超临界水体系下Ni基双金属催化剂对苯酚的催化气化研究

发布时间：2018-01-14 17:36

本文关键词：超临界水体系下Ni基双金属催化剂对苯酚的催化气化研究　出处：《昆明理工大学》2017年硕士论文　论文类型：学位论文

【摘要】：随着化石燃料的枯竭、环境污染的恶化,以生物质为原料生产生物燃油或生物燃气的方法被认为是缓解这些问题最有效的方法之一。本论文是以环境污染物苯酚作为生物质的模型化合物,负载型镍基双金属纳米颗粒为催化剂在超临界水中催化气化苯酚,通过分析其反应产物,探究生物质在超临界水中的气化情况。用浸渍法制备的一系列xNi-yRu/Ce02双金属催化剂在超临界水中气化苯酚的研究结果表明双金属纳米催化剂比单金属纳米催化剂有更好的催化效果。其中10Ni-1Ru/CeO2催化剂对苯酚的气化效果最好,将该双金属催化剂在500℃下催化气化苯酚时,反应达到平衡后苯酚的碳气化效率达到了 90%。GC-MS的结果显示,在气化过程中,10Ni-lRu/CeO2催化剂能够有效的抑制二聚体如二苯并呋喃以及多环芳香烃的生成。建立动力学模型对超临界水催化气化苯酚过程进行模拟显示气体生成反应过程的活化能为110 ± 17 kJ/mol及频率因子为16.7 ± 2.6,而结焦过程的活化能和频率因子分别为38 ± 5 kJ/mol以及3.9 ± 0.8。对10Ni-1Ru/CeO2催化剂进行回收再利用显示其在500℃的超临界水体系中具有良好的稳定性。综合来看,利用10Ni-1Ru/CeO2双金属催化剂在超临界水体系下催化气化苯酚可以成为苯酚处理的一个有效方法,并为生物质的气化提供理论基础。在制备催化剂过程中,本研究开发了用超临界水沉积制备双金属纳米催化剂的新方法,并通过超临界水同时沉积法和连续沉积法成功的制备了以镍钴为例的双金属纳米催化剂。在超临界水催化气化苯酚实验中同时沉积和分步沉积法形成的纳米催化剂的催化活性都有所不同,其中Co-Ni/AC催化剂催化效果最好,在500℃时,反应达到平衡后苯酚的碳气化效率达到了 95%。对催化剂进行回收使用,Ni-Co/AC催化剂和Mix/AC催化剂的活性都有一定程度的下降,而Co-Ni/AC催化剂碳气化效率没发生改变,说明该方法合成的Co-Ni/AC催化剂可用于苯酚的有效处理。
[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.

【学位授予单位】：昆明理工大学
【学位级别】：硕士
【学位授予年份】：2017
【分类号】：O643.36;X703

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