cu改性vwti催化剂低温nh3scr性能研究word格式论文.docxVIP

中文摘要目前 NOx 污染物的大量排放导致光化学烟雾，酸雨及人体危害等影响，因此 受到广泛关注。SCR 是一种常用的消除 NOx 技术，V/WTi 催化剂因其具有优异的 中温活性及抗硫性能而被广泛应用于固定源脱硝。当燃煤电厂出现低负荷运行时， 由于其烟气温度不足导致 SCR 脱硝系统不能正常启动。为了避免上述问题，开发 出优异低温活性的 NH3-SCR 催化剂成为迫在眉睫的任务。本论文通过浸渍法将 CuO 引入到 V/WTi 催化剂体系中，考察改性催化剂 NH3-SCR 性能影响，并对其 组成-结构-性能之间的关系进行详细论述，同时提出 CuO 改性钒钨钛催化剂的机 理。研究发现 CuO 改性样品较 V/WTi 表现出优异的较低温度 NH3-SCR 性能。利 用 XRD, Raman, EPR, H2-TPR, XPS 及 in situ DRIFTS 等表征手段详细考察了铜改 性催化剂低温活性提高原因。结构表征表明钒及铜物种负载后，对载体晶型结构 没有影响；两种负载物种在催化剂表面都以高度分散态存在。EPR, H2-TPR, XPS 表明催化剂表面亲密接触的钒和铜物种形成双还原对（V5+/V4+和 Cu2+/Cu+），二者通过 Cu2++V4+?V5++Cu+发生电子相互传导作用。结合相关吸附实验结果表明二者通过还原对的电子相互传导作用能够显著提高催化剂表面钒物种的氧化还原性能从而提高其表面的吸附 NH3 物种催化活性；另一方面该电子交互作用能够诱导 铜物种表面形成更高活性的硝酸盐物种。动力学结果表明 CuO 改性能够显著降低催化反应 Ea 值从而进一步证明铜和钒之间的电子交互作用促进催化剂低温活性。关键词： V(Cu)/WTi 催化剂NH3-SCR低温活性 CuOIAbstractNitrogen oxides (NOx), are one of the most dangerous air pollutants that cause acid rain and photochemical smog, as well as directly do harm to human health. The selective reduction of NOx by NH3 is one of the most efficient NOx emission control technologies. V2O5-WO3/TiO2 has been a well-known NH3-SCR catalyst and shows optimum performance within a narrow temperature window of 300-400?C and the high resistance to SO2 poisoning. Under the condition of low-load operation, the temperature of exhausted gas cannot reach to the lowest operation temperature, causing the SCR denitrification system not operation. Hence, it is urgent to develop a novel NH3-SCR catalyst with excellent NOx conversion at low temperature to avoid the problems associated with the existing commercial system, especially for the coal power plant. The V/WTi was first prepared by traditional incipient wetness impregnation method, and then, Cu was added to gain the V(Cu)/WTi catalyst with the same method. The promoting effect of Cu on the SCR active was evaluated and the structure-performance correlation on NH3-SCR performance was investigated. Meanwhile, a mechanism of NH3-SCR over V(Cu)/WTi catalyst at low temperature is proposed to further understand the pro