Improved capture capacity of SeO2 by sorbents with anti-sintering at high temperature

doi:10.16085/j.issn.1000-6613.2022-0234

Abstract

Abstract:

Selenium (Se) capture capacity by different oxides (MgO, Fe₂O₃, Al₂O₃ and CaO) at 700—1100℃ were performed by a gas-solid instant reaction system to determine characteristics of adsorption products. Then, corresponding typical minerals and bicomponent composite sorbents with anti-sintering were chosen to improve Se capture capacity at high temperature. Results showed that the capacity of CaO was highest before 900℃, but noticeably decreased to 167.59μg/g as temperature rose to 1100℃. Capture capacity of γ-Al₂O₃ was greater at high temperature, which could reach 415.04μg/g at 1100℃ likely due to its great pore structure. Calcite, one of typical Ca-based minerals, indicated great high-temperature capture capacity because of its great anti-sintering and pore structure, and the capacity could be improved to 1064.97μg/g at 1100℃. Capture capacity of bicomponent composite sorbents at high temperature presented some improvement. Capacity of Ca-Al based sorbent increased slightly, while that of Ca-Si based sorbent was much higher than that of monocomponent based sorbents, which increased by 1787.21μg/g than that of CaO.

Key words: selenium, minerals, bicomponent sorbents, high-temperature capture, anti-sintering

摘要：

使用气固瞬时反应装置在700~1100℃下对不同氧化物（氧化镁、氧化铁、氧化铝、氧化钙）的硒捕集性能进行研究，确定吸附产物性质。基于此选取相应的典型矿物及双组分抗烧结吸附剂改善硒高温吸附能力。结果表明：900℃前氧化钙捕集效果最好，但1100℃时其吸附量迅速降低到167.59μg/g；γ-氧化铝在高温下捕集效果较好，1100℃时吸附量可达415.04μg/g，这与其优异的孔隙结构有关。钙基矿物方解石因其具有一定的抗烧结能力和发达的孔隙结构，表现出更好的高温捕集能力，1100℃时吸附量可提高到1064.97μg/g。双组分吸附剂高温捕集能力展现出不同程度的提高。钙-铝基吸附剂高温捕集性能提高相对较小；而钙-硅基吸附剂在高温下效果远高于单组分吸附剂，与氧化钙相比，1100℃时可提高1787.21μg/g。

关键词: 硒, 矿物, 双组分吸附剂, 高温捕集, 抗烧结性

CLC Number:

X511

YANG Xiaoyu, YU Mengzhu, HUANG Yaji, LI Jinlei, ZHU Zhicheng, LI Zhiyuan, WANG Sheng, LI Qiubai. Improved capture capacity of SeO₂ by sorbents with anti-sintering at high temperature[J]. Chemical Industry and Engineering Progress, 2022, 41(12): 6711-6722.

杨晓域, 于梦竹, 黄亚继, 李金壘, 朱志成, 李志远, 王圣, 李秋白. 高温抗烧结吸附剂对SeO₂捕集性能[J]. 化工进展, 2022, 41(12): 6711-6722.

Figures/Tables 22

References 42

1	中华人民共和国国家统计局. 中华人民共和国2008年国民经济和社会发展统计公报[J]. 中国统计, 2009(3): 4-10.
	National Bureau of Statistics. Statistical bulletin of the People’s Republic of China on national economic and social development, 2020[J]. China Statistics, 2009(3): 4-10.
2	夏文青, 黄亚继, 王昕晔, 等. 非碳基吸附剂高温捕集氯化铅蒸气[J]. 化工进展, 2017, 36(9): 3508-3513.
	XIA Wenqing, HUANG Yaji, WANG Xinye, et al. Experimental study on high temperature adsorption of lead chloride by non-carbon adsorbents[J]. Chemical Industry and Engineering Progress, 2017, 36(9): 3508-3513.
3	FAN Yuyang, LIU Chao, KONG Xiangchen, et al. A new perspective on polyethylene-promoted lignin pyrolysis with mass transfer and radical explanation[J]. Green Energy & Environment, 2022, 7(6): 1318-1326.
4	ZHOU Chuncai, LIU Guijian, XU Zhongyu, et al. Retention mechanisms of ash compositions on toxic elements (Sb, Se and Pb) during fluidized bed combustion[J]. Fuel, 2018, 213: 98-105.
5	程运, 王昕晔, 吕文婷, 等. 高岭土高温吸附重金属和碱金属的研究进展[J]. 化工进展, 2019, 38(8): 3852-3865.
	CHENG Yun, WANG Xinye, Wenting LYU, et al. A review on heavy and alkali metals adsorption by Kaolin at high temperature[J]. Chemical Industry and Engineering Progress, 2019, 38(8): 3852-3865.
6	WANG Lei, JU Yiwen, LIU Guijian, et al. Selenium in Chinese coals: distribution, occurrence, and health impact[J]. Environmental Earth Sciences, 2010, 60(8): 1641-1651.
7	TIAN H Z, ZHU C Y, GAO J J, et al. Quantitative assessment of atmospheric emissions of toxic heavy metals from anthropogenic sources in China: historical trend, spatial distribution, uncertainties, and control policies[J]. Atmospheric Chemistry and Physics, 2015, 15(17): 10127-10147.
8	FAN Yaming, ZHUO Yuqun, LI Liangliang. SeO₂ adsorption on CaO surface: DFT and experimental study on the adsorption of multiple SeO₂ molecules[J]. Applied Surface Science, 2017, 420: 465-471.
9	National emission standards for hazardous air pollutants from coal and oil-fired electric utility steam generating units and standards of performance for fossil-fuel-fired electric utility, industrial-commercial-institutional, and small industrial [S]. Federal Register, 2016.
10	黄永达, 胡红云, 龚泓宇, 等. 燃煤电厂砷、硒、铅的排放与控制技术研究进展[J]. 燃料化学学报, 2020, 48(11): 1281-1297.
	HUANG Yongda, HU Hongyun, GONG Hongyu, et al. Research progress on emission and control technologies of arsenic, selenium and lead in coal-fired power plants[J]. Journal of Fuel Chemistry and Technology, 2020, 48(11): 1281-1297.
11	HU Jianjun, SUN Qiang, HE Huan. Thermal effects from the release of selenium from a coal combustion during high-temperature processing: a review[J]. Environmental Science and Pollution Research, 2018, 25(14): 13470-13478.
12	张军营, 任德贻, 许德伟, 等. 煤中硒的研究现状[J]. 煤田地质与勘探, 1999, 27(2): 16-18.
	ZHANG Junying, REN Deyi, XU Dewei, et al. Advances in the studies of selenium in coal[J]. Coal Geology & Exploration, 1999, 27(2): 16-18.
13	JAMES D W, KRISHNAMOORTHY G, BENSON S A, et al. Modeling trace element partitioning during coal combustion[J]. Fuel Processing Technology, 2014, 126: 284-297.
14	SENIOR C L, TYREE C A, MEEKS N D, et al. Selenium partitioning and removal across a wet FGD scrubber at a coal-fired power plant[J]. Environmental Science & Technology, 2015, 49(24): 14376-14382.
15	LI Yuzhong, TONG Huiling, ZHUO Yuqun, et al. Simultaneous removal of SO₂ and trace SeO₂ from flue gas: effect of product layer on mass transfer[J]. Environmental Science & Technology, 2006, 40(13): 4306-4311.
16	ZOU Renjie, ZHANG Haoyu, LUO Guangqian, et al. Selenium migration behaviors in wet flue gas desulfurization slurry and an in situ treatment approach[J]. Chemical Engineering Journal, 2020, 385: 123891.
17	DIAZ-SOMOANO M, MARTINEZ-TARAZONA M R. Retention of arsenic and selenium compounds using limestone in a coal gasification flue gas[J]. Environmental Science & Technology, 2004, 38(3): 899-903.
18	GHOSH-DASTIDAR A, MAHULI S, AGNIHOTRI R, et al. Selenium capture using sorbent powders: mechanism of sorption by hydrated lime[J]. Environmental Science & Technology, 1996, 30(2): 447-452.
19	AGNIHOTRI R, CHAUK S, MAHULI S, et al. Selenium removal using Ca-based sorbents: reaction kinetics[J]. Environmental Science & Technology, 1998, 32(12): 1841-1846.
20	LOU Yu, FAN Yaming, PANG Chengkai, et al. The promotion by steam on CaO adsorbing SeO₂ at medium temperature[J]. IOP Conference Series: Earth and Environmental Science, 2018, 159: 012010.
21	LI Yuzhong, TONG Huiling, ZHUO Yuqun, et al. Simultaneous removal of SO₂ and trace SeO₂ from flue gas: effect of SO₂ on selenium capture and kinetics study[J]. Environmental Science & Technology, 2006, 40(24): 7919-7924.
22	SENIOR Constance, OTTEN Brydger Van, WENDT Jost O L, et al. Modeling the behavior of selenium in pulverized-coal combustion systems[J]. Combustion and Flame, 2010, 157(11): 2095-2105.
23	XU Shengrui, SHUAI Qin, HUANG Yunjie, et al. Se capture by a CaO-ZnO composite sorbent during the combustion of Se-rich stone coal[J]. Energy & Fuels, 2013, 27(11): 6880-6886.
24	FRANDSEN Flemming, Kim DAM-JOHANSEN, RASMUSSEN Peter. Trace elements from combustion and gasification of coal—An equilibrium approach[J]. Progress in Energy and Combustion Science, 1994, 20(2): 115-138.
25	WANG Jiawei, ZHANG Yongsheng, WANG Tao, et al. Effect of modified fly ash injection on As, Se, and Pb emissions in coal-fired power plant[J]. Chemical Engineering Journal, 2020, 380: 122561.
26	FURUZONO Takuya, NAKAJIMA Tsunenori, FUJISHIMA Hiroki, et al. Behavior of selenium in the flue gas of pulverized coal combustion system: influence of kind of coal and combustion conditions[J]. Fuel Processing Technology, 2017, 167: 388-394.
27	ZENG T, SAROFIM A F, SENIOR C L. Vaporization of arsenic, selenium and antimony during coal combustion[J]. Combustion and Flame, 2001, 126(3): 1714-1724.
28	刘忠, 王硕, 白宝泉. 燃煤飞灰中矿物质对烟气中As、Se、Pb形态分布影响的热力学研究[J]. 燃料化学学报, 2020, 48(12): 1530-1536.
	LIU Zhong, WANG Shuo, BAI Baoquan. Thermodynamic study on effect of minerals in fly ash on morphological distribution of As, Se and Pb in flue gas[J]. Journal of Fuel Chemistry and Technology, 2020, 48(12): 1530-1536.
29	于梦竹, 王海, 黄亚继, 等. 典型钙/镁基吸附剂对二氧化硒吸附特性研究[J]. 燃料化学学报, 2020, 48(11): 1335-1344.
	YU Mengzhu, WANG Hai, HUANG Yaji, et al. Characteristics of selenium capture by typical Ca-/ Mg-based sorbents[J]. Journal of Fuel Chemistry and Technology, 2020, 48(11): 1335-1344.
30	王昕晔, 黄亚继, 仲兆平, 等. 炉内添加剂对垃圾焚烧过程中重金属捕集影响的试验研究[J]. 中国电机工程学报, 2012, 32(32): 15-21, 4.
	WANG Xinye, HUANG Yaji, ZHONG Zhaoping, et al. Experimental study on the capture of heavy metals by in-furnace additives during MSW incineration[J]. Proceedings of the CSEE, 2012, 32(32): 15-21, 4.
31	CAO Yue, SONG Bing, SONG Min, et al. Capture of arsenic in coal combustion flue gas at high temperature in the presence of CaSiO₃ with good anti-sintering[J]. Fuel Processing Technology, 2020, 205: 106428.
32	CHENG Haoqiang, HUANG Yaji, ZHU Zhicheng, et al. Enhanced PbCl₂ adsorption capacity of modified Kaolin in the furnace using a combined method of thermal pre-activation and acid impregnation[J]. Chemical Engineering Journal, 2021, 414: 128672.
33	刘瑞卿, 王钧伟. 矿物质与矿物离子对煤中硒释放行为的影响[J]. 环境化学, 2013, 32(1): 100-105.
	LIU Ruiqing, WANG Junwei. Influence of minerals and mineral ions on selenium release behaviors during coal pyrolysis[J]. Environmental Chemistry, 2013, 32(1): 100-105.
34	YUAN Changle, ZHANG Cheng, YU Shenghui, et al. Experimental and density functional theory study of the adsorption characteristics of CaO for SeO₂ in simulated flue gas and the effect of CO₂ [J]. Energy & Fuels, 2020, 34(9): 10872-10881.
35	SHENASA Mohsen, SAINKAR Sudhakar, LICHTMAN David. XPS study of some selected selenium compounds[J]. Journal of Electron Spectroscopy and Related Phenomena, 1986, 40(4): 329-337.
36	SARODE P R, RAO K J, HEGDE M S, et al. Study of As₂(Se, Te)₃ glasses by X-ray absorption and photoelectron spectroscopy[J]. Journal of Physics C: Solid State Physics, 1979, 12(19): 4119-4128.
37	BAHL M K, WATSON R L, IRGOLIC K J. LMM Auger spectra of selenium and some of its compounds[J]. The Journal of Chemical Physics, 1980, 72(7): 4069-4077.
38	SATOH Kenji, TAKAHASHI Takashi, Hiroshi KATAYAMA-YOSHIDA, et al. Bound states in copper-based Cu-Ge and Cu-Se alloys studied by X-ray photoelectron spectroscopy[J]. Journal of the Physical Society of Japan, 1985, 54(3): 1214-1215.
39	CAHEN David, IRELAND P J, KAZMERSKI L L, et al. X-ray photoelectron and Auger electron spectroscopic analysis of surface treatments and electrochemical decomposition of CuInSe₂ photoelectrodes[J]. Journal of Applied Physics, 1985, 57(10): 4761-4771.
40	FAN Yaming, ZHUO Yuqun, LOU Yu, et al. SeO₂ adsorption on CaO surface: DFT study on the adsorption of a single SeO₂ molecule[J]. Applied Surface Science, 2017, 413: 366-371.
41	ZHA Jianrui, HUANG Yaji, CLOUGH Peter T, et al. Green production of a novel sorbent from Kaolin for capturing gaseous PbCl₂ in a furnace[J]. Journal of Hazardous Materials, 2021, 404(Pt B): 124045.
42	YU Mengzhu, HUANG Yaji, XIA Wenqing, et al. PbCl₂ capture by Kaolin and metakaolin under different influencing factors of thermal treatment[J]. Energy & Fuels, 2020, 34(2): 2284-2292.

T/°C	ΔH/kcal	ΔS/cal·K^-1	ΔG/kcal	lgK	T/°C	ΔH/kcal	ΔS/cal·K^-1	ΔG/kcal	lgK
500	84.156	108.146	0.543	-0.153	900	94.349	118.762	-44.976	8.379
600	86.677	111.212	-10.428	2.610	1000	96.937	120.878	-56.959	9.779
700	89.218	113.967	-21.689	4.871	1100	99.539	122.846	-69.147	11.006
800	91.776	116.469	-33.213	6.764	1200	102.156	124.686	-81.524	12.096

T/°C	ΔH/kcal	ΔS/cal·K^-1	ΔG/kcal	lgK	T/°C	ΔH/kcal	ΔS/cal·K^-1	ΔG/kcal	lgK
500	84.156	108.146	0.543	-0.153	900	94.349	118.762	-44.976	8.379
600	86.677	111.212	-10.428	2.610	1000	96.937	120.878	-56.959	9.779
700	89.218	113.967	-21.689	4.871	1100	99.539	122.846	-69.147	11.006
800	91.776	116.469	-33.213	6.764	1200	102.156	124.686	-81.524	12.096

T/°C	ΔH/kcal	ΔS/cal·K^-1	ΔG/kcal	lgK
500	166.491	403.340	-145.351	41.090
600	173.289	411.606	-186.105	46.586
700	180.202	419.101	-227.647	51.129
800	187.199	425.945	-269.904	54.971
900	194.266	432.241	-312.817	58.281
1000	201.390	438.069	-356.336	61.174
1100	208.565	443.493	-400.418	63.736

T/°C	ΔH/kcal	ΔS/cal·K^-1	ΔG/kcal	lgK
500	166.491	403.340	-145.351	41.090
600	173.289	411.606	-186.105	46.586
700	180.202	419.101	-227.647	51.129
800	187.199	425.945	-269.904	54.971
900	194.266	432.241	-312.817	58.281
1000	201.390	438.069	-356.336	61.174
1100	208.565	443.493	-400.418	63.736

T/°C	ΔH/kcal	ΔS/cal·K^-1	ΔG/kcal	lgK
600	41.565	39.117	7.409	-1.855
700	40.699	38.179	3.544	-0.796
800	39.717	37.220	-0.226	0.046
900	38.615	36.239	-3.899	0.726
1000	37.389	35.237	-7.473	1.283
1100	36.039	34.217	-10.946	1.742

Improved capture capacity of SeO₂ by sorbents with anti-sintering at high temperature

高温抗烧结吸附剂对SeO₂捕集性能

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Figures/Tables 22

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样品	比表面积/m²·g^-1	孔容/cm³·g^-1	孔径/nm
MgO（700℃）	3.58	0.0096	10.75
Fe₂O₃（700℃）	2.92	0.0074	10.08
高岭土（700℃）	2.61	0.0094	14.45
方解石（900℃）	6.55	0.0203	12.39
CaSiO₃（700℃）	3.44	0.0110	12.81
CaSiO₃（900℃）	3.17	0.0056	7.08

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