BiPO4@Ag3PO4核/壳异质结的制备及光催化性能

doi:10.7503/cjcu20140266

摘要/Abstract

摘要：

采用简单的水热法结合离子交换法制备了BiPO₄@Ag₃PO₄核/壳异质结光催化剂, 采用场发射扫描电子显微镜(FE-SEM)、透射电子显微镜(TEM)、紫外-可见漫反射光谱仪(DRS)和X射线光电子能谱仪(XPS)等对催化剂的形貌、组成、晶型和光物理性质等进行了研究, 用罗丹明B(RhB)为模拟水体中有机污染物分别在可见光和模拟太阳光照条件下对催化剂的催化活性进行了测试. 结果表明, 负载Ag₃PO₄的BiPO₄微米棒具有较高的可见光响应, 其核/壳异质结结构有利于光生电子-空穴对的有效分离和提高对RhB的光催化降解效率, 在可见光和模拟太阳光照射条件下分别在60和40 min可使RhB完全脱色降解. 活性物种检测实验结果证明, 该催化剂在污染物降解过程中主要的机理是光生空穴的直接氧化.

关键词: BiPO4@Ag3PO4, 核/壳结构, 异质结, 空穴氧化

Abstract:

BiPO₄@Ag₃PO₄ core/shell heterojuction photocatalyst was synthesized through a facile hydrothermal process followed by the ion-exchange method. The morphology, crystallinity, composition, and photophy-sical properties of the catalyst were systematically investigated by scanning electron microscope(SEM), X-ray diffraction(XRD), energy dispersive X-ray analysis, UV-Vis diffuse reflectance spectrophotometer(DRS) and X-ray photoelectron spectroscopy(XPS). Meanwhile, Rhodamine B(RhB) was chosen as the target pollutant to evaluate the photocatalytic activity of BiPO₄@Ag₃PO₄ photocatalyst under the visible light and simulated sunlight irradiation, respectively. The results show that RhB was almost totally degraded in 60 min under visible-light irradiation and in 40 min under sunlight irradiation, respectively. The BiPO₄@Ag₃PO₄ core/shell heterojunction photocatalyst displayed enhanced photocatalytic activity against RhB, which is attributed to the effective charge separation by the core/shell heterojuction between the Ag₃PO₄ and BiPO₄. Active species detection experiments proved that during the process of degradation of pollutants over the core/shell microrods, the main mechanism was the direct oxidation process by the photo-induced holes. Ag₃PO₄ shell can improve the absorption of the visible light effectively and also enhance the stability, dispersibility and photocatalytic activity of the photocatalyst. The BiPO₄@AgPO₄ photocatalysts show attractive potential applications in pollution control, water splitting and solar cell.

Key words: BiPO4@Ag3PO4, Core/shell structure, Heterojunction, Holeoxidation

中图分类号:

O644
O613.62

TrendMD:

任延琳, 李新勇, 肇启东. BiPO₄@Ag₃PO₄核/壳异质结的制备及光催化性能. 高等学校化学学报, 2014, 35(11): 2435.

REN Yanlin, LI Xinyong, ZHAO Qidong. Fabrication and Photocatalytic Activity of BiPO₄@Ag₃PO₄ Core/Shell Heterojunction^†. Chem. J. Chinese Universities, 2014, 35(11): 2435.

图/表 9

Fig.1 SEM images of BiPO4@Ag3PO4 core-shell heterostructure photocatalyst(A,B) and BiPO4 microrods(C,D) with different magnifications

Fig.2 TEM images of BiPO4microrods(A) and BiPO4@Ag3PO4 core-shell heterostructure photocatalyst with different magnifications(B, C) and HRTEM image of BiPO4@Ag3PO4(D) Inset of (B) is the magnified view of local TEM image.

Fig.3 XRD patterns of BiPO4(a) and BiPO4@Ag3PO4(b)

Fig.4 Overall XPS spectrum(A) and Ag3d(B), Bi4f(C), P2p XPS spectra(D) for BiPO4@Ag3PO4

Fig.5 DRS spectra of the as-prepared Ag3PO4(a), BiPO4(b) and BiPO4@Ag3PO4(c)

Fig.6 Photocatalytic degradation efficiencies of RhB over BiPO4@Ag3PO4(a), BiPO4 mixed with Ag3PO4(b), BiPO4(c) and photolysis without catalyst(d) under visible light(A) and simulant solar light(B) irradiation

Table 1 Reaction kinetic constants under different conditions*

Sample	k₁/min^-1	$R 12$	k₂/min^-1	$R 22$
BiPO₄@Ag₃PO₄	1.42×10^-2	0.8810	1.79×10^-2	0.9735
BiPO₄ mixed with Ag₃PO₄	1.16×10^-3	0.9781	3.62×10^-3	0.9818
BiPO₄	3.26×10^-5	0.9560	8.95×10^-4	0.9883
Photolysis	2.84×10^-6	0.9414	1.48×10^-5	0.9516

Table 1 Reaction kinetic constants under different conditions*

Sample	k₁/min^-1	$R 12$	k₂/min^-1	$R 22$
BiPO₄@Ag₃PO₄	1.42×10^-2	0.8810	1.79×10^-2	0.9735
BiPO₄ mixed with Ag₃PO₄	1.16×10^-3	0.9781	3.62×10^-3	0.9818
BiPO₄	3.26×10^-5	0.9560	8.95×10^-4	0.9883
Photolysis	2.84×10^-6	0.9414	1.48×10^-5	0.9516

Fig.7 Plots of photogenerated carriers trapping in different systems of photodegradation of RhB on BiPO4@Ag3PO4 a. BiPO4@Ag3PO4; b. purging N2; c. 1 mmol/L t-BuOH; d. 1 mmol/L EDTA.

Fig.8 Proposed photodegradation mechanism of RhB on the surface of BiPO4@Ag3PO4 core/shell heterojunction photocatalyst The potential values of CB and VB edges are cited vs. NHE.

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BiPO₄@Ag₃PO₄核/壳异质结的制备及光催化性能

Fabrication and Photocatalytic Activity of BiPO₄@Ag₃PO₄ Core/Shell Heterojunction^†

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