NiWO4/g-C3N4的制备及其在离子液体中氧化脱硫性能的研究

李秀萍; 赵荣祥; 邢鹏飞

NiWO₄/g-C₃N₄的制备及其在离子液体中氧化脱硫性能的研究

1.
辽宁石油化工大学化学化工与环境学部化学与材料科学学院, 辽宁抚顺 113001
2.
辽宁石油化工大学化学化工与环境学部石油化工学院, 辽宁抚顺 113001

详细信息

中图分类号: TE624
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出版历程
- 收稿日期: 2017-04-12
- 修回日期: 2017-07-27
- 网络出版日期: 2021-01-23
- 刊出日期: 2017-11-10

Preparation of NiWO₄/g-C₃N₄ and its ultra-deep desulfurization properties in ionic liquid

1.
School of chemistry and Materials Science, College of Chemistry, Chemical Engineering and Environmental Engineering, Liaoning University of Petroleum & Chemical Technology, Fushun 113001, China
2.
School of Petrochemical Engineering, College of Chemistry, Chemical Engineering and Environmental Engineering, Liaoning University of Petroleum & Chemical Technology, Fushun 113001, China

More Information

Corresponding author: ZHAO Rong-xiang, Tel:024-56860937, E-mail:zylhzrx@126.com

摘要

摘要: 采用水热法合成了NiWO₄纳米粒子，然后通过混合煅烧法成功地制备了负载型催化剂NiWO₄/g-C₃N₄。采用XRD、FT-IR、EDS、SEM、BET和XPS表征了NiWO₄/g-C₃N₄的形貌和结构特征。以NiWO₄/g-C₃N₄为催化剂，过氧化氢为氧化剂，1-丁基-3-甲基咪唑四氟硼酸盐离子液体（[BMIM]BF₄）为萃取剂。考察了催化剂的负载量，过氧化氢、离子液体和催化剂使用量，反应温度，反应时间，不同种类的含硫化合物对脱硫效果的影响。结果表明，在5 mL模拟油，0.2 mL过氧化氢，1.0 mL的[BMIM]BF₄，0.03 g的NiWO₄/g-C₃N₄，反应温度为80 ℃，反应时间为140 min的最佳的反应条件下，脱硫率可以达到97.35%。实验表明，NiWO₄/g-C₃N₄具有很好的催化稳定性，催化剂重复使用五次后催化活性并没有明显地降低。
- NiWO₄/g-C₃N₄ /
- 氧化脱硫 /
- 二苯并噻吩 /
- 离子液体
Abstract: The NiWO₄ nanoparticles were synthesized by hydrothermal method. The supported catalysts NiWO₄/g-C₃N₄ were prepared by a simple mixing-calcination method. XRD, FT-IR, EDS, SEM, BET and XPS were used to characterize the morphology and structure of NiWO₄/g-C₃N₄. The prepared NiWO₄/g-C₃N₄ was used as catalyst, hydrogen peroxide as oxidant, 1-butyl-3-methylimidazolium tetrafluoroborate ionic liquid ([BMIM]BF₄) as extractant for oxidative desulfurization. The effects of catalyst loading, the amount of hydrogen peroxide, ionic liquid and catalyst, reaction temperature, reaction time, and different sulfur compounds on desulfurization efficiency were studied. The desulfurization rate can reach 97.35% at the optimum reaction conditions:5 mL of model oil, 0.2 mL of hydrogen peroxide, 1.0 mL of [BMIM] BF₄, 0.03 g of NiWO₄/g-C₃N₄, 80 ℃ of reaction temperature and 140 min of reaction time. The results showed that NiWO₄/g-C₃N₄ had good catalytic stability, and the catalytic activity was not significantly reduced after 5 repeated reactions.
- NiWO₄/g-C₃N₄ /
- oxidative desulfurization /
- dibenzothiophene /
- ionic liquid

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图 1 g-C₃N₄和NiWO₄/g-C₃N₄的XRD谱图

Figure 1 XRD patterns of g-C₃N₄ and NiWO₄/g-C₃N₄

a: g-C₃N₄; b: 5%-NiWO₄/g-C₃N₄; c: 10%-NiWO₄/g-C₃N₄; d: 15%-NiWO₄/g-C₃N₄; e: 20%-NiWO₄/g-C₃N₄

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图 2 NiWO₄/g-C₃N₄的红外光谱谱图

Figure 2 FT-IR spectra of NiWO₄/g-C₃N₄

a: g-C₃N₄; b: 5%-NiWO₄/g-C₃N₄; c: 10%-NiWO₄/g-C₃N₄; d: 15%-NiWO₄/g-C₃N₄; e: 20%-NiWO₄/g-C₃N₄

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图 3 20%-NiWO₄/g-C₃N₄的EDS能谱谱图

Figure 3 EDS spectrum of 20%-NiWO₄/g-C₃N₄

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图 4 g-C₃N₄ NiWO₄和20%-NiWO₄/g-C₃N₄的SEM照片

Figure 4 SEM images of (a) g-C₃N₄, (b) NiWO₄ and (c) 20%-NiWO₄/g-C₃N₄

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图 5 20%-NiWO₄/g-C₃N₄的XPS谱图

Figure 5 XPS spectra of 20%-NiWO₄/g-C₃N₄

(a): the survey spectrum；(b): W 4f；(c): C 1s；(d): N 1s；(e): O 1s；(f): Ni 2p

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图 6 NiWO₄负载量对脱硫率的影响

Figure 6 Effect of catalyst loading amount on the desulfurization rate

V(DBT, oil)=5 mL; V([BMIM]BF₄)=1.0 mL; m(NiWO₄/g-C₃N₄)=0.02 g; V(H₂O₂)=0.2 mL; t=80 ℃; t=180 min

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图 7 H₂O₂加入量对脱硫率的影响

Figure 7 Effect of amount of H₂O₂ on the desulfurization rate

V(DBT, oil)=5 mL; V([BMIM]BF₄)=1.0 mL; m(20%-NiWO₄/g-C₃N₄)=0.02 g; t=80 ℃; t=180 min

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图 8 离子液体使用量对脱硫率的影响

Figure 8 Effect of the amount of IL on the desulfurization rate

V(DBT, oil)=5 mL; m(20%-NiWO₄/g-C₃N₄)=0.02 g; V(H₂O₂)=0.2 mL; t=80℃; t=180 min

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图 9 催化剂使用量对脱硫率的影响

Figure 9 Effect of the amount of catalyst on the desulfurization rate

V(DBT, oil)=5 mL; V([BMIM]BF₄)=1.0 mL; V(H₂O₂)=0.2 mL; t=80 ℃; t=180 min

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图 10 反应温度对脱硫率的影响

Figure 10 Effect of the reaction temperature on the desulfurization rate

V(DBT, oil)=5 mL; V([BMIM]BF₄)=1.0 mL; V(H₂O₂)=0.2 mL; m(20%-NiWO₄/g-C₃N₄)=0.03 g; t=180 min

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图 11 不同含硫化合物对脱硫率的影响

Figure 11 Effect of different sulfur compounds on the desulfurization rate

V(oil)=5 mL; V([BMIM]BF₄)=1.0 mL; V(H₂O₂)=0.2 mL; m(20%-NiWO₄/g-C₃N₄)=0.03 g; t=80 ℃; t=140 min

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图 12 NiWO₄/g-C₃N₄催化氧化脱硫机理示意图

Figure 12 Mechanism of oxidative desulfurization catalyzed by NiWO₄/g-C₃N₄

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表 1 不同负载量的NiWO₄/g-C₃N₄催化剂的比表面积

Table 1 Specific surface area of g-C₃N₄, NiWO₄ and NiWO₄/g-C₃N₄ with different loading amount

Catalyst	Specific surface area A/(m²·g^-1)
g-C₃N₄	18.15
NiWO₄	112.60
5%-NiWO₄/g-C₃N₄	40.12
10%-NiWO₄/g-C₃N₄	43.60
15%-NiWO₄/g-C₃N₄	46.76
20%-NiWO₄/g-C₃N₄	48.58

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表 2 20%-NiWO₄/g-C₃N₄循环次数使用对脱硫效果的影响

Table 2 Influence of the recycle times of 20%-NiWO₄/g-C₃N₄ on the desulfurization rate

Number of recycle	1	2	3	4	5
Desulfurization rate η /%	97.35	96.33	96.18	95.87	95.47

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