ru/CeO2 catalyst for recycling. In general, the use of 10Ni-1Ru/CeO2 bimetallic catalyst in supercritical water gasification of phenol can be an effective method for treatment of phenol, and provide a theoretical basis for biomass gasification. In the preparation of catalyst in the process of the research and development of Supercritical A new method of community water deposited Nanobimetallic catalyst, and through supercritical water and deposition method and continuous deposition method was successfully prepared with Nanobimetallic catalyst with cobalt and nickel as an example. The catalytic activity of nano catalyst formation deposited in supercritical water catalytic gasification experiment of phenol and the fractional precipitation method different, the catalytic effect of Co-Ni/AC catalyst is the best, at 500 DEG C, the reaction reached equilibrium after the carbon gasification efficiency of phenol reached 95%. for recycling of catalysts, Ni-Co/AC catalyst and Mix/AC catalyst activity have a certain degree of decline, while the Co-Ni/AC catalyst carbon gasification efficiency did not change, effective treatment method of the Co-Ni/AC catalyst can be used for the synthesis of phenol.

【學(xué)位授予單位】：昆明理工大學(xué)
【學(xué)位級(jí)別】：碩士
【學(xué)位授予年份】：2017
【分類號(hào)】：O643.36;X703

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