过渡金属负载Silicalite-1分子筛的制备及其催化糠醛加氢性能研究

doi:10.19964/j.issn.1006-4990.2023-0423

Abstract

Abstract:

Furfural is an important biomass-derived platform molecule，and developing robust catalysts with high activity and stability for furfural hydrogenation is a research hotspot.However，noble metal catalysts suffer from high costs，which cannot satisfy the demand towards large-scale industrial production.Herein，the transition metal-supported Silicalite-1 zeolite catalysts were successfully synthesized by a one-step hydrothermal method，and the influence of the introduction of four different types of transition metal elements on the structure of the Silicalite-1 zeolite was studied.Comprehensive characterization results showed that the crystallinity of the zeolite was not affected by low metal loading，and the metal species were uniformly dispersed on the surface of zeolite.In the hydrogenation of furfural，Ni-based catalyst S-Ni2 showed excellent catalytic activity toward furfural transformation with 96% furfural conversion and 71% furan selectivity.Cu-based catalyst S-Cu1 showed extraordinary selectivity toward furfuryl alcohol（100%），which was much higher than that over Cu-based catalyst prepared by impregnation method（76%）.Therefore，compared with the impregnation method，one-step hydrothermal method could be used to obtain a catalyst with high selectivity，and the method wass also simple and easy to operate.This work would open up a new direction for developing highly efficient，stable，and low-cost hydrogenation catalysts，and promote the valorization of biomass.

Key words: metal-supported zeolite, Silicalite-1 zeolite, furfural hydrogenation, one-step hydrothermal method

CLC Number:

O643.36

DI Lu, WANG Weiguo, CHEN Juexian, WU Chuanshu. Study on preparation of transition metal-supported Silicalite-1 zeolite catalyst and its catalytic performance for furfural hydrogenation[J]. Inorganic Chemicals Industry, 2024, 56(4): 125-132.

Figures/Tables 10

Table 1

Fig.1

Table 2

Fig.2

Fig.3

Fig.4

Fig.5

Fig.6

Fig.7

Fig.8

References 15

1	王鹏，赵山山，卢雁飞，等. 铜系材料的制备及其催化丁二酸二甲酯加氢的性能探究［J］. 无机盐工业， 2023， 55（10）：145-152.
	WANG Peng， ZHAO Shanshan， LU Yanfei， et al. Study on preparation of copper-based materials and its catalytic performance for hydrogenation of dimethyl succinate［J］. Inorganic Chemicals Industry， 2023， 55（10）：145-152.
2	李亮荣，付兵，刘艳，等. 生物质衍生物重整制氢研究进展［J］. 无机盐工业， 2021， 53（9）：12-17.
	LI Liangrong， FU Bing， LIU Yan， et al. Research progress of hydrogen production by reforming biomass-derived compounds［J］. Inorganic Chemicals Industry， 2021， 53（9）：12-17.
3	LEE K， JING Yaxuan， WANG Yanqin， et al. A unified view on catalytic conversion of biomass and waste plastics［J］. Nature Reviews Chemistry， 2022， 6（9）：635-652. doi: 10.1038/s41570-022-00411-8
4	JASWAL A， SINGH P P， MONDAL T. Furfural：A versatile，biomass-derived platform chemical for the production of renewable chemicals［J］. Green Chemistry， 2022， 24（2）：510-551. doi: 10.1039/D1GC03278J
5	郑修新，蒋志魁，孙国方，等. 糠醇加氢制1，2-戊二醇催化剂的制备及性能研究［J］. 无机盐工业， 2020， 52（6）：96-100.
	ZHENG Xiuxin， JIANG Zhikui， SUN Guofang， et al. Study on preparation and properties of 1，2-pentanediol catalyst by hydrogenation of furfuryl alcohol［J］. Inorganic Chemicals Industry， 2020， 52（6）：96-100.
6	XIAO Tao， YAN Peijian， LI Kaijie， et al. Hollow mesoporous nanoreactors with encaged PtSn alloy nanoparticles for selective hydrogenation of furfural to furfuryl alcohol［J］. Industrial & Engineering Chemistry Research， 2021， 60（17）：6078-6088. doi: 10.1021/acs.iecr.1c00293
7	SITTHISA S， RESASCO D E. Hydrodeoxygenation of furfural over supported metal catalysts：A comparative study of Cu，Pd and Ni［J］. Catalysis Letters， 2011， 141（6）：784-791. doi: 10.1007/s10562-011-0581-7
8	GUERRERO-TORRES A， JIMÉNEZ-GÓMEZ C P， CECILIA J A， et al. Ni supported on sepiolite catalysts for the hydrogenation of furfural to value-added chemicals：Influence of the synthesis method on the catalytic performance［J］. Topics in Catalysis， 2019， 62（5）：535-550. doi: 10.1007/s11244-019-01168-z
9	SUNYOL C， ENGLISH OWEN R， GONZÁLEZ M D， et al. Catalytic hydrogenation of furfural to tetrahydrofurfuryl alcohol using competitive nickel catalysts supported on mesoporous clays［J］. Applied Catalysis A：General， 2021， 611：117903.
10	MENG Xiaoyu， YANG Yusen， CHEN Lifang， et al. A control over hydrogenation selectivity of furfural via tuning exposed facet of Ni catalysts［J］. ACS Catalysis， 2019， 9（5）：4226-4235. doi: 10.1021/acscatal.9b00238
11	LUO Lin， YUAN Fulong， ZAERA F， et al. Catalytic hydrogenation of furfural to furfuryl alcohol on hydrotalcite-derived Cu _x Ni_3- _x AlO _y mixed-metal oxides［J］. Journal of Catalysis， 2021， 404：420-429. doi: 10.1016/j.jcat.2021.10.009
12	JIMÉNEZ-GÓMEZ C P， CECILIA J A， DURÁN-MARTÍN D， et al. Gas-phase hydrogenation of furfural to furfuryl alcohol over Cu/ZnO catalysts［J］. Journal of Catalysis， 2016， 336：107-115. doi: 10.1016/j.jcat.2016.01.012
13	洪美花，郭子峰，刘冠锋，等. 碱处理方法合成多级孔分子筛的进展与挑战［J］. 无机盐工业， 2023， 55（6）：36-42.
	HONG Meihua， GUO Zifeng， LIU Guanfeng， et al. Progress and challenges of alkaline treatment for synthesis of hierarchical zeolites［J］. Inorganic Chemicals Industry， 2023， 55（6）：36-42.
14	YUAN Qiang， PANG Jifeng， YU Wenguang， et al. Vapor-phase furfural decarbonylation over a high-performance catalyst of 1%Pt/SBA-15［J］. Catalysts， 2020， 10（11）：1304. doi: 10.3390/catal10111304
15	YE Tiantian， LIU Hanfang， WANG Fupeng， et al. Pd@silicate-1 synthesized by steam-assisted-crystallization strategy for high-efficient catalytic hydrogenation of furfural［J］. Journal of Porous Materials， 2022， 29（5）：1479-1487. doi: 10.1007/s10934-022-01269-3

M	样品编号	原料物质的量配比	过渡金属（M）占 SiO₂的质量分数/%
M	样品编号	n（SiO₂）∶n（TPAOH）∶n（H₂O）∶n（MO _x ）∶n（柠檬酸）	过渡金属（M）占 SiO₂的质量分数/%
Ni	S-Ni1	1∶0.125∶30∶0.01∶0.01	1.0
	S-Ni2	1∶0.125∶30∶0.02∶0.02	2.0
	S-Ni3	1∶0.125∶30∶0.05∶0.05	4.9
	S-Ni4	1∶0.125∶30∶0.1∶0.1	9.8
Co	S-Co1	1∶0.125∶30∶0.01∶0.01	1.0
	S-Co2	1∶0.125∶30∶0.02∶0.02	2.0
	S-Co3	1∶0.125∶30∶0.05∶0.05	4.9
	S-Co4	1∶0.125∶30∶0.1∶0.1	9.8
Cu	S-Cu1	1∶0.125∶30∶0.01∶0.01	1.1
	S-Cu2	1∶0.125∶30∶0.02∶0.02	2.1
	S-Cu3	1∶0.125∶30∶0.05∶0.05	5.3
	S-Cu4	1∶0.125∶30∶0.09∶0.1	9.6
Fe	S-Fe1	1∶0.125∶30∶0.01∶0.01	0.9
	S-Fe2	1∶0.125∶30∶0.02∶0.02	1.9
	S-Fe3	1∶0.125∶30∶0.05∶0.05	4.7
	S-Fe4	1∶0.125∶30∶0.11∶0.11	10.3

样品	金属负载量^a/%	S_total^b/ （m²·g^-1）	S_micro^c/ （m²·g^-1）	S_ext^c/ （m²·g^-1）	V_micro^c/ （cm³·g^-1）
S-Ni1	1.0	389	367	22	0.173
S-Ni2	1.7	368	323	45	0.157
S-Co1	1.0	390	370	19	0.174
S-Co2	2.1	265	237	28	0.113
S-Fe1	1.1	409	383	27	0.166
S-Cu1	1.4	301	283	18	0.137

[1]	TANG Bei. Preparation of ZnO/g-C₃N₄ heterojunction photocatalytic material and its degradation of pyridine [J]. Inorganic Chemicals Industry, 2024, 56(4): 133-142.
[2]	ZHU Jinjian, YANG Xiaxia, MU Zhanpeng, SONG Guoliang, LI Zihan, LIU Wei, XU Yan, ZHANG Jingcheng. Effect of different additives on liquid phase selective hydrogenation performance of maleic anhydride over Ni/Al₂O₃ [J]. Inorganic Chemicals Industry, 2024, 56(4): 143-150.
[3]	HU Mingliang, ZHOU Wei, LI Bin, LAI Xiaoling. Research progress of synergistic effect catalytic reforming of methane and carbon dioxide [J]. Inorganic Chemicals Industry, 2024, 56(1): 23-32.
[4]	WU Luming, YU Haibin, WANG Yaquan. Research progress of porous carbon-based non noble metal electrocatalysts for oxygen reduction [J]. Inorganic Chemicals Industry, 2023, 55(10): 13-23.
[5]	WANG Peng, ZHAO Shanshan, LU Yanfei, LI Shisong, WANG Chunlei, SHU Chang, ZHANG Dongsheng. Study on preparation of copper-based materials and its catalytic performance for hydrogenation of dimethyl succinate [J]. Inorganic Chemicals Industry, 2023, 55(10): 145-152.
[6]	ZHAO Hongjuan, WANG Jiujiang, LIU Yuhang, LI Ning, CAO Gengzhen, LIU Honghai. Impact of heterogenous crystal seeds on synthesis of NaY zeolite [J]. Inorganic Chemicals Industry, 2023, 55(4): 120-124.
[7]	LI Liangrong, YANG Xiaozhe, CHEN Chuxin, LIU Yan, ZHANG Mengling, DING Yonghong. Research progress of photocatalytic water splitting of semiconductor core-shell materials for hydrogen production [J]. Inorganic Chemicals Industry, 2023, 55(3): 10-20.
[8]	WEN Yuan, ZHOU Chenliang, ZHANG Qiang, YU Linfei, HE Wenxiu, LIU Quansheng. Research progress of electronic and structure promoters of iron-based catalysts for FTO reaction [J]. Inorganic Chemicals Industry, 2023, 55(3): 36-46.
[9]	LI Xiangyang,LIU Ziwei,LI Keyan,GUO Xinwen. Study on preparation and performance of FeMn-MOF/CN heterojunction photo-Fenton catalyst [J]. Inorganic Chemicals Industry, 2022, 54(12): 126-132.
[10]	YU Wohui,ZHANG Pan,ZHAO Yiming,ZHA Zhongfa,WU Ruilong,QI Liqiang. Research progress on low-temperature denitration catalysts [J]. Inorganic Chemicals Industry, 2022, 54(10): 57-68.
[11]	CUI Jiaxin,WANG Lianyong,LI Yao,HE Yan,WANG Rui,HAN Jianli. Preparation and properties characterization of water quenching slag-fly ash based 4A zeolite [J]. Inorganic Chemicals Industry, 2022, 54(4): 135-140.
[12]	YANG Wenbo,WU Pan,HE Jian,LIU Changjun,JIANG Wei. Study on effect of heating rate on structure-activity of g-C₃N₄photocatalyst by pyrolysis of urea [J]. Inorganic Chemicals Industry, 2022, 54(4): 169-174.
[13]	JI Chang,WANG Guosheng. Degradation of berberine by visible light over Ag₃PO₄ /g-C₃N₄ heterojunction catalyst [J]. Inorganic Chemicals Industry, 2022, 54(4): 175-180.
[14]	ZHOU Wei,YU Haibin,MA Xinbin. Oxidative dehydrogenation of ethane with carbon dioxide to ethylene over Cr/SSZ-13 catalyst [J]. Inorganic Chemicals Industry, 2021, 53(12): 43-48.
[15]	Chang Ruopeng,Hu Xu,He Lei,Hao Guangping. Preparation of nickel-nitrogen co-doped carbon-based carbon dioxide electrocatalyst through complex-assisted method [J]. Inorganic Chemicals Industry, 2021, 53(9): 97-103.

National Inorganic Salts Information Center

Inorganic Acid-Base-Salt Committee of CIESC

Study on preparation of transition metal-supported Silicalite-1 zeolite catalyst and its catalytic performance for furfural hydrogenation

RichHTML

PDF (PC)

Knowledge

Abstract

Cite this article

share this article

Figures/Tables 10

References 15

Related Articles 15

Metrics

Comments

Recommended 0