Photocatalytic water splitting is beneficial for the effective mitigation of global energy and environmental crises.Owing to multi-exciton generation,impressive light harvesting,and excellent photochemical properties,...Photocatalytic water splitting is beneficial for the effective mitigation of global energy and environmental crises.Owing to multi-exciton generation,impressive light harvesting,and excellent photochemical properties,the quantum dot(QD)-based catalysts reveal a considerable potential in photocatalytic hydrogen(H_(2))production compared with bulk competitors.In this review,we summarize the recent advances in QDs for photocatalytic H_(2) production by enumerating different synthetic and characterization strategies for QDs.Various QDs-based photocatalysts are introduced and summarized in categories,and the role of different QDs in varied systems,as well as the mechanism and key factors that enhance the photocatalytic H_(2) generation performance,is discussed.Finally,conclusions and future perspectives in the exploration of highly efficient QDs-based photocatalysts for innovative applications are highlighted.展开更多
Plasmonic nonmetal semiconductors with localized surface plasmon resonance(LSPR)effects possess extended light-response ranges and can act as highly efficient H2 generation photocatalysts.Herein,an LSPR-enhanced 0D/2D...Plasmonic nonmetal semiconductors with localized surface plasmon resonance(LSPR)effects possess extended light-response ranges and can act as highly efficient H2 generation photocatalysts.Herein,an LSPR-enhanced 0D/2D CdS/MoO3‒x heterojunction has been synthesized by the growth of 0D CdS nanoparticles on 2D plasmonic MoO3‒x elliptical nanosheets via a simple coprecipitation method.Taking advantage of the LSPR effect of the MoO3‒x elliptical nanosheets,the light absorption of the CdS/MoO3‒x heterojunction was extended from 600 nm to the near-infrared region(1400 nm).Furthermore,the introduction of 2D plasmonic MoO3‒x elliptical nanosheets not only provided a platform for the growth of CdS nanoparticles,but also contributed to the construction of an LSPR-enhanced S-scheme structure due to the interface between the MoO3‒x and CdS,accelerating the separation of light-induced electrons and holes.Therefore,the CdS/MoO3‒x heterojunction exhibited higher photocatalytic H2 generation activity than pristine CdS under visible light irradiation,including under 420,450,550,and 650 nm monochromic light,as well as improved photo-corrosion performance.展开更多
Silver nanoparticles (Ag NPs) can effectively address the issue of antibiotic-resistant bacterial infections to reduce the potential toxicity of Ag NPs. Although challenging, it is, therefore, necessary to achieve the...Silver nanoparticles (Ag NPs) can effectively address the issue of antibiotic-resistant bacterial infections to reduce the potential toxicity of Ag NPs. Although challenging, it is, therefore, necessary to achieve the sustainable release of Ag+ ions from a finite amount of Ag NPs. This study aims at designing an efficient and benign antimicrobial silver-based ternary composite composed of photocatalysis zinc oxide (ZnO) and reduced graphene oxide (rGO) as a carrier, in which the reactive oxygen species (ROS) excited from ZnO and Ag+ ions released from the Ag NPs cooperate to realize an effective antibacterial activity against E. coli and S. aureus. The constant effective bacterial performance of the ternary photocatalyst with minimum Ag content can be attributed to the increase in the available quantity of ROS, which results from the enhanced separation efficiency of the photogenerated carriers. The proposed system notably realized the long-term sustainable release of Ag+ ions with low concentration for 30 days when compared with an equivalent amount of silver nitrate. Moreover, the use of the composite prevents biotoxicity and silver wastage, and imparts enhanced stability to the long-lasting antibacterial efficacy.展开更多
Extended light absorption and dynamic charge separation are vital factors that determine the effectivenessof photocatalysts.In this study,a nonmetallic plasmonic S‐scheme photocatalyst was fabricatedby loading 1D pla...Extended light absorption and dynamic charge separation are vital factors that determine the effectivenessof photocatalysts.In this study,a nonmetallic plasmonic S‐scheme photocatalyst was fabricatedby loading 1D plasmonic W_(18)O_(49)nanowires onto 2D g‐C_(3)N_(4)nanosheets.W_(18)O_(49)nanowiresplay the dual role of a light absorption antenna—that extends light adsorption—and a hot electrondonor—that assists the water reduction reaction in a wider light spectrum range.Moreover,S‐scheme charge transfer resulting from the matching bandgaps of W_(18)O_(49)and g‐C_(3)N_(4)can lead tostrong redox capability and high migration speed of the photoinduced charges.Consequently,in thisstudy,W_(18)O_(49)/g‐C_(3)N_(4)hybrids exhibited higher photocatalytic H2 generation than that of pristineg‐C_(3)N_(4)under light irradiation of 420–550 nm.Furthermore,the H2 production rate of thebest‐performing W_(18)O_(49)/g‐C_(3)N_(4)hybrid was 41.5μmol·g^(−1)·h^(−1)upon exposure to monochromaticlight at 550 nm,whereas pure g‐C_(3)N_(4)showed negligible activity.This study promotes novel andenvironmentally friendly hot‐electron‐assisted S‐scheme photocatalysts for the broad‐spectrumutilization of solar light.展开更多
Accelerating the separation efficiency of photoexcited electron-hole pairs with the help of highly active co-catalysts has proven to be a promising approach for improving photocatalytic activity. Thus far, the most de...Accelerating the separation efficiency of photoexcited electron-hole pairs with the help of highly active co-catalysts has proven to be a promising approach for improving photocatalytic activity. Thus far, the most developed co-catalysts for semiconductor-based photocatalysis are inorganic materials;the employment of a specific organic molecule as a co-catalyst for photocatalytic hydrogen evolution and pollutant photodegradation is rare and still remains a challenging task. Herein, we report on the use of an organic molecule, oxamide (OA), as a novel co-catalyst to enhance electron- hole separation, photocatalytic H2 evolution, and dye degradation over TiO2 nanosheets. OA-modified TiO2 samples were prepared by a wet chemical route and demonstrated improved light absorption in the visible-light region and more efficient charge transport. The photocatalytic performance of H2 evolution from water splitting and rhodamine B (RhB) degradation for an optimal OA-modified TiO2 photocatalyst reached 2.37 mmol g^–1 h^–1 and 1.43 × 10^-2 min^-1, respectively, which were 2.4 and 3.8 times higher than those of pristine TiO2, respectively. A possible mechanism is proposed, in which the specific π-conjugated structure of OA is suggested to play a key role in the enhancement of the charge transfer and catalytic capability of TiO2. This work may provide advanced insight into the development of a variety of metal-free organic molecules as functional co-catalysts for improved solar-to-fuel conversion and environmental remediation.展开更多
Construction of multi-channels of photo-carrier migration in photocatalysts is favor to boost conversion efficiency of solar energy by promoting the charge separation and transfer.Herein,a ternary ZnIn_(2)S_(4)/g-C_(3...Construction of multi-channels of photo-carrier migration in photocatalysts is favor to boost conversion efficiency of solar energy by promoting the charge separation and transfer.Herein,a ternary ZnIn_(2)S_(4)/g-C_(3)N_(4)/Ti_(3)C_(2) MXene hybrid composed of S-scheme junction integrated Schottky-junction was fabricated using a simple hydrothermal approach.All the components(g-C_(3)N_(4),ZnIn_(2)S_(4) and Ti_(3)C_(2) MXene)demonstrated two-dimensional(2D)nanosheets structure,leading to the formation of a 2D/2D/2D sandwich-like structure with intimate large interface for carrier migration.Furthermore,the photogenerated carriers on the g-C_(3)N_(4) possessed dual transfer channels,including one route in S-scheme transfer mode between the g-C_(3)N_(4) and ZnIn_(2)S_(4) and the other route in Schottky-junction between g-C_(3)N_(4) and Ti_(3)C_(2) MXene.Consequently,a highly efficient carrier separation and transport was realized in the ZnIn_(2)S_(4)/g-C_(3)N_(4)/Ti_(3)C_(2) MXene heterojunction.This ternary sample exhibited wide light response from 200 to 1400 nm and excellent photocatalytic H_(2) evolution of 2452.1μmol∙g^(–1)∙h^(–1),which was 200,3,1.5 and 1.6 times of g-C_(3)N_(4),ZnIn_(2)S_(4),ZnIn_(2)S_(4)/Ti_(3)C_(2) MXene and g-C_(3)N_(4)/ZnIn_(2)S_(4) binary composites.This work offers a paradigm for the rational construction of multi-electron pathways to regulate the charge separation and migration via the introduction of dual-junctions in catalytic system.展开更多
Graphitic carbon nitride(g-C3N4)-based photocatalysts have shown great potential in the splitting of water.However,the intrinsic drawbacks of g-C3N4,such as low surface area,poor diffusion,and charge separation effici...Graphitic carbon nitride(g-C3N4)-based photocatalysts have shown great potential in the splitting of water.However,the intrinsic drawbacks of g-C3N4,such as low surface area,poor diffusion,and charge separation efficiency,remain as the bottleneck to achieve highly efficient hydrogen evolution.Here,a hollow oxygen-incorporated g-C3N4 nanosheet(OCN)with an improved surface area of 148.5 m2 g^−1 is fabricated by the multiple thermal treatments under the N2/O2 atmosphere,wherein the C–O bonds are formed through two ways of physical adsorption and doping.The physical characterization and theoretical calculation indicate that the O-adsorption can promote the generation of defects,leading to the formation of hollow morphology,while the O-doping results in reduced band gap of g-C3N4.The optimized OCN shows an excellent photocatalytic hydrogen evolution activity of 3519.6μmol g^−1 h^−1 for~20 h,which is over four times higher than that of g-C3N4(850.1μmol g^−1 h^−1)and outperforms most of the reported g-C3N4 catalysts.展开更多
Durable and inexpensive graphitic carbon nitride(g-C_(3)N_(4))demonstrates great potential for achieving efficient photocatalytic hydrogen evolution reduction(HER).To further improve its activity,g-C_(3)N_(4)was subje...Durable and inexpensive graphitic carbon nitride(g-C_(3)N_(4))demonstrates great potential for achieving efficient photocatalytic hydrogen evolution reduction(HER).To further improve its activity,g-C_(3)N_(4)was subjected to atomic-level structural engineering by doping with transition metals(M=Fe,Co,or Ni),which simultaneously induced the formation of metal-N active sites in the g-C_(3)N_(4)framework and modulated the bandgap of g-C_(3)N_(4).Experiments and density functional theory calculations further verified that the as-formed metal-N bonds in M-doped g-C_(3)N_(4)acted as an"electron transfer bridge",where the migration of photo-generated electrons along the bridge enhanced the efficiency of separation of the photogenerated charges,and the optimized bandgap of g-C_(3)N_(4)afforded stronger reduction ability and wider light absorption.As a result,doping with either Fe,Co,or Ni had a positive effect on the HER activity,where Co-doped g-C_(3)N_(4)exhibited the highest performance.The findings illustrate that this atomic-level structural engineering could efficiently improve the HER activity and inspire the design of powerful photocatalysts.展开更多
Graphite‐like carbon nitride(g‐C3N4)‐based compounds have attracted considerable attention because of their excellent photocatalytic performance.In this work,a novel direct Z‐scheme system constructed from two‐di...Graphite‐like carbon nitride(g‐C3N4)‐based compounds have attracted considerable attention because of their excellent photocatalytic performance.In this work,a novel direct Z‐scheme system constructed from two‐dimensional(2D)g‐C3N4nanoplates and zero‐dimensional(0D)MoS2quantum dots(QDs)was prepared through the combination of a hydrothermal process and microemulsion preparation.The morphologies,structures,and optical properties of the as‐prepared photocatalysts were characterized by X‐ray diffraction,X‐ray photoelectron spectroscopy,atomic force microscopy,transmission electron microscopy,and UV‐vis diffuse reflectance spectroscopy.In addition,the photocatalytic performances of the prepared2D/0D hybrid composites were evaluated based on the photodegradation of rhodamine B under visible‐light irradiation.The results demonstrated that the introduction of MoS2QDs to g‐C3N4greatly enhanced the photocatalytic efficiency.For the optimum7%MoS2QD/g‐C3N4photocatalyst,the degradation rate constant was8.8times greater than that of pure g‐C3N4under visible‐light irradiation.Photocurrent and electrochemical impedance spectroscopy results further demonstrated that the MoS2QD/g‐C3N4composites exhibited higher photocurrent density and lower chargetransfer resistance than those of the pure g‐C3N4or MoS2QDs.Active species trapping,terephthalic acid photoluminescence,and nitro blue tetrazolium transformation experiments were performed to investigate the evolution of reactive oxygen species,including hydroxyl radicals and superoxide radicals.The possible enhanced photocatalytic mechanism was attributed to a direct Z‐scheme system,which not only can increase the separation efficiency of photogenerated electron‐hole pairs but also possesses excellent oxidation and reduction ability for high photocatalytic performances.This work provides an effective synthesis approach and insight to help develop other C3N4‐based direct Z‐scheme photocatalytic systems for environmental purification and energy conversion.展开更多
g-C3N4 is a metal-free semiconductor and a potential candidate for photocatalytic H2 production,however,the drawbacks,rapid recombination rate and limited migration efficiency of photogenerated carriers,restrict its p...g-C3N4 is a metal-free semiconductor and a potential candidate for photocatalytic H2 production,however,the drawbacks,rapid recombination rate and limited migration efficiency of photogenerated carriers,restrict its photocatalytic activity.Herein,Co(II)as a hole cocatalyst modified P-doped g-C3N4 were successfully prepared to ameliorate the separation efficiency of photoinduced carriers and enhance the photocatalytic hydrogen production.The photocatalytic results demonstrated that the P-doped g-C3N4(PCN)exhibited higher photocatalytic activity compared with pure g-C3N4,while Co(II)/PCN photocatalyst exhibited further enhancement of photocatalytic performance.The proposed possible mechanism based on various characterizations is that P-doping can modulate the electronic structure of g-C3N4 to boost the separation of photogenerated-e-and h+;while the synergistic effect of both Co(II)(as hole cocatalyst)and Pt(as electron cocatalyst)can not only lead to the directional shunting of photogenerated e+-h?pairs,but further accelerate the photogenerated electrons transfer to Pt in order to join the photocatalytic reduction process for hydrogen evolution.As a result,the transportation and separation of photoinduced carriers were accelerated to greatest extent in the Pt/Co(II)/PCN photocatalyst.展开更多
Aiming to develop a photocatalyst that can simultaneously produce valuable chemicals and clean H_(2) fuel for promoting the utilization efficiency of solar energy,herein,a sea-urchin-like CoP@Ni_(2)P binary nanojuncti...Aiming to develop a photocatalyst that can simultaneously produce valuable chemicals and clean H_(2) fuel for promoting the utilization efficiency of solar energy,herein,a sea-urchin-like CoP@Ni_(2)P binary nanojunction was employed as an efficient photothermal cocatalyst to couple with zero-dimensional CdZnS(CZS)solid solution for achieving superior coordinative redox reaction.The CoP@Ni_(2)P/CZS hybrid displayed a high solar-driven H_(2) generation rate of 40.92 mmol g^(–1) h^(–1) coupling with a benzaldehyde formation rate of 20.33 mmol g^(–1) h^(–1),which was 16.4 and 8.0 times higher than that of bare CZS.Furthermore,the CoP@Ni_(2)P/CZS hybrid also achieved a high photothermal H_(2) production under a broad light range from 420 to 720 nm,and the H_(2) production reached 44.48μmol g^(–1) h^(–1) under the 720 nm light illumination.The enhanced catalytic performance can be ascribed to that the CoP@Ni_(2)P nanojunction with photothermal effect can speed up the separation and transport of carriers,offer more catalytic active sites,and induce an increase in temperature to optimize reaction kinetics.This study may open a facile route to design novel binary metal phosphides with dual functions in photocatalysis for the full exploitation of solar energy.展开更多
Background:Nontraumatic acute abdominal pain(AAP)accounts for a large proportion of emergency department(ED)admissions.This study aimed to explore the underlying correlations among basic information,imaging examinatio...Background:Nontraumatic acute abdominal pain(AAP)accounts for a large proportion of emergency department(ED)admissions.This study aimed to explore the underlying correlations among basic information,imaging examinations,and diagnoses.Methods:A total of 7453 patients complaining of AAP,admitted to the ED of Zhongnan Hospital of Wuhan University,were enrolled in this retrospective study from January 1 to December 30,2019.We collected the following information from the patients:sex,age,date of visit,pain location,nature of pain,level of severity,imaging(computed tomography,x-ray,and ultrasound),diagnosis,and outcomes(re-lease from the hospital,transfer to another hospital,transfer to another department,observation room,hospitalization,or death).Results:According to this study,AAP was more common in female than male.A total of 82.11%patients of AAP were in level 3 of se-verity,while 0.19%patients were in level 1.A total of 77.20%of the patients had undergone imaging.Swelling pain and colic are the 2 most common types of AAP.Nonspecific abdominal pain(NSAP)is the most common diagnosis.In the diagnosis of NSAP and gastroenteritis,female patients were more prevalent than male patients,but for renal colic,male patients were 3 times as many as female patients.Non-specific abdominal pain,biliary colic,and cholecystitis are the 3 leading causes in patients 65 years or older.Nonspecific abdominal pain,renal colic,and gastroenteritis are the 3 leading causes of AAP in patients younger than 65 years.Conclusion:With the help of imaging,clinicians can specify a diagnosis and perform corresponding treatment in most cases.However,making a precise diagnosis of AAP within a short period is still challenging.Further research should be conducted to seek safer and more effective techniques to streamline clinicians’work.展开更多
A simple one-step thermal polymerization method was developed for synthesis of holey graphitic carbon nitride nanotubes,involving direci eating of mixtures of melamine and urea or melamine and cyanuric acid in specifi...A simple one-step thermal polymerization method was developed for synthesis of holey graphitic carbon nitride nanotubes,involving direci eating of mixtures of melamine and urea or melamine and cyanuric acid in specific mass ratios.Supramolecular structures formed betweer the precursor molecules guided nanotube formation.The porous and nanotubular structure of the nanotubes facilitated efficient charge carrier nigration and separation,thereby enhancing photocatalytic Hz production in 20 vol.%lactic acid under visible light irradiation.Nanotubes synthesized using melamine and urea in a 1:10 mass ratio(denoted herein as CN-MU nanotubes)exhibited a photocatalytic hydroger production rate of 1,073.6μmol·h^-1·^-g with Pt as the cocatalyst,a rate of 4.7 and 3.1 times higher than traditional Pt/g-CN4 photocatalysts prepared from graphitic carbon nitride(g-CN4)obtained by direct thermal polymerization of melamine or urea,respectively.On the basis of their outstanding performance for photocatalytic H2 production,it is envisaged that the holey g-C3N4 nanotubes will find widespread uptake in other areas,including photocatalytic CO2 reduction,dye-sensitized solar cells and photoelectrochemical sensors.展开更多
It is still of gigantic challenging to design and to optimize photocatalytic systems with cost-efficiency for photocatalytic hydrogen evolution from water splitting.Herein,noble-metal-free 2D CoP nanosheets were prepa...It is still of gigantic challenging to design and to optimize photocatalytic systems with cost-efficiency for photocatalytic hydrogen evolution from water splitting.Herein,noble-metal-free 2D CoP nanosheets were prepared by a phosphorization method using Co(OH)2 nanosheets as precursors,and then employed as photocatalytic cocatalyst and template to make 0D Ti O2 nanoparticles in-situ grow on the surface for construction of 0D/2D TiO_(2)/CoP hybrid by a simple hydrothermal method.The TiO2/CoP hybrid with the optimal ratio of CoP cocatalyst(1 wt.%)manifested significantly improved photocatalytic H_(2) evolution rate of 0.604 mmol g^(-1) h^(-1),which is tenfold in comparison to pure TiO2(0.06 mmol g^(-1) h^(-1).The mechanism of performance enhancement was fully investigated and supposed that 2D CoP nanosheets cocatalyst can enhance the photo-absorption and provide more active sites for water reduction reaction;furthermore,2D CoP nanosheets with smaller work function and high conductivity would form an Ohmicjunction with TiO_(2) nanoparticles,which can significantly accelerate the separation of photo-generated charge carriers and improve the exploitation of the photoexcited electrons in water redox reaction.This work is anticipated to impel more perspicacity into synthesizing innovative photocatalytic systems with 2D transition metal phosphides cocatalysts for attaining high photocatalytic H_(2) evolving pursuit.展开更多
Converting water into hydrogen fuel and oxidizing benzyl alcohol to benzaldehyde simultaneously under visible light illumination is of great significance,but the fast recombination of photogenerated carriers in photoc...Converting water into hydrogen fuel and oxidizing benzyl alcohol to benzaldehyde simultaneously under visible light illumination is of great significance,but the fast recombination of photogenerated carriers in photocatalysts seriously decreases the conversion efficiency.Herein,a novel dual-functional 0D Cd_(0.5)Zn_(0.5)S/2D Ti_(3)C2 hybrid was fabricated by a solvothermally in-situ generated assembling method.The Cd_(0.5)Zn_(0.5)S nano-spheres with a fluffy surface completely and uniformly covered the ultrathin Ti_(3)C2 nanosheets,leading to the increased Schottky barrier(SB)sites due to a large contact area,which could accelerate the electron–hole separation and improve the light utilization.The optimized Cd_(0.5)Zn_(0.5)S/Ti_(3)C2 hybrid simultaneously presents a hydrogen evolution rate of 5.3 mmol/(g·h)and a benzaldehyde production rate of 29.3 mmol/(g·h),which are~3.2 and 2 times higher than those of pristine Cd_(0.5)Zn_(0.5)S,respectively.Both the multiple experimental measurements and the density functional theory(DFT)calculations further demonstrate the tight connection between Cd_(0.5)Zn_(0.5)S and Ti_(3)C2,formation of Schottky junction,and efficient photogenerated electron–hole separation.This paper suggests a dual-functional composite catalyst for photocatalytic hydrogen evolution and benzaldehyde production,and provides a new strategy for preventing the photogenerated electrons and holes from recombining by constructing a 0D/2D heterojunction with increased SB sites.展开更多
Four artificial composite soil treatment systems(ACSTs)fed with reclaimed water containing trimethoprim(TMP)and sulfamethoxazole(SMX)were constructed to investigate SMX and TMP biodegradation efficiency,ammonia and ni...Four artificial composite soil treatment systems(ACSTs)fed with reclaimed water containing trimethoprim(TMP)and sulfamethoxazole(SMX)were constructed to investigate SMX and TMP biodegradation efficiency,ammonia and nitrite removal conditions and the microbial community within ACST layers.Results showed SMX and TMP removal rates could reach 80% and 95%,respectively,and removal rates of ammonia and nitrite could reach 80% and 90%,respectively,in ACSTs.The MiSeq sequencing results showed that microbial community structures of the ACSTs were similar.The dominant microbial community in the adsorption and biodegradation layers of the ACSTs contained Proteobacteria,Chloroflexi,Acidobacteria,Firmicutes,Actinobacteria and Nitrospirae.Firmicutes and Proteobacteria were considerably dominant in the ACST biodegradation layers.The entire experimental results indicated that Nitrosomonadaceae_uncultured,Nitrospira and Bacillus were associated with nitrification processes,while Bacillus and Lactococcus were associated with SMX and TMP removal processes.The findings suggest that ACSTs are appropriate for engineering applications.展开更多
The low separation/migration efficiency is a major obstacle that limits the practical application of semiconductor-photocatalysts. Constructing S-scheme heterojunction is an ideal strategy for providing high photocata...The low separation/migration efficiency is a major obstacle that limits the practical application of semiconductor-photocatalysts. Constructing S-scheme heterojunction is an ideal strategy for providing high photocatalytic activity via accelerating charge separation. Herein, an AgPO/CNcomposite was synthesized by coupling AgPOparticle with CNhollow spheres in-situ via a precipitation method. The S-scheme hete-rojunction between AgPOand CNcould accelerate the charge separation and retain high photoredox ability, which synchronously realized high photocatalytic oxygen production and hexavalent chromium reduction. The optimized Ag3PO4/CNcomposite shows a high oxygen production rate up to 803.31 μmol·g·hand a high conversion(87.9%) of Cr(Ⅵ) to Cr(Ⅲ). In addition, CNhollow spheres affords higher reaction efficiency than that of CNtube, CNbulk and CNsheet, which indicates that the hollow sphere structure can provide more active sites and adsorption sites in the photocatalytic process. This work offers an effective way in developing a dual-function S-scheme heterojunction for clean energy production and environmental protection.展开更多
The conversion of solar energy in a wide spectrum region to clean fuel,H_(2),remains a challenge in the field of photocatalysis.Herein,plasmonic TiN nanobelts,as a novel cocatalyst,were coupled with CdS nanoparticles ...The conversion of solar energy in a wide spectrum region to clean fuel,H_(2),remains a challenge in the field of photocatalysis.Herein,plasmonic TiN nanobelts,as a novel cocatalyst,were coupled with CdS nanoparticles to construct a 0D/1D CdS/TiN heterojunction.Utilization of the localized surface plasmon resonance(LSPR)effect generated from TiN nanobelts was effective in promoting light absorption in the near-infrared region,accelerating charge separation,and generating hot electrons,which can effectively improve the photocatalytic H_(2) generation activity of the 0D/1D CdS/TiN heterojunction over a wide spectral range.Furthermore,owing to the high metallicity and low work function,an ohmic-junction was formed between the CdS and TiN,favoring the transfer of hot electrons generated from TiN nanobelts the CdS nanoparticles,followed by the reaction with water to generate H_(2).Consequently,the 0D/1D CdS/TiN heterojunction demonstrated H_(2) generation activity even under light irradiation at 760 nm,while the pure CdS and Pt nanoparticles modified CdS presented no activity.This work opens a new insight into coupling plasmonic cocatalysts to realize full spectrum H_(2) production.展开更多
基金Taishan Youth Scholar Program of Shandong ProvinceNational Natural Science Foundation of China,Grant/Award Numbers:21972058,21975110,22088102,51825205+3 种基金Postgraduate Practice Research Innovation Program of Jiangsu Province,Grant/Award Number:SJCX21_1707CAS Project for Young Scientists in Basic Research,Grant/Award Number:YSBR‐004DNL Cooperation Fund,CAS,Grant/Award Number:DNL202016National Key Projects for Fundamental Research and Development of China,Grant/Award Number:2018YFB1502002。
文摘Photocatalytic water splitting is beneficial for the effective mitigation of global energy and environmental crises.Owing to multi-exciton generation,impressive light harvesting,and excellent photochemical properties,the quantum dot(QD)-based catalysts reveal a considerable potential in photocatalytic hydrogen(H_(2))production compared with bulk competitors.In this review,we summarize the recent advances in QDs for photocatalytic H_(2) production by enumerating different synthetic and characterization strategies for QDs.Various QDs-based photocatalysts are introduced and summarized in categories,and the role of different QDs in varied systems,as well as the mechanism and key factors that enhance the photocatalytic H_(2) generation performance,is discussed.Finally,conclusions and future perspectives in the exploration of highly efficient QDs-based photocatalysts for innovative applications are highlighted.
文摘Plasmonic nonmetal semiconductors with localized surface plasmon resonance(LSPR)effects possess extended light-response ranges and can act as highly efficient H2 generation photocatalysts.Herein,an LSPR-enhanced 0D/2D CdS/MoO3‒x heterojunction has been synthesized by the growth of 0D CdS nanoparticles on 2D plasmonic MoO3‒x elliptical nanosheets via a simple coprecipitation method.Taking advantage of the LSPR effect of the MoO3‒x elliptical nanosheets,the light absorption of the CdS/MoO3‒x heterojunction was extended from 600 nm to the near-infrared region(1400 nm).Furthermore,the introduction of 2D plasmonic MoO3‒x elliptical nanosheets not only provided a platform for the growth of CdS nanoparticles,but also contributed to the construction of an LSPR-enhanced S-scheme structure due to the interface between the MoO3‒x and CdS,accelerating the separation of light-induced electrons and holes.Therefore,the CdS/MoO3‒x heterojunction exhibited higher photocatalytic H2 generation activity than pristine CdS under visible light irradiation,including under 420,450,550,and 650 nm monochromic light,as well as improved photo-corrosion performance.
基金supported by the National Natural Science Foundation of China(51472101,51572114,21773062,21577036)the Jiangsu Key Laboratory for Chemistry of Low-Dimensional Materials(JSKC17003)~~
文摘Silver nanoparticles (Ag NPs) can effectively address the issue of antibiotic-resistant bacterial infections to reduce the potential toxicity of Ag NPs. Although challenging, it is, therefore, necessary to achieve the sustainable release of Ag+ ions from a finite amount of Ag NPs. This study aims at designing an efficient and benign antimicrobial silver-based ternary composite composed of photocatalysis zinc oxide (ZnO) and reduced graphene oxide (rGO) as a carrier, in which the reactive oxygen species (ROS) excited from ZnO and Ag+ ions released from the Ag NPs cooperate to realize an effective antibacterial activity against E. coli and S. aureus. The constant effective bacterial performance of the ternary photocatalyst with minimum Ag content can be attributed to the increase in the available quantity of ROS, which results from the enhanced separation efficiency of the photogenerated carriers. The proposed system notably realized the long-term sustainable release of Ag+ ions with low concentration for 30 days when compared with an equivalent amount of silver nitrate. Moreover, the use of the composite prevents biotoxicity and silver wastage, and imparts enhanced stability to the long-lasting antibacterial efficacy.
文摘Extended light absorption and dynamic charge separation are vital factors that determine the effectivenessof photocatalysts.In this study,a nonmetallic plasmonic S‐scheme photocatalyst was fabricatedby loading 1D plasmonic W_(18)O_(49)nanowires onto 2D g‐C_(3)N_(4)nanosheets.W_(18)O_(49)nanowiresplay the dual role of a light absorption antenna—that extends light adsorption—and a hot electrondonor—that assists the water reduction reaction in a wider light spectrum range.Moreover,S‐scheme charge transfer resulting from the matching bandgaps of W_(18)O_(49)and g‐C_(3)N_(4)can lead tostrong redox capability and high migration speed of the photoinduced charges.Consequently,in thisstudy,W_(18)O_(49)/g‐C_(3)N_(4)hybrids exhibited higher photocatalytic H2 generation than that of pristineg‐C_(3)N_(4)under light irradiation of 420–550 nm.Furthermore,the H2 production rate of thebest‐performing W_(18)O_(49)/g‐C_(3)N_(4)hybrid was 41.5μmol·g^(−1)·h^(−1)upon exposure to monochromaticlight at 550 nm,whereas pure g‐C_(3)N_(4)showed negligible activity.This study promotes novel andenvironmentally friendly hot‐electron‐assisted S‐scheme photocatalysts for the broad‐spectrumutilization of solar light.
基金supported by the National Natural Science Foundation of China(51672113,51602132)the Six Talent Peaks Project in Jiangsu Province(2015-XCL-026)+2 种基金the Natural Science Foundation of Jiangsu Province(BK20171299)the Training Project of Jiangsu University for Young Cadre Teachers(5521220009)the Youth Research Project of Jiangsu Health and Family Planning Commission in 2016(Q201609)~~
文摘Accelerating the separation efficiency of photoexcited electron-hole pairs with the help of highly active co-catalysts has proven to be a promising approach for improving photocatalytic activity. Thus far, the most developed co-catalysts for semiconductor-based photocatalysis are inorganic materials;the employment of a specific organic molecule as a co-catalyst for photocatalytic hydrogen evolution and pollutant photodegradation is rare and still remains a challenging task. Herein, we report on the use of an organic molecule, oxamide (OA), as a novel co-catalyst to enhance electron- hole separation, photocatalytic H2 evolution, and dye degradation over TiO2 nanosheets. OA-modified TiO2 samples were prepared by a wet chemical route and demonstrated improved light absorption in the visible-light region and more efficient charge transport. The photocatalytic performance of H2 evolution from water splitting and rhodamine B (RhB) degradation for an optimal OA-modified TiO2 photocatalyst reached 2.37 mmol g^–1 h^–1 and 1.43 × 10^-2 min^-1, respectively, which were 2.4 and 3.8 times higher than those of pristine TiO2, respectively. A possible mechanism is proposed, in which the specific π-conjugated structure of OA is suggested to play a key role in the enhancement of the charge transfer and catalytic capability of TiO2. This work may provide advanced insight into the development of a variety of metal-free organic molecules as functional co-catalysts for improved solar-to-fuel conversion and environmental remediation.
文摘Construction of multi-channels of photo-carrier migration in photocatalysts is favor to boost conversion efficiency of solar energy by promoting the charge separation and transfer.Herein,a ternary ZnIn_(2)S_(4)/g-C_(3)N_(4)/Ti_(3)C_(2) MXene hybrid composed of S-scheme junction integrated Schottky-junction was fabricated using a simple hydrothermal approach.All the components(g-C_(3)N_(4),ZnIn_(2)S_(4) and Ti_(3)C_(2) MXene)demonstrated two-dimensional(2D)nanosheets structure,leading to the formation of a 2D/2D/2D sandwich-like structure with intimate large interface for carrier migration.Furthermore,the photogenerated carriers on the g-C_(3)N_(4) possessed dual transfer channels,including one route in S-scheme transfer mode between the g-C_(3)N_(4) and ZnIn_(2)S_(4) and the other route in Schottky-junction between g-C_(3)N_(4) and Ti_(3)C_(2) MXene.Consequently,a highly efficient carrier separation and transport was realized in the ZnIn_(2)S_(4)/g-C_(3)N_(4)/Ti_(3)C_(2) MXene heterojunction.This ternary sample exhibited wide light response from 200 to 1400 nm and excellent photocatalytic H_(2) evolution of 2452.1μmol∙g^(–1)∙h^(–1),which was 200,3,1.5 and 1.6 times of g-C_(3)N_(4),ZnIn_(2)S_(4),ZnIn_(2)S_(4)/Ti_(3)C_(2) MXene and g-C_(3)N_(4)/ZnIn_(2)S_(4) binary composites.This work offers a paradigm for the rational construction of multi-electron pathways to regulate the charge separation and migration via the introduction of dual-junctions in catalytic system.
基金This work was supported by the National Science Foundation of China(51772152,51702129,51572114,51972150,21908110,and 51902161)Fundamental Research Funds for the Central Universities(30919011269,30919011110,and 1191030558)+3 种基金Y.W.thanks the Key University Science Research Project of Jiangsu province(16KJB430009)Y.Z.thanks for the support from the Postdoctoral Science Foundation(2018M630527)China Scholarship Council(201708320150)J.S.thanks the Natural Science Foundation of Jiangsu Province(BK20190479,1192261031693).
文摘Graphitic carbon nitride(g-C3N4)-based photocatalysts have shown great potential in the splitting of water.However,the intrinsic drawbacks of g-C3N4,such as low surface area,poor diffusion,and charge separation efficiency,remain as the bottleneck to achieve highly efficient hydrogen evolution.Here,a hollow oxygen-incorporated g-C3N4 nanosheet(OCN)with an improved surface area of 148.5 m2 g^−1 is fabricated by the multiple thermal treatments under the N2/O2 atmosphere,wherein the C–O bonds are formed through two ways of physical adsorption and doping.The physical characterization and theoretical calculation indicate that the O-adsorption can promote the generation of defects,leading to the formation of hollow morphology,while the O-doping results in reduced band gap of g-C3N4.The optimized OCN shows an excellent photocatalytic hydrogen evolution activity of 3519.6μmol g^−1 h^−1 for~20 h,which is over four times higher than that of g-C3N4(850.1μmol g^−1 h^−1)and outperforms most of the reported g-C3N4 catalysts.
文摘Durable and inexpensive graphitic carbon nitride(g-C_(3)N_(4))demonstrates great potential for achieving efficient photocatalytic hydrogen evolution reduction(HER).To further improve its activity,g-C_(3)N_(4)was subjected to atomic-level structural engineering by doping with transition metals(M=Fe,Co,or Ni),which simultaneously induced the formation of metal-N active sites in the g-C_(3)N_(4)framework and modulated the bandgap of g-C_(3)N_(4).Experiments and density functional theory calculations further verified that the as-formed metal-N bonds in M-doped g-C_(3)N_(4)acted as an"electron transfer bridge",where the migration of photo-generated electrons along the bridge enhanced the efficiency of separation of the photogenerated charges,and the optimized bandgap of g-C_(3)N_(4)afforded stronger reduction ability and wider light absorption.As a result,doping with either Fe,Co,or Ni had a positive effect on the HER activity,where Co-doped g-C_(3)N_(4)exhibited the highest performance.The findings illustrate that this atomic-level structural engineering could efficiently improve the HER activity and inspire the design of powerful photocatalysts.
基金supported by National Natural Science Foundation of China(51672113)Six Talent Peaks Project in Jiangsu Province(2015-XCL-026)+3 种基金Natural Science Foundation of Jiangsu Province(BK20171299)State Key Laboratory of Photocatalysis on Energy and Environment(SKLPEE-KF201705),Fuzhou UniversityState Key Laboratory of Advanced Technology for Materials Synthesis and Processing(2016-KF-10),Wuhan University of Technologythe Qing Lan Project Foundation of Jiangsu Province~~
文摘Graphite‐like carbon nitride(g‐C3N4)‐based compounds have attracted considerable attention because of their excellent photocatalytic performance.In this work,a novel direct Z‐scheme system constructed from two‐dimensional(2D)g‐C3N4nanoplates and zero‐dimensional(0D)MoS2quantum dots(QDs)was prepared through the combination of a hydrothermal process and microemulsion preparation.The morphologies,structures,and optical properties of the as‐prepared photocatalysts were characterized by X‐ray diffraction,X‐ray photoelectron spectroscopy,atomic force microscopy,transmission electron microscopy,and UV‐vis diffuse reflectance spectroscopy.In addition,the photocatalytic performances of the prepared2D/0D hybrid composites were evaluated based on the photodegradation of rhodamine B under visible‐light irradiation.The results demonstrated that the introduction of MoS2QDs to g‐C3N4greatly enhanced the photocatalytic efficiency.For the optimum7%MoS2QD/g‐C3N4photocatalyst,the degradation rate constant was8.8times greater than that of pure g‐C3N4under visible‐light irradiation.Photocurrent and electrochemical impedance spectroscopy results further demonstrated that the MoS2QD/g‐C3N4composites exhibited higher photocurrent density and lower chargetransfer resistance than those of the pure g‐C3N4or MoS2QDs.Active species trapping,terephthalic acid photoluminescence,and nitro blue tetrazolium transformation experiments were performed to investigate the evolution of reactive oxygen species,including hydroxyl radicals and superoxide radicals.The possible enhanced photocatalytic mechanism was attributed to a direct Z‐scheme system,which not only can increase the separation efficiency of photogenerated electron‐hole pairs but also possesses excellent oxidation and reduction ability for high photocatalytic performances.This work provides an effective synthesis approach and insight to help develop other C3N4‐based direct Z‐scheme photocatalytic systems for environmental purification and energy conversion.
基金supported by the National Natural Science Foundation of China(51672113)QingLan Project Foundation of Jiangsu Province(201611)~~
文摘g-C3N4 is a metal-free semiconductor and a potential candidate for photocatalytic H2 production,however,the drawbacks,rapid recombination rate and limited migration efficiency of photogenerated carriers,restrict its photocatalytic activity.Herein,Co(II)as a hole cocatalyst modified P-doped g-C3N4 were successfully prepared to ameliorate the separation efficiency of photoinduced carriers and enhance the photocatalytic hydrogen production.The photocatalytic results demonstrated that the P-doped g-C3N4(PCN)exhibited higher photocatalytic activity compared with pure g-C3N4,while Co(II)/PCN photocatalyst exhibited further enhancement of photocatalytic performance.The proposed possible mechanism based on various characterizations is that P-doping can modulate the electronic structure of g-C3N4 to boost the separation of photogenerated-e-and h+;while the synergistic effect of both Co(II)(as hole cocatalyst)and Pt(as electron cocatalyst)can not only lead to the directional shunting of photogenerated e+-h?pairs,but further accelerate the photogenerated electrons transfer to Pt in order to join the photocatalytic reduction process for hydrogen evolution.As a result,the transportation and separation of photoinduced carriers were accelerated to greatest extent in the Pt/Co(II)/PCN photocatalyst.
基金supported by the Program for the National Natural Science Foundation of China(No.21972058)Prof.H.Tang also appreciates the support from the Taishan Youth Scholar Program of Shandong Province.
文摘Aiming to develop a photocatalyst that can simultaneously produce valuable chemicals and clean H_(2) fuel for promoting the utilization efficiency of solar energy,herein,a sea-urchin-like CoP@Ni_(2)P binary nanojunction was employed as an efficient photothermal cocatalyst to couple with zero-dimensional CdZnS(CZS)solid solution for achieving superior coordinative redox reaction.The CoP@Ni_(2)P/CZS hybrid displayed a high solar-driven H_(2) generation rate of 40.92 mmol g^(–1) h^(–1) coupling with a benzaldehyde formation rate of 20.33 mmol g^(–1) h^(–1),which was 16.4 and 8.0 times higher than that of bare CZS.Furthermore,the CoP@Ni_(2)P/CZS hybrid also achieved a high photothermal H_(2) production under a broad light range from 420 to 720 nm,and the H_(2) production reached 44.48μmol g^(–1) h^(–1) under the 720 nm light illumination.The enhanced catalytic performance can be ascribed to that the CoP@Ni_(2)P nanojunction with photothermal effect can speed up the separation and transport of carriers,offer more catalytic active sites,and induce an increase in temperature to optimize reaction kinetics.This study may open a facile route to design novel binary metal phosphides with dual functions in photocatalysis for the full exploitation of solar energy.
文摘Background:Nontraumatic acute abdominal pain(AAP)accounts for a large proportion of emergency department(ED)admissions.This study aimed to explore the underlying correlations among basic information,imaging examinations,and diagnoses.Methods:A total of 7453 patients complaining of AAP,admitted to the ED of Zhongnan Hospital of Wuhan University,were enrolled in this retrospective study from January 1 to December 30,2019.We collected the following information from the patients:sex,age,date of visit,pain location,nature of pain,level of severity,imaging(computed tomography,x-ray,and ultrasound),diagnosis,and outcomes(re-lease from the hospital,transfer to another hospital,transfer to another department,observation room,hospitalization,or death).Results:According to this study,AAP was more common in female than male.A total of 82.11%patients of AAP were in level 3 of se-verity,while 0.19%patients were in level 1.A total of 77.20%of the patients had undergone imaging.Swelling pain and colic are the 2 most common types of AAP.Nonspecific abdominal pain(NSAP)is the most common diagnosis.In the diagnosis of NSAP and gastroenteritis,female patients were more prevalent than male patients,but for renal colic,male patients were 3 times as many as female patients.Non-specific abdominal pain,biliary colic,and cholecystitis are the 3 leading causes in patients 65 years or older.Nonspecific abdominal pain,renal colic,and gastroenteritis are the 3 leading causes of AAP in patients younger than 65 years.Conclusion:With the help of imaging,clinicians can specify a diagnosis and perform corresponding treatment in most cases.However,making a precise diagnosis of AAP within a short period is still challenging.Further research should be conducted to seek safer and more effective techniques to streamline clinicians’work.
基金The authors are grateful for the financial support from the National Key R&D Program of China(Nos.2018YFB1502002,2017YFA0206904,2017YFA0206900,and 2016YFB0600901)the National Natural Science Foundation of China(Nos.51825205,U1662U&51772305,51572270,21871279,and 21802154)+4 种基金the Beijing Natural Science Foundation(Nos.2191002,218207&and 2194089)the Beijing Municipal Science and Technology Project(No.Z181100005118007)the Strategic Priority Research Program of the Chinese Academy of Sciences(No.XDB17000000)the Royal Society-Newton Advanced Fellowship(No.NA170422)the International Partnership Program of Chinese Academy of Sciences(No.GJHZ1819)and the K.C.Wong Education Foundation.G.I.N.W.acknowledges funding support from the Energy Education Trust of New Zealand and the University of Auckland Faculty Research Development Fund.
文摘A simple one-step thermal polymerization method was developed for synthesis of holey graphitic carbon nitride nanotubes,involving direci eating of mixtures of melamine and urea or melamine and cyanuric acid in specific mass ratios.Supramolecular structures formed betweer the precursor molecules guided nanotube formation.The porous and nanotubular structure of the nanotubes facilitated efficient charge carrier nigration and separation,thereby enhancing photocatalytic Hz production in 20 vol.%lactic acid under visible light irradiation.Nanotubes synthesized using melamine and urea in a 1:10 mass ratio(denoted herein as CN-MU nanotubes)exhibited a photocatalytic hydroger production rate of 1,073.6μmol·h^-1·^-g with Pt as the cocatalyst,a rate of 4.7 and 3.1 times higher than traditional Pt/g-CN4 photocatalysts prepared from graphitic carbon nitride(g-CN4)obtained by direct thermal polymerization of melamine or urea,respectively.On the basis of their outstanding performance for photocatalytic H2 production,it is envisaged that the holey g-C3N4 nanotubes will find widespread uptake in other areas,including photocatalytic CO2 reduction,dye-sensitized solar cells and photoelectrochemical sensors.
基金financially supported by the National Natural Science Foundation of China(Nos.51672113,21975110 and 21972058)。
文摘It is still of gigantic challenging to design and to optimize photocatalytic systems with cost-efficiency for photocatalytic hydrogen evolution from water splitting.Herein,noble-metal-free 2D CoP nanosheets were prepared by a phosphorization method using Co(OH)2 nanosheets as precursors,and then employed as photocatalytic cocatalyst and template to make 0D Ti O2 nanoparticles in-situ grow on the surface for construction of 0D/2D TiO_(2)/CoP hybrid by a simple hydrothermal method.The TiO2/CoP hybrid with the optimal ratio of CoP cocatalyst(1 wt.%)manifested significantly improved photocatalytic H_(2) evolution rate of 0.604 mmol g^(-1) h^(-1),which is tenfold in comparison to pure TiO2(0.06 mmol g^(-1) h^(-1).The mechanism of performance enhancement was fully investigated and supposed that 2D CoP nanosheets cocatalyst can enhance the photo-absorption and provide more active sites for water reduction reaction;furthermore,2D CoP nanosheets with smaller work function and high conductivity would form an Ohmicjunction with TiO_(2) nanoparticles,which can significantly accelerate the separation of photo-generated charge carriers and improve the exploitation of the photoexcited electrons in water redox reaction.This work is anticipated to impel more perspicacity into synthesizing innovative photocatalytic systems with 2D transition metal phosphides cocatalysts for attaining high photocatalytic H_(2) evolving pursuit.
基金This work was supported by the National Natural Science Foundation of China(Grant Nos.51902137 and 51672113)the Key Research and Development Plan(Grant No.BE2019094)+1 种基金the Qing Lan Project([2016]15)of Jiangsu ProvinceThe calculations were carried out by the Advanced Computing East China Sub-center and Big Data Center of Southeast University。
文摘Converting water into hydrogen fuel and oxidizing benzyl alcohol to benzaldehyde simultaneously under visible light illumination is of great significance,but the fast recombination of photogenerated carriers in photocatalysts seriously decreases the conversion efficiency.Herein,a novel dual-functional 0D Cd_(0.5)Zn_(0.5)S/2D Ti_(3)C2 hybrid was fabricated by a solvothermally in-situ generated assembling method.The Cd_(0.5)Zn_(0.5)S nano-spheres with a fluffy surface completely and uniformly covered the ultrathin Ti_(3)C2 nanosheets,leading to the increased Schottky barrier(SB)sites due to a large contact area,which could accelerate the electron–hole separation and improve the light utilization.The optimized Cd_(0.5)Zn_(0.5)S/Ti_(3)C2 hybrid simultaneously presents a hydrogen evolution rate of 5.3 mmol/(g·h)and a benzaldehyde production rate of 29.3 mmol/(g·h),which are~3.2 and 2 times higher than those of pristine Cd_(0.5)Zn_(0.5)S,respectively.Both the multiple experimental measurements and the density functional theory(DFT)calculations further demonstrate the tight connection between Cd_(0.5)Zn_(0.5)S and Ti_(3)C2,formation of Schottky junction,and efficient photogenerated electron–hole separation.This paper suggests a dual-functional composite catalyst for photocatalytic hydrogen evolution and benzaldehyde production,and provides a new strategy for preventing the photogenerated electrons and holes from recombining by constructing a 0D/2D heterojunction with increased SB sites.
文摘Four artificial composite soil treatment systems(ACSTs)fed with reclaimed water containing trimethoprim(TMP)and sulfamethoxazole(SMX)were constructed to investigate SMX and TMP biodegradation efficiency,ammonia and nitrite removal conditions and the microbial community within ACST layers.Results showed SMX and TMP removal rates could reach 80% and 95%,respectively,and removal rates of ammonia and nitrite could reach 80% and 90%,respectively,in ACSTs.The MiSeq sequencing results showed that microbial community structures of the ACSTs were similar.The dominant microbial community in the adsorption and biodegradation layers of the ACSTs contained Proteobacteria,Chloroflexi,Acidobacteria,Firmicutes,Actinobacteria and Nitrospirae.Firmicutes and Proteobacteria were considerably dominant in the ACST biodegradation layers.The entire experimental results indicated that Nitrosomonadaceae_uncultured,Nitrospira and Bacillus were associated with nitrification processes,while Bacillus and Lactococcus were associated with SMX and TMP removal processes.The findings suggest that ACSTs are appropriate for engineering applications.
基金supported by the National Natural Science Foundation of China(21975110,21972058 and 22102064)the financial support from Taishan Youth Scholar Program of Shandong Province。
文摘The low separation/migration efficiency is a major obstacle that limits the practical application of semiconductor-photocatalysts. Constructing S-scheme heterojunction is an ideal strategy for providing high photocatalytic activity via accelerating charge separation. Herein, an AgPO/CNcomposite was synthesized by coupling AgPOparticle with CNhollow spheres in-situ via a precipitation method. The S-scheme hete-rojunction between AgPOand CNcould accelerate the charge separation and retain high photoredox ability, which synchronously realized high photocatalytic oxygen production and hexavalent chromium reduction. The optimized Ag3PO4/CNcomposite shows a high oxygen production rate up to 803.31 μmol·g·hand a high conversion(87.9%) of Cr(Ⅵ) to Cr(Ⅲ). In addition, CNhollow spheres affords higher reaction efficiency than that of CNtube, CNbulk and CNsheet, which indicates that the hollow sphere structure can provide more active sites and adsorption sites in the photocatalytic process. This work offers an effective way in developing a dual-function S-scheme heterojunction for clean energy production and environmental protection.
基金sustained by the National Natural Science Foundation of China(Nos.21975110 and 21972058)financial support from Taishan Youth Scholar Program of Shandong Provincesupported by the Open Project Program of the State Key Laboratory of Photocatalysis on Energy and Environment(No.SKLPEE-KF202102)。
文摘The conversion of solar energy in a wide spectrum region to clean fuel,H_(2),remains a challenge in the field of photocatalysis.Herein,plasmonic TiN nanobelts,as a novel cocatalyst,were coupled with CdS nanoparticles to construct a 0D/1D CdS/TiN heterojunction.Utilization of the localized surface plasmon resonance(LSPR)effect generated from TiN nanobelts was effective in promoting light absorption in the near-infrared region,accelerating charge separation,and generating hot electrons,which can effectively improve the photocatalytic H_(2) generation activity of the 0D/1D CdS/TiN heterojunction over a wide spectral range.Furthermore,owing to the high metallicity and low work function,an ohmic-junction was formed between the CdS and TiN,favoring the transfer of hot electrons generated from TiN nanobelts the CdS nanoparticles,followed by the reaction with water to generate H_(2).Consequently,the 0D/1D CdS/TiN heterojunction demonstrated H_(2) generation activity even under light irradiation at 760 nm,while the pure CdS and Pt nanoparticles modified CdS presented no activity.This work opens a new insight into coupling plasmonic cocatalysts to realize full spectrum H_(2) production.
