多种碳材料与碳酸钠复合后脱硫性能对比

doi:10.16085/j.issn.1000-6613.2022-0781

摘要/Abstract

摘要：

碳材料本身对于H₂S的净化效果有限，通过将活性催化剂负载到活性炭上可以弥补碳材料脱除H₂S气体能力的不足。本文选用三种具有典型孔隙结构的碳材料：微孔活性碳纤维、中孔活性炭以及孔隙更大的单壁碳纳米管，等体积浸渍不同浓度的碳酸钠溶液制作负载活性材料的脱硫剂，应用固定床反应实验评价不同负载量下制得脱硫剂的脱硫性能，并对材料进行表征测试。经过对比，具有发达微孔结构的活性碳纤维材料整体上具有最佳的脱硫性能，且活性物质的负载量并不是越大越好。实验条件下，在出口逐渐检测到SO₂以及H₂S两种气体，其中SO₂气体出现较早。测定各类碳材料负载以及脱硫前后的表面pH，发现负载Na₂CO₃后材料表面pH得到大幅度提升，而脱硫后的材料表面pH均有不同程度的下降。

关键词: 安全工程, 硫化氢, 活性碳纤维, 活性炭, 碳纳米管, 浸渍浓度

Abstract:

The carbon material itself has limited purification effect on H₂S. Loading the activated catalyst on the activated carbon can make up for the lack of H₂S removal capacity of the carbon material. In this paper, three kinds of carbon materials with typical pore structure: microporous activated carbon fiber, mesoporous activated carbon and single-walled carbon nanotubes with larger pores were impregnated with different concentrations of sodium carbonate solution in equal volume to make desulfurizer loaded with active materials. The desulfurization performance of desulfurizer prepared under different loads was evaluated by fixed bed reaction experiment, and the materials were characterized and tested. After comparison, the activated carbon fiber material with developed microporous structure had the best desulfurization performance as a whole, and the larger the load of active substances, the better. Under the experimental conditions, SO₂ and H₂S were gradually detected at the outlet. SO₂ gas appeared earlier. When this gas appeared, it indicated that the desulfurizer would be inactivated. The surface pH of various carbon materials loaded and before and after desulfurization were measured. It was found that the pH of the material surface increased greatly after loading Na₂CO₃, while the pH of the material surface decreased in varying degrees after desulfurization.

Key words: safety engineering, hydrogen sulfide, activated carbon fiber, activated carbon, carbon nanotubes, impregnation concentration

中图分类号:

TQ127.11

张辛亥, 赵思琛, 朱辉, 张首石, 王凯. 多种碳材料与碳酸钠复合后脱硫性能对比[J]. 化工进展, 2022, 41(S1): 424-435.

ZHANG Xinhai, ZHAO Sichen, ZHU Hui, ZHANG Shoushi, WANG Kai. Comparative study on desulfurization performance of various carbon materials combined with sodium carbonate[J]. Chemical Industry and Engineering Progress, 2022, 41(S1): 424-435.

图/表 22

参考文献 19

1	中华人民共和国国家职业卫生标准 [S]. 北京: 中国标准出版社, 2019.
	National occupational health standards of the People’s Republic of China [S]. Beijing: Standards Press of China, 2019.
2	黄新, 朱道平. 硫化氢脱除方法述评[J]. 化学工业与工程技术, 2004, 25(5): 47-49, 62.
	HUANG Xin, ZHU Daoping. Review on removal technology of H₂S[J]. Journal of Chemical Industry & Engineering, 2004, 25(5): 47-49, 62.
3	DALRYMPLE D A, TROFE T W, EVANS J M. An overview of liquid redox sulfur recovery[J]. Chemical Engineering Progress, 1989, 85.
4	LIU Xinpeng, WANG Rui. H₂S removal by peroxo heteropoly compound/ionic liquid solution[J]. Fuel Processing Technology, 2017, 160: 78-85.
5	梁锋, 徐丙根, 施小红, 等. 湿式氧化法脱硫的技术进展[J]. 现代化工, 2003, 23(5): 21-24.
	LIANG Feng, XU Binggen, SHI Xiaohong, et al. Advances in desulfurization with wet oxidation process[J]. Modern Chemical Industry, 2003, 23(5): 21-24.
6	李石雷, 张冬冬, 宁平, 等. 液相催化氧化法脱除硫化氢的研究进展[J]. 广州化学, 2017, 42(5): 57-64.
	LI Shilei, ZHANG Dongdong, NING Ping, et al. Progress of liquid phase catalytic oxidation removing hydrogen sulfide[J]. Guangzhou Chemistry, 2017, 42(5): 57-64.
7	刘岱. 氧化铜基脱硫剂低温脱硫与再生性能研究[D]. 大连: 大连理工大学, 2017.
	LIU Dai. Low temperature desulfurization and regeneration performance of CuO-based adsorbents[D]. Dalian: Dalian University of Technology, 2017.
8	XUE Mei, CHITRAKAR Ramesh, SAKANE Kohji, et al. Screening of adsorbents for removal of H₂S at room temperature[J]. Green Chemistry, 2003, 5(5): 529-534.
9	JIANG Dahao, SU Lianghu, MA Lei, et al. Cu-Zn-Al mixed metal oxides derived from hydroxycarbonate precursors for H₂S removal at low temperature[J]. Applied Surface Science, 2010, 256(10): 3216-3223.
10	DHAGE Priyanka, SAMOKHVALOV Alexander, REPALA Divya, et al. Copper-promoted ZnO/SiO₂ regenerable sorbents for the room temperature removal of H₂S from reformate gas streams[J]. Industrial & Engineering Chemistry Research, 2010, 49(18): 8388-8396.
11	颜杰, 李红, 刘科财, 等. 干法脱除硫化氢技术研究进展[J]. 四川化工, 2011, 14(5): 27-31.
	YAN Jie, LI Hong, LIU Kecai, et al. Research progress of removing H₂S by dry method[J]. Sichuan Chemical Industry, 2011, 14(5): 27-31.
12	常化振, 赵朝成. 浸渍铜盐改性活性炭吸附/催化氧化低浓度H₂S[J]. 石油化工, 2008, 37(11): 1195-1200.
	CHANG Huazhen, ZHAO Chaocheng. Adsorption & catalytic oxidation of low concentration H₂S on activated carbon modified by copper salts[J]. Petrochemical Technology, 2008, 37(11): 1195-1200.
13	陈勇, 赖小林. 氧化铁/活性炭负载型硫化氢脱除剂制备及性能评价[J]. 工业催化, 2014, 22(9): 680-682.
	CHEN Yong, LAI Xiaolin. Preparation and performance evaluation of iron oxide/activated carbon supported hydrogen sulfide scavenger[J]. Industrial Catalysis, 2014, 22(9): 680-682.
14	LI Yuran, LIN Yuting, XU Zhicheng, et al. Oxidation mechanisms of H₂S by oxygen and oxygen-containing functional groups on activated carbon[J]. Fuel Processing Technology, 2019, 189: 110-119.
15	鲍勇强. 活性碳纤维负载掺铜BiVO₄光催化剂降解车内甲醛的研究[D]. 重庆: 重庆大学, 2018.
	BAO Yongqiang. Study on the degradation of formaldehyde in car by activated carbon fiber loaded with copper-doped BiVO₄ composite photocatalyst[D]. Chongqing: Chongqing University, 2018.
16	刘飞. 活性碳纤维负载金属氧化物复合材料的制备及其性能研究[D]. 成都: 西南交通大学, 2019.
	LIU Fei. Preparation and properties of activated carbon fiber supported metal oxide composites[D]. Chengdu: Southwest Jiaotong University, 2019.
17	钱佳燕, 赵彤, 吴逸雨, 等. 改性活性炭的制备及其吸附解析效果研究[J]. 辽宁化工, 2022, 51(2): 160-162.
	QIAN Jiayan, ZHAO Tong, WU Yiyu, et al. Study on preparation of modified activated carbon and its adsorption and resolution effect[J]. Liaoning Chemical Industry, 2022, 51(2): 160-162.
18	刘楠, 李伟, 张伟, 等. 碳纳米管在天然橡胶中的应用研究[J]. 中国橡胶, 2022, 38(1): 45-51.
	LIU Nan, LI Wei, ZHANG Wei, et al. Application of carbon nanotubes in natural rubber[J]. China Rubber, 2022, 38(1): 45-51.
19	包宗尧, 李永贵, 杨建忠, 等. 聚酰胺基碳纳米管复合纤维的研究现状与进展[J]. 丝绸, 2022, 59(2): 40-47.
	BAO Zongyao, LI Yonggui, YANG Jianzhong, et al. Research progress of polyamide-based carbon nanotube composite fibers[J]. Journal of Silk, 2022, 59(2): 40-47.

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原料	提供方	型号
活性碳纤维粉	江苏科净碳纤维有限公司	KJF1500型，孔隙以微孔为主，具有大的比表面积
活性炭	苏州旋风活性炭有限公司	椰壳炭粉，具有丰富的微孔以及中孔结构
碳纳米管	苏州碳丰石墨烯科技有限公司	单壁碳纳米管，孔隙结构以中孔和大孔为主
去离子水	江苏沐阳环境工程科技有限公司	—
碳酸钠	天津致远化学试剂有限公司	分析纯（AR）

原料	提供方	型号
活性碳纤维粉	江苏科净碳纤维有限公司	KJF1500型，孔隙以微孔为主，具有大的比表面积
活性炭	苏州旋风活性炭有限公司	椰壳炭粉，具有丰富的微孔以及中孔结构
碳纳米管	苏州碳丰石墨烯科技有限公司	单壁碳纳米管，孔隙结构以中孔和大孔为主
去离子水	江苏沐阳环境工程科技有限公司	—
碳酸钠	天津致远化学试剂有限公司	分析纯（AR）

材料	pH
AFC	6.01
AC	8.04
SWNT	7.97

材料	pH
AFC	6.01
AC	8.04
SWNT	7.97

脱硫剂名称	H₂S出现时间/min	SO₂出现时间/min	穿透时间 /min	穿透硫容 /g-S·g^-1
AFC	110	75	175	0.0272
AFC-Na₂CO₃-4%	170	135	190	0.0330
AFC-Na₂CO₃-7%	275	215	300	0.0523
AFC-Na₂CO₃-10%	235	185	260	0.0456
AFC-Na₂CO₃-15%	180	90	200	0.0335
AFC-Na₂CO₃-20%	235	90	255	0.0439