In-duct injection mercury removal characteristics of biochar prepared under biomass reburning condition

doi:10.16085/j.issn.1000-6613.2018-1647

Abstract

Abstract:

Biochars (called RH1050, RH 1150, WS1050 and WS1150) were prepared under reburning with biomass of rice husk and wheat straw at 1050°C and 1105°C in an entrained flow reactor, and four kinds of sorbents for mercury removal were obtained through blending above biochars and calcined coal-fired flyash, respectively. Elenmental mercury (Hg⁰) removal characteristics of different sorbents was carried out in an in-duct sorbent injection apparatus. The effects of biomass species, adsorption temperature, initial mercury concentration, and flue gas components (SO₂, NO and HCl) on Hg⁰ removal were analyzed, and mercury removal mechanism was also discussed. The obtained results indicated that the average mercury removal efficiency of four biochars is around 30%, and mercury removal efficiency of RH-biochar is a little bit larger than that of WS-biochar. Mercury removal efficiency of RH1050 continuously increases with the increase of adsorption temperature, but mercury removal efficiency of RH1150 presents fluctuating trend. The average mercury removal efficiency of RH-biochar behaves the trend of increase first and decrease later, and the maximum average mercury removal efficiencies of 35.6% and 37.1% through in-duct injection of RH1050 and RH1150 are achieved at initial mercury concentration of 25μg/m³. The presence of SO₂ suppresses Hg⁰ removal, NO enhances Hg⁰ removal, and HCl has a significant promoting effect. The average mercury removal efficiency can achieve more than 90% while HCl content in the simulated flue gas is larger than 50μL/L.

Key words: biomass reburning, biochar, in-duct sorbent injection, mercury removal, flue gas component

摘要：

采用高温携带流反应装置在1050℃和1150℃条件下制备了稻壳再燃焦（RH1050和RH1150）和小麦秸秆再燃焦（WS1050和WS1150），并分别将其与燃煤灼烧飞灰混合制成相应的脱汞吸附剂。在吸附剂管道喷射脱汞实验装置上，研究了生物质种类、吸附温度、初始汞浓度和烟气组分（SO₂、NO和HCl）对生物质再燃焦管道喷射脱汞性能的影响，并结合生物质及其再燃焦的理化特性分析，探讨了单质汞（Hg⁰）脱除机理。结果表明：4种生物质再燃焦平均脱汞效率相差不大，约为30%，稻壳再燃焦的脱汞效率略高于小麦秸秆焦。随着吸附温度的升高，RH1050脱汞效率持续增加，RH1150脱汞效率则呈现波动变化趋势。随着初始汞浓度的升高，稻壳再燃焦的平均脱汞效率均呈现先增大后减小的趋势，初始汞浓度为25μg/m³时RH1050和RH1150的平均脱汞效率最大，分别为35.6%和37.1%。SO₂对生物质再燃焦管道喷射脱汞具有一定的抑制作用，NO具有一定促进作用，而HCl的促进作用更为显著，且当HCl浓度大于50μL/L时，生物质再燃焦的平均脱汞效率均在90%以上。

关键词: 生物质再燃, 生物质焦, 管道喷射, 脱汞, 烟气组分

CLC Number:

X511

Ping LU, Jiateng SHI, Yangtian YE, Hewei JIANG. In-duct injection mercury removal characteristics of biochar prepared under biomass reburning condition[J]. Chemical Industry and Engineering Progress, 2019, 38(05): 2471-2478.

卢平, 史加腾, 叶扬天, 蒋何伟. 生物质再燃焦管道喷射脱汞性能[J]. 化工进展, 2019, 38(05): 2471-2478.

Figures/Tables 9

References 30

1	HUI M , WU Q , WANG S , et al . Mercury flows in China and global drivers[J]. Environmental Science & Technology, 2017, 51(1): 222-231.
2	DRISCOLL C T , MASON R P , CHAN H M , et al . Mercury as a global pollutant: sources, pathways, and effects[J]. Environmental Science Technoloy, 2013, 47(10): 4967-4983.
3	HU Y , CHENG H . Control of mercury emissions from stationary coal combustion sources in China: current status and recommendations[J]. Environmental Pollution, 2016, 218: 1209-1221.
4	YAN R , LIANG D T , TAY J H . Control of mercury vapor emissions from combustion flue gas[J]. Environmental Science and Pollution Research, 2003, 10(6): 399-407.
5	MUKHERJEE A B , ZEVENHOVEN R , BHATTACHARY P , et al . Mercury flow via coal and coal utilization by-products: a global perspective[J]. Resources, Conservation and Recycling, 2008, 52(4): 571-591.
6	韩粉女，钟秦 . 燃煤烟气脱汞技术的研究进展[J]. 化工进展，2011, 30(4): 878-885.
	HAN F N , ZHONG Q . Research progress of removal of mercury from coal-fired flue gas[J]. Chemical Industry and Engineering Progress, 2011, 30(4): 878-885.
7	XU Y , ZENG X , ZHANG B , et al . Experiment and kinetic study of elemental mercury adsorption over a novel chlorinated sorbent derived from coal and waste polyvinyl chloride[J]. Energy & Fuels, 2016, 30(12): 10635-10642.
8	LIU Z , YANG W , XU W , et al . Removal of elemental mercury by bio-chars derived from seaweed impregnated with potassium iodine[J]. Chemical Engineering Journal, 2018, 339(1): 468-478.
9	SI H L , RHIM Y J , CHO S P, et al . Carbon-based novel sorbent for removing gasphase mercury[J]. Fuel, 2006, 85(2): 219-226.
10	DE M, AZARGOHAR R , DALAI A K . Mercury removal by bio-char based modified activated carbons[J]. Fuel, 2013, 103: 570-578.
11	SHU T , LU P , HE N . Mercury adsorption of modified mulberry twig chars in a simulated flue gas[J]. Bioresource Technology, 2013, 136: 182-187.
12	LI G , WANG S , WANG F , et al . Role of inherent active constituents on mercury adsorption capacity of chars from four solid wastes[J]. Chemical Engineering Journal, 2017, 307: 544-552.
13	任建莉, 周劲松, 骆仲泱,等 . 活性碳吸附烟气中气态汞的试验研究[J]. 中国电机工程学报, 2004, 24(2): 171-175.
	REN J L , ZHOU J S , LUO Z Y , et al . Experimental study on adsorption of gaseous mercury in flue gas by activated carbon[J]. Proceedings of the CSEE, 2004, 24(2): 171-175.
14	洪亚光，段钰锋，朱纯，等 . 载硫椰壳活性炭喷射脱尿实验研究[J]. 工程热物理学报，2015, 36(5): 1135-1138.
	HONG Y G , DUAN Y F , ZHU C , et al . Experimental study on mercury adsorption of S-impregnated coconut shell activated carbon by duct injection[J]. Journal of Engineering Thermophysics, 2015, 36(5): 1135-1138.
15	SERRE S D , SILCOX G D . Adsorption of elemental mercury on the residual carbon in coal fly ash[J]. Ind. Eng. Chem. Res., 2000, 39(6): 1723-1730.
16	LU P , HAO J , YU W , et al . Effects of water vapor and Na/K additives on NO reduction through advanced biomass reburning[J]. Fuel, 2016, 170: 60-66.
17	BALLESTER J , ICHASO R , PINA A , et al . Experimental evaluation and detailed characterisation of biomass reburning[J]. Biomass & Bioenergy, 2008, 32(10): 959-970.
18	史加腾，尹欣怡，卢平，等 . 再燃温度对稻壳焦理化结构演变的影响[J]. 燃料化学学报， 2017, 45(8): 924-931.
	SHI J T , YIN X Y , LU P , et al . Effect of reburning temperature on physico-chemical characteristics evolution of rice husk char[J]. Journal of Fuel Chemistry & Technology, 2017, 45(8): 924-931.
19	郝江涛，于伟，卢平，等 . 生物质高级再燃脱硝的影响因素与元素释放特性[J]. 燃料化学学报, 2014, 42(5): 552-559.
	HAO J T , YU W , LU P , et al . The influence factors and element release properties of NO reduction through biomass advanced reburning[J]. Journal of Fuel Chemistry and Technology, 2014, 42(5): 552-559.
20	鲁许鳌，冉旭，郑小龙，等 . 热解温度对生物质半焦特征的影响[J]. 动力工程学报，2012, 32(11): 865-870.
	LU X A , RAN X , ZHENG X L , et al . Effects of pyrolysis temperature on characteristics of biomass char[J]. Journal of Chinese Society of Power Engineering, 2012, 32(11): 865-870.
21	周军, 张海, 吕俊复, 等 . 高温下热解温度对煤焦孔隙结构的影响[J]. 燃料化学学报, 2007, 35(2): 155-159.
	ZHOU J , ZHANG H , LU J F , et al . Effect of pyrolysis temperature on porous structure of anthracite chars produced at high temperatures[J]. Journal of Fuel Chemistry and Technology, 2007, 35(2): 155-159.
22	顾永正，王树民 . 改性燃煤飞灰吸附氧化脱汞机理研究进展[J]. 化工进展，2017, 36(11): 4257-4263.
	GU Y Z , WANG S M . Research progress of mercury adsorption and oxidation mechanism on modified coal-fired fly ash [J]. Chemical Industry and Engineering Progress, 2017, 36(11): 4257-4263.
23	王鹏，吴江，任建兴，等 . 飞灰未燃尽碳对吸附烟气汞影响的试验研究[J]. 动力工程学报，2012, 32(4): 332-337.
	WANG P , WU J , REN J X , et al . Experimental study on influence of unburned carbon in fly ash on mercury adsorption in flue gas[J]. Journal of Chinese Society of Power Engineering, 2012, 32(4): 332-337.
24	熊银伍, 杜铭华, 步学鹏, 等 . 改性活性焦脱除烟气中汞的实验研究[J]. 中国电机工程学报, 2007, 27(35): 17-22.
	XIONG Y W , DU M H , BU X P , et al . Experimental study on removal of mercury from flue gas by modified activated coke[J]. Proceedings of the CSEE, 2007, 27(35): 17-22.
25	ZENG H , FENG J , GUO J . Removal of elemental mercury from coal combustion flue gas by chloride-impregnated activated carbon[J]. Fuel, 2004, 83(1): 143-146.
26	周强，段钰锋，洪亚光，等．模拟烟气活性炭喷射脱汞实验研究[J]. 中国电机工程学报，2013, 33(35): 36-43.
	ZHOU Q , DUAN Y F , HONG Y G , et al . Experimental study on simulated flue gas activated carbon injection for mercury removal[J]. Proceedings of the CSEE, 2013, 33(35): 36-43.
27	MILLER S J , DUNHAM G E , OLSON E S , et al . Flue gas effects on a carbon-based mercury sorbent[J]. Fuel Processing Technology, 2000, 65(99): 343-363.
28	DIAMANTOPOULOU I , SKODRAS G , SAKELLAROPOULOS G P . Sorption of mercury by activated carbon in the presence of flue gas components[J]. Fuel Processing Technology, 2010, 91(2): 158-163.
29	李兵，张立强，蒋海涛，等 . 活性炭孔隙结构和表面化学性质对吸附氧化NO的影响[J]. 煤炭学报，2011, 36(11): 1906-1910.
	LI B ， ZHANG L Q ， JIANG H T , et al . Effect of pore structure and surface chemical properties of activated carbon on the adsorption and oxidation of NO[J]. Journal of China Coal Society, 2011, 36(11): 1906-1910.
30	OCHIAI R , UDDIN M A , SASAOKA E , et al . Effects of HCl and SO₂ concentration on mercury removal by activated carbon sorbents in coal-derived flue gas[J]. Energy & Fuels, 2009, 23(10): 4734-4739.

样品	工业分析			元素分析					Cl	Y	R₁
样品	A_d	FC_d	V_d	C_d	H_d	O_d	N_d	S_d	Cl	Y	R₁
RH	13.14	17.88	68.98	44.30	6.35	35.30	0.58	0.32	0.24	—	—
WS	9.83	17.46	72.71	39.17	5.63	42.34	2.55	0.48	0.72	—	—
RH1050	66.16	22.01	11.82	28.40	1.38	3.36	0.51	0.19	0.13	19.86	89.36
RH1150	69.88	22.91	7.21	27.11	1.24	1.10	0.52	0.15	0	18.80	100
WS1050	52.57	38.27	9.16	42.73	1.98	2.17	0.46	0.09	0.16	18.69	95.87
WS1150	56.66	43.34	7.36	39.87	1.85	1.06	0.44	0.12	0	17.34	100

样品	工业分析			元素分析					Cl	Y	R₁
样品	A_d	FC_d	V_d	C_d	H_d	O_d	N_d	S_d	Cl	Y	R₁
RH	13.14	17.88	68.98	44.30	6.35	35.30	0.58	0.32	0.24	—	—
WS	9.83	17.46	72.71	39.17	5.63	42.34	2.55	0.48	0.72	—	—
RH1050	66.16	22.01	11.82	28.40	1.38	3.36	0.51	0.19	0.13	19.86	89.36
RH1150	69.88	22.91	7.21	27.11	1.24	1.10	0.52	0.15	0	18.80	100
WS1050	52.57	38.27	9.16	42.73	1.98	2.17	0.46	0.09	0.16	18.69	95.87
WS1150	56.66	43.34	7.36	39.87	1.85	1.06	0.44	0.12	0	17.34	100

样品	S _BET/m²·g^-1	V _M/mm³·g^-1	V _T/mm³·g^-1	X/%	D _a/nm
飞灰	1.55	0.81	2.87	28.22	7.41
RH	1.23	0.67	1.96	34.18	6.37
WS	1.28	0.66	2.11	31.28	6.59
RH1050	176.92	93.87	111.40	84.26	2.52
RH1150	190.31	99.88	119.40	83.64	2.51
WS1050	146.27	77.05	93.12	82.74	2.55
WS1150	169.45	89.90	113.70	79.06	2.69

样品	S _BET/m²·g^-1	V _M/mm³·g^-1	V _T/mm³·g^-1	X/%	D _a/nm
飞灰	1.55	0.81	2.87	28.22	7.41
RH	1.23	0.67	1.96	34.18	6.37
WS	1.28	0.66	2.11	31.28	6.59
RH1050	176.92	93.87	111.40	84.26	2.52
RH1150	190.31	99.88	119.40	83.64	2.51
WS1050	146.27	77.05	93.12	82.74	2.55
WS1150	169.45	89.90	113.70	79.06	2.69

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