双金属掺杂SBA-15催化合成双酚F及其同分异构体调控

doi:10.19964/j.issn.1006-4990.2023-0380

Abstract

Abstract:

Using metal salts of Al and Zr as precursors and ethyl orthosilicate as a silicon source，the catalyst M-SBA-15 doped with different n（Si）/n（M）（M=Al，Zr or Al-Zr） was prepared by direct hydrothermal method. The synthesized samples were characterized by X-ray diffraction，N₂ adsorption-desorption and pyridine infrared spectroscopy，and were used to catalyze the hydroxylalkylation reaction of phenol and formaldehyde to synthesize bisphenol F. The results showed that Al and Zr atoms were successfully doped into the skeleton of SBA-15，and there were both Brønsted and Lewis acid sites on M-SBA-15. When n（Si）/n（M） was 20，the catalytic effect was the best，and the yield of bisphenol F reached 82.4%. In addition，the content of 4，4′-，2，4′-，2，2′-bisphenol F could be adjusted by adjusting n（Al）/n（Zr） in raw materials. Finally，the possible reaction mechanism of M-SBA-15 catalytic synthesis of bisphenol F was proposed.

Key words: bimetal doped SBA-15, catalytic synthesis, bisphenol F, isomer regulation

CLC Number:

TAN Ying, LI Chongyi, YU Xiaoguang, LIAO Hongguang, YAN Xin. Bimetal doped SBA-15 catalytic synthesis of bisphenol F and its isomers regulation[J]. Inorganic Chemicals Industry, 2023, 55(11): 147-152.

Figures/Tables 11

Fig.1

Table 1

Fig.2

Fig.3

Table 2

Fig.4

Fig.5

Fig.6

Fig.7

Fig.8

Fig.9

References 15

1	ZHAO Yun， ZHANG Xinkai， CHEN Yanxia，et al.Application of in situ ATR-IR spectroscopy for the synthesis of bisphenol F：Optimization，mechanistic and kinetics studies［J］.Analytical Methods，2023，15（22）：2736-2744.
2	吴献章.两种介孔固体酸的制备及催化合成双酚F的性能研究［D］.长沙：湖南大学，2017：42-55.
	WU Xianzhang.The preparation of two kinds of mesoporous solid acid and their application in the hydroxyalkylation of phenol to bisphenol F［D］.Changsha：Hunan University，2017：42-55.
3	刘宁，周唤宇，夏志文，等.Bronsted酸性离子液体改性SBA-15分子筛催化合成双酚F［J］.能源化工，2020，41（5）：29-33.
	LIU Ning， ZHOU Huanyu， XIA Zhiwen，et al.Synthesis of bispheol F catalyzed by SBA-15 modified by Bronsted acid ionic liquids［J］.Energy Chemical Industry，2020，41（5）：29-33.
4	严家其，谈瑛，李勇飞，等.金属有机框架MIL-100（Cr）和MIL-101（Cr）负载磷钨酸催化合成双酚F［J］.化工学报，2015，66（2）：576-583.
	YAN Jiaqi， TAN Ying， LI Yongfei，et al.Synthesis of bisphenol F catalyzed by phosphotungstic acid encapsulated in metal-organic frameworks MIL-100（Cr） and MIL-101（Cr）［J］.CIESC Journal，2015，66（2）：576-583.
5	JANA S K， OKAMOTO T， KUGITA T，et al.Selective synthesis of bisphenol F catalyzed by microporous H-beta zeolite［J］.Applied Catalysis A：General，2005，288（1/2）：80-85.
6	谈瑛，廖红光，罗晴.Al-SBA-15催化合成双酚F的研究［J］.广东化工，2022，49（21）：7-10，37.
	TAN Ying， LIAO Hongguang， LUO Qing.Study on the catalytic synthesis of bisphenol F by Al-SBA-15［J］.Guangdong Chemical Industry，2022，49（21）：7-10，37.
7	杨晨，唐晓东，李晶晶，等.双酚A型环氧树脂合成技术进展［J］.中国塑料，2023，37（2）：106-112.
	YANG Chen， TANG Xiaodong， LI Jingjing，et al.Research progress in synthetic technology of bisphenol-A epoxy resin［J］.China Plastics，2023，37（2）：106-112.
8	朱金剑，张景成，南军，等.金属负载方式对Al-SBA-15/USY分子筛加氢裂化催化剂的影响［J］.无机盐工业，2019，51（6）：72-75.
	ZHU Jinjian， ZHANG Jingcheng， Jun NAN，et al.Effect of metal loading method on the Al-SBA-15/USY molecular sieve to hydrogen cracking catalyst［J］.Inorganic Chemicals Industry，2019，51（6）：72-75.
9	WEI Yuanfeng， LI Yongfei， TAN Ying，et al.A facile route for one-pot synthesis of short-channeled bimetallic Zr-Al-SBA-15［J］.Materials Letters，2015，141：145-148.
10	吴南，沈继军，周志彬.棒状SBA-15的制备与调控［J］.材料与冶金学报，2019，18（4）：293-299.
	WU Nan， SHEN Jijun， ZHOU Zhibin.Review on typical preparations of SBA-15 rods［J］.Journal of Materials and Metallurgy，2019，18（4）：293-299.
11	RESTREPO-GARCIA J R， GOMORA-HERRERA D，TORRES-MANCERA P，et al.Hydro-co-processing of a jatropha oil and gas oil blend with a sulfided Ni-W catalyst supported on mesostructured materials Al（x）-SBA-15 type for cleaner hybrid diesel production：Effect of the Al/Si molar ratio［J］.Fuel，2023，351：128890.
12	CAI Wenlan， NI Xiaoyan， MENG Fanyong，et al.From Al-SBA-15 to Ga-SBA-15：Morphology and acidity evolution in the acid-free synthesis［J］.Microporous and Mesoporous Materials，2022，335：111823.
13	YU Haibiao， JIA Xiu， WANG Peng，et al.High efficiency Al modified mesoporous SBA-15 catalyst for biomass-derived γ-val-erolactone decarboxylation to butene［J］.Microporous and Mesoporous Materials，2021，327：111432.
14	盖媛媛，李建法，孙瑞霞，等.Zr-SBA-15催化肉桂醛的MPV转移加氢性能［J］.精细化工，2019，36（5）：935-939，950.
	GE Yuanyuan， LI Jianfa， SUN Ruixia，et al.MPV transfer hydrogenation of cinnamaldehyde over Zr-SBA-15 catalyst［J］.Fine Chemicals，2019，36（5）：935-939，950.
15	LIU Xiumei， LIU Min， GUO Xinwen，et al. SO₃H-functionalized ionic liquids for selective alkylation of m-cresol with tert-butanol［J］. Catalysis Communications，2008，9（1）：1-7.

样品	比表面积/ （m²·g^-1）	孔径/ nm	孔容量/ （cm³·g^-1）
SBA-15	817	6.654	0.814
M-10	815	6.648	0.887
M-20	727	6.628	0.921
M-30	825	5.679	0.856
M-50	849	6.644	0.896

催化剂	反应4 h后双酚F收率/%	反应4 h后双酚F同分异构体分布/%
催化剂	反应4 h后双酚F收率/%	4，4′-双酚F	2，4′-双酚F	2，2′-双酚F
SBA-15	—	—	—	—
M-10	57.1	20.0	51.0	29.0
M-20	76.6	19.4	56.8	23.8
M-30	62.8	17.1	56.2	26.7
M-50	48.6	20.4	55.0	24.6

[1]	Cao Maoqi,Long Chengmei,Sun Sailan,Xu Ping,Wu Dawang. High efficiency electrocatalytic synthesis of ammonia by oxygen deficient WO₃ nanowire arrays [J]. Inorganic Chemicals Industry, 2021, 53(5): 100-104.
[2]	LONG Jin-Qiao, LUO Zhi-Rong. Catalytic synthesis of cyclohexanone glycol ketal with silicotungstic acid lanthanum prepared by solid-state interaction under microwave heating [J]. INORGANICCHEMICALSINDUSTRY, 2014, 46(12): 67-.
[3]	ZHANG Xia-Yan, LIU Ding-Hua, LIU Xiao-Qin- . Research progress in preparation and catalytic application of cuprous halide [J]. INORGANICCHEMICALSINDUSTRY, 2012, 44(7): 56-.
[4]	Shi Dejun;Hu Qingxun;Cui Yongli;Qiao Ke;Yan Zifeng. Progress in synthesis process of calcium carbide [J]. INORGANICCHEMICALSINDUSTRY, 2010, 0(5): 0-0.

National Inorganic Salts Information Center

Inorganic Acid-Base-Salt Committee of CIESC

Bimetal doped SBA-15 catalytic synthesis of bisphenol F and its isomers regulation

RichHTML

PDF (PC)

Knowledge

Abstract

Cite this article

share this article

Figures/Tables 11

References 15

Related Articles 4

Metrics

Comments

Recommended 0