硫掺杂氮化硼的制备及其对气相重金属的吸附特性研究

Preparation of Sulfur-Doped Boron Nitride and Its Adsorption Characteristics of Heavy Metal in Gas Phase

  • 摘要: 目前对焚烧烟气中重金属的控制以活性炭烟气喷射技术为主,然而该吸附剂高温(>150℃)下性能较差,吸附温度窗口较窄,因此开发耐高温非碳基吸附剂对于焚烧烟气中重金属的控制意义较大.以硼酸及三聚氰胺作为前驱体原料,将硫脲作为硫源掺杂进前驱体,经高温扩散后制备得到一种新型硫掺杂改性氮化硼(S-BN)吸附剂,并进行气相重金属高温吸附试验研究.结果表明:①S-BN吸附剂表面呈棱状结构,内部孔隙结构明显,不同S掺杂摩尔比下的形貌结构有一定差异.S-BN吸附剂内部孔体积范围为0.17~0.39 cm3/g,孔径分布范围为0.85~284.39 nm,平均孔径为2.95~4.19 nm,属于典型的中介孔多孔吸附剂.②当S掺杂摩尔比为0.50且1 300℃下煅烧5 h时,获得的S-BN吸附剂比表面积最大,达524.17 m2/g.S-BN吸附剂对气相重金属的最佳吸附温度为150~200℃.吸附过程中前5 min的吸附速率较快,并且在10 min内基本达到吸附饱和状态.③吸附过程动力学拟合分析发现,低温下S-BN吸附剂对重金属的吸附过程以物理吸附为主导,随着温度的升高,吸附过程逐渐转变为以化学吸附为主导.研究显示,该试验制得的新型S-BN吸附剂拥有较高的比表面积,其对气相重金属的饱和吸附量可以达到54.15~74.13 mg/g,对于气相重金属锌的吸附能力是活性炭的1.9~10.0倍,并且在相对高温(300℃)的吸附条件下仍可以保持较好的吸附能力.

     

    Abstract: Activated carbon flue gas injection is currently the main technology to control the concentration of heavy metals in incineration flue gas. However, the efficiency of the adsorption performance of activated carbon at high temperature (>150℃) is low. Therefore, the development of high-temperature resistant non-carbon-based adsorbents is of great significance to the control of heavy metals in high temperature flue gas. Sulfur-doped boron nitride (S-BN) is a non-carbon-based high-temperature resistant heavy metal adsorbent used for high-temperature adsorption of gaseous heavy metals. In this study, boric acid and melamine were used as precursor materials, thiourea was used as sulfur source to be doped into the precursor, and S-BN adsorbent was prepared by high temperature diffusion. The results showed that the surface of S-BN had a rib-like structures and the internal pore structure was obvious. The morphology and structure of S-BN varied with the molar ratio of S doping. It was found that S-BN was a typical mesoporous porous adsorbent, and its internal pore volume, pore size distribution, and average pore size were 0.17-0.39 cm3/g, 0.85-284.39 nm, and 2.95-4.19 nm, respectively. The maximum specific surface area of the adsorbent obtained after pyrolysis at 1300℃ for 5 h was 524.17 m2/g, and the molar ratio of S doping was 0.50. It was also found that 150-200℃ was the optimal temperature range for S-BN to control the adsorption of gaseous heavy metals. The adsorption rate was relatively faster in the first 5 min of the adsorption process, and the adsorption saturation could be basically reached within 10 min. Finally, it was found that the adsorption mechanism at low temperature was dominated by physical adsorption. With the increase of temperature, the adsorption mechanism changed from physical adsorption to chemical adsorption. The study has shown that the new S-BN adsorbent prepared in this experiment has a higher specific surface area. Its saturated adsorption capacity for heavy metals in gas phase was 54.15-74.13 mg/g. Compared with activated carbon, the adsorption capacity of Zn was 1.9-10.0 times., and it still has good performance at relatively high temperature (300℃).

     

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