过渡金属硫化物对Claus尾气催化加氢制备硫化氢的影响

Influence of transition-metal sulfide for hydrogenation of Claus tail gas on hydrogen sulfide

以γ-Al2O3为载体,考察了第一过渡金属亲硫元素和Cr系元素及其负载量对Claus尾气加氢生成H2S的催化活性。结果表明,经预硫化后上述负载量为10%质量分数的各元素,其催化活性按大小可以划分为4组:Ni、Co、Fe>Mo、W、Cu>Cr>Zn、Mn。针对第一组的3种元素进行物相分析表明,在反应气体积比为SO2/H2/N2=0.5/3/96.5,重量时间空速(WHSV)=6 000mL/(h.g)的强还原气氛下,Ni的催化活性相为稳定的NiS2,但Co和Fe除主晶相CoS2和FeS2外,还分别具有Co3S4和Co9S8或FeS和Fe7S8的贫硫相。

The catalytic activity of a series of γ-Al2O3 supported first row transition-metal sulfides for hydrogenating Claus tail gas to H2S was studied. The resuhs showed that when the metal content was 10 wt. %, after presulfiding, the catalysts can be divided into four groups as the following order according to the activity： Ni, Co and Fe 〉 Mo, W and Cu 〉 Cr 〉 Zn and Mn. Research on metal phase of the first group showed that under the condition of a molar feed ratio of SO2/H2/N2 = 0.5/3/96.5, the gas hourly space velocity per g（WHSV）of 6 000 mL/（h·g）, the metal phase of Ni catalyst was stable NiS2. However, for Co and Fe, besides the main phase CoS2 and FeS2, there are some sulfur-deficient phase, Co3S4 and Co9S8 phase existing in Co catalysts, and FeS and FeTSs in Fe catalysts.