0D/2D Z-Scheme Heterojunctions of Bismuth Tantalate Quantum Dots/Ultrathin g-C3N4 Nanosheets for Highly Efficient Visible Light Photocatalytic Degradation of Antibiotics.

Constructing 0D/2D Z-scheme photocatalysts is a great promising path to improve photocatalytic activity by  efficiently enhancing charge separation. Herein, we fabricated a visible-light-responsive Bi3TaO7 quantum dots (QDs)/g-C3N4 nanosheets (NSs) 0D/2D Z-scheme composite via a facile ultrasound method, and Bi3TaO7 QDs could be interspersed on the surface of g-C3N4 NSs uniformly. Furthermore, the strong interaction between Bi3TaO7 QDs and g-C3N4 NSs disturbed the CN heterocycles by forming C═O bonds between C atoms of the N-(C)3 group and O atoms of the Ta-O bond. The optimum composite with 20 wt % g-C3N4 NSs showed the superior photocatalytic activity for degradation of ciprofloxacin (CIP) over the composites prepared by mechanical mixing and solid-state methods, the photocatalytic efficiency of which were 4 and 12.2 times higher than those of bare Bi3TaO7 and g-C3N4. Photoluminescence (PL), time-resolved transient PL decay spectra, and photocurrent together verify that the photogenerated hole-electron pairs in this 0D/2D Z-scheme composite have been effectively separated. The enhanced photocatalytic activity of as-synthesized photocatalysts could be attributed to the synergistic effect of efficient Z-scheme charge separation, highly dispersed 0D Bi3TaO7 nanocrystals, coordinating sites of 2D g-C3N4 NSs and the strong coupling between them. This study might pave the way toward designing novel visible-light-induced 0D/2D photocatalyst systems for highly efficient degradation of antibiotics.

[1]  Juncheng Hu,et al.  In-situ topotactic synthesis and photocatalytic activity of plate-like BiOCl/2D networks Bi2S3 heterostructures , 2018 .

[2]  Xiaoyong Wu,et al.  Vacancy-Rich Monolayer BiO2-x as a Highly Efficient UV, Visible, and Near-Infrared Responsive Photocatalyst. , 2018, Angewandte Chemie.

[3]  W. Shi,et al.  Characterization and photocatalytic activity of Bi 3 TaO 7 prepared by hydrothermal method , 2017 .

[4]  Changling Yu,et al.  Novel fluorinated Bi2MoO6 nanocrystals for efficient photocatalytic removal of water organic pollutants under different light source illumination , 2017 .

[5]  M. Jaroniec,et al.  All‐Solid‐State Z‐Scheme Photocatalytic Systems , 2014, Advanced materials.

[6]  Ying-hua Liang,et al.  A stable Ag3PO4@g-C3N4 hybrid core@shell composite with enhanced visible light photocatalytic degradation , 2016 .

[7]  Zhanghua Wu,et al.  An interesting Eu,F-codoped BiVO4 microsphere with enhanced photocatalytic performance , 2017 .

[8]  S. Yin,et al.  Facile preparation of BiOX (X = Cl, Br, I) nanoparticles and up-conversion phosphors/BiOBr composites for efficient degradation of NO gas: Oxygen vacancy effect and near infrared light responsive mechanism , 2017 .

[9]  P. Feng,et al.  Enhanced photocatalytic activity and photostability for novel g-C3N4 decorated Bi2O4 microrod composites , 2017 .

[10]  Jiang Tang,et al.  Synergistic Effect of Hybrid PbS Quantum Dots/2D‐WSe2 Toward High Performance and Broadband Phototransistors , 2017 .

[11]  Wei Chen,et al.  In situ fabrication of novel Z-scheme Bi2WO6 quantum dots/g-C3N4 ultrathin nanosheets heterostructures with improved photocatalytic activity , 2015 .

[12]  A. Krasheninnikov,et al.  Effects of confinement and environment on the electronic structure and exciton binding energy of MoS2 from first principles , 2012 .

[13]  Jianpeng Shi,et al.  Highly Efficient Photocatalyst Based on a CdS Quantum Dots/ZnO Nanosheets 0D/2D Heterojunction for Hydrogen Evolution from Water Splitting. , 2017, ACS applied materials & interfaces.

[14]  Yongyou Hu,et al.  CdS nanoparticles immobilized on porous carbon polyhedrons derived from a metal-organic framework with enhanced visible light photocatalytic activity for antibiotic degradation , 2017 .

[15]  M. Gao,et al.  Fabrication of Z-scheme g-C3N4/RGO/Bi2WO6 photocatalyst with enhanced visible-light photocatalytic activity , 2016 .

[16]  Jiancheng Zhou,et al.  Enhancement of SrTiO3/BiPO4 heterostructure for simulated organic wastewater degradation under UV light irradiation , 2017, Research on Chemical Intermediates.

[17]  C. Niu,et al.  Enhanced Photocatalytic Degradation of Tetracycline by AgI/BiVO4 Heterojunction under Visible-Light Irradiation: Mineralization Efficiency and Mechanism. , 2016, ACS applied materials & interfaces.

[18]  K. Suslick,et al.  Applications of Ultrasound to the Synthesis of Nanostructured Materials , 2010, Advanced materials.

[19]  Alireza Nezamzadeh-Ejhieh,et al.  Enhanced activity of clinoptilolite-supported hybridized PbS–CdS semiconductors for the photocatalytic degradation of a mixture of tetracycline and cephalexin aqueous solution , 2015 .

[20]  Jiaguo Yu,et al.  Synthesis of nanometer-size Bi3TaO7 and its visible-light photocatalytic activity for the degradation of a 4BS dye. , 2010, Journal of colloid and interface science.

[21]  J. Shang,et al.  Efficient Visible Light Nitrogen Fixation with BiOBr Nanosheets of Oxygen Vacancies on the Exposed {001} Facets. , 2015, Journal of the American Chemical Society.

[22]  R. Jin,et al.  Phase Transformation Synthesis of Novel Ag2O/Ag2CO3 Heterostructures with High Visible Light Efficiency in Photocatalytic Degradation of Pollutants , 2014, Advanced materials.

[23]  Fangfang Zhu,et al.  Fabrication of nitrogen doped graphene quantum dots-BiOI/MnNb2O6 p-n junction photocatalysts with enhanced visible light efficiency in photocatalytic degradation of antibiotics , 2017 .

[24]  Yanjun Xin,et al.  Synthesis of Au–CuS–TiO2 nanobelts photocatalyst for efficient photocatalytic degradation of antibiotic oxytetracycline , 2016 .

[25]  Weidong Shi,et al.  Fabrication of a Ag/Bi3TaO7 Plasmonic Photocatalyst with Enhanced Photocatalytic Activity for Degradation of Tetracycline. , 2015, ACS applied materials & interfaces.

[26]  Tian-Yi Ma,et al.  0D/2D Heterojunctions of Vanadate Quantum Dots/Graphitic Carbon Nitride Nanosheets for Enhanced Visible-Light-Driven Photocatalysis. , 2017, Angewandte Chemie.

[27]  Hua Tang,et al.  In situ hydrothermal synthesis of g-C3N4/TiO2 heterojunction photocatalysts with high specific surface area for Rhodamine B degradation , 2017 .

[28]  Yihe Zhang,et al.  Anionic Group Self-Doping as a Promising Strategy: Band-Gap Engineering and Multi-Functional Applications of High-Performance CO32–-Doped Bi2O2CO3 , 2015 .

[29]  Zhenyi Zhang,et al.  Ultrathin hexagonal SnS2 nanosheets coupled with g-C3N4 nanosheets as 2D/2D heterojunction photocatalysts toward high photocatalytic activity , 2015 .

[30]  Yongfa Zhu,et al.  Preparation of visible light-driven g-C₃N₄@ZnO hybrid photocatalyst via mechanochemistry. , 2014, Physical chemistry chemical physics : PCCP.

[31]  J. Shang,et al.  Correction to "Efficient Visible Light Nitrogen Fixation with BiOBr Nanosheets of Oxygen Vacancies on the Exposed {001} Facets". , 2018, Journal of the American Chemical Society.

[32]  S. Yin,et al.  Novel visible-light-driven Z-scheme Bi12GeO20/g-C3N4 photocatalyst: Oxygen-induced pathway of organic pollutants degradation and proton assisted electron transfer mechanism of Cr(VI) reduction , 2017 .

[33]  Jinlong Zhang,et al.  Efficient Solar Light Harvesting CdS/Co9 S8 Hollow Cubes for Z-Scheme Photocatalytic Water Splitting. , 2017, Angewandte Chemie.

[34]  G. Zeng,et al.  Visible-light photocatalytic degradation of multiple antibiotics by AgI nanoparticle-sensitized Bi5O7I microspheres: Enhanced interfacial charge transfer based on Z-scheme heterojunctions , 2017 .

[35]  T. Hayat,et al.  Hybrid 0D-2D Nanoheterostructures: In Situ Growth of Amorphous Silver Silicates Dots on g-C3N4 Nanosheets for Full-Spectrum Photocatalysis. , 2016, ACS applied materials & interfaces.

[36]  M. Salavati‐Niasari,et al.  Enhanced photodegradation of dye in waste water using iron vanadate nanocomposite; ultrasound-assisted preparation and characterization. , 2017, Ultrasonics sonochemistry.

[37]  Yongxiu Li,et al.  Synthesis and photocatalytic activity of BiOBr nanosheets with tunable exposed {0 1 0} facets , 2016 .

[38]  Yihe Zhang,et al.  Fabrication of multiple heterojunctions with tunable visible-light-active photocatalytic reactivity in BiOBr-BiOI full-range composites based on microstructure modulation and band structures. , 2015, ACS applied materials & interfaces.

[39]  Zhouping Wang,et al.  Enhanced Visible-Light-Driven Photocatalytic Disinfection Performance and Organic Pollutant Degradation Activity of Porous g-C3N4 Nanosheets. , 2017, ACS applied materials & interfaces.

[40]  Gaoke Zhang,et al.  Ultrasonic-assistant fabrication of cocoon-like Ag/AgFeO2 nanocatalyst with excellent plasmon enhanced visible-light photocatalytic activity. , 2017, Ultrasonics sonochemistry.

[41]  Wei Wei,et al.  Formation of g-C3N4@Ni(OH)2 Honeycomb Nanostructure and Asymmetric Supercapacitor with High Energy and Power Density. , 2017, ACS applied materials & interfaces.

[42]  Hui‐Ming Cheng,et al.  Nitrogen Vacancy-Promoted Photocatalytic Activity of Graphitic Carbon Nitride , 2012 .

[43]  H. Schmalz,et al.  Clinical wastewater treatment: Photochemical removal of an anionic antibiotic (ciprofloxacin) by mesostructured high aspect ratio ZnO nanotubes , 2017 .

[44]  Can Li,et al.  Enhancement of photocatalytic H2 evolution on CdS by loading MoS2 as Cocatalyst under visible light irradiation. , 2008, Journal of the American Chemical Society.

[45]  Jinshui Zhang,et al.  Sol processing of conjugated carbon nitride powders for thin-film fabrication. , 2015, Angewandte Chemie.

[46]  C. Liang,et al.  Facile synthesis of Z-scheme graphitic-C3N4/Bi2MoO6 nanocomposite for enhanced visible photocatalytic properties , 2015 .

[47]  W. Ho,et al.  Noble Metal-Like Behavior of Plasmonic Bi Particles as a Cocatalyst Deposited on (BiO)2CO3 Microspheres for Efficient Visible Light Photocatalysis , 2014 .

[48]  T. Schmidt,et al.  Dependence of transformation product formation on pH during photolytic and photocatalytic degradation of ciprofloxacin. , 2016, Journal of hazardous materials.

[49]  A. Alivisatos Semiconductor Clusters, Nanocrystals, and Quantum Dots , 1996, Science.

[50]  Weidong Shi,et al.  Highly efficient visible-light-driven photocatalytic degradation of tetracycline by a Z-scheme g-C3N4/Bi3TaO7 nanocomposite photocatalyst. , 2017, Dalton transactions.