项目名称: 等离子体催化CH4与NH3反应直接合成腈类精细化学品
项目编号: No.21503032
项目类型: 青年科学基金项目
立项/批准年度: 2016
项目学科: 有机化学
项目作者: 易颜辉
作者单位: 大连理工大学
项目金额: 21万元
中文摘要: 腈类在合成医药和精细化学品等领域有重要用途。然而,许多腈类的生产技术存在严重的环境问题。本项目旨在探索基于非平衡等离子体和非贵金属催化剂协同催化,以CH4和NH3为原料的腈类绿色合成新途径。研究重点包括:(1)以CH4高效活化产生C、CH、CH2、CH3和C2-C4自由基物种,和NH3高效活化产生NH和NH2自由基物种为目标,开展介质阻挡放电反应器的结构研究;(2)在选定的介质阻挡放电反应器中,以CH4和NH3等离子体反应生成各种腈类为基本目标,开展负载型Fe、Co、Ni、Cu等非贵金属催化剂的制备研究;(3)以高效合成特定腈类为目标,优化放电参数和反应条件,开展等离子体与非贵金属催化剂的协同催化研究;(4)通过原位发射光谱诊断、激光诱导荧光和红外光谱分析,研究电子密度和能量、激发态物种、自由基和催化剂表面吸附态物种及其与特定腈类生成的内在联系,揭示反应机理。
中文关键词: 等离子体催化;合成腈类;甲烷利用;非贵金属催化剂;协同效应
英文摘要: Nitriles are very important for the synthesis of medicines and fine chemicals. However, many nitriles are not available due to the serious environment problems of their synthesis processes. This proposal is aimed at pioneering a green and simple one-step way for the synthesis of different nitriles with raw materials no more than CH4 and NH3, based on the synergy of non-equilibrium plasma and non-noble metal catalyst, i.e., the plasma-catalysis. Research emphases include: first, the study of the configuration of dielectric barrier discharge reactor for efficient transforming of CH4 into radical species such as C, CH, CH2, CH3 and C2-C4 , and NH3 into radical species such as NH and NH2; second, the preparation of supported non-noble metal catalysts ( Fe, Co, Ni, Cu, et al.) for selected reactor in order to obtain different nitriles from the plasma reactions of CH4 and NH3; third, the investigation of the synergetic effect between plasma and different non-noble metal catalysts under suitable reaction conditions and optimized discharge parameters for efficient synthesis of some desired nitriles; finally, the reveal of the plasma-catalysis reaction mechanism by getting insight into the relationships of special nitrile synthesis with electron density and energy, excited-state species, radical species and adsorption species on the surface of the catalysts, using in situ OES, LIF and FT-IR spectroscopy methods.
英文关键词: plasma-catalysis;synthesis of nitriles;exploitation of methane;non-noble metal catalyst;synergy effect