Graphitic carbon nitride(g-C_(3)N_(4))has been extensively doped with alkali metals to enlarge photocatalytic output,in which cesium(Cs)doping is predicted to be the most efficient.Nevertheless,the sluggish diffusion ...Graphitic carbon nitride(g-C_(3)N_(4))has been extensively doped with alkali metals to enlarge photocatalytic output,in which cesium(Cs)doping is predicted to be the most efficient.Nevertheless,the sluggish diffusion and doping kinetics of precursors with high melting points,along with imprecise regulation,have raised the debate on whether Cs doping could make sense.For this matter,we attempt to confirm the positive effects of Cs doping on multifunctional photocatalysis by first using cesium acetate with the character of easy manipulation.The optimized Csdoped g-C_(3)N_(4)(CCN)shows a 41.6-fold increase in visible-light-driven hydrogen evolution reaction(HER)compared to pure g-C_(3)N_(4) and impressive degradation capability,especially with 77%refractory tetracycline and almost 100%rhodamine B degradedwithin an hour.The penetration ofCs+is demonstrated to be a mode of interlayer doping,and Cs–N bonds(especially with sp^(2) pyridine N in C═N–C),along with robust chemical interaction and electron exchange,are fabricated.This atomic configuration triggers the broadened spectral response,the improved charge migration,and the activated photocatalytic capacity.Furthermore,we evaluate the CCN/cadmium sulfide hybrid as a Z-scheme configuration,promoting the visible HER yield to 9.02 mmol g^(−1) h^(−1),which is the highest ever reported among all CCN systems.This work adds to the rapidly expanding field of manipulation strategies and supports further development of mediating served for photocatalysis.展开更多
Photocatalysis,a critical strategy for harvesting sunlight to address energy demand and environmental concerns,is underpinned by the discovery of high-performance photocatalysts,thereby how to design photocatalysts is...Photocatalysis,a critical strategy for harvesting sunlight to address energy demand and environmental concerns,is underpinned by the discovery of high-performance photocatalysts,thereby how to design photocatalysts is now generating widespread interest in boosting the conversion effi-ciency of solar energy.In the past decade,computational technologies and theoretical simulations have led to a major leap in the development of high-throughput computational screening strategies for novel high-efficiency photocatalysts.In this viewpoint,we started with introducing the challenges of photocatalysis from the view of experimental practice,especially the inefficiency of the traditional“trial and error”method.Sub-sequently,a cross-sectional comparison between experimental and high-throughput computational screening for photocatalysis is presented and discussed in detail.On the basis of the current experimental progress in photocatalysis,we also exemplified the various challenges associated with high-throughput computational screening strategies.Finally,we offered a preferred high-throughput computational screening procedure for pho-tocatalysts from an experimental practice perspective(model construction and screening,standardized experiments,assessment and revision),with the aim of a better correlation of high-throughput simulations and experimental practices,motivating to search for better descriptors.展开更多
It is a challenge to coordinate carrier-kinetics performance and the redox capacity of photogenerated charges synchronously at the atomic level for boosting photocatalytic activity.Herein,the atomic Ni was introduced ...It is a challenge to coordinate carrier-kinetics performance and the redox capacity of photogenerated charges synchronously at the atomic level for boosting photocatalytic activity.Herein,the atomic Ni was introduced into the lattice of hexagonal ZnIn_(2)S_(4) nanosheets(Ni/ZnIn_(2)S_(4))via directionalsubstituting Zn atom with the facile hydrothermal method.The electronic structure calculations indicate that the introduction of Ni atom effectively extracts more electrons and acts as active site for subsequent reduction reaction.Besides the optimized light absorption range,the elevation of Efand ECBendows Ni/ZnIn_(2)S_(4) photocatalyst with the increased electron concentration and the enhanced reduction ability for surface reaction.Moreover,ultrafast transient absorption spectroscopy,as well as a series of electrochemical tests,demonstrates that Ni/ZnIn_(2)S_(4) possesses 2.15 times longer lifetime of the excited charge carriers and an order of magnitude increase for carrier mobility and separation efficiency compared with pristine ZnIn_(2)S_(4).These efficient kinetics performances of charge carriers and enhanced redox capacity synergistically boost photocatalytic activity,in which a 3-times higher conversion efficiency of nitrobenzene reduction was achieved upon Ni/ZnIn_(2)S_(4).Our study not only provides in-depth insights into the effect of atomic directional-substitution on the kinetic behavior of photogenerated charges,but also opens an avenue to the synchronous optimization of redox capacity and carrier-kinetics performance for efficient solar energy conversion.展开更多
Photocatalysis driven by abundant yet intermittent solar energy has considerable potential in renewable energy generation and environmental remediation.The outstanding electronic structure and physicochemical properti...Photocatalysis driven by abundant yet intermittent solar energy has considerable potential in renewable energy generation and environmental remediation.The outstanding electronic structure and physicochemical properties of graphitic carbon nitride(g-C_(3)N_(4)),together with unique metal-free characteristic,make them ideal candidates for advanced photocatalysts construction.This review summarizes the up-to-date advances on g-C_(3)N_(4)based photocatalysts from ingenious-design strategies and diversified photocatalytic applications.Notably,the advantages,fabrication methods and limitations of each design strategy are systemically analyzed.In order to deeply comprehend the inner connection of theory–structure–performance upon g-C_(3)N_(4)based photocatalysts,structure/composition designs,corresponding photocatalytic activities and reaction mechanisms are jointly discussed,associated with introducing their photocatalytic applications toward water splitting,carbon dioxide/nitrogen reduction and pollutants degradation,etc.Finally,the current challenges and future perspectives for g-C_(3)N_(4)based materials for photocatalysis are briefly proposed.These design strategies and limitations are also instructive for constructing g-C_(3)N_(4) based materials in other energy and environment-related applications.展开更多
The bulk/surface states of semiconductor photocatalysts are imperative parameters to maneuver their performance by significantly affecting the key processes of photocatalysis including light absorption,separation of c...The bulk/surface states of semiconductor photocatalysts are imperative parameters to maneuver their performance by significantly affecting the key processes of photocatalysis including light absorption,separation of charge carrier,and surface site reaction.Recent years have witnessed the encouraging progress of self-adaptive bulk/surface engineered Bi_(x)O_(y)Br_(z) for photocatalytic applications spanning various fields.However,despite the maturity of current research,the interaction between the bulk/surface state and the performance of Bi_(x)O_(y)Br_(z) has not yet been fully understood and highlighted.In this regard,a timely tutorial overview is quite urgent to summarize the most recent key progress and outline developing obstacles in this exciting area.Herein,the structural characteristics and fundamental principles of Bi_(x)O_(y)Br_(z)for driving photocatalytic reaction as well as related key issues are firstly reviewed.Then,we for the first time summarized different self-adaptive engineering processes over Bi_(x)O_(y)Br_(z)followed by a classification of the generation approaches towards diverse Bi_(x)O_(y)Br_(z)materials.The features of different strategies,the up-to-date characterization techniques to detect bulk/surface states,and the effect of bulk/surface states on improving the photoactivity of Bi_(x)O_(y)Br_(z)in expanded applications are further discussed.Finally,the present research status,challenges,and future research opportunities of self-adaptive bulk/surface engineered Bi_(x)O_(y)Br_(z)are prospected.It is anticipated that this critical review can trigger deeper investigations and attract upcoming innovative ideas on the rational design of Bi_(x)O_(y)Br_(z)-based photocatalysts.展开更多
We report a new facile light-induced strategy to disperse micron-sized aggregated bulk covalent organic frameworks(COFs)into isolated COFs nanoparticles.This was achieved by a series of metal-coordinated COFs,namely C...We report a new facile light-induced strategy to disperse micron-sized aggregated bulk covalent organic frameworks(COFs)into isolated COFs nanoparticles.This was achieved by a series of metal-coordinated COFs,namely COF-909-Cu,-Co or-Fe,where for the first time the diffusio-phoretic propulsion was utilized to design COF-based micro/nanomotors.The mechanism studies revealed that the metal ions decorated in the COF-909 backbone could promote the separation of electron and holes and trigger the production of sufficient ionic and reactive oxygen species under visible light irradiation.In this way,strong light-induced self-diffusiophoretic effect is achieved,resulting in good dispersion of COFs.Among them,COF-909-Fe showed the highest dispersion performance,along with a drastic decrease in particle size from 5μm to500 nm,within only 30 min light irradiation,which is inaccessible by using traditional magnetic stirring or ultrasonication methods.More importantly,benefiting from the outstanding dispersion efficiency,COF-909-Fe micro/nanomotors were demonstrated to be efficient in photocatalytic degradation of tetracycline,about 8 times faster than using traditional magnetic stirring method.This work opens up a new avenue to prepare isolated nanosized COFs in a high-fast,simple,and green manner.展开更多
In this paper, we present a proof-of-concept study of the enhancement of photocatalytic activity via a combined strategy of fabricating a visible-light responsive ternary heterostructure and improving overall photosta...In this paper, we present a proof-of-concept study of the enhancement of photocatalytic activity via a combined strategy of fabricating a visible-light responsive ternary heterostructure and improving overall photostability by incorporating magnetic zinc oxide/graphene/iron oxide (ZGF). A solvothermal approach was used to synthesize the catalyst. X-ray diffraction (XRD), scanning electron microscopic, energy dispersive X-ray, transmission electron microscopic, vibrating sample magnetometric, and ultraviolet–visible diffuse reflectance spectroscopic techniques were used to characterize the synthesized samples. The obtained optimal Zn(NO_(3))_(2) concentration, temperature, and heating duration were 0.10 mol/L, 600℃, and 1 h, respectively. The XRD pattern revealed the presence of peaks corresponding to zinc oxide, graphene, and iron oxide, indicating that the ZGF catalyst was effectively synthesized. Furthermore, when the developed ZGF was used for methylene blue dye degradation, the optimum irradiation time, dye concentration, catalyst dosage, irradiation intensity, and solution pH were 90 min, 10 mg/L, 0.03 g/L, 100 W, and 8.0, respectively. Therefore, the synthesized ZGF system could be used as a catalyst to degrade dyes in wastewater samples. This hybrid nanocomposite consisting of zinc oxide, graphene, and iron oxide could also be used as an effective photocatalytic degrader for various dye pollutants.展开更多
This present study comes in addition to overcome the problems of separation of fine particles of TiO<sub>2</sub> in heterogeneous photocatalysis after treatment. It aims to show the potential for using tit...This present study comes in addition to overcome the problems of separation of fine particles of TiO<sub>2</sub> in heterogeneous photocatalysis after treatment. It aims to show the potential for using titaniferous sand as a new semiconductor under solar irradiation. The photocatalytic efficiency of this titaniferous sand was tested on a pesticide (Azadirachtin). A tubular photocatalytic reactor with recirculation of the polluting solution was designed for the elimination of the pesticide in an aqueous solution. Before its use as a photocatalyst, the titaniferous sand has undergone a specific treatment that consists of calcination at 600℃ followed by extraction of the calcined natural organic materials, which can interfere with the measurement of analytical parameters such as COD. The titaniferous sand was also characterized by X-ray fluorescence spectroscopy (XRF). XRF analyses have shown that TiO<sub>2</sub> is predominant in the titaniferous sand with a percentage that has been estimated at 46.34%. The influence of various experimental parameters such as the flow rate of the polluting solution, the concentration of titaniferous sand, the presence of oxygen and the intensity of the overall rate of sunshine, was studied to optimize the photocatalytic degradation of the pesticide. The results showed that the highest removal rate (70%) was observed under the following conditions: a pH of 6, a titaniferous sand concentration of 150 g/L, a flow rate of 0.3 mL/min, and a sunshine rate of 354 W/m<sup>2</sup> and in the presence of atmospheric oxygen. Under these experimental conditions, the rate of photodegradation of the pesticide follows the pseudo first order kinetic model of Langmuir Hinshelwood with a coefficient of determination R<sup>2</sup> of 0.9869 and an apparent rate constant of 0.0029 min<sup>-1</sup>. The results clearly demonstrated the potential of titaniferous sand as a photocatalyst sensitive to sunlight for the effective removal of pesticides in the aquatic environment.展开更多
Since their seminal discovery in 2011,two-dimensional(2D)transition metal carbides/nitrides known as MXenes,that constitute a large family of 2D materials,have been targeted toward various applications due to their ou...Since their seminal discovery in 2011,two-dimensional(2D)transition metal carbides/nitrides known as MXenes,that constitute a large family of 2D materials,have been targeted toward various applications due to their outstanding electronic properties.MXenes functioning as co-catalyst in combination with certain photocatalysts have been applied in photocatalytic systems to enhance photogenerated charge separation,suppress rapid charge recombination,and convert solar energy into chemical energy or use it in the degradation of organic compounds.The photocatalytic performance greatly depends on the composition and morphology of the photocatalyst,which,in turn,are determined by the method of preparation used.Here,we review the four different synthesis methods(mechanical mixing,self-assembly,in situ decoration,and oxidation)reported for MXenes in view of their application as co-catalyst in photocatalysis.In addition,the working mechanism for MXenes application in photocatalysis is discussed and an outlook for future research is also provided.展开更多
g-C_(3)N_(4) emerges as a star 2D photocatalyst due to its unique layered structure,suitable band structure and low cost.However,its photocatalytic application is limited by the fast charge recombination and low photo...g-C_(3)N_(4) emerges as a star 2D photocatalyst due to its unique layered structure,suitable band structure and low cost.However,its photocatalytic application is limited by the fast charge recombination and low photoabsorption.Rationally designing g-C_(3)N_(4)-based heterojunction is promising for improving photocatalytic activity.Besides,g-C_(3)N_(4) exhibits great potentials in electrochemical energy storage.In view of the excellent performance of typical transition metal oxides(TMOs)in photocatalysis and energy storage,this review summarized the advances of TMOs/g-C_(3)N_(4) heterojunctions in the above two areas.Firstly,we introduce several typical TMOs based on their crystal structures and band structures.Then,we summarize different kinds of TMOs/g-C_(3)N_(4) heterojunctions,including type Ⅰ/Ⅱ heterojunction,Z-scheme,p-n junction and Schottky junction,with diverse photocatalytic applications(pollutant degradation,water splitting,CO_(2) reduction and N_(2) fixation)and supercapacitive energy storage.Finally,some promising strategies for improving the performance of TMOs/g-C_(3)N_(4) were proposed.Particularly,the exploration of photocatalysis-assisted supercapacitors was discussed.展开更多
Photocatalysis and electrocatalysis have been essential parts of electrochemical processes for over half a century.Recent progress in the controllable synthesis of 2D nanomaterials has exhibited enhanced catalytic per...Photocatalysis and electrocatalysis have been essential parts of electrochemical processes for over half a century.Recent progress in the controllable synthesis of 2D nanomaterials has exhibited enhanced catalytic performance compared to bulk materials.This has led to significant interest in the exploitation of 2D nanomaterials for catalysis.There have been a variety of excellent reviews on 2D nanomaterials for catalysis,but related issues of differences and similarities between photocatalysis and electrocatalysis in 2D nanomaterials are still vacant.Here,we provide a comprehensive overview on the differences and similarities of photocatalysis and electrocatalysis in the latest 2D nanomaterials.Strategies and traps for performance enhancement of 2D nanocatalysts are highlighted,which point out the differences and similarities of series issues for photocatalysis and electrocatalysis.In addition,2D nanocatalysts and their catalytic applications are discussed.Finally,opportunities,challenges and development directions for 2D nanocatalysts are described.The intention of this review is to inspire and direct interest in this research realm for the creation of future 2D nanomaterials for photocatalysis and electrocatalysis.展开更多
As a new member of carbon material family, carbon quantum dots(CQDs) have attracted tremendous attentions for their potentials in the heterogeneous photocatalysis applications. Due to the unique microstructure and opt...As a new member of carbon material family, carbon quantum dots(CQDs) have attracted tremendous attentions for their potentials in the heterogeneous photocatalysis applications. Due to the unique microstructure and optical properties, the roles of CQDs played in the CQDs-based photocatalytic systems have been found to be diverse with the continuous researches in this regard. Herein, we provide a concise minireview to elaborate the multifarious roles of CQDs in photocatalysis, including photoelectron mediator and acceptor, photosensitizer, photocatalyst, reducing agent for metal salt, enhancing adsorption capacity and spectral converter. In addition, the perspectives on future research trends and challenges are proposed, which are anticipated to stimulate further research into this promising field on designing a variety of efficient CQDs-based photocatalysts for solar energy conversion.展开更多
To improve the visible light absorption and photocatalytic activity of titanium dioxide nanotube arrays(TONTAs), ZnFe_2O_4(ZFO) nanocrystals were perfused into pristine TONTA pipelines using a novel bias voltageassist...To improve the visible light absorption and photocatalytic activity of titanium dioxide nanotube arrays(TONTAs), ZnFe_2O_4(ZFO) nanocrystals were perfused into pristine TONTA pipelines using a novel bias voltageassisted perfusion method. ZFO nanocrystals were well anchored on the inner walls of the pristine TONTAs when the ZFO suspensions(0.025 mg m L^(-1)) were kept under a60 V bias voltage for 1 h. After annealing at 750 °C for2 h, the heterostructured ZFO/Fe_2 TiO_5(FTO)/TiO_2 composite nanotube arrays were successfully obtained. Furthermore, Fe^(3+)was reduced to Fe^(2+)when solid solution reactions occurred at the interface of ZFO and the pristine TONTAs. Introducing ZFO significantly enhanced thevisible light absorption of the ZFO/FTO/TONTAs relative to that of the annealed TONTAs. The coexistence of type I and staggered type II band alignment in the ZFO/FTO/TONTAs facilitated the separation of photogenerated electrons and holes, thereby improving the efficiency of the ZFO/FTO/TONTAs for photocatalytic degradation of methylene blue when irradiated with simulated sunlight.展开更多
Pyrolysis of the Ta_(2)_(O5)/melamine mixture in molten chlorides is herein demonstrated as a facile and controllable method to nitridize and functionalize Ta_(2)_(O5).The influence of the stoichiometry and compositio...Pyrolysis of the Ta_(2)_(O5)/melamine mixture in molten chlorides is herein demonstrated as a facile and controllable method to nitridize and functionalize Ta_(2)_(O5).The influence of the stoichiometry and composition of Ta_(2)_(O5)/melamine in molten salts on the nitridation process is rationalized to ensure the controllable preparation of Ta_(3)N_(5) and Ta_(3)N_(5)/TaON.The characterization results,including scanning electron microscopy,transmission electron microscopy,elemental mapping,X-ray photoelectron spectroscopy,and photoluminescence spectroscopy,all confirm the existence of the Ta_(3)N_(5)/TaON heterojunction,in which the TaON nanoparticles are closely anchored to the Ta_(3)N_(5) nanorods.Benefiting from its composition and structure,the Ta_(3)N_(5)/TaON composites show enhanced photocatalytic activity for the degradation of methylene blue.The present study highlights that the molten salt method using a solid nitrogen source can be a new technique for rationalizing the design of nitrides and oxynitrides.展开更多
Porous photocatalysts are promising materials capable of simultaneously adsorbing and oxidizing/reducing target species,showing great potentials in environmental remediation and energy generation.This review offered a...Porous photocatalysts are promising materials capable of simultaneously adsorbing and oxidizing/reducing target species,showing great potentials in environmental remediation and energy generation.This review offered a comprehensive overview of the recent progress in design,fabrication,and applications of porous photocatalysts,including carbon-based semiconductors,metal oxides/sulfides,metal–organic frameworks,and adsorbent–photocatalyst hybrids.The fundamental understanding of the structure–performance relationships of porous materials together with the in-depth insights into the synergetic effects between adsorption and photocatalysis was presented.The strategies to further improve the photocatalytic activity of porous photocatalysts were proposed.This review would provide references and outlooks of constructing efficient porous materials for adsorptive and photocatalytic removal of pollutants and energy production.展开更多
Due to the strict regulations and reuse policies that govern wastewater's use as an irrigation water resource for agricultural purposes, especially in dry climates, optimization of the disinfection process is of t...Due to the strict regulations and reuse policies that govern wastewater's use as an irrigation water resource for agricultural purposes, especially in dry climates, optimization of the disinfection process is of the utmost importance. The effects of solar radiation along with Titanium dioxide(TiO_2) nanoparticles applied to optimization of the photolysis and photocatalysis processes for inactivating heterotrophic bacteria were investigated. Temperature, p H, and dissolved oxygen fluctuations in the dairy wastewater effluent treated by activated sludge were examined. In addition,different dosages of TiO_2 were tested in the solar photocatalysis(ph-C S) and concentrated solar photocatalysis(ph-C CS) processes. The results show that the disinfection efficiencies of the solar photolysis(ph-L S) and concentrated solar photolysis(ph-L CS) processes after 30 min were about 10.5% and 68.9%, respectively, and that the ph-C S and ph-C CS processes inactivated 41% and 97% of the heterotrophic bacteria after 30 min, respectively. The p H variation in these processes was negligible. Using the ph-L CS and ph-C CS processes, the synergistic effect between the optical and thermal inactivation caused complete disinfection after three hours. However, disinfection was faster in the ph-C CS process than in the ph-L CS process. Significant correlations were found between the disinfection efficiency and the variation of the dissolved oxygen concentration in the ph-C S and ph-C CS processes, while the correlations between the disinfection efficiency and temperature variation were not significant in the ph-L S and ph-C S processes. Moreover, the oxygen consumption rate was greatest(3.2 mg··L^(-1)) in the ph-C CS process. Hence,it could be concluded that the ph-C CS process is an efficient photocatalysis process for disinfection of dairy wastewater effluent.展开更多
Semiconductor-based photocatalytic and photoelectrochemical(PEC) processes can convert solar energy into high-density chemical energy or for the treatment of environmental pollutants, which are ideal ways to deal with...Semiconductor-based photocatalytic and photoelectrochemical(PEC) processes can convert solar energy into high-density chemical energy or for the treatment of environmental pollutants, which are ideal ways to deal with environmental and energy crises. The development of high-efficiency photocatalysts and photoelectrodes is the key to the in-depth development and practical application of the two technologies.Black phosphorus(BP) has excellent physicalcochemical properties such as adjustable band gap, high carrier mobility, large specific surface area and anisotropy, making it one of the most promising catalysts.BP-based heterostructure can not only realize the effective separation of photogenerated carriers but also improve the stability of BP, and is widely used in photocatalytic and PEC reactions. In this review, we first introduce the crystal structure, band structure, anisotropy, and preparation of BP with different dimensions(bulk, zero-dimension and two-dimension). Then, according to the transfer path of the photogenerated carriers and the components, the BP-based heterostructures are divided into type I heterojunction, type II heterojunction, Z-scheme heterojunction, S-scheme heterojunction, BP/carbonbased material heterostructure, BP/metal heterostructure and multi-component heterostructure.Highlighted are the diverse photocatalytic applications of BP-based heterostructure, such as water splitting and CO_(2)reduction, N_(2)fixation, pollutant degradation, photothermal and photodynamic therapy.Finally, some concluding views and opinions are stated on the challenges and opportunities faced by the further development of BP-based heterostructures in photocatalysis and PEC water splitting.展开更多
The effects of Humic Acid (HA) concentration,pH value and aeration on the photocatalysis degradation of HA by the silica gel supported TiO2 were studied.Moreover,the effect of aeration on the generation of hydroxyl ra...The effects of Humic Acid (HA) concentration,pH value and aeration on the photocatalysis degradation of HA by the silica gel supported TiO2 were studied.Moreover,the effect of aeration on the generation of hydroxyl radicals are investigated.The experimental results indicated that the hydroxyl radicals are generated during the photocatalysis process.The generation of hydroxyl radicals is increasing linearly with the reaction time,approximately.Moreover,the generation rate of hydroxyl under the condition of aeration is 1.57 times of that under the condition without aeration,which is the main influent factor on the reaction rate.Therefore,the reaction rate constant with and without aeration is 0.012 min-1 and 0.0063 min-1,respectively.The degradation rate decreases when the initial HA concentration increases,which is due to that more TiO2 active sites are occupied by HA when the HA concentration is higher.Moreover,HA can absorb large amount of photons,which can prevent those available photons to arrive at the activate TiO2 particles.The degradation rate decreases when increasing pH value,which is due to that the adsorption of HA on the TiO2 particles is weakened and not benefit for the degradation process of HA.展开更多
A new zinc coordination polymer(CP) {[Zn1.5(ttb)0.5(phen)(H2O)]·2 H2O}n(1),(H6ttb = 3,4,5-tricarboxyl-(3',4',5'-tricarboxylazophenyl)benzene, phen = 1,10-phenanthroline), has been hydrothermally synth...A new zinc coordination polymer(CP) {[Zn1.5(ttb)0.5(phen)(H2O)]·2 H2O}n(1),(H6ttb = 3,4,5-tricarboxyl-(3',4',5'-tricarboxylazophenyl)benzene, phen = 1,10-phenanthroline), has been hydrothermally synthesized and structurally characterized by single-crystal X-ray determination, IR and thermogravimetric analysis(TGA). CP 1 crystallizes in the monoclinic system, space group C2/c with a = 12.402(3), b = 15.231(3), c = 22.233(4)A, β = 94.388(3)°, Zn1.5C21H16N3O9, Mr = 552.42, V = 4187.3(15) A^3, Dc = 1.753 g/cm^3, F(000) = 2240, μ = 1.795 mm^-1, S = 1.041, GOF = 1.041, Rint = 0.0169, 2.36°<θ<30.95°, and Z = 8. The final refinement gave R = 0.0340 and w R = 0.0927 for 5791 observed reflections with I > 2σ(I). The completely deprotonated(ttb)^6- ion in 1 adopts an octadentate coordination mode(μ8-η^2-η^1-η^1-η^1-η^1-η^2). Four of the carboxyl groups are coordinated with four zinc ions by monodentate, respectively. While the other two carboxyl groups are coordinated with four zinc ions by bidentate, respectively. So, CP 1 possesses a 3 D network structure cross-linked by(ttb)6-ion. The XRD, UV and photoluminescence properties of CP 1 were also studied. Remarkably, 1 exhibits photocatalytic activities for the degradation of dye(MO) under UV light irradiation and shows good stabilities towards UV-light photocatalysis.展开更多
Bi_2WO_6 was modified by two-dimensional g-C_3N_4(2D g-C_3N_4)via a hydrothermal method.The structure,morphology,optical and electronic properties were investigated by multiple techniques,including X-ray diffraction(X...Bi_2WO_6 was modified by two-dimensional g-C_3N_4(2D g-C_3N_4)via a hydrothermal method.The structure,morphology,optical and electronic properties were investigated by multiple techniques,including X-ray diffraction(XRD),X-ray photoelectron spectroscopy spectra(XPS),Fourier transform infrared spectroscopy(FT-IR),scanning electron microscopy(SEM),transmission electron microscopy(TEM),Ultravioletvisible diffuse reflection spectroscopy(DRS),photocurrent and electrochemical impedance spectroscopy(EIS),electron spin resonance(ESR),respectively.Rhodamine B(Rh B)was used as the target organic pollutant to research the photocatalytic performance of as-prepared composites.The Bi_2WO_6/2D g-C_3N_4exhibited a remarkable improvement compared with the pure Bi_2WO_6.The enhanced photocatalytic activity was because the photogenerated electrons and holes can quickly separate by Z-Scheme passageway in composites.The photocatalytic mechanism was also researched in detail through ESR analysis.展开更多
基金supported primarily by the National Natural Science Foundation of China(Contract No.21975245,51972300,62274155,and U20A20206)the National Key Research and Development Program of China(Grant No.2018YFE0204000)+2 种基金the Strategic Priority Research Program of the Chinese Academy of Sciences(Grant No.XDB43000000)the National Natural Science Foundation of China under Grant No.62175231.Prof.Kong Liu appreciates the support from the Youth Innovation Promotion Association,the Chinese Academy of Sciences(No.2020114)the Beijing Nova Program(No.2020117).
文摘Graphitic carbon nitride(g-C_(3)N_(4))has been extensively doped with alkali metals to enlarge photocatalytic output,in which cesium(Cs)doping is predicted to be the most efficient.Nevertheless,the sluggish diffusion and doping kinetics of precursors with high melting points,along with imprecise regulation,have raised the debate on whether Cs doping could make sense.For this matter,we attempt to confirm the positive effects of Cs doping on multifunctional photocatalysis by first using cesium acetate with the character of easy manipulation.The optimized Csdoped g-C_(3)N_(4)(CCN)shows a 41.6-fold increase in visible-light-driven hydrogen evolution reaction(HER)compared to pure g-C_(3)N_(4) and impressive degradation capability,especially with 77%refractory tetracycline and almost 100%rhodamine B degradedwithin an hour.The penetration ofCs+is demonstrated to be a mode of interlayer doping,and Cs–N bonds(especially with sp^(2) pyridine N in C═N–C),along with robust chemical interaction and electron exchange,are fabricated.This atomic configuration triggers the broadened spectral response,the improved charge migration,and the activated photocatalytic capacity.Furthermore,we evaluate the CCN/cadmium sulfide hybrid as a Z-scheme configuration,promoting the visible HER yield to 9.02 mmol g^(−1) h^(−1),which is the highest ever reported among all CCN systems.This work adds to the rapidly expanding field of manipulation strategies and supports further development of mediating served for photocatalysis.
基金The authors are grateful for financial support from the National Key Projects for Fundamental Research and Development of China(2021YFA1500803)the National Natural Science Foundation of China(51825205,52120105002,22102202,22088102,U22A20391)+1 种基金the DNL Cooperation Fund,CAS(DNL202016)the CAS Project for Young Scientists in Basic Research(YSBR-004).
文摘Photocatalysis,a critical strategy for harvesting sunlight to address energy demand and environmental concerns,is underpinned by the discovery of high-performance photocatalysts,thereby how to design photocatalysts is now generating widespread interest in boosting the conversion effi-ciency of solar energy.In the past decade,computational technologies and theoretical simulations have led to a major leap in the development of high-throughput computational screening strategies for novel high-efficiency photocatalysts.In this viewpoint,we started with introducing the challenges of photocatalysis from the view of experimental practice,especially the inefficiency of the traditional“trial and error”method.Sub-sequently,a cross-sectional comparison between experimental and high-throughput computational screening for photocatalysis is presented and discussed in detail.On the basis of the current experimental progress in photocatalysis,we also exemplified the various challenges associated with high-throughput computational screening strategies.Finally,we offered a preferred high-throughput computational screening procedure for pho-tocatalysts from an experimental practice perspective(model construction and screening,standardized experiments,assessment and revision),with the aim of a better correlation of high-throughput simulations and experimental practices,motivating to search for better descriptors.
基金the National Natural Science Foundation of China (22209091)the Natural Science Foundation of Shandong Province (ZR2020QB057)+1 种基金the Key Program of National Natural Science Foundation of China (22133006)the Yankuang Group 2019 Science and Technology Program (YKKJ2019AJ05JG-R60)。
文摘It is a challenge to coordinate carrier-kinetics performance and the redox capacity of photogenerated charges synchronously at the atomic level for boosting photocatalytic activity.Herein,the atomic Ni was introduced into the lattice of hexagonal ZnIn_(2)S_(4) nanosheets(Ni/ZnIn_(2)S_(4))via directionalsubstituting Zn atom with the facile hydrothermal method.The electronic structure calculations indicate that the introduction of Ni atom effectively extracts more electrons and acts as active site for subsequent reduction reaction.Besides the optimized light absorption range,the elevation of Efand ECBendows Ni/ZnIn_(2)S_(4) photocatalyst with the increased electron concentration and the enhanced reduction ability for surface reaction.Moreover,ultrafast transient absorption spectroscopy,as well as a series of electrochemical tests,demonstrates that Ni/ZnIn_(2)S_(4) possesses 2.15 times longer lifetime of the excited charge carriers and an order of magnitude increase for carrier mobility and separation efficiency compared with pristine ZnIn_(2)S_(4).These efficient kinetics performances of charge carriers and enhanced redox capacity synergistically boost photocatalytic activity,in which a 3-times higher conversion efficiency of nitrobenzene reduction was achieved upon Ni/ZnIn_(2)S_(4).Our study not only provides in-depth insights into the effect of atomic directional-substitution on the kinetic behavior of photogenerated charges,but also opens an avenue to the synchronous optimization of redox capacity and carrier-kinetics performance for efficient solar energy conversion.
基金supported by the National Natural Science Foundation of China(21875118,22111530112)the support from the Smart Sensing Interdisciplinary Science Center,Nankai University。
文摘Photocatalysis driven by abundant yet intermittent solar energy has considerable potential in renewable energy generation and environmental remediation.The outstanding electronic structure and physicochemical properties of graphitic carbon nitride(g-C_(3)N_(4)),together with unique metal-free characteristic,make them ideal candidates for advanced photocatalysts construction.This review summarizes the up-to-date advances on g-C_(3)N_(4)based photocatalysts from ingenious-design strategies and diversified photocatalytic applications.Notably,the advantages,fabrication methods and limitations of each design strategy are systemically analyzed.In order to deeply comprehend the inner connection of theory–structure–performance upon g-C_(3)N_(4)based photocatalysts,structure/composition designs,corresponding photocatalytic activities and reaction mechanisms are jointly discussed,associated with introducing their photocatalytic applications toward water splitting,carbon dioxide/nitrogen reduction and pollutants degradation,etc.Finally,the current challenges and future perspectives for g-C_(3)N_(4)based materials for photocatalysis are briefly proposed.These design strategies and limitations are also instructive for constructing g-C_(3)N_(4) based materials in other energy and environment-related applications.
基金the National Natural Science Foundation of China(22102126)the Natural Science Foundation of Hubei Province(2020CFB124)+2 种基金the Key Laboratory of Hubei Province for Coal Conversion and New Carbon Materials(Wuhan University of Science and Technology)the Hubei Provincial Department of Education for the"Chutian Scholar"programthe support of the"CUG Scholar"Scientific Research Funds at China University of Geosciences(Wuhan)(Project No.2022187)。
文摘The bulk/surface states of semiconductor photocatalysts are imperative parameters to maneuver their performance by significantly affecting the key processes of photocatalysis including light absorption,separation of charge carrier,and surface site reaction.Recent years have witnessed the encouraging progress of self-adaptive bulk/surface engineered Bi_(x)O_(y)Br_(z) for photocatalytic applications spanning various fields.However,despite the maturity of current research,the interaction between the bulk/surface state and the performance of Bi_(x)O_(y)Br_(z) has not yet been fully understood and highlighted.In this regard,a timely tutorial overview is quite urgent to summarize the most recent key progress and outline developing obstacles in this exciting area.Herein,the structural characteristics and fundamental principles of Bi_(x)O_(y)Br_(z)for driving photocatalytic reaction as well as related key issues are firstly reviewed.Then,we for the first time summarized different self-adaptive engineering processes over Bi_(x)O_(y)Br_(z)followed by a classification of the generation approaches towards diverse Bi_(x)O_(y)Br_(z)materials.The features of different strategies,the up-to-date characterization techniques to detect bulk/surface states,and the effect of bulk/surface states on improving the photoactivity of Bi_(x)O_(y)Br_(z)in expanded applications are further discussed.Finally,the present research status,challenges,and future research opportunities of self-adaptive bulk/surface engineered Bi_(x)O_(y)Br_(z)are prospected.It is anticipated that this critical review can trigger deeper investigations and attract upcoming innovative ideas on the rational design of Bi_(x)O_(y)Br_(z)-based photocatalysts.
基金supported by Huazhong University of Science and Technology(No.2021XXJS036,3004013134)National Natural Science Foundation of China(No.51903099,82002879,22102059)+2 种基金the Innovation and Talent Recruitment Base of New Energy Chemistry and Device(No.B21003)China Postdoctoral Science Foundation(2021M692475,2021T140524,XJ2021037)support from the 100 Talents Program of the Hubei Provincial Government。
文摘We report a new facile light-induced strategy to disperse micron-sized aggregated bulk covalent organic frameworks(COFs)into isolated COFs nanoparticles.This was achieved by a series of metal-coordinated COFs,namely COF-909-Cu,-Co or-Fe,where for the first time the diffusio-phoretic propulsion was utilized to design COF-based micro/nanomotors.The mechanism studies revealed that the metal ions decorated in the COF-909 backbone could promote the separation of electron and holes and trigger the production of sufficient ionic and reactive oxygen species under visible light irradiation.In this way,strong light-induced self-diffusiophoretic effect is achieved,resulting in good dispersion of COFs.Among them,COF-909-Fe showed the highest dispersion performance,along with a drastic decrease in particle size from 5μm to500 nm,within only 30 min light irradiation,which is inaccessible by using traditional magnetic stirring or ultrasonication methods.More importantly,benefiting from the outstanding dispersion efficiency,COF-909-Fe micro/nanomotors were demonstrated to be efficient in photocatalytic degradation of tetracycline,about 8 times faster than using traditional magnetic stirring method.This work opens up a new avenue to prepare isolated nanosized COFs in a high-fast,simple,and green manner.
基金supported by the Research and Development Institute at Nakhon Si Thammarat Rajabhat University and the Nanomaterials Chemistry Research Unit at Nakhon Si Thammarat Rajabhat University,Nakhon Si Thammarat,Thailand(Grant No.004/2563).
文摘In this paper, we present a proof-of-concept study of the enhancement of photocatalytic activity via a combined strategy of fabricating a visible-light responsive ternary heterostructure and improving overall photostability by incorporating magnetic zinc oxide/graphene/iron oxide (ZGF). A solvothermal approach was used to synthesize the catalyst. X-ray diffraction (XRD), scanning electron microscopic, energy dispersive X-ray, transmission electron microscopic, vibrating sample magnetometric, and ultraviolet–visible diffuse reflectance spectroscopic techniques were used to characterize the synthesized samples. The obtained optimal Zn(NO_(3))_(2) concentration, temperature, and heating duration were 0.10 mol/L, 600℃, and 1 h, respectively. The XRD pattern revealed the presence of peaks corresponding to zinc oxide, graphene, and iron oxide, indicating that the ZGF catalyst was effectively synthesized. Furthermore, when the developed ZGF was used for methylene blue dye degradation, the optimum irradiation time, dye concentration, catalyst dosage, irradiation intensity, and solution pH were 90 min, 10 mg/L, 0.03 g/L, 100 W, and 8.0, respectively. Therefore, the synthesized ZGF system could be used as a catalyst to degrade dyes in wastewater samples. This hybrid nanocomposite consisting of zinc oxide, graphene, and iron oxide could also be used as an effective photocatalytic degrader for various dye pollutants.
文摘This present study comes in addition to overcome the problems of separation of fine particles of TiO<sub>2</sub> in heterogeneous photocatalysis after treatment. It aims to show the potential for using titaniferous sand as a new semiconductor under solar irradiation. The photocatalytic efficiency of this titaniferous sand was tested on a pesticide (Azadirachtin). A tubular photocatalytic reactor with recirculation of the polluting solution was designed for the elimination of the pesticide in an aqueous solution. Before its use as a photocatalyst, the titaniferous sand has undergone a specific treatment that consists of calcination at 600℃ followed by extraction of the calcined natural organic materials, which can interfere with the measurement of analytical parameters such as COD. The titaniferous sand was also characterized by X-ray fluorescence spectroscopy (XRF). XRF analyses have shown that TiO<sub>2</sub> is predominant in the titaniferous sand with a percentage that has been estimated at 46.34%. The influence of various experimental parameters such as the flow rate of the polluting solution, the concentration of titaniferous sand, the presence of oxygen and the intensity of the overall rate of sunshine, was studied to optimize the photocatalytic degradation of the pesticide. The results showed that the highest removal rate (70%) was observed under the following conditions: a pH of 6, a titaniferous sand concentration of 150 g/L, a flow rate of 0.3 mL/min, and a sunshine rate of 354 W/m<sup>2</sup> and in the presence of atmospheric oxygen. Under these experimental conditions, the rate of photodegradation of the pesticide follows the pseudo first order kinetic model of Langmuir Hinshelwood with a coefficient of determination R<sup>2</sup> of 0.9869 and an apparent rate constant of 0.0029 min<sup>-1</sup>. The results clearly demonstrated the potential of titaniferous sand as a photocatalyst sensitive to sunlight for the effective removal of pesticides in the aquatic environment.
基金supported by the National Natural Science Foundation of China(No.11574111 and No.11974129 to X.-F.W.)“the Fundamental Research Funds for the Central Universities.”.
文摘Since their seminal discovery in 2011,two-dimensional(2D)transition metal carbides/nitrides known as MXenes,that constitute a large family of 2D materials,have been targeted toward various applications due to their outstanding electronic properties.MXenes functioning as co-catalyst in combination with certain photocatalysts have been applied in photocatalytic systems to enhance photogenerated charge separation,suppress rapid charge recombination,and convert solar energy into chemical energy or use it in the degradation of organic compounds.The photocatalytic performance greatly depends on the composition and morphology of the photocatalyst,which,in turn,are determined by the method of preparation used.Here,we review the four different synthesis methods(mechanical mixing,self-assembly,in situ decoration,and oxidation)reported for MXenes in view of their application as co-catalyst in photocatalysis.In addition,the working mechanism for MXenes application in photocatalysis is discussed and an outlook for future research is also provided.
基金financially supported by the National Natural Science Foundation (No.52072347, 51972288, 51672258 and 51572246)the Fundamental Research Funds for the Central Universities (No. 2652019144 and 2652018287)+1 种基金the financial supports from the Science and Technology Program of Guangdong Province (2019A050510012)Shenzhen Science, Technology and Innovation Commission (SGDX2019081623240364).
文摘g-C_(3)N_(4) emerges as a star 2D photocatalyst due to its unique layered structure,suitable band structure and low cost.However,its photocatalytic application is limited by the fast charge recombination and low photoabsorption.Rationally designing g-C_(3)N_(4)-based heterojunction is promising for improving photocatalytic activity.Besides,g-C_(3)N_(4) exhibits great potentials in electrochemical energy storage.In view of the excellent performance of typical transition metal oxides(TMOs)in photocatalysis and energy storage,this review summarized the advances of TMOs/g-C_(3)N_(4) heterojunctions in the above two areas.Firstly,we introduce several typical TMOs based on their crystal structures and band structures.Then,we summarize different kinds of TMOs/g-C_(3)N_(4) heterojunctions,including type Ⅰ/Ⅱ heterojunction,Z-scheme,p-n junction and Schottky junction,with diverse photocatalytic applications(pollutant degradation,water splitting,CO_(2) reduction and N_(2) fixation)and supercapacitive energy storage.Finally,some promising strategies for improving the performance of TMOs/g-C_(3)N_(4) were proposed.Particularly,the exploration of photocatalysis-assisted supercapacitors was discussed.
基金supported by the National Key R&D Project from Minister of Science and Technology in China(No.2016YFA0202701,No.2018YFB2200500)the National Natural Science Foundation of China(No.52072041,No.61604012,No.61974170)the University of Chinese Academy of Sciences(Grant No.Y8540XX2D2)。
文摘Photocatalysis and electrocatalysis have been essential parts of electrochemical processes for over half a century.Recent progress in the controllable synthesis of 2D nanomaterials has exhibited enhanced catalytic performance compared to bulk materials.This has led to significant interest in the exploitation of 2D nanomaterials for catalysis.There have been a variety of excellent reviews on 2D nanomaterials for catalysis,but related issues of differences and similarities between photocatalysis and electrocatalysis in 2D nanomaterials are still vacant.Here,we provide a comprehensive overview on the differences and similarities of photocatalysis and electrocatalysis in the latest 2D nanomaterials.Strategies and traps for performance enhancement of 2D nanocatalysts are highlighted,which point out the differences and similarities of series issues for photocatalysis and electrocatalysis.In addition,2D nanocatalysts and their catalytic applications are discussed.Finally,opportunities,challenges and development directions for 2D nanocatalysts are described.The intention of this review is to inspire and direct interest in this research realm for the creation of future 2D nanomaterials for photocatalysis and electrocatalysis.
基金financial support from the key project of the National Natural Science Foundation of China (U1463204)the project of National Natural Science Foundation of China (NSFC) (20903023,21173045)+4 种基金the Award Program for Minjiang Scholar Professorshipthe Natural Science Foundation (NSF) of Fujian Province for Distinguished Young Investigator Grant (2012J06003)the Independent Research Project of State Key Laboratory of Photocatalysis on Energy and Environment (No.2014A05)the 1st Program of Fujian Province for Top Creative Young Talentsthe Program for Returned High-Level Overseas Chinese Scholars of Fujian Province
文摘As a new member of carbon material family, carbon quantum dots(CQDs) have attracted tremendous attentions for their potentials in the heterogeneous photocatalysis applications. Due to the unique microstructure and optical properties, the roles of CQDs played in the CQDs-based photocatalytic systems have been found to be diverse with the continuous researches in this regard. Herein, we provide a concise minireview to elaborate the multifarious roles of CQDs in photocatalysis, including photoelectron mediator and acceptor, photosensitizer, photocatalyst, reducing agent for metal salt, enhancing adsorption capacity and spectral converter. In addition, the perspectives on future research trends and challenges are proposed, which are anticipated to stimulate further research into this promising field on designing a variety of efficient CQDs-based photocatalysts for solar energy conversion.
基金financially supported by National Nature Science Foundation of China(Grant No.51402247 and 41630646)Sichuan Province Education Department Innovation Team Foundation(16zd1104)+2 种基金Sichuan Province Science Foundation for Young Scientists(No.15zs2111)Open Project of State Key Laboratory Cultivation Base for Nonmetal Composites and Functional Materials(No.13zxfk11)Doctoral Research Foundation of Southwest University of Science and Technology(No.14zx7119)
文摘To improve the visible light absorption and photocatalytic activity of titanium dioxide nanotube arrays(TONTAs), ZnFe_2O_4(ZFO) nanocrystals were perfused into pristine TONTA pipelines using a novel bias voltageassisted perfusion method. ZFO nanocrystals were well anchored on the inner walls of the pristine TONTAs when the ZFO suspensions(0.025 mg m L^(-1)) were kept under a60 V bias voltage for 1 h. After annealing at 750 °C for2 h, the heterostructured ZFO/Fe_2 TiO_5(FTO)/TiO_2 composite nanotube arrays were successfully obtained. Furthermore, Fe^(3+)was reduced to Fe^(2+)when solid solution reactions occurred at the interface of ZFO and the pristine TONTAs. Introducing ZFO significantly enhanced thevisible light absorption of the ZFO/FTO/TONTAs relative to that of the annealed TONTAs. The coexistence of type I and staggered type II band alignment in the ZFO/FTO/TONTAs facilitated the separation of photogenerated electrons and holes, thereby improving the efficiency of the ZFO/FTO/TONTAs for photocatalytic degradation of methylene blue when irradiated with simulated sunlight.
基金the National Natural Science Foundation of China(Nos.51722404,51674177,51804221,and 91845113)the National Key R&D Program of China(No.2018YFE0201703)+2 种基金the China Postdoctoral Science Foundation(Nos.2018M642906 and 2019T120684)the Fundamental Research Funds for the Central Universities(No.2042019kf0230)the Hubei Provincial Natural Science Foundation of China(No.2019CFA065)。
文摘Pyrolysis of the Ta_(2)_(O5)/melamine mixture in molten chlorides is herein demonstrated as a facile and controllable method to nitridize and functionalize Ta_(2)_(O5).The influence of the stoichiometry and composition of Ta_(2)_(O5)/melamine in molten salts on the nitridation process is rationalized to ensure the controllable preparation of Ta_(3)N_(5) and Ta_(3)N_(5)/TaON.The characterization results,including scanning electron microscopy,transmission electron microscopy,elemental mapping,X-ray photoelectron spectroscopy,and photoluminescence spectroscopy,all confirm the existence of the Ta_(3)N_(5)/TaON heterojunction,in which the TaON nanoparticles are closely anchored to the Ta_(3)N_(5) nanorods.Benefiting from its composition and structure,the Ta_(3)N_(5)/TaON composites show enhanced photocatalytic activity for the degradation of methylene blue.The present study highlights that the molten salt method using a solid nitrogen source can be a new technique for rationalizing the design of nitrides and oxynitrides.
基金financially supported by the National Natural Science Foundation of China(21706224,21671075)the China Postdoctoral Science Foundation(2020M672810)+3 种基金the Science and Technology Innovation Commission of Shenzhen Municipality(JCYJ20180307123906004 and JCYJ20190808181003717)the Research Grants Council of Hong Kong(CityU 21301817,11215518)the Strategic Research Grants from City University of Hong Kong(Ref:CityU 11306419 and 11308420)the Applied Research Grant from City University of Hong Kong(Ref:CityU 9667217)。
文摘Porous photocatalysts are promising materials capable of simultaneously adsorbing and oxidizing/reducing target species,showing great potentials in environmental remediation and energy generation.This review offered a comprehensive overview of the recent progress in design,fabrication,and applications of porous photocatalysts,including carbon-based semiconductors,metal oxides/sulfides,metal–organic frameworks,and adsorbent–photocatalyst hybrids.The fundamental understanding of the structure–performance relationships of porous materials together with the in-depth insights into the synergetic effects between adsorption and photocatalysis was presented.The strategies to further improve the photocatalytic activity of porous photocatalysts were proposed.This review would provide references and outlooks of constructing efficient porous materials for adsorptive and photocatalytic removal of pollutants and energy production.
基金supported by the Foundation of the Gonabad University of Medical Sciences,in Gonabad,Iran(Grant No.92131)
文摘Due to the strict regulations and reuse policies that govern wastewater's use as an irrigation water resource for agricultural purposes, especially in dry climates, optimization of the disinfection process is of the utmost importance. The effects of solar radiation along with Titanium dioxide(TiO_2) nanoparticles applied to optimization of the photolysis and photocatalysis processes for inactivating heterotrophic bacteria were investigated. Temperature, p H, and dissolved oxygen fluctuations in the dairy wastewater effluent treated by activated sludge were examined. In addition,different dosages of TiO_2 were tested in the solar photocatalysis(ph-C S) and concentrated solar photocatalysis(ph-C CS) processes. The results show that the disinfection efficiencies of the solar photolysis(ph-L S) and concentrated solar photolysis(ph-L CS) processes after 30 min were about 10.5% and 68.9%, respectively, and that the ph-C S and ph-C CS processes inactivated 41% and 97% of the heterotrophic bacteria after 30 min, respectively. The p H variation in these processes was negligible. Using the ph-L CS and ph-C CS processes, the synergistic effect between the optical and thermal inactivation caused complete disinfection after three hours. However, disinfection was faster in the ph-C CS process than in the ph-L CS process. Significant correlations were found between the disinfection efficiency and the variation of the dissolved oxygen concentration in the ph-C S and ph-C CS processes, while the correlations between the disinfection efficiency and temperature variation were not significant in the ph-L S and ph-C S processes. Moreover, the oxygen consumption rate was greatest(3.2 mg··L^(-1)) in the ph-C CS process. Hence,it could be concluded that the ph-C CS process is an efficient photocatalysis process for disinfection of dairy wastewater effluent.
基金jointly supported by the National Natural Science Foundation of China(51972288 and 51672258)the Fundamental Research Funds for the Central Universities(2652018287)。
文摘Semiconductor-based photocatalytic and photoelectrochemical(PEC) processes can convert solar energy into high-density chemical energy or for the treatment of environmental pollutants, which are ideal ways to deal with environmental and energy crises. The development of high-efficiency photocatalysts and photoelectrodes is the key to the in-depth development and practical application of the two technologies.Black phosphorus(BP) has excellent physicalcochemical properties such as adjustable band gap, high carrier mobility, large specific surface area and anisotropy, making it one of the most promising catalysts.BP-based heterostructure can not only realize the effective separation of photogenerated carriers but also improve the stability of BP, and is widely used in photocatalytic and PEC reactions. In this review, we first introduce the crystal structure, band structure, anisotropy, and preparation of BP with different dimensions(bulk, zero-dimension and two-dimension). Then, according to the transfer path of the photogenerated carriers and the components, the BP-based heterostructures are divided into type I heterojunction, type II heterojunction, Z-scheme heterojunction, S-scheme heterojunction, BP/carbonbased material heterostructure, BP/metal heterostructure and multi-component heterostructure.Highlighted are the diverse photocatalytic applications of BP-based heterostructure, such as water splitting and CO_(2)reduction, N_(2)fixation, pollutant degradation, photothermal and photodynamic therapy.Finally, some concluding views and opinions are stated on the challenges and opportunities faced by the further development of BP-based heterostructures in photocatalysis and PEC water splitting.
基金Sponsored by the Fundamental Research Funds for the Central Universities (Grant No. 2009BO1614)the Ministry of Water Resources' Special Funds for Scientific Research on Public Causes(Grant No. 201101052)the Natural Found of Hohai University(Grant No. 2009423311)
文摘The effects of Humic Acid (HA) concentration,pH value and aeration on the photocatalysis degradation of HA by the silica gel supported TiO2 were studied.Moreover,the effect of aeration on the generation of hydroxyl radicals are investigated.The experimental results indicated that the hydroxyl radicals are generated during the photocatalysis process.The generation of hydroxyl radicals is increasing linearly with the reaction time,approximately.Moreover,the generation rate of hydroxyl under the condition of aeration is 1.57 times of that under the condition without aeration,which is the main influent factor on the reaction rate.Therefore,the reaction rate constant with and without aeration is 0.012 min-1 and 0.0063 min-1,respectively.The degradation rate decreases when the initial HA concentration increases,which is due to that more TiO2 active sites are occupied by HA when the HA concentration is higher.Moreover,HA can absorb large amount of photons,which can prevent those available photons to arrive at the activate TiO2 particles.The degradation rate decreases when increasing pH value,which is due to that the adsorption of HA on the TiO2 particles is weakened and not benefit for the degradation process of HA.
基金Supported by the National Natural Science Foundation of China(No.21763028)Scientific Research Program Project of Yan’an University(No.YDY2017-07)+2 种基金Key Project of Natural Science of Shaanxi Provincial Education Department(No.16JS121)the Natural Science Foundation of Yan’an(2018KN-22)Yan’an University Training Program for Innovation and Entrepreneurship(No.D2018017)
文摘A new zinc coordination polymer(CP) {[Zn1.5(ttb)0.5(phen)(H2O)]·2 H2O}n(1),(H6ttb = 3,4,5-tricarboxyl-(3',4',5'-tricarboxylazophenyl)benzene, phen = 1,10-phenanthroline), has been hydrothermally synthesized and structurally characterized by single-crystal X-ray determination, IR and thermogravimetric analysis(TGA). CP 1 crystallizes in the monoclinic system, space group C2/c with a = 12.402(3), b = 15.231(3), c = 22.233(4)A, β = 94.388(3)°, Zn1.5C21H16N3O9, Mr = 552.42, V = 4187.3(15) A^3, Dc = 1.753 g/cm^3, F(000) = 2240, μ = 1.795 mm^-1, S = 1.041, GOF = 1.041, Rint = 0.0169, 2.36°<θ<30.95°, and Z = 8. The final refinement gave R = 0.0340 and w R = 0.0927 for 5791 observed reflections with I > 2σ(I). The completely deprotonated(ttb)^6- ion in 1 adopts an octadentate coordination mode(μ8-η^2-η^1-η^1-η^1-η^1-η^2). Four of the carboxyl groups are coordinated with four zinc ions by monodentate, respectively. While the other two carboxyl groups are coordinated with four zinc ions by bidentate, respectively. So, CP 1 possesses a 3 D network structure cross-linked by(ttb)6-ion. The XRD, UV and photoluminescence properties of CP 1 were also studied. Remarkably, 1 exhibits photocatalytic activities for the degradation of dye(MO) under UV light irradiation and shows good stabilities towards UV-light photocatalysis.
基金supported by National Nature Science Foundation of China (21476097, 21776118)Six talent peaks project in Jiangsu Province (2014-JNHB-014)Project Funded by the Priority Academic Program Development of Jiangsu Higher Education Institutions
文摘Bi_2WO_6 was modified by two-dimensional g-C_3N_4(2D g-C_3N_4)via a hydrothermal method.The structure,morphology,optical and electronic properties were investigated by multiple techniques,including X-ray diffraction(XRD),X-ray photoelectron spectroscopy spectra(XPS),Fourier transform infrared spectroscopy(FT-IR),scanning electron microscopy(SEM),transmission electron microscopy(TEM),Ultravioletvisible diffuse reflection spectroscopy(DRS),photocurrent and electrochemical impedance spectroscopy(EIS),electron spin resonance(ESR),respectively.Rhodamine B(Rh B)was used as the target organic pollutant to research the photocatalytic performance of as-prepared composites.The Bi_2WO_6/2D g-C_3N_4exhibited a remarkable improvement compared with the pure Bi_2WO_6.The enhanced photocatalytic activity was because the photogenerated electrons and holes can quickly separate by Z-Scheme passageway in composites.The photocatalytic mechanism was also researched in detail through ESR analysis.
