铁基碳铝催化剂的制备及其催化玉米秸秆热解制氢研究

doi:10.3969/j.issn.0253-2417.2024.02.008

Abstract

Abstract:

An iron-based carbon-aluminum catalyst(Fe/CS-AWA) was prepared using hydrothermal carbonization(HTC) method, using corn stover(CS) biomass as the raw material, activated aluminum ash(AWA) activated by waste aluminum ash(WA) as a carrier and Fe as the active component. The Fe/CS-AWA was applied in catalyzing the pyrolysis of CS for hydrogen production. By investigating the influence of Fe loading on the catalyst performance, the hydrothermal carbonization conditions on the structural properties of Fe/CS-AWA and the effect of catalytic CS pyrolysis on hydrogen production were further optimized using response surface methodology(RSM).The results indicated that compared with CS pyrolysis, AWA and CS mixed hydrothermal carbonization as a catalyst increased the hydrogen production capacity of CS pyrolysis by 19. 11 mL/g. More importantly, Fe enhanced the catalytic activity of CS-AWA, with a gas total yield of 160. 93 mL/g and hydrogen proportion of 39.96% when the Fe loading was 10%. The optimized process conditions from RSM were as follows: m_AWA ∶ m_CS of 2 ∶ 1, residence time of 60 min at 250 ℃, and a carbonization temperature of 500 ℃. Under these conditions, the gas total yield for Fe/CS-AWA catalyzing CS pyrolysis was 267. 43 mL/g, with a H₂ proportion of 37. 80%. It was found that characterization revealed the formation of irregular iron carbides and Al—O—C intermediates on the surface of Fe/CS-AWA, enhancing the catalytic activity of Fe/CS-AWA.

Key words: aluminum ash, hydrothermal carbon, carbon aluminum catalyst, response surface method, hydrogen production through pyrolysis

CLC Number:

TQ35

Yan LU, Xueqin LI, Yanling LI, Tanglei SUN, Peng LIU, Tingzhou LEI. Preparation of Iron Based Carbon Aluminum Catalyst and Its Catalytic for Hydrogen Production from Corn Straw Pyrolysis[J]. Chemistry and Industry of Forest Products, 2024, 44(2): 55-63.

Figures/Tables 9

Table 1

Fig.1

Table 2

Table 3

Table 4

Fig.2

Fig.3

Fig.4

Table 5

References 31

1	MOHAN S V , MOHANAKRISHNA G , SARMA P N . Integration of acidogenic and methanogenic processes for simultaneous production of biohydrogen and methane from wastewater treatment[J]. International Journal of Hydrogen Energy, 2008, 33 (9): 2156- 2166. doi: 10.1016/j.ijhydene.2008.01.055
2	SANSANIWAL S K , PAL K , ROSEN M A , et al. Recent advances in the development of biomass gasification technology: A comprehensive review[J]. Renewable and Sustainable Energy Reviews, 2017, 72, 363- 384. doi: 10.1016/j.rser.2017.01.038
3	ISAHAK W , HISHAM M , YARMO M , et al. A review on bio-oil production from biomass by using pyrolysis method[J]. Renewable and Sustainable Energy Reviews, 2012, 16 (8): 5910- 5923. doi: 10.1016/j.rser.2012.05.039
4	KAN T , STREZOV V , EVANS T J . Lignocellulosic biomass pyrolysis: A review of product properties and effects of pyrolysis parameters[J]. Renewable and Sustainable Energy Reviews, 2016, 57, 1126- 1140. doi: 10.1016/j.rser.2015.12.185
5	李湘萍, 张建光. 生物质热解制备多孔炭材料的研究进展[J]. 石油学报(石油加工), 2020, 36 (5): 1101- 1110.
	LI X P , ZHANG J G . Progress on biochar preparation through pyrolysis process[J]. Acta Petrolei Sinica(Petroleum Processing Section), 2020, 36 (5): 1101- 1110.
6	LI X Q, LIU P, LEI T Z, et al. Pyrolysis of biomass tar model compound with various Ni-based catalysts: Influence of promoters characteristics on hydrogen-rich gas formation[J/OL]. Energy, 2022, 244: 123137[2023-03-18]. https://doi.org/10.1016/j.energy.2022.123137.
7	LANG P P , LU A , LIU P , et al. Pyrolysis of wood waste to enhance hydrogen production on iron-based aluminum dross[J]. Fuel, 2023, 334, 126781- 126791. doi: 10.1016/j.fuel.2022.126781
8	邢万丽, 孙秋双, 杨天华, 等. 基于Ni/Al₂O₃整体式催化剂的生物质气化合成气甲烷化研究[J]. 太阳能学报, 2020, 41 (3): 363- 370.
	XING W L , SUN Q S , YANG T H , et al. Study on methanation of biomass gasification syngas based on Ni/Al₂O₃ monolithic catalysts[J]. Acta Energiae Solaris Sinica, 2020, 41 (3): 363- 370.
9	MAHINROOSTA M , ALLAHVERDI A . Hazardous aluminum dross characterization and recycling strategies: A critical review[J]. Journal of the Energy Institute, 2018, 223, 452- 468.
10	李文英, 喻长连, 李晓红, 等. 褐煤固体热载体催化热解研究进展[J]. 煤炭科学技术, 2012, 40 (5): 111- 115.
	LI W Y , YU C L , LI X H , et al. Research progress on catalytic themolysis of lignite solid heat carriers[J]. Coal Science and Technology, 2012, 40 (5): 111- 115.
11	毛俏婷, 胡俊豪, 姚丁丁, 等. 生物炭催化生物质热化学转化利用的研究进展[J]. 化工进展, 2020, 39 (4): 1302- 1307.
	MAO Q T , HU J H , YAO D D , et al. Biochar for thermo-chemical conversion of biomass: A review[J]. Chemical Industry and Engineering Progress, 2020, 39 (4): 1302- 1307.
12	王敬茹, 姚宗路, 丛宏斌, 等. 生物质炭催化玉米秸秆热解气重整提质研究[J]. 农业工程学报, 2019, 35 (16): 258- 264.
	WANG J R , YAO Z L , CONG H B , et al. Upgrading biomass pyrolysis gas from corn stalk by charcoal catalytic reforming[J]. Transactions of the Chinese Society of Agricultural Engineering, 2019, 35 (16): 258- 264.
13	SUN H L, FENG D D, ZHAO Y J, et al. Mechanism of catalytic tar reforming over biochar: Description of volatile-H₂O-char interaction[J/OL]. Fuel, 2020, 275: 117954[2023-03-18]. https://doi.org/10.1016/j.fuel.2020.117954.
14	LU Q , GUO H Q , ZHOU M X , et al. Selective preparation of monocyclic aromatic hydrocarbons from catalytic cracking of biomass fast pyrolysis vapors over Mo₂N/HZSM-5 catalyst[J]. Fuel Processing Technology, 2018, 173, 134- 142. doi: 10.1016/j.fuproc.2018.01.017
15	CLAUDE V, MAHY J G, DOUVEN S, et al. Ni- and Fe-doped γ-Al₂O₃ or olivine as primary catalyst for toluene reforminga[J/OL]. Materials Today Chemistry, 2019, 14: 100197[2023-03-18]. https://doi.org/10.1016/j.mtchem.2019.100197.
16	UDDIN M A , TSUDA H , WU S , et al. Catalytic decomposition of biomass tars with iron oxide catalysts[J]. Fuel, 2008, 87 (4/5): 451- 459.
17	LI X Q, LIU P, LEI T Z, et al. Catalytic pyrolysis of biomass tar using different Ni-based HZMS-5: Influence of promoters characteristics on hydrogen-rich gas formation[J/OL]. Social Science Electronic Publishing, 2021: 240175053[2023-03-18]. https://doi.org/10.2139/ssrn.3947557.
18	GUO F Q, DONG Y C, DONG K M, et al. Role of biochar-based catalysts in microwave-induced biomass pyrolysis: Structural properties and modification with Fe-series metals[J/OL]. Fuel, 2023, 341: 127769[2023-03-18]. https://doi.org/10.1016/j.fuel.2023.127769.
19	庞赟佶, 孟浩楠, 陈义胜, 等. Ca/Fe强化生物炭催化秸秆热解挥发分蒸汽重整产氢[J]. 农业工程学报, 2019, 35 (22): 187- 192.
	PANG Y J , MENG H N , CHEN Y S , et al. Biomass charcoal catalytic with Ca/Fe enhancing hydrogen production by pyrolysis volatile steam reforming[J]. Transactions of the Chinese Society of Agricultural Engineering, 2019, 35 (22): 187- 192.
20	项飞鹏, 王智化, 况敏, 等. Fe₂O₃添加剂对宝日希勒褐煤热解特性的影响[J]. 中国电机工程学, 2016, 36 (1): 172- 178.
	XIANG F P , WANG Z H , KUANG M , et al. Effect of Fe₂O₃ additive on pyrolysis characteristics of baorixile lignite[J]. Lignite Proceedings of the CSEE, 2016, 36 (1): 172- 178.
21	栾艳春. 铁基催化剂对生物质高温蒸汽气化影响的实验研究[D]. 包头: 内蒙古科技大学, 2015.
	LUAN Y C. Experimental study on the influence of iron-based catalysts for high-temperature steam gasification of biomass[D]. Baotou: Inner Mongolia University of Science and Technology, 2015.
22	李学琴, 时君友, 亓伟, 等. 响应面法优化生物质基固体酸催化剂的制备[J]. 太阳能学报, 2015, 36 (5): 1029- 1033.
	LI X Q , SHI J Y , QI W , et al. The preparation methods of biomass based solid acid catalyst by response surface methodology[J]. Journal of Solar Energy, 2015, 36 (5): 1029- 1033.
23	陈建峰. 生物质碳源制备铁碳化物纳米催化剂及其在费托合成的应用[D]. 广州: 广东工业大学, 2022.
	CHEN J F. Preparation of iron carbide nanocatalysts derived from biomass for Fischer-Tropsch synthesis[D]. Guangzhou: Guangdong University of Technology, 2022.
24	吴桢芬, 苏有勇, 王华. 响应面法优化碳基固体酸催化剂的制备及催化性能评价[J]. 化工新型材料, 2013, 41 (12): 152- 155.
	WU Z F , SU Y Y , WANG H . Optimization of synthsis and catalytic performance of carbon-based solid catalyst with response surface methodology[J]. New Chemical Materials, 2013, 41 (12): 152- 155.
25	刘浅. 铁基催化剂条件下煤与生物质共热解的协同作用研究[D]. 北京: 北京化工大学, 2021.
	LIU Q. Study on the synergistic effect of co-pyrolysis of coal and biomass under the condition of iron-based catalyst[D]. Beijing: Beijing University of Chemical Technology, 2021.
26	赵文祥. LDH衍生铁基催化剂强化木屑热解制备富氢合成气研究[D]. 济南: 齐鲁工业大学, 2022.
	ZHAO W X. Study on the hydrogen-rich syngas production from biomass pyrolysis enhanced by Fe-based catalyst derived from LDH[D]. Jinan: Qilu University of Technology, 2022.
27	TERZYK A P . The influence of activated carbon surface chemical composition on the adsorption of acetaminophen(paracetamol) in vitro: Part ⅡTG, FTIR, and XPS analysis of carbons and the temperature dependence of adsorption kinetics at the neutral pH[J]. Colloids and Surfaces A: Physicochemical and Engineering Aspects, 2001, 177 (1): 23- 45.
28	KUNKES E L , SIMONETTI D A , WEST R M , et al. Catalytic conversion of biomass to monofunctional hydrocarbons and targeted liquid-fuel classes[J]. Science, 2008, 322 (5900): 417- 421. doi: 10.1126/science.1159210
29	胡沔. 半焦载Fe-Ni催化剂的制备及其对生物质催化热解的机理研究[D]. 武汉: 华中科技大学, 2015.
	HU M. Preparation and mehanism for char supported Fe-Ni catalytic on biomass catalytic pyrolysis[D]. Wuhan: Huazhong University of Science and Technology, 2015.
30	SHEN Y F , ZHAO P T , SHAO Q F , et al. In-situ catalytic conversion of tar using rice husk char-supported nickel-iron catalysts for biomass pyroly-sis/gasification[J]. Applied Catalysis B: Environmental, 2014, 152, 140- 151.
31	周智超, 王焦飞, 白永辉, 等. 典型城市生活垃圾一次性竹筷子水热炭结构与气化反应特性关联机制研究[J]. 燃料化学学报, 2023, 51 (6): 718- 728.
	ZHOU Z C , WANG J F , BAI Y H , et al. Correlation mechanism between structure and gasification characteristics of typical municipal solid waste(MSW) disposable bamboo chopsticks hydrochar[J]. Journal of Fuel Chemistry and Technology, 2023, 51 (6): 718- 728.

编号No.	条件condition	H₂/(mL·g^-1)	CO/(mL·g^-1)	CH₄/(mL·g^-1)	CO₂/(mL·g^-1)	总产率/(mL·g^-1)total gas yield	气体转化率/% gas conversion(y_g)
1	CS	43.65	25.75	14.55	48.77	132.73	39.41
2	CS(HTC)	58.52	15.11	10.61	23.67	107.91	40.33
3	CS+WA(HTC)	49.98	23.14	15.16	49.39	137.68	36.67
4	CS+AWA(HTC)	62.76	28.82	18.25	50.73	160.56	41.54
5	Fe/CS-AWA(HTC)	64.36	30.02	16.89	49.78	161.06	43.77

编号No.	A m_AWA∶m_CS	B 停留时间(250 ℃)/minresidence time	C 炭化温度/℃carbonization temp.	R₁ H₂产率/%H₂ yield
1	2∶1	40	500	61.48
2	4∶1	40	500	60.06
3	2∶1	60	500	98.16
4	4∶1	60	500	69.06
5	2∶1	40	700	54.28
6	4∶1	40	700	76.57
7	2∶1	60	700	70.72
8	4∶1	60	700	63.44
9	1∶1	50	600	78.51
10	5∶1	50	600	63.49
11	3∶1	30	600	56.10
12	3∶1	70	600	69.64
13	3∶1	50	400	82.57
14	3∶1	50	800	74.27
15	3∶1	50	600	59.80
16	3∶1	50	600	64.03
17	3∶1	50	600	64.47
18	3∶1	50	600	56.83
19	3∶1	50	600	66.49
20	3∶1	50	600	56.51

来源sources	平方和sum of squares	自由度df	均方mean square	F值F value	P值P value	显著性significant
模型model	2 038.89	9	226.54	16.27	< 0.001	**
A	129.83	1	129.83	9.33	0.012 2	*
B	361.73	1	361.73	25.98	0.000 5	**
C	101.81	1	101.81	7.31	0.022 1	*
AB	409.55	1	409.55	29.42	0.000 3	**
AC	259.14	1	259.14	18.62	0.001 5	**
BC	224.26	1	224.26	16.11	0.002 5	**
A²	155.20	1	155.20	11.15	0.007 5	**
B²	5.15	1	5.15	0.37	0.556 8
C²	473.52	1	473.52	34.02	0.000 2	**
残差residual	139.21	0	13.92	0.55	0.733 6
失拟项lack of fit	49.64	5	9.93
纯误差pure error	89.57	5	17.91
总和sum	2 178.10	9

编号No.	H₂/(mL·g^-1)	CO/(mL·g^-1)	CH₄/(mL·g^-1)	CO₂/(mL·g^-1)	总产率/(mL·g^-1)total yield	y_g/%
1	104.32	60.25	23.07	94.81	282.44	38.04
2	100.68	55.53	22.24	89.42	267.87	32.10
3	98.23	53.31	20.84	79.60	251.99	34.33

催化剂catalyst	S_BET/(m²·g^-1)	S_Mic/(m²·g^-1)	S_Ext/(m²·g^-1)	孔容/(cm³·g^-1)pore volume	孔径/nmpore size	平均粒径/nmaverage particle size
AWA	77.09	28.10	48.99	0.015 0	4.38	77.83
CS-AWA	30.19	13.56	16.63	0.007 3	6.81	198.73
Fe/CS-AWA	40.72	15.78	24.94	0.008 1	4.84	147.34

Preparation of Iron Based Carbon Aluminum Catalyst and Its Catalytic for Hydrogen Production from Corn Straw Pyrolysis

RichHTML

PDF (PC)

Knowledge

Abstract

Cite this article

share this article

Figures/Tables 9

References 31

Related Articles 15

Recommended Articles

Metrics

Comments

[1]	Junhao YOU, Bao ZHANG, Hang XUN, Xi YAO, Jin WANG, Feng TANG. Optimization of Pressurized Hot Water Extraction Technology and Chemical Composition Analysis from Moso Bamboo Stalks [J]. Chemistry and Industry of Forest Products, 2023, 43(4): 107-114.
[2]	Mengru ZHAN, Yanbin WANG, Shuhe KANG, Xingping LUO. Purification of Polysaccharides from Codonopsis pilosula by Macroporous Adsorption Resin and Its Whitening, Moisture Absorption and Moisturizing Properties [J]. Chemistry and Industry of Forest Products, 2023, 43(3): 79-88.
[3]	Yong LIU, Caihong ZHANG, Pujun XIE, Yejun DENG, Lixin HUANG. Optimization of Ultrasonic-assisted Extraction Technology of Saponins from Gleditsia sinensis Thorn by RSM and Its Hypoglycemic Activity [J]. Chemistry and Industry of Forest Products, 2023, 43(2): 12-18.
[4]	Mei ZHANG, Yanjie ZHANG, Weijian CHEN, Huafang JING, Benyong LOU. Preparation of Rhododendron×pulchrum Sweet Flowers Anthocyanins Microcapsule and Its Stability [J]. Chemistry and Industry of Forest Products, 2023, 43(2): 19-26.
[5]	Shitao WEN, Linxin DAI, Zhihui WANG, Zhenrui LI, Jiajun WANG, Xing'er LIU. Preparation of Bamboo Pulp Fiber Hydrothermal Carbon Microspheres with Controllable Structure [J]. Chemistry and Industry of Forest Products, 2023, 43(2): 127-134.
[6]	Yangyang YAN, Changwei ZHANG, Chuan LI, Hao ZHOU, Chengzhang WANG. Preparation of Different Purity Indigo Extracts and Study of Their Antibacterial Activities [J]. Chemistry and Industry of Forest Products, 2023, 43(1): 104-112.
[7]	Jia FU, Yujian WU, Zhiming LIU, Haiying WANG. Chemical Constituents Analysis and Process Optimization of Ethanol Extract from Mulberry Leaves [J]. Chemistry and Industry of Forest Products, 2023, 43(1): 120-126.
[8]	Moran CHEN, Huazhong YU, Leilei LIU, Kehua TANG. Application of Response Surface Methodology for Optimication of Reducing the Content of Militarine in Bletilla striata by Rinsing [J]. Chemistry and Industry of Forest Products, 2022, 42(6): 117-122.
[9]	Tian HUANG, Xiaotong ZHANG, Jianglin ZHAO, Jianming GUO, Xin ZHOU, Yong XU. Preparation of Xylooligosaccharides by Xylonic Acid Assisted Hydrolysis of Xylan and Its Separation and Recovery Process [J]. Chemistry and Industry of Forest Products, 2021, 41(5): 8-14.
[10]	Shuqin CHEN, Yanyan YE, Yingxuan QUAN, Linhai LI, Lin NI, Shuangquan ZOU. Extraction Process and Components Analysis of Oil from the Seeds of Euscaphis konishii Hayata [J]. Chemistry and Industry of Forest Products, 2021, 41(1): 53-59.
[11]	Yiwei JIANG, Na GUO, Zhiguo LIU, Chunjian ZHAO, Yujie FU, Xiqing WANG. Optimization of Extraction Technology of Blue Honeysuckle Seed Oil and Analysis of Its Fatty Acid Composition [J]. Chemistry and Industry of Forest Products, 2020, 40(6): 30-36.
[12]	Aihua ZHANG,Juan TANG,Pengying LAI,Yidan HE,Jilie LI,Zhihong XIAO. Bio-hydrocarbon Fuel Preparation from Pyrolysate of Swida wilsoniana Fruit Oil by Catalytic Hydrogenation [J]. Chemistry and Industry of Forest Products, 2020, 40(5): 43-49.
[13]	Tingting ZHANG,Xiuli HAN,Ying LIU,Chunling DONG,Chun CHANG. Adsorption Characteristics of Ciprofloxacin by Biomass-based Activated Carbon [J]. Chemistry and Industry of Forest Products, 2020, 40(4): 71-78.
[14]	Liang CHEN,Guiping ZHAN,Ying LU,Jiaxing LI,Ji YU,Chengjin MA,Maojun YAO. Preparation and Stability of Eucommia ulmoides Oliv.Seed Oil Liposomes [J]. Chemistry and Industry of Forest Products, 2020, 40(1): 68-76.
[15]	Zhexuan LÜ,Weiwei ZHANG,Dandan LIU,Liwei ZHU,Jianxin JIANG. Extraction Technology and Surface Tension Characterization of Gymnocladus chinensis Saponin [J]. Chemistry and Industry of Forest Products, 2019, 39(6): 102-108.