论文总字数：27213字

摘 要

2吸附脱附、BET比表面积和孔隙结构分析仪、X射线能谱仪等仪器，对高温热解和活化处理后的高硫石油焦的物理化学性质进行了表征；在模拟烟气固定床汞吸附实验台上，进行了高温热解高硫石油焦和高温活化高硫石油焦的吸附Hg⁰实验研究，考察了热解温度、活化温度等对高硫石油焦脱汞特性的影响，并对实验结果进行了理论分析和讨论。试验结果表明，低温时原始高硫石油焦表面硫形态主要是硫化物、亚砜等向噻吩转化，高温时主要是噻吩向亚砜和砜等高价态的硫转化。KOH作为强氧化剂对于高硫石油焦表面的硫具有一定的氧化作用，主要发生的是低价态的噻吩等向高价态的砜和硫酸盐转化。高硫石油焦吸附剂对于Hg⁰同时存在物理吸附和化学吸附，其吸附效率受到比表面积、孔隙结构以及表面硫形态的共同影响。比表面积越大，孔隙结构越发达，低价态的硫含量越高，脱汞性能越好。本实验首次研究了高硫石油焦吸附剂在活化处理后硫形态的转变，以及对于单质汞的吸附能力。

关键词：高硫石油焦；硫形态转化；脱汞特性；高温热解；高温活化

High-sulfur Petroleum Coke’s Sulfur Transformation and Removal Characteristics of Mercury

03211736 Zhou Yongsu

Supervised by Liu Meng

Abstract：Author preparates high-sulfur petroleum coke adsorbent by put high-sulfur petroleum coke forwards high temperature pyrolysis and activation. Characterize the physical and chemical characterization of high-sulfur petroleum coke adsorbent, while analysis the results of experimental of fixed-bed of simulated flue gas, study the surface sulfur transformation and the characteristics of mercury removal from simulated flue gas fixed bed experimental device. Author puts sulfur petroleum coke in 300℃, 500℃, 700℃, 900℃, 1100℃ high temperature pyrolysis conditions and KOH and high sulfur petroleum coke mixing in accordance with 1: 1 weight ratio then activate in 650 ℃, 750 ℃, 850 ℃, 950 ℃; by N₂ adsorption-desorption, BET specific surface area and pore structure analyzers, X-ray spectrometer and other equipment, characterize the physical and chemistry characterization of high sulfur petroleum coke adsorbents after high temperature pyrolysis and activation; experiment high sulfur petroleum coke adsorbent , adsorption of Hg⁰, knowing the the effects of pyrolysis temperature, activation temperature on sulfur petroleum coke mercury removal characteristics, the theoretical and the experimental results were analyzed and discussed. The results show that at low temperatures the original surface sulfur forms sulfur petroleum coke is mainly sulfide, sulfoxide to thiophene conversion, when the high temperature is mainly thiophene sulfur to sulfoxide and sulfone and other high state of transformation. As a strong oxidizing agent, KOH has a certain oxidation for sulfur surfaced sulfur petroleum coke, low-cost states such as thiophene conversion to high state of sulfone and sulfates.Physical adsorption and chemisorption present in sulfur petroleum coke adsorbent adsorb Hg0，adsorption efficiency by the combined effect of the specific surface area, pore structure and surface morphology of sulfur. The larger the specific surface area, pore structure more developed, the higher valence state of sulfur content, the better the mercury removal performance. The experiment first study the transformation of sulfur forms sulfur petroleum coke adsorbent after activation, and elemental mercury adsorption capacity.

Key words：sulfur petroleum coke, sulfur form transformation, mercury removal feature, pyrolysis, high-temperature activation

目 录

1绪论……………………………………………………………………………1

1.1 课题研究背景…………………………………………………………………………1

1.2 燃煤汞污染…………………………………………………………………………1

1.2.1 煤中汞的赋存形态…………………………………………………………………………1

1.2.2 燃煤汞排放特性…………………………………………………………………………2

1.2.3 燃煤汞污染控制技术………………………………………………………………3

1.3 高硫石油焦………………………………………………………………………………… 4

1.3.1 高硫石油焦中硫的赋存形态……………………………………………………………4

1.3.2 高硫石油焦的利用技术……………………………………………………………5

1.4 本文研究内容和方法…………………………………………………………………… 5

2 试验系统与方法……………………………………………………………………………7

2.1 引言………………………………………………………………………………… 7

2.2 试验系统……………………………………………………………………………7

2.2.1管式炉实验系统…………………………………………………………………………… 7

2.2.2 模拟烟气固定床实验系统………………………………………………………………… 7

2.3 测试仪器……………………………………………………………………………8

2.3.1 VM-3000在线测汞仪……………………………………………………………………… 8

2.3.2 比表面积及孔隙度分析仪（BET）…………………………………………………………9

2.3.3 X射线光电子能谱仪（XPS）………………………………………………………… 10

2.4 本章小结……………………………………………………………………………10

3 高硫石油焦吸附剂的制备及其物理化学性能表征……………………………………… 11

3.1 高硫石油焦吸附剂的制备………………………………………………………………11

3.2 高硫石油焦吸附剂物理性能表征………………………………………………………… 11

3.2.1 比表面积和孔隙结构分析………………………………………………………………11

3.3 高硫石油焦吸附剂化学性能表征……………………………………………………………12

3.4 本章小结……………………………………………………………………………………14

4 高硫石油焦吸附剂固定床脱汞性能试验………………………………………………… 15

4.1 实验方法………………………………………………………………………………15

4.2 吸附剂脱汞性能评价指标……………………………………………………………………15

4.3 原始高硫石油焦的脱汞性能……………………………………………………………17

4.4 热解活化后高硫石油焦的脱汞性能………………………………………………………18

4.4.1 不同温度热解………………………………………………………………………………18

4.4.2 不同温度活化…………………………………………………………………………19

4.5 本章小结……………………………………………………………………………………20

5结论………………………………………………………………………………………21

5.1全文总结………………………………………………………………………………………21

5.1.1高硫石油焦吸附剂的制备及其物理化学性能表征…………………………………21

5.1.2不同高硫石油焦吸附剂固定床吸附特性……………………………………………21

致谢……………………………………………………………………………………………22

参考文献………………………………………………………………………………………23

高硫石油焦硫形态转化及脱汞特性研究

1、绪论

1.1 课题研究背景

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