亲水性FePt纳米颗粒协同催化有机污染物的降解

doi:10.7503/cjcu20190661

摘要/Abstract

摘要：

以半胱氨酸为配体, 采用一锅法简便合成了亲水性的FePt纳米颗粒(NPs). 超小的FePt NPs对水中常见有机污染物表现出良好的催化降解性能, 以NaBH₄为还原剂时可实现对染料罗丹明B(RhB)和有害物质4-硝基苯酚(4-NP)的有效还原; 以H₂O₂为氧化剂时可实现亚甲基蓝(MB)的高效降解. 实验结果表明, FePt NPs对3种有机污染物的降解率均高于90%. 对FePt原子对之间的协同催化机理进行了探讨, 揭示了不同反应体系中微观反应历程和催化机理的区别. 磁性测试结果表明, FePt催化剂可以通过外加磁场进行收集并重复利用, 解决了催化剂二次污染问题. 该研究为设计合成绿色环保催化剂提供了思路.

关键词: 亲水性FePt NPs, 协同催化, 有机污染物, 降解, 可回收

Abstract:

Hydrophilic ultra-small FePt nanoparticles(NPs) stabilized with cysteine were facile synthesized in water phase by one pot method. As-prepared FePt NPs showed good catalytic degradation activity of common organic pollutants in water. NaBH₄ and H₂O₂ were chose as the co-reactant to degrade rhodamine B(RhB), 4-nitrophenol(4-NP) and methylene blue(MB), respectively. The results showed that the degradation rates were more than 90% for three organic pollutants by FePt NPs. At the same time, we focus on the discussion of the collaborative catalytic mechanism between FePt atom pairs, and reveal the difference between the microscopic reaction process and catalytic mechanism in different reaction systems. Moreover, magnetic test results show that FePt catalyst can be collected and reused by external magnetic field, which solves the problem of secondary pollution of the catalyst. This study provides an idea for the design of green catalyst.

Key words: Hydrophilic FePt NPs, Collaborative catalysis, Degradation, Organic pollutant, Recyclable

中图分类号:

O614.8

TrendMD:

刘丛远, 刘佳, 杜佩瑶, 张振, 卢小泉. 亲水性FePt纳米颗粒协同催化有机污染物的降解. 高等学校化学学报, 2020, 41(4): 697.

LIU Congyuan, LIU Jia, DU Peiyao, ZHANG Zhen, LU Xiaoquan. Preparation of Hydrophilic FePt Nanoparticles and co-Catalyze Degrade Organic Pollutants ^†. Chem. J. Chinese Universities, 2020, 41(4): 697.

图/表 13

Scheme 1 Schematic illustration of the preparation of FePt NPs and their application for degradation of organic pollutants

Fig.1 TEM images(A—C) and size distribution(D) of FePt NPs

Fig.2 XRD patterns(A) and EDS profile(B) of FePt NPs

Fig.3 XPS survey scan Fe2p(A), Pt4f (B), C1s(C) and N1s(D) of FePt NPs

Fig.4 FTIR spectra of FePt NPs(a) and L-Cys(b)(A) and UV-Vis spectrum of FePt NPs(B) Inset of (B) is the photograph of FePt NPs solution.

Fig.5 Degradation of RhB with(A) and without(B) FePt catalyst(A) a. RhB; b.—h. RhB+FePt+NaBH4. Reaction time/min, b.—h.: 0, 1, 3, 5, 10, 15, 20. (B) a. RhB; b.—i. RhB+NaBH4. Reaction time/min, b.—i.: 0, 1, 3, 5, 10, 15, 20, 25, 30. Inset of (A) show the color change of RhB solution before and after degradation.

Scheme 2 Catalytic mechanism of FePt for the degradation of RhB with NaBH4 as reducing agent

Scheme 3 Reduction process of RhB by FePt NPs under the help of NaBH4

Fig.6 Degradation of 4-NP with(A) and without(B) PePt catalyst(A) a. 4-NP; b. 4-NP+NaBH4; c.—e. 4-NP+NaBH4+FePt. Reaction time/min, c.—e.: 1, 3, 5.^ (B) 4-NP+NaBH4. Reaction time/min, a.—e.: 0, 1, 3, 5, 7.

Fig.90 Scheme 4 Reduction process of 4-NP catalyzed by ePt NPs under the help of NaBH4

Fig.7 Degradation of MB P with(A) and without(B) PePt catalyst(A) a. MB; b. MB+FePt; c.—f. MB+FePt+H2O2. Reaction time/min, c.—f.: 1, 3, 8, 15. (B) a. MB; b. MB+H2O2, 20 min.

Fig.91 Scheme 5 Mechanism of degradation of MB by FePt NPs with the participation of H2O2

Fig.8 Magnetization hysteresis curves of FePt NPs at 300 K

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