Abstract: A series of Ce-Cu-Al-O mixed metal oxide adsorbents for deep removal of H₂S at low temperature was prepared by a co-precipitation method. Characterization methods such as XRD, N₂ physical adsorption, SEM, XPS were used to analyze the samples before and after desulfurization. The influence of Ce content, calcination temperature, space velocity, adsorption temperature and impurity gas on the removal of H₂S was investigated. It was found that Ce-Cu-Al-O adsorbents were able to remove H₂S from CO₂ at 40℃and the adsorbent with 10% Ce (10Ce-Cu-Al-O) exhibited the highest breakthrough capacity of 94.1mg/g. The characterization results show that the addition of CeO₂ could effectively improve the dispersion of CuO, the BET surface areas and pore volumes of the adsorbents. A relatively high calcination temperature, high space velocity and balance gas CO₂ will all inhibit the H₂S adsorption. The H₂S breakthrough capacity of 10Ce-Cu-Al-O increased with temperature and there was no COS impurities generated when the desulfurization temperature was not higher than 100℃. The characterization results of the used adsorbents showed that the aggregate components resulted in the decrease of the BET surface areas and pore volumes. In addition, the regeneration experiment indicated that a relatively low temperature of 100℃ can be applied to regenerate the used 10Ce-Cu-Al-O adsorbents in air.

Key words: mixed metal oxides, low temperature, hydrogen sulfide, adsorption, regeneration

摘要： 用共沉淀法制备了一系列Ce-Cu-Al-O复合金属氧化物吸附剂，用于低温下脱除CO₂气体中的微量H₂S。采用XRD、N₂物理吸附、SEM及XPS等手段对脱硫前后的吸附剂结构进行表征。研究了Ce含量、煅烧温度、气体空速、杂质气体及吸附温度对吸附剂脱除H₂S性能的影响。结果表明，Ce-Cu-Al-O系列吸附剂在40℃条件下可有效脱除CO₂气体中的H₂S，Ce含量为10%的吸附剂（10Ce-Cu-Al-O）具有最大H₂S穿透吸附量，为94.1mg/g。研究发现，引入CeO₂能有效改善CuO的分散性，提高吸附剂的比表面积和孔容。提高煅烧温度，较大空速均不利于吸附剂的脱硫效果；平衡气CO₂会抑制H₂S的吸附；吸附温度不高于100℃时，10Ce-Cu-Al-O的穿透吸附量随温度升高而增加且不会生成COS副产物。表征结果显示，硫化后吸附剂的组分团聚导致了比表面积和孔容降低。此外，失活后的脱硫剂可在100℃用空气再生。

关键词: 复合金属氧化物, 低温, 硫化氢, 吸附, 再生