One-pot synthesis of ternary Ag2CO3/Ag/AgCl photocatalyst in natural geothermal water with enhanced photocatalytic activity under visible light irradiation

doi:10.1016/j.jhazmat.2014.07.079

Journal of Hazardous Materials

Volume 280, 15 September 2014, Pages 260-268

https://doi.org/10.1016/j.jhazmat.2014.07.079 Get rights and content

Highlights

•
Ag₂CO₃/Ag/AgCl composite was synthesized in geothermal water by a one-pot method.
•
Geothermal water served as the source of chlorine and carbonate.
•
Ag₂CO₃/Ag/AgCl exhibited the enhanced photocatalytic activity and stability.
•
The efficient charge carrier separation is attributed to the Z-scheme construction.

Abstract

Geothermal water is a clean, cheap and renewable resource and it is widely distributed all over the world. In this work, ternary Ag₂CO₃/Ag/AgCl photocatalyst has been successfully synthesized via a one-pot precipitation method in natural geothermal water at room temperature, wherein the geothermal water serves as the source of chlorine and carbonate. The results suggest that the Ag/AgCl nanoparticles are anchored on the surface of Ag₂CO₃ and Ag₂CO₃/Ag/AgCl composite shows strong absorption ability in the visible light region. The evaluation of the photocatalytic activity indicates that the as-synthesized Ag₂CO₃/Ag/AgCl photocatalyst exhibits higher photocatalytic performance for the degradation of methylene blue (MB) aqueous solution under visible light irradiation than one-component (Ag₂CO₃), two-component (Ag/AgCl, Ag₂CO₃/AgCl) and the mechanical mixture of Ag₂CO₃ and Ag/AgCl. The trapping experiments confirmed that holes (h⁺) and ^•O₂⁻ were the two main active species in the photocatalytic process. Finally, a possible Z-scheme photocatalytic mechanism of the charge transfer was proposed for the enhanced photocatalytic performance. This work may open up new insights into the application of cheap geothermal water resources in the word and provide new opportunities for facile fabrication of Ag/AgCl-based photocatalysts.

Graphical abstract

Introduction

Semiconductor photocatalysis has attracted considerable attention since Fujishima and Honda reported the photoelectrochemcial evolution of H₂ on the TiO₂ electrode in 1972 [1]. Many researches focused on the photocatalytic degradation of organic pollutants [2], [3], [4], [5] and the photocatalytic H₂-generation from water splitting [6], [7], [8], [9]. TiO₂, as a typical semiconductor, has been widely used for the application in photocatalysis due to its high chemical stability and prefect photocatalytic activity [10], [11], [12]. Unfortunately, TiO₂ can only be activated by UV light which accounts for ca. 5% of the solar energy because of its large band gap (3.2 eV for anatase TiO₂), resulting in the low quantum efficiency. Many efforts have been devoted to finding and designing visible-light-responsive photocatalysts according to the band gap and energy levels of the valence band and conduction band. It is worth noting that the coupling of various semiconductors with different band gap levels has been widely investigated to enhance the visible-light absorption capability. Compared with the single-component photocatalysts, semiconductor-semiconductor composites, mainly including sensitization, p–n heterojunction and Z-scheme, usually show excellent photocatalytic activity [13], [14], [15], [16], [17]. In the case of a Z-scheme system, photoexcited electrons transferred from the valence band to conduction band in both semiconductors. The photoexcited electrons of the semiconductor with a higher conduction band acted as the reduction sites and the holes of the semiconductor with a lower valence band are used for the oxidation. Meanwhile, the photoinduced electrons of the semiconductor with a lower conduction band recombined with the photogenerated holes of the semiconductor with a higher valance band. As a result, the Z-scheme photocatalysts have stronger reduction and oxidation potential than the individual photocatalyst [16], [18]. Recently, Ag-based nanomaterials have been considered as promising photocatalysts for the degradation of organic pollutants under visible light irradiation, such as Ag/AgCl [19], [20], [21], Ag₃PO₄ [22], Ag₂O [23], [24], Ag₂CO₃ [25], [26]. Among them, Ag/AgX (X = Cl or Br) plasmonic photocatalysts stand out owing to the high efficiency and excellent stability under visible light irradiation [3], [21], [27], [28]. The absorption ability in visible light region results from the strong localized surface plasmon resonance (LSPR) of photoexcited Ag nanoparticles. In order to further improve their photocatalytic performance, many hierarchical nanostructures have been reported, including Ag/AgCl/WO₃ [29], Ag/AgBr/Bi₂MoO₆ [30], Ag₃VO₄/AgBr/Ag [31], AgCl/Ag/γ-TaON [32], and Ag/AgCl/Bi₂₀TiO₃₂ [33]. Compared with the one-component or two-component products, these hierarchical composites indeed enhanced the photocatalytic activity. Therefore, it is critically important to design novel visible-light-driven photocatalysts for the efficient degradation of toxic organic compounds and high energy conversion of solar energy to chemical energy.

Natural geothermal water is a clean, renewable and cheap resource, which is widely distributed and has been used in many fields of industry and life in the world, such as the generation of electric power and physical therapy [34], [35], [36]. Geothermal energy is the natural heat energy contained in the depth of the earth, primarily attributed to the magma and the decay of the radioactive isotopes [37]. Geothermal resource is a kind of renewable energy, which can provide clean and green energy. The development and utilization of renewable energies have been considered as important measures to solve resource shortage and relieve environment pollution pressure. The formation of geothermal water originates from the ground water heated by geothermal energy and hot magma. Then the heated water gushes out of the surface cracks owing to the existence of hydrostatic pressure gradient. It is general that geothermal water contains Cl⁻, HCO₃⁻, SO₄²⁻, Na⁺, Mg²⁺ and so on. To the best of our knowledge, there has been no report about the synthesis of visible-light-driven photocatalysts using geothermal water as raw material. In this work, we firstly report a one-pot precipitation method for the direct synthesis of Ag₂CO₃/Ag/AgCl composite photocatalyst by dropwise addition of silver nitrate (AgNO₃) aqueous solution into natural geothermal water which served as chlorine and carbonate sources. Herein, the representative geothermal water was chose from Changbai Mountain, Jilin Province, China. The physical-chemical properties of the as-obtained products were characterized by powder X-ray diffraction (XRD), scanning electron microscopy (SEM), transmission electron microscopy (TEM), ultraviolet-visible diffuse reflectance spectroscopy (DRS) and X-ray photoelectron spectra (XPS). The Ag₂CO₃/Ag/AgCl photocatalyst exhibited excellent photocatalytic performance and stability for the visible-light-driven photocatalytic degradation of methylene blue (MB) dye due to the efficient charge carrier separation through a Z-scheme system. This new work might extend the potential application of cheap geothermal water in environment purification.

Section snippets

Synthesis of Ag₂CO₃/Ag/AgCl composite

All the chemicals were of analytical grade and used as purchased without any further treatment. The geothermal water in this work was taken from Changbai Mountain, Jilin Province, China. The ternary Ag₂CO₃/Ag/AgCl composite was synthesized by a one-pot precipitation method under ambient conditions. In a typical process, 20 mL of AgNO₃ aqueous solution (0.01 M) was dropwise added into 20 mL of natural geothermal water at room temperature with strongly magnetic stirring under sunlight. Then, the

Results and discussion

The Ag₂CO₃/Ag/AgCl composite was successfully synthesized via a one-pot precipitation method by simply adding an aqueous solution of AgNO₃ into natural geothermal water. A white suspension could be observed immediately while AgNO₃ solution was dropped into the geothermal water and the color of the product gradually changed to dark gray after being stirred for 0.5 h. The phase structure of the as-synthesized products was investigated by XRD and the typical XRD patterns of Ag₂CO₃, Ag/AgCl, and Ag₂

Conclusion

In this work, a plasmonic Z-scheme photocatalyst of ternary Ag₂CO₃/Ag/AgCl has been successfully synthesized by a one-pot green method in geothermal water at room temperature, wherein silver nitrate serves as silver source and geothermal water serves as the source of chlorine and carbonate. The as-prepared Ag₂CO₃/Ag/AgCl shows a higher photocatalytic performance than Ag₂CO₃, Ag/AgCl, Ag₂CO₃/AgCl and the mechanical mixture of Ag₂CO₃ and Ag/AgCl for the degradation of methyl blue (MB) aqueous

Acknowledgements

This project is supported financially by the National Natural Science Foundation of China (No. 51272107), the Natural Science Foundation of Jiangsu Province, China (No. BK2011024), the Specialized Research Fund for the Doctoral Program of Higher Education, China (20133219110015), and A Project Funded by the Priority Academic Program Development (PAPD) of Jiangsu Higher Education Institutions.

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One-pot synthesis of ternary Ag2CO3/Ag/AgCl photocatalyst in natural geothermal water with enhanced photocatalytic activity under visible light irradiation

Highlights

Abstract

Graphical abstract

Introduction

Section snippets

Synthesis of Ag2CO3/Ag/AgCl composite

Results and discussion

Conclusion

Acknowledgements

Appl. Surf. Sci.

Appl. Catal. A

Appl. Catal. B

Geothermics

J. Alloys Compd.

J. Hazard. Mater.

Micropor. Mesopor. Mater.

Appl. Catal. B

Chem. Eng. J.

Desalination

J. Colloid Interface Sci.

J. Electron. Spectrosc. Relat. Phenom.

J. Mol. Catal. A

J. Hazard. Mater.

Mater. Chem. Phys.

Appl. Catal. B

Electrochemical photolysis of water at a semiconductor electrode

Nature

Direct synthesis of anatase TiO2 nanowires with enhanced photocatalytic activity

Adv. Mater.

Ag@AgCl: a highly efficient and stable photocatalyst active under visible light

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Synthesis of few-layer MoS2 nanosheet-coated TiO2 nanobelt heterostructures for enhanced photocatalytic activities

Small

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Formation of 1D hierarchical structures composed of Ni3S2 nanosheets on CNTs backbone for supercapacitors and photocatalytic H2 production

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Enhanced photocatalytic activity and electron transfer mechanisms of graphene/TiO2 with exposed {001} facets

J. Phys. Chem. C

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High-efficiency visible-light-driven Ag3PO4/AgI photocatalysts: Z-scheme photocatalytic mechanism for their enhanced photocatalytic activity

J. Phys. Chem. C

One-pot synthesis of ternary Ag₂CO₃/Ag/AgCl photocatalyst in natural geothermal water with enhanced photocatalytic activity under visible light irradiation

Synthesis of Ag₂CO₃/Ag/AgCl composite

Direct synthesis of anatase TiO₂ nanowires with enhanced photocatalytic activity

Synthesis of few-layer MoS₂ nanosheet-coated TiO₂ nanobelt heterostructures for enhanced photocatalytic activities

Selective growth of Ag₃PO₄ submicro-cubes on Ag nanowires to fabricate necklace-like heterostructures for photocatalytic applications

Nanostructured Cu/TiO₂ photocatalysts for H₂ production from ethanol and glycerol aqueous solutions

The potential of supported Cu₂O and CuO nanosystems in photocatalytic H₂ production

Formation of 1D hierarchical structures composed of Ni₃S₂ nanosheets on CNTs backbone for supercapacitors and photocatalytic H₂ production

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Tunable photocatalytic selectivity of hollow TiO₂ microspheres composed of anatase polyhedra with exposed {001} facets

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Photocatalytic overall water splitting promoted by an α-β phase junctionon Ga₂O₃

High-efficiency visible-light-driven Ag₃PO₄/AgI photocatalysts: Z-scheme photocatalytic mechanism for their enhanced photocatalytic activity