Manifestation of enhanced and durable photocatalytic H2 production using hierarchically structured Pt@Co3O4/TiO2 ternary nanocomposite

A hierarchical structure composed of Pt@Co₃O₄/TiO₂ (CTP) ternary nanocomposite was synthesized and demonstrated for its enhanced and durable production of hydrogen from glycerol under simulated solar light irradiation. The rate of hydrogen production over the optimized composition was found to be 19.2 mmol h^?1 g^?1_cat. The obtained XRD and XPS results revealed the facile formation of the composite. The heterojunction formed in the ternary system remarkably enhanced the visible light absorption properties and charge separation in CTP as evidenced from their UV–visible absorption and PL spectra, respectively. The optimized union of the materials with specific properties and their intimate physical contacts might be the origin for the manifested, improved and durable photocatalytic efficiency towards hydrogen production.     

Facile fabrication of 3D interconnected porous boron doped polymeric g-C3N4 with enhanced visible light photocatalytic hydrogen evolution and dye contaminant elimination

Researchers have attempted to developing high-efficiency catalysts for photocatalytic hydrogen evolution and organic pollution elimination simultaneously to alleviate the issues of energy shortage and water pollution. In this work, we fabricated 3D interconnected porous boron doped polymeric g-C₃N₄ catalysts with efficient photocatalytic activity for hydrogen evolution and dye contaminant elimination under visible-light irradiation. The as-fabricated catalysts exhibited significantly enhanced hydrogen evolution (4.37 mmol g ^?1 h^?1) and RhB contaminant elimination (96.37%) activity. Based on characterization and photocatalytic tests, an enhanced mechanism of the superior photocatalytic performance was proposed: 3D interconnected porous structure and B-doping have a synergistic effect on the greatly improved photocatalytic activity. The 3D interconnected structures endowed g-C₃N₄ with a higher specific surface area and abundant active sites and improved the capacity of rapid absorption to facilitate the photocatalytic process. B doping provided enhanced visible-light absorption capacity and a narrowed bandgap and served as a “highway” for electron-hole pairs to facilitate migration and separation and suppress the combination of photogenerated carriers. Besides, the possible mechanism of enhanced photocatalytic performance was elucidated according to the results of characterization measurements and active species analysis.     

Ionic liquid-assisted preparation of g-C3N4/RGO co-intercalated CuBi2O4 hierarchical nanoflower and enhancement of the photocatalytic activity

A new p-n type CBO/CN/RGO ternary heterojunction photocatalyst combining three-dimensional multi-stage rosette CuBi₂O₄ and two-dimensional g-C₃N₄ and RGO flakes was successfully prepared by ionic liquid-assisted hydrothermal method. The successful construction of p-n heterojunctions of CBO/CN/RGO composites was verified by means of UV–vis diffuse reflection, Mott Schottky curves and TEM, and construction the heterojunctions significantly improved that of the transfer and transport speed of photogenerated carriers. The photocatalytic degradation of MO by CBO/CN/RGO-6% reached 91.83% within 150 min, while the kinetic constants of degradation k were 9.7 and 7.9 times greater than those of single-phase CBO and g-C₃N₄, respectively. Three cycles of experiments demonstrated that the degradation efficiency of CBO/CN/RGO-6% composites remained above 88% for RhB, which fully proved that the CBO/CN/RGO-6% composites possessed good chemical stability. Based on its excellent photocatalytic performance and good stability, CBO/CN/RGO-6% is expected to be the preferred material for environmental wastewater treatment.     

MoS2/g-C3N4复合光催化剂催化降解H2S的研究

采用热处理法合成了g-C3N4,通过光照沉积法将MoS2原位沉积到g-C3N4表面的活性位点,制备了MoS2/g-C3N4复合光催化剂,采用XRD、XPS和BET对MoS2/g-C3N4复合光催化剂的结构进行了表征:MoS2负载到g-C3N4表面,且未改变g-C3N4的晶体结构,同时具有较大的比表面积.考察了MoS2负...     

氮化碳的梯度热分解法制备与产氢研究

以三聚氰胺为原料,采用梯度升温热解法制备了石墨状氮化碳(g-C_3N_4),采用XRD、XPS、FTIR、SEM及UV-Vis、PL等技术手段对氮化碳材料的微观结构和光学性能进行了表征,并分析其光解水产氢性能。结果表明:采用梯度升温热解法制备的g-C_3N_4结构良好;620°C才开始快速分解,对热稳定性良好;几乎不溶于常见试剂,化学稳定性较好;在400~550 nm的可见光波长范围内对可见光有着明显吸收,禁带宽度达到2.42 e V,具有较高的光催化分解水制氢能力(18.95μmol/h).     

Facile fabrication of ordered assembled TiO2/g-C3N4 nanosheets with enhanced photocatalytic activity

A series of assembled porous TiO₂/g-C₃N₄ (TC) powders composed of spherical nanoparticles were synthesized by controlling the molar ratio of urea to tetrabutyl titanate (TBOT) in a facile hydrothermal process. A nanosheets-constructed hierarchical structure was obtained at the molar ratio of urea to TBOT of 10:1, which possessed uniform mesopores with bimodal distribution (0.5–1.5 nm and 2–20 nm) and interconnected macropores between TC nanosheets. The specific surface area achieved 98.4 m² g^?1. X-ray diffraction (XRD) patterns and high resolution transmission electron microscope (HRTEM) analysis proved that the nanosheets are made of overlapping TC nanocomposite. Photoluminescence (PL) spectra results illustrated that a well-defined hierarchical porous structure is particularly desired for the low recombination rate of carriers. Further, the TC-decorated carbon fiber (CF) cloth was obtained based on the nanosheets assembled hierarchical structure, which showed more outstanding photocatalytic behavior with high degradation capability for Rhodamine B (RhB) (99.9%) and tetracycline hydrochloride (89.8%) at 60 min by 500 W Xe lamp irradiation. After five consecutive cycles, the degradation efficiencies of TC/CF cloth for both RhB and tetracycline hydrochloride all remained above 90% of the initial value.     

Fabrication of heterogeneous photocatalysts for insight role of carbon nanofibre in hierarchical WO3/ MoSe2 composite for enhanced photocatalytic hydrogen generation

Mimicking the natural photosynthesis system, artificial photocatalysis facilitates effective utilization of solar energy for environmental sustainability and hydrogen energy production. In this work, the robust and efficient carbon fiber has been successfully incorporated into the interface between WO₃ nanodots and MoSe₂ needles using the facile hydrothermal and solvothermal method. The suitable interfacial contact of heterogeneous photocatalysts plays a significant role in the separation/transfer of interfacial photogenerated electron-hole pairs and hetero-junction. It seems an efficient approach for enhanced photocatalytic performance since the greater area of contact could improve the interfacial rate of charge transfer. The phase structure of prepared WO₃ nanodots changed from the monoclinic to hexagonal phase by the addition of co-catalyst. The experimental results exhibited that carbon fiber played a tri-functional role to boost up the photocatalytic activity over MoSe₂ nanostructures. It's not only act as operative co-catalyst but could also serve as the conductive electron bridges, rather than general cocatalyst, to accumulate electrons and encourage the hydrogen generation kinetics over the WO₃ photocatalysts. More interestingly, the WO₃?1% MoSe₂?1.5% carbon fiber and WO₃?1%MoSe₂ nanocomposites demonstrated the excellent rates of hydrogen evolution 438.7 and 356.2?mmol/g.h, which were 7.6 and 6.17 times higher when compared to that of pure MoSe₂, respectively. Under the visible light excitation, the atomically junction encourages fast electron transfer from nanofibers to MoSe₂ to suppress the rapid recombination kinetics within WO₃ nanodots and extend the lifetime of WO₃ charge carrier's, thereby releasing more photogenerated electrons with higher reducing power for hydrogen evolution. The current work can contribute with new perspectives and mechanistic insight for the design and development of heterogeneous photocatalysts WO₃ based nanostructures using the combination of MoSe₂ and trifunctional carbon nanofibers for environment and energy harvesting applications.     

ZnIn2S4/g-C3N4 Nanocomposite for Proficient Elimination of Hg (II) under Visible Light

Journal of Inorganic and Organometallic Polymers and Materials - The present work offers beneficial method for Hg (II) elimination from aqueous solution. ZnIn2S4/g-C3N4 nanocomposites were...     

Fabrication of direct Z-scheme FeIn2S4/Bi2WO6 hierarchical heterostructures with enhanced photocatalytic activity for tetracycline hydrochloride photodagradation

A series of direct Z-scheme FeIn₂S₄/Bi₂WO₆ hierarchical heterostructures with intimate interface contacts were synthesized by in-situ growth route and characterized by systematical analyses. All as-prepared FeIn₂S₄/Bi₂WO₆ nanocomposites showed significantly enhanced photocatalytic activity towards photodegradation for the removal of tetracycline hydrochloride (TCH) in comparison with individual FeIn₂S₄ and Bi₂WO₆. Meanwhile, the highest photocatalytic degradation activity can be achieved by modulating adding amount of FeIn₂S₄ in FeIn₂S₄/Bi₂WO₆ nanocomposites and the optimized component ratio of FeIn₂S₄ to Bi₂WO₆ is determined to be 10 wt%. The enhanced photocatalytic activity could be ascribed to efficient separation between photogenerated holes and electrons based on the construction of direct Z-scheme system. The high photocatalytic stability of resultant 10 wt% FeIn₂S₄/Bi₂WO₆ nanocomposites was revealed through six successive recycling reactions. The main intermediate generated during TCH photodegradation was explored by HPLC-MS. Besides, the direct Z-scheme photocatalytic mechanism was confirmed by band position analysis, electron spin resonance (ESR) and active species capture experiment.     

Amino group-rich porous g-C3N4 nanosheet photocatalyst: Facile oxalic acid-induced synthesis and improved H2-evolution activity

The reasonable modulation of tri-s-triazine structure units of g-C₃N₄ is an effective method to optimize its intrinsic electronic and optical properties, thus boosting its photocatalytic hydrogen-evolution activity. Herein, amino groups are successfully introduced into the tri-s-triazine structure units of g-C₃N₄ nanosheets to improve their H₂-evolution activity via a facile oxalic acid-induced supramolecular assembly strategy. In this case, the resulting amino group-rich porous g-C₃N₄ nanosheets display a loose and fluffy structure with a large specific surface area (70.41 m² g^?1) and pore volume (0.50 cm³? g^??1), and enhanced visible-light absorption (450–800 nm). Photocatalytic tests reveal that the amino group-rich porous g-C₃N₄ nanosheets (AP-CN1.0 nanosheets) exhibit a significantly elevated photocatalytic H₂-production activity (130.7 μmol h^?1, AQE = 5.58%), which is much greater than that of bulk g-C₃N₄ by a factor of 4.9 times. The enhanced hydrogen-generation performance of amino group-rich porous g-C₃N₄ nanosheets can be mainly attributed to the introduction of more amino groups, which can reinforce the visible-light absorption and work as the interfacial hydrogen-generation active centers to boost the photocatalytic hydrogen production. The present facile and effective regulation of tri-s-triazine structure units may provide an ideal route for the exploitation of novel and highly efficient g-C₃N₄ photocatalysts.     

Preparation of g-C3N4/MoS2 Composite Material and Its Visible Light Catalytic Performance

The g-C₃N₄ nanosheet was prepared by calcination method, the MoS₂ nanosheet was prepared by hydrothermal method. The g-C₃N₄/MoS₂ composites were prepared by ultrasonic composite in anhydrous ethanol. X-ray diffraction, scanning electron microscopy, transmission electron microscopy, X-ray photoelectron spectroscopy, ultraviolet–visible spectroscopy, and photoluminescence techniques were used to characterize the materials. The photocatalytic degradation of Rhodamine B (Rh B) by g-C₃N₄/MoS₂ composites with different mass ratios was investigated under visible light. The results show that a small amount of MoS₂ combined with g-C₃N₄ can significantly improve photocatalytic activity. The g-C₃N₄/MoS₂ composite with a mass ratio of 1:8 has the highest photocatalytic activity, and the degradation rate of Rh B increases from 50 to 99.6%. The main reason is that MoS₂ and g-C₃N₄ have a matching band structure. The separation rate of photogenerated electron–hole pairs is enhanced. So the g-C₃N₄/MoS₂ composite can improve the photocatalytic activity. Through the active material capture experiment, it is found that the main active material in the photocatalytic reaction process is holes, followed by superoxide radicals.

     

g-C_3N_4/BiVO_4复合光催化剂的制备与光催化性能研究

通过原位复合的方法制备不同配比的g-C3N4/BiVO4复合光催化剂,利用傅里叶红外光谱(FTIR)、X-射线衍射(XRD)、扫描电子显微镜(SEM)、透射电子显微镜(TEM)、紫外-可见光漫反射光谱(UV-Vis DRS)和N2吸附-脱附对所制备的材料进行表征。并通过光催化降解有机染料罗丹明B对其光催化活性进行测试。结果表明,部分g-C3N4附着在BiVO4表面,g-C3N4/BiVO4复合光催化剂比纯的BiVO4光催化效果要好,并且确定了最佳复合比例,同时对复合光催化剂性能提高的机理进行了讨论。     

Sea urchin shaped ZnO coupled with MoS2 and polyaniline as highly efficient photocatalysts for organic pollutant decomposition and hydrogen evolution

In this work, an attempt has been made to fabricate multifunctional composite photocatalysts by coupling sea urchin shaped ZnO with MoS₂ and polyaniline (PANI) sheets, and a significant improvement in photocatalytic activity was perceived with composites in comparison to pristine components. It was found that the ternary ZnO–MoS₂-PANI photocatalyst showed excellent adsorptive decomposition of organic pollutants natural sunlight irradiation. In addition, enhanced photocatalytic hydrogen evolution was also evidenced, which revealed the multifunctional nature of the photocatalysts. In the case of organic pollutant decomposition, the presence of MoS₂ in ZnO–MoS₂-PANI offers abundant catalytic active sites which result in adsorption of the pollutants and boost the photocatalytic activity. While for the photocatalytic hydrogen evolution, the binary ZnO-PANI composite showed the utmost activity in comparison to the pristine components and ZnO–MoS₂-PANI, which is due to the fact that the higher loading of MoS₂ in the composite increases the number of S atoms on the basal planes, which are inactive for H₂ evolution, and hence results in decreased photocatalytic activity. The results discussed in this work may pave the approach for the design and development of ZnO based multifunctional materials for diverse photocatalytic applications.     

Constructing 0D/1D/2D Z-scheme heterojunctions of Ag nanodots/SiC nanofibers/g-C3N4 nanosheets for efficient photocatalytic water splitting

Efficiently constructing nanostructured Z-scheme heterojunctions with good interface contact is a desired route to optimize the photocatalytic property of the materials. In this work, novel 0D/1D/2D Z-scheme silver/silicon carbide/graphitic carbon nitride (Ag/SiC/CN) photocatalysts were prepared from Ag nanodots loaded on SiC nanofibers/CN nanosheets (SiC/CN) composite, using the calcination and chemical reduction routes. The Ag/SiC/CN composite with an optimal 3% Ag loading dose performs the best H₂ evolution rate of 2971 μmol g^?1 h^?1, which is approximately 8.8, 1.5 and 4.5 times compared to CN, SiC/CN and 3% Ag/CN, respectively. Besides the Ag/SiC/CN composite presents a high apparent quantum efficiency (7.3%) and outstanding photo-corrosion resistance stability. The Ag nanodots are served as efficient carriers transfer center and cocatalyst to construct Z-scheme heterojunction interface, which can help to generate more photo-generated carries, shorten the electron transmission distance and increase the electron transfer rate, certifying that 0D/1D/2D Z-scheme photocatalytic system is high-efficiency and has great advantages in photocatalytic applications.     

A Facile One Step Synthesis of MoS2/g-C3N4 Photocatalyst with Enhanced Visible Light Photocatalytic Hydrogen Production

Catalysis Letters - Noble metal-free MoS2/g-C3N4 photocatalysts have been synthetized by one step thermal treatment of thiourea and sodium molybdate, which has intimate contact interfaces between...     

有机酸介导合成WO3/g-C3N4及其光催化性能

采用水热法制备了WO3/g-C3N4复合物,并探讨了草酸、柠檬酸、乙酸和水杨酸对复合物结构、形貌及催化活性的影响.结果表明,复合物中棒状WO3分布在片层状的g-C3N4上,二者结合紧密形成异质结构.以1 mol/L草酸为介导剂制备的WO3/g-C3N4的光催化活性最佳,当WO3和g-C3N4质量比为1:1时,可见光下反...     

花簇状g-C3N4/Bi2MoO6微球的制备及其光催化降解模拟染料废水

以酵母为生物模板,通过水热-牺牲模板法制备了花簇状g-C3N4/Bi2MoO6微球.利用XRD、SEM、TEM、FTIR、UV-Vis DRS、光电流响应以及氮气吸附-脱附等手段对样品的晶体结构、微观形貌、光吸收和比表面积等性能进行了表征,并对样品可见光催化降解亚甲基蓝(MB)模拟染料废水的性能和机理进行了探讨.结果表...     

Construction of highly efficient 0D/2D Bi2MoO6/g-C3N4 heterojunctions for visible-light-driven photodegradation of 1-naphthol

Photocatalytic degradation is an ecologically benign method of reducing organic contaminants in wastewater. To remove the pollutant 1-naphthol, highly efficient 0D/2D Bi₂MoO₆/g-C₃N₄ heterojunctions were successfully assembled by a one-step hydrothermal method, where zero-dimension (0D) Bi₂MoO₆ nanoparticles were firmly bonded to two-dimension (2D) g-C₃N₄ nanosheets. 0D/2D Bi₂MoO₆/g-C₃N₄ exhibited exceptional degradation efficiency for 1-naphthol with a removal rate of 81.5% after 60 min of visible light irradiation. The enhanced photocatalytic ability was attributed to the matched band structures and tightly connected heterojunctions, which effectively prevented the recombination of photogenerated carriers. Besides, the photodegradation mechanism was revealed by investigating the catalysts' crystal phase, morphology, physicochemical and optical properties. This work introduces a novel method for one-step preparation of 0D/2D photocatalysts and advances the utilization of photodegradation for organic pollutants.     

Heterogeneous photocatalytic removal of the herbicide clopyralid and its comparison with UV/H2O2 and ozone oxidation techniques

Clopyralid is a herbicide that has recently been reported to occur in drinking water at concentrations above the Permitted Concentration Value (PCV) of 0.1 μg/L for an individual pesticide (EU directive 98/83/EC). An extensive laboratory study on clopyralid removal with UV/TiO₂, was carried out and was compared to UV/H₂O₂ and O₃ removal efficiencies. The effectiveness of three TiO₂ photocatalysts (Degussa P25, VP Aeroperl, Hombifine N) was studied and Degussa P25 was selected since it outperformed the other two. Complete removal of clopyralid was achieved with UV/TiO₂ in about 90 min at an optimum catalyst concentration of 1 g/L. Pseudo-zero-order kinetics were suitable to describe the first stage of the photocatalytic reaction in the concentration range 0.078–0.521 mM. pH was found to significantly affect the removal rates of clopyralid due to changes in TiO₂ surface charges and clopyralid ionisation degree. The rate constant was maximum at pH 5 and its value was 2.1 × 10⁻⁶ ± 4.3 × 10⁻⁷ M min⁻¹. Pure oxygen bubbled in solution was found to slightly affect unfavourably the photocatalytic removal of clopyralid as compared to air. With UV/H₂O₂ and O₃ systems, the initial removal rates were high but these systems were not effective in achieving high removal percentages overall.     

Enhancement of photoinduced hydrogen production from irradiated Pt/TiO2 suspensions with simultaneous degradation of azo-dyes

The production of hydrogen from aqueous Pt/TiO₂ suspensions illuminated with UV–vis light has been examined in the absence and in presence of azo-dyes in solution. The effects of operational variables, including dye concentration, solution pH and temperature, on the rate of hydrogen production were investigated. It has been found that deposition of Pt (0.5 wt.%) on the semiconductor surface results in an increase of the H₂ production rate, which goes through a maximum with time of irradiation and then drops to steady-state values comparable to those obtained over bare TiO₂. Both, maximum and steady-state rates obtained over Pt/TiO₂ suspensions were found to increase with increasing solution pH and temperature. Addition of small quantities of azo-dyes in solution results in significantly enhanced rates of H₂ production for a period which depends on dye concentration, solution pH and, to a lesser extent, solution temperature. It is proposed that the dye acts as a scavenger of photogenerated oxidizing species while it is degraded toward CO₂ and inorganic ions. When complete mineralization is achieved, oxygen can no longer be removed from the photocatalyst surface and the rate drops to steady-state values, comparable to those obtained in the absence of azo-dye in solution. The amount of additional H₂ produced is directly proportional to the amount of dye added in the solution. The rate increases with increasing solution pH, where dye degradation is faster, indicating that the process is limited by the rate of consumption of photogenerated oxygen. It is concluded that, under certain experimental conditions, it is possible to obtain significantly enhanced rates of photoinduced hydrogen production from Pt/TiO₂ suspensions with simultaneous mineralization of azo-dyes. The process could be used for combined production of fuel H₂ and degradation of organic pollutants present in water.