The growing presence of emerging pollutants in the environment has led to a focus on developing new treatment technologies to address the limitations of traditional methods.Recent advancements in combining photocataly...The growing presence of emerging pollutants in the environment has led to a focus on developing new treatment technologies to address the limitations of traditional methods.Recent advancements in combining photocatalysis with biodegradation for pollutant treatment have garnered significant attention.This is due to the rapid and uncontrolled chemical reactions in single photocatalytic processes,which often result in the buildup of harmful by-products and over-oxidation residues.Additionally,relying solely on biodegradation is challenging for breaking down emerging pollutants that possess high concentrations and intricate structures.Therefore,the intimately coupled photocatalysis and biodegradation(ICPB)systems,along with the photocatalytic microbial fuel cells(PMFCs),as a new approach to treat pollutants.These systems combine the benefits of biodegradation and photocatalytic reactions,providing cost-effective,eco-friendly,and sustainable solutions with significant promise.In order to demonstrate the ICPB system and the PMFCs system as rational options for pollutant removal,the mechanisms of pollutant degradation by the two systems have been analyzed in depth,and recent advances in photocatalysts,biofilms,and carriers/configurations in the two systems have been summarized.Furthermore,the practical applications of the ICPB system versus the PMFCs system for pollutant removal are also summarized and highlighted.This review further points out the current limitations,such as photocatalytic materials that are still challenging in terms of commercial viability for practical applications,and looks forward to the prospects of the ICPB system versus the PMFCs system for the treatment of pollutants to promote practical applications.展开更多
The mass production and widespread use of Pharmaceuticals and Personal Care Products(PPCPs)have posed a serious threat to the water environment and public health.In this work,a green metal-based Metal Organic Framewor...The mass production and widespread use of Pharmaceuticals and Personal Care Products(PPCPs)have posed a serious threat to the water environment and public health.In this work,a green metal-based Metal Organic Framework(MOF)Bi-NH_(2)-BDC was prepared and characterized,and the adsorption characteristics of Bi-NH_(2)-BDCwere investigated with typical PPCPs-diclofenac sodium(DCF).It was found that DCF mainly covered the adsorbent surface as a single molecular layer,the adsorption reaction was a spontaneous,entropyincreasing exothermic process and the adsorption mechanisms between Bi-NH_(2)-BDC and DCF were hydrogen bonding,π-πinteractions and electrostatic interactions.In addition,Bi-NH_(2)-BDC also had considerable photocatalytic properties,and its application in adsor-bent desorption treatment effectively solved the problem of secondary pollution,achieving a green and sustainable adsorption desorption cycle.展开更多
The production of renewable methanol(CH_(3)OH)via the photocatalytic hydrogenation of CO_(2) is an ideal method to ameliorate energy shortages and mitigate CO_(2) emissions:however,the highly selective synthesis of me...The production of renewable methanol(CH_(3)OH)via the photocatalytic hydrogenation of CO_(2) is an ideal method to ameliorate energy shortages and mitigate CO_(2) emissions:however,the highly selective synthesis of methanol at atmospheric pressure remains challenging owing to the competing reverse water-gas shift(RWGS)reaction.Herein,we present a novel approach for the synthesis of CH_(3)OH via photocatalytic CO_(2) hydrogenation using a catalyst featuring highly dispersed Au nanoparticles loaded on oxygen vacancy(OV)-rich molybdenum dioxide(MoO_(2)),resulting in a remarkable selectivity of 43.78%.The active sites in the Au/MoO_(2) catalyst are high-density Au-oxygen vacancies,which synergistically promote the tandem methanol synthesis via an initial RWGS reaction and subsequent CO hydrogenation.This work provides comprehensive insights into the design of metal-vacancy synergistic sites for the highly selective photocatalytic hydrogenation of CO_(2) to CH_(3)OH.展开更多
Semi-heterogeneous photocatalysis has emerged as a powerful and productive platform in organic chemistry,which provides mild and eco-friendly conditions for a diverse range of bond-forming reactions.The synergy of hom...Semi-heterogeneous photocatalysis has emerged as a powerful and productive platform in organic chemistry,which provides mild and eco-friendly conditions for a diverse range of bond-forming reactions.The synergy of homogeneous catalysts and heterogeneous catalysts inherits their main advantages,such as higher activities,easy separation and superior recyclability.In this review,we summarize the recent advances in recyclable semi-heterogenous protocols for the light promoted bond-forming reactions and identify directions for future research according to the different photocatalysts/metal/redox catalysts involved.Notably,this review is not a comprehensive description of reported literature but aim to highlight and illustrate key concepts,strategies,reaction model,reaction conditions and mechanisms.展开更多
Achieving artificial simulations of multi-step energy transfer processes and conversions in nature remains a challenge.In this study,we present a three-step sequential energy transfer process,which was constructed thr...Achieving artificial simulations of multi-step energy transfer processes and conversions in nature remains a challenge.In this study,we present a three-step sequential energy transfer process,which was constructed through host-vip interactions between a piperazine derivative(PPE-BPI)with aggregationinduced emission(AIE)and cucurbit[7]uril(CB[7])in water to serve as ideal energy donors.To achieve multi-step sequential energy transfer,we employ three distinct fluorescent dyes Eosin B(EsB),Sulforhodamine 101(SR101),and Cyanine 5(Cy5)as energy acceptors.The PPE-PBI-2CB[7]+EsB+SR101+Cy5 system demonstrates a highly efficient three-step sequential energy transfer mechanism,starting with PPEPBI-2CB[7]and transferring energy successively to EsB,SR101,and finally to Cy5,with remarkable energy transfer efficiencies.More interestingly,with the progressive transfer of energy in the multi-step energy transfer system,the generation efficiency of superoxide anion radical(O_(2)•-)increased gradually,which can be used as photocatalysts for selectively photooxidation of N-phenyltetrahydroisoquinoline in an aqueous medium with a high yield of 86%after irradiation for 18 h.This study offers a valuable investigation into the simulation of multi-step energy transfer processes and transformations in the natural world,paving the way for further research in the field.展开更多
Carbon quantum dots are a new type of fluorescent nanomaterials with broad applications in drug delivery,bioimaging,solar cells,and photocatalysis due to their unique biocompatibility,optical properties and easy funct...Carbon quantum dots are a new type of fluorescent nanomaterials with broad applications in drug delivery,bioimaging,solar cells,and photocatalysis due to their unique biocompatibility,optical properties and easy functionalization.In the meantime,because of its high carbon content,renewable nature,and environmental friendliness,lignin has drawn the attention of researchers as a desirable raw material for creating carbon quantum dots.Here we review the synthesis of carbon quantum dots from lignin,focusing on synthetic methods,properties,and applications in energy,and photocatalysis.Later,we propose some new development prospects from preparation methods,luminescence mechanism research,application,and commercial cost of lignin carbon quantum dots.Finally,based on this,the development prospects of this field are prospected and summarized.展开更多
Photocatalysis(PC)and photoelectrocatalysis(PEC)represent promising and efficient avenues for harnessing solar energy to produce sustainable clean energy products and environmental remediation.Yet the current reaction...Photocatalysis(PC)and photoelectrocatalysis(PEC)represent promising and efficient avenues for harnessing solar energy to produce sustainable clean energy products and environmental remediation.Yet the current reaction efficiencies remain inadequate,limiting their efficiencies for practice.Despite the growing interest in photo thermal-driven PC/PEC systems,there is no comprehensive review that systematically summarises the role of the photothermal effect in bridging the gap between PC and PEC efficiencies.This review initially introduces the fundamental principles of PC and PEC,alongside the primary photothermal materials and relevant conversion mechanisms.Subsequently,the key influences of photothermal effects on PC and PEC performance(e.g.,light absorption,charge separation and transport,and surface reactions)and optimization strategies are discussed.In addition,the latest advancements in solar photothermal conversion are discussed,mainly focused on the widely application of different types of photothermal drive PC and PEC applications,such as PC and PEC oxygen evolution reaction(OER),hydrogen evolution reaction(HER),CO_(2)reduction reaction(CO_(2)RR),pollutant degradation,and sterilization,serving to illustrate the widespread applicability of the photothermal conversion.Finally,the development prospects and challenges of photothermal-assisted PC and PEC are discussed from the perspective of basic research and practical application.This work provides a timely and systematic framework to guide the rational design of photothermal-enhanced PC/PEC systems for sustainable energy and environmental applications.展开更多
Natural fibers,as a typical renewable and biodegradable material,have shown great potential for many applications(e.g.,catalysis,hydrogel,biomedicine)in recent years.Recently,the growing importance of natural fibers i...Natural fibers,as a typical renewable and biodegradable material,have shown great potential for many applications(e.g.,catalysis,hydrogel,biomedicine)in recent years.Recently,the growing importance of natural fibers in these photo-driven applications is reflected by the increasing number of publications.The utilization of renewable materials in photo-driven applications not only contributes to mitigating the energy crisis but also facilitates the transition of society toward a low-carbon economy,thus enabling harmonious coexistence between humans and the environment within the context of sustainable development.This paper provides an overview of the recent advances of natural fibers which acted as substrates or precursors to construct an efficient system of light utilization.The different chemical properties and pretreatment methods of cellulose affect its performance in final photo-driven applications,including solar-driven water purification,photocatalysis,and photothermal biomedical applications.Nevertheless,current research rarely conducts a comprehensive comparisonof themfromabroadperspective.As a whole,this review first reveals the different structural advantages as well as thematching degree between natural fibers(bacterial cellulose,plant cellulose,and animal fiber)and three typical photo-driven applications.Besides,new strategies for optimizing the utilization of natural fibers are an important subject under the background of low-carbon and circular economy.Finally,some suggestions and prospects are put forward for the limitations and research prospects of natural fibers in photo-driven applications,which provides a new idea for the synthesis of renewable functional materials.展开更多
Crystal defects and morphological modifications are popular strategies to enhance the catalytic activity of heterogeneous semiconductor photocatalysts.Despite defect engineering and morphology control show their succe...Crystal defects and morphological modifications are popular strategies to enhance the catalytic activity of heterogeneous semiconductor photocatalysts.Despite defect engineering and morphology control show their successful applications in ZnO,the effects of curved surface modifications on the photocatalytic performance of ZnO and their interplay with the defect formation remain unclear.To resolve this puzzle,we systemically investigate the joint effects of curvature and defect formation on the electronic structure,optoelectronic properties,and photocatalytic performance of ZnO slabs using first-principles calculations.We find that curvature deformation effectively narrows the electronic bandgap by up to 1.6 eV and shifts the p-/d-band centers,thereby enhancing light absorption in the visible and near-ultraviolet regions.Besides,curvature deformation stimulates self-polarization,facilitating the separation of photogenerated electrons and holes.Also,curvature deformation promotes the formation of defects by reducing defect formation energy(by up to 1.0 eV),thus creating abundant reaction sites for photocatalysis.Intriguingly,the synergistic interaction between curvature and defect deformation further strengthens the self-polarization,narrows the electronic bandgaps,adjusts the p-/d-band centers to improve the optoelectronic properties,and influences the dissociation and free energy barriers of intermediates.Consequently,our findings reveal that this synergy substantially enhances the photocatalytic performance of ZnO slabs,providing deeper insights into the role of defect engineering and morphology control on photocatalysis.展开更多
The introduction of metal single atoms(SAs)into semiconductors can effectively optimize their electronic configuration and enhance their photocatalytic properties.Therefore,it is crucial to clarify the corresponding p...The introduction of metal single atoms(SAs)into semiconductors can effectively optimize their electronic configuration and enhance their photocatalytic properties.Therefore,it is crucial to clarify the corresponding principles and photocatalytic mechanisms for efficient and sustainable photocatalytic water remediation systems.Herein,a promising Fe single-atom photocatalyst(Fe_(SA)-CN)is obtained by anchoring Fe SAs in graphitic carbon nitride using a simple calcination strategy.Characterization and experimental results indicate that the modification of Fe SAs not only introduces a doping energy level,but also changes the valence band position,which expands the light absorption range,enhances the reduction ability of photogenerated electrons,and improves the separation and transfer of photogenerated charge carriers.Subsequently,contaminants adsorbed on the FeSA-CN surface trigger their oxidation removal by h^(+),and the H_(2)O_(2)generated via two-electron direct reductions is converted in situ into OH by self-Fenton reaction for the synergistic contaminant degradation.In summary,FeSA-CN offers a promising pathway for single-atom photocatalysts in water remediation because of outstanding contamination removal efficiency,adaptability,and stability.展开更多
Covalent organic frameworks(COFs)based photocatalysts utilizing infrared light remains unexplored due to the limitation of electronic absorption.Herein,two novel two-dimensional(2D)polyimide-linked phthalocyanine COFs...Covalent organic frameworks(COFs)based photocatalysts utilizing infrared light remains unexplored due to the limitation of electronic absorption.Herein,two novel two-dimensional(2D)polyimide-linked phthalocyanine COFs,namely MPc-DPA-COFs(M=Zn/Cu),were prepared from the imidization reaction of metal tetraanhydrides of 2,3,9,10,16,17,23,24-octacarboxyphthalocyaninato(M(TAPc))with 9,10-diphenyl anthracene(DPA).Both COFs possess highly crystalline eclipsed AA stacking structure with neighboring layer distance of 0.33 nm on the basis of powder X-ray diffraction analysis and high-resolution transmission electron microscopy.Effective π–π interaction between phthalocyanine chromophores in neighboring layers of 2D COFs leads to significant bathochromic-shift of narrow Q band from 697 nm for M(TAPc)to the infrared light absorption range of 760–1000 nm for MPc-DPA-COFs according to solid UV-vis diffuse reflectance spectra.This endows them in particular ZnPc-DPA-COF with excellent reactive oxygen species of•O_(2)^(–)and 1O_(2) generation activity under infrared light radiation(λ>760 nm)based on the electron spin resonance spectroscopy measurement,in turn resulting in the excellent photocatalytic capacity towards oxidation of sulfides under infrared light radiation.Corresponding quenching experiments reveal the contribution of both•O_(2)^(–)and 1O_(2) to the oxidation of sulfides,but the former•O_(2)^(–)species plays a leading role in this photocatalytic process.The present result not only provides a new efficient infrared light photocatalyst but also unveils the good potentials of phthalocyanine-based COFs in photocatalysis.展开更多
In conjugated polymers(CPs)photocatalytic system,the generation of reactive oxygen species(ROS)is regulated by cross-scale factors involving active site,excitonic behavior,and O_(2)activation process on the surface.Ho...In conjugated polymers(CPs)photocatalytic system,the generation of reactive oxygen species(ROS)is regulated by cross-scale factors involving active site,excitonic behavior,and O_(2)activation process on the surface.However,research on exploring the domino effect of“structure→excitonic behavior→O_(2)activation→photocatalytic reaction”through structural modification at the atomic scale remains at its early stages.Herein,two heptazine-based CPs,CP-DPA,and CP-CZ were successfully prepared by polymerization of precursors formed by reacting diphenylamine(DPA)and carbazole(CZ)with cyameluric chloride,respectively.The minute difference in single bond between DPA and CZ endows the polymers with distinct physicochemical properties.Owing to the rotation between benzene rings,CP-DPA exhibits relatively lower conjugation,resulting in increased exciton binding energy(Eb)and inhibited exciton dissociation.Meanwhile,its more triplet state excitons facilitate energy transfer to generate singlet oxygen.Therefore,CP-DPA shows excellent activity for phenylboronic acid oxidation.Conversely,CP-CZ possesses relatively higher conjugation,minimal Eb and intensified exciton dissociation,which promotes charge transfer to produce superoxide radical.Consequently,CP-CZ displays optimal activity for phe-nylacetylene oxidation and[3+2]cycloaddition.This work provides new insights into regulating ROS gener-ation by modulating the composition and structure of photocatalysts at the atomic scale.展开更多
Peroxymonosulfate(PMS)is commonly used in advanced oxidation processes to degrade organic pollutants in wastewater.In this work,to obtain better PMS activation efficiency,Bi_(4)O_(5)Br_(2)/BCZT(BBT)piezoelectric photo...Peroxymonosulfate(PMS)is commonly used in advanced oxidation processes to degrade organic pollutants in wastewater.In this work,to obtain better PMS activation efficiency,Bi_(4)O_(5)Br_(2)/BCZT(BBT)piezoelectric photocatalyst was designed.Abundant active radicals produced by BBT under visible light irradiation and ultrasonic vibration were used to activate PMS,thereby achieving rapid degradation of high concentration pollutants.With the introduction of BCZT,the catalyst has a strong internal electric field and three-dimensional lamellar structure,which promotes the separation and transfer of electrons and holes.It is worth noting that under optimal reaction conditions,the degradation rate of ARB reached 93%by BBT15 within 10 min.The catalytic experiment combined with the piezoelectric performance test results revealed the key role of piezoelectric photocatalytic reaction in PMS activation.This provides an important prospect for PMS to effectively deal with the degradation of high concentrations of organic pollutants.展开更多
Reactive oxygen species(ROS),including singlet oxygen(^(1)O_(2)),hydroxyl radicals(·OH),and superoxide anions(O_(2)^(·-)),are highly reactive molecules that play central roles in many chemical,biological,and...Reactive oxygen species(ROS),including singlet oxygen(^(1)O_(2)),hydroxyl radicals(·OH),and superoxide anions(O_(2)^(·-)),are highly reactive molecules that play central roles in many chemical,biological,and environmental processes due to their strong oxidative power[1].Generating ROS in a controlled manner under mild conditions is essential for achieving selective oxidation reactions.Light-driven methods are especially appealing for this purpose,as they offer precise control over where and when ROS are produced.展开更多
Herein,a simple and effective outer-surface interactions assisted supramolecular hierarchical assembly has been first exploited to uniformly distribute tungstosilicic acid(TSA)inside the porous structure of cucurbit[1...Herein,a simple and effective outer-surface interactions assisted supramolecular hierarchical assembly has been first exploited to uniformly distribute tungstosilicic acid(TSA)inside the porous structure of cucurbit[10]uril-based single-layer 2D supramolecular-organic-frameworks(Q[10]-SOFs)in water.Importantly,the 2D Q[10]-SOFs can further serve as light harvesting antenna,achieving fast energy transfer to the embedded redox-active TSA upon photoexcitation,resulting in efficient visible light-driven selective oxidation of benzyl alcohols into the corresponding aldehydes in high yield at room temperature.Further studies revealed that the integrated of 2D Q[10]-SOFs and TSA played a key role in the catalytic process,due to the presence of a novel stepwise electron transfer route in the single-layer hybrid 2D structures.展开更多
Ce-β-Bi_(2)O_(3)/AgI was prepared using solvothermal calcination and in-situ deposition methods.The introduction of Ce can inhibit the conversion of Bi_(2)O_(3)fromβtoαphase at high temperatures,promoting the forma...Ce-β-Bi_(2)O_(3)/AgI was prepared using solvothermal calcination and in-situ deposition methods.The introduction of Ce can inhibit the conversion of Bi_(2)O_(3)fromβtoαphase at high temperatures,promoting the formation of oxygen vacancies(OVs)in the photocatalyst.OVs can adsorb more dissolved oxygen to promote the formation rate of·O^(-)_(2).Moreover,the interaction between Ce-Bi_(2)O_(3)and AgI results in the formation of Z-scheme heterojunctions,which can broaden the light absorption region,facilitate photogenerated carrier separation and transfer and enhance the ability to produce more active oxygen species(ROS).The morphology,crystal,element distribution and photo-electric chemical properties of the Ce-Bi_(2)O_(3)/AgI were analyzed,and the result shows that the optimal ratio of Ce-Bi_(2)O_(3)/AgI photocatalyst achieves a removal rate of 88.63%(180 min)of tetracycline(TC)(20 mg/L)and 100%(120 min)of methyl orange(MO)(20 mg/L).This work clarified the photocatalytic degradation mechanism,providing a promising avenue for developing photocatalytic composites by rare earth metal doping in environme ntal remediation applications.展开更多
Water purification systems based on transition metal dichalcogenides face significant challenges,including lack of reactivity under dark conditions,scarcity of catalytically active sites,and rapid recombination of pho...Water purification systems based on transition metal dichalcogenides face significant challenges,including lack of reactivity under dark conditions,scarcity of catalytically active sites,and rapid recombination of photogenerated charge carriers.Simultaneously increasing the number of active sites and improving charge separation efficiency has proven difficult.In this study,we present a novel approach combining molybdenum(Mo) monoatomic doping and size engineering to produce a series of Mo-ReS_(2) quantum dots(MR QDs) with controllable dimensions.High-resolution structural characterization,first-principle calculations,and piezo force microscopy reveal that Mo monoatomic doping enhances the lattice asymmetry,thereby improving the piezoelectric properties.The resulting piezoelectric polarization and the generated built-in electric field significantly improve charge separation efficiency,leading to optimized photocatalytic performance.Additionally,the doping strategy increases the number of active sites and improves the adsorption of intermediate radicals,substantially boosting photo-sterilization efficiency.Our results demonstrate the elimination of 99.95% of Escherichia coli and 100.00% of Staphylococcus aureus within 30 min.Furthermore,we developed a self-purification system simulating water drainage,utilizing low-frequency water streams to trigger the piezoelectric behavior of MR QDs,achieving piezoelectric synergistic photodegradation.This innovative approach provides a more environmentally friendly and economical method for water self-purification,paving the way for advanced water treatment technologies.展开更多
This work reports a soft chemistry approach for the synthesis of magnesium oxide nanoparticles(MgO)incorporated in a polyaniline(PANI)matrix to give PANI/MgO nanocomposite.Using spin coating method,three different per...This work reports a soft chemistry approach for the synthesis of magnesium oxide nanoparticles(MgO)incorporated in a polyaniline(PANI)matrix to give PANI/MgO nanocomposite.Using spin coating method,three different percentages of MgO/PVC(1,2,and 3%in wt.%)were deposited on glass substrates.These films of PANI/MgO nanocomposite were characterized by X-ray diffraction(XRD),atomic force microscopy(AFM),and UV-visible spectroscopy.The results of the XRD pattern revealed the embedding of MgO nanoparticles in the PANI matrix with cubic phase,with the average size of nanoparticles varying from 35.12 to 59.55 nm.The AFM images displayed a significant change in the morphology of the PANI/MgO NPs composite films as MgO concentration was increased.The optical transmittance analysis revealed that at very low concentrations of MgO in PANI/MgO nanocomposite films,there is a high transparency,reaching close to 90%.However,this transmittance decreases significantly as the concentration of MgO increases.The photocatalytic activity of the nanocomposite film was then evaluated for the degradation of methylene blue(MB)dye under UV light irradiation.The results indicated a strong potential for PANI/MgO nanocomposite films in effectively degrading MB,supported by a proposed mechanism for the photocatalytic reaction.Compared with other composites such as PVC/MgO,PANI/MgO nanocomposite presented better MB degradation efficiency.展开更多
This article systematically reviewed the applications of single-atom catalysts(SACs)in the domain of photocatalytic reactions,with a particular emphasis on the indispensable role of H_(2)O in these processes.SACs,due ...This article systematically reviewed the applications of single-atom catalysts(SACs)in the domain of photocatalytic reactions,with a particular emphasis on the indispensable role of H_(2)O in these processes.SACs,due to their distinct active sites and superior catalytic efficacy,found their applications in the fields of energy conversion and environmental protection.The review elaborated on the potential carriers,preparation methods,and characterization techniques for single-atom photocatalysts.Subsequently,the article provided an in-depth explanation of the crucial role of H_(2)O in photocatalytic reactions,serving as an important green solvent and an oxygen/proton source.The adsorption of water could also change the surface energy structure and charge distribution of the photocatalyst.Conversely,the presence of H_(2)O might also inhibit the target reaction.Additionally,the distinct roles of water in both liquid and gas phases were discussed.Furthermore,the review systematically summarized the applications of single-atom photocatalysts in H_(2)generation,CO_(2)reduction,N2fixation,H_(2)O_(2)production,and environmentalremediation.It delved into the mechanisms by which water molecules participated in photocatalytic processes and their interactions with competing pathways,thereby revealing the complexity and critical importance of water in photocatalytic reactions.Finally,the article discusses the opportunities and challenges of SACs in photocatalytic reactions with H_(2)O.This article provides a comprehensive perspective for understanding the role of SACs in waterinvolved photocatalytic reactions.展开更多
Photocatalysis,harnessing abundant solar energy,presents a sustainable strategy to address the dual chal-lenges of fossil fuel depletion and environmental degradation.Among the emerging materials for photo-catalytic a...Photocatalysis,harnessing abundant solar energy,presents a sustainable strategy to address the dual chal-lenges of fossil fuel depletion and environmental degradation.Among the emerging materials for photo-catalytic applications,reticular framework materials,including metal-organic frameworks(MOFs),cova-lent organic frameworks(COFs),and hydrogen-bonded organic frameworks(HOFs),have attracted signif-icant attention due to their high surface area,tunable architectures,and versatile chemical compositions.These properties enable efficient light harvesting and charge separation,making them promising candi-dates for various photocatalytic processes.This review systematically explores recent advancements in the synthesis and structural properties of MOFs,COFs,and HOFs,elucidating the complex mechanisms governing solar-driven photocatalysis and comparing their performance with a particular focus on their applications in CO_(2)reduction,H_(2)generation,H_(2)O_(2)production,N_(2)fixation,and pollutant degradation.Key strategies for enhancing photocatalytic performance,including structural modifications,bandgap en-gineering,defect engineering,hybridization,and heterojunction formation,are critically analyzed.A com-parative evaluation of reticular framework materials against traditional semiconductors is provided,con-sidering factors such as efficiency,cost,and long-term stability.Furthermore,this review highlights the challenges related to stability and scalability,along with key achievements and barriers to practical im-plementation.This work offers possible insights to overcome existing limitations and improve efficiency.Ultimately,this comprehensive assessment highlights the pivotal role of reticular frameworks in advanc-ing sustainable energy solutions and provides a roadmap for future research and innovation in this rapidly evolving field.展开更多
文摘The growing presence of emerging pollutants in the environment has led to a focus on developing new treatment technologies to address the limitations of traditional methods.Recent advancements in combining photocatalysis with biodegradation for pollutant treatment have garnered significant attention.This is due to the rapid and uncontrolled chemical reactions in single photocatalytic processes,which often result in the buildup of harmful by-products and over-oxidation residues.Additionally,relying solely on biodegradation is challenging for breaking down emerging pollutants that possess high concentrations and intricate structures.Therefore,the intimately coupled photocatalysis and biodegradation(ICPB)systems,along with the photocatalytic microbial fuel cells(PMFCs),as a new approach to treat pollutants.These systems combine the benefits of biodegradation and photocatalytic reactions,providing cost-effective,eco-friendly,and sustainable solutions with significant promise.In order to demonstrate the ICPB system and the PMFCs system as rational options for pollutant removal,the mechanisms of pollutant degradation by the two systems have been analyzed in depth,and recent advances in photocatalysts,biofilms,and carriers/configurations in the two systems have been summarized.Furthermore,the practical applications of the ICPB system versus the PMFCs system for pollutant removal are also summarized and highlighted.This review further points out the current limitations,such as photocatalytic materials that are still challenging in terms of commercial viability for practical applications,and looks forward to the prospects of the ICPB system versus the PMFCs system for the treatment of pollutants to promote practical applications.
基金supported by Liaoning Revitalization Talents Program(No.XLYC1907173)the Science and Technology General Project of Liaoning Provincial Education Department(No.LJKMZ20221835)the National Natural Science Foundation of China(Nos.22006073 and 22205027).
文摘The mass production and widespread use of Pharmaceuticals and Personal Care Products(PPCPs)have posed a serious threat to the water environment and public health.In this work,a green metal-based Metal Organic Framework(MOF)Bi-NH_(2)-BDC was prepared and characterized,and the adsorption characteristics of Bi-NH_(2)-BDCwere investigated with typical PPCPs-diclofenac sodium(DCF).It was found that DCF mainly covered the adsorbent surface as a single molecular layer,the adsorption reaction was a spontaneous,entropyincreasing exothermic process and the adsorption mechanisms between Bi-NH_(2)-BDC and DCF were hydrogen bonding,π-πinteractions and electrostatic interactions.In addition,Bi-NH_(2)-BDC also had considerable photocatalytic properties,and its application in adsor-bent desorption treatment effectively solved the problem of secondary pollution,achieving a green and sustainable adsorption desorption cycle.
文摘The production of renewable methanol(CH_(3)OH)via the photocatalytic hydrogenation of CO_(2) is an ideal method to ameliorate energy shortages and mitigate CO_(2) emissions:however,the highly selective synthesis of methanol at atmospheric pressure remains challenging owing to the competing reverse water-gas shift(RWGS)reaction.Herein,we present a novel approach for the synthesis of CH_(3)OH via photocatalytic CO_(2) hydrogenation using a catalyst featuring highly dispersed Au nanoparticles loaded on oxygen vacancy(OV)-rich molybdenum dioxide(MoO_(2)),resulting in a remarkable selectivity of 43.78%.The active sites in the Au/MoO_(2) catalyst are high-density Au-oxygen vacancies,which synergistically promote the tandem methanol synthesis via an initial RWGS reaction and subsequent CO hydrogenation.This work provides comprehensive insights into the design of metal-vacancy synergistic sites for the highly selective photocatalytic hydrogenation of CO_(2) to CH_(3)OH.
文摘Semi-heterogeneous photocatalysis has emerged as a powerful and productive platform in organic chemistry,which provides mild and eco-friendly conditions for a diverse range of bond-forming reactions.The synergy of homogeneous catalysts and heterogeneous catalysts inherits their main advantages,such as higher activities,easy separation and superior recyclability.In this review,we summarize the recent advances in recyclable semi-heterogenous protocols for the light promoted bond-forming reactions and identify directions for future research according to the different photocatalysts/metal/redox catalysts involved.Notably,this review is not a comprehensive description of reported literature but aim to highlight and illustrate key concepts,strategies,reaction model,reaction conditions and mechanisms.
基金the National Natural Science Foundation of China(No.52205210)the Natural Science Foundation of Shandong Province(Nos.ZR2020MB018,ZR2022QE033 and ZR2021QB049).
文摘Achieving artificial simulations of multi-step energy transfer processes and conversions in nature remains a challenge.In this study,we present a three-step sequential energy transfer process,which was constructed through host-vip interactions between a piperazine derivative(PPE-BPI)with aggregationinduced emission(AIE)and cucurbit[7]uril(CB[7])in water to serve as ideal energy donors.To achieve multi-step sequential energy transfer,we employ three distinct fluorescent dyes Eosin B(EsB),Sulforhodamine 101(SR101),and Cyanine 5(Cy5)as energy acceptors.The PPE-PBI-2CB[7]+EsB+SR101+Cy5 system demonstrates a highly efficient three-step sequential energy transfer mechanism,starting with PPEPBI-2CB[7]and transferring energy successively to EsB,SR101,and finally to Cy5,with remarkable energy transfer efficiencies.More interestingly,with the progressive transfer of energy in the multi-step energy transfer system,the generation efficiency of superoxide anion radical(O_(2)•-)increased gradually,which can be used as photocatalysts for selectively photooxidation of N-phenyltetrahydroisoquinoline in an aqueous medium with a high yield of 86%after irradiation for 18 h.This study offers a valuable investigation into the simulation of multi-step energy transfer processes and transformations in the natural world,paving the way for further research in the field.
基金Sponsorship Program by CAST(2023QNRC001)University-Industry Collaborative Education Program(220901115200913,220901115201954)+2 种基金Hunan Provincial Natural Science Foundation of China(2022JJ40007)Jiangsu Agricultural Science and Technology Innovation Fund(CX(22)3047)the National Natural Science Foundation of China(32201491)。
文摘Carbon quantum dots are a new type of fluorescent nanomaterials with broad applications in drug delivery,bioimaging,solar cells,and photocatalysis due to their unique biocompatibility,optical properties and easy functionalization.In the meantime,because of its high carbon content,renewable nature,and environmental friendliness,lignin has drawn the attention of researchers as a desirable raw material for creating carbon quantum dots.Here we review the synthesis of carbon quantum dots from lignin,focusing on synthetic methods,properties,and applications in energy,and photocatalysis.Later,we propose some new development prospects from preparation methods,luminescence mechanism research,application,and commercial cost of lignin carbon quantum dots.Finally,based on this,the development prospects of this field are prospected and summarized.
基金partly supported by the National Natural Science Foundation of China(21978276)。
文摘Photocatalysis(PC)and photoelectrocatalysis(PEC)represent promising and efficient avenues for harnessing solar energy to produce sustainable clean energy products and environmental remediation.Yet the current reaction efficiencies remain inadequate,limiting their efficiencies for practice.Despite the growing interest in photo thermal-driven PC/PEC systems,there is no comprehensive review that systematically summarises the role of the photothermal effect in bridging the gap between PC and PEC efficiencies.This review initially introduces the fundamental principles of PC and PEC,alongside the primary photothermal materials and relevant conversion mechanisms.Subsequently,the key influences of photothermal effects on PC and PEC performance(e.g.,light absorption,charge separation and transport,and surface reactions)and optimization strategies are discussed.In addition,the latest advancements in solar photothermal conversion are discussed,mainly focused on the widely application of different types of photothermal drive PC and PEC applications,such as PC and PEC oxygen evolution reaction(OER),hydrogen evolution reaction(HER),CO_(2)reduction reaction(CO_(2)RR),pollutant degradation,and sterilization,serving to illustrate the widespread applicability of the photothermal conversion.Finally,the development prospects and challenges of photothermal-assisted PC and PEC are discussed from the perspective of basic research and practical application.This work provides a timely and systematic framework to guide the rational design of photothermal-enhanced PC/PEC systems for sustainable energy and environmental applications.
基金supported by the Jiangsu Province Key Laboratory of Fine Petrochemical Engineering(No.KF2204).
文摘Natural fibers,as a typical renewable and biodegradable material,have shown great potential for many applications(e.g.,catalysis,hydrogel,biomedicine)in recent years.Recently,the growing importance of natural fibers in these photo-driven applications is reflected by the increasing number of publications.The utilization of renewable materials in photo-driven applications not only contributes to mitigating the energy crisis but also facilitates the transition of society toward a low-carbon economy,thus enabling harmonious coexistence between humans and the environment within the context of sustainable development.This paper provides an overview of the recent advances of natural fibers which acted as substrates or precursors to construct an efficient system of light utilization.The different chemical properties and pretreatment methods of cellulose affect its performance in final photo-driven applications,including solar-driven water purification,photocatalysis,and photothermal biomedical applications.Nevertheless,current research rarely conducts a comprehensive comparisonof themfromabroadperspective.As a whole,this review first reveals the different structural advantages as well as thematching degree between natural fibers(bacterial cellulose,plant cellulose,and animal fiber)and three typical photo-driven applications.Besides,new strategies for optimizing the utilization of natural fibers are an important subject under the background of low-carbon and circular economy.Finally,some suggestions and prospects are put forward for the limitations and research prospects of natural fibers in photo-driven applications,which provides a new idea for the synthesis of renewable functional materials.
基金supported by the National Key R&D Program of China(No.2021YFA1502300)the National Natural Science Foundation of China(Nos.22103012,22173105)+2 种基金the Natural Science Foundation of Fujian Province(Nos.2024J01456,2024J01191)the Selfdeployment Project Research Program of Haixi Institutes,Chinese Academy of Sciences(No.CXZX-2022-GH10)the CAS Youth Interdisciplinary Team.
文摘Crystal defects and morphological modifications are popular strategies to enhance the catalytic activity of heterogeneous semiconductor photocatalysts.Despite defect engineering and morphology control show their successful applications in ZnO,the effects of curved surface modifications on the photocatalytic performance of ZnO and their interplay with the defect formation remain unclear.To resolve this puzzle,we systemically investigate the joint effects of curvature and defect formation on the electronic structure,optoelectronic properties,and photocatalytic performance of ZnO slabs using first-principles calculations.We find that curvature deformation effectively narrows the electronic bandgap by up to 1.6 eV and shifts the p-/d-band centers,thereby enhancing light absorption in the visible and near-ultraviolet regions.Besides,curvature deformation stimulates self-polarization,facilitating the separation of photogenerated electrons and holes.Also,curvature deformation promotes the formation of defects by reducing defect formation energy(by up to 1.0 eV),thus creating abundant reaction sites for photocatalysis.Intriguingly,the synergistic interaction between curvature and defect deformation further strengthens the self-polarization,narrows the electronic bandgaps,adjusts the p-/d-band centers to improve the optoelectronic properties,and influences the dissociation and free energy barriers of intermediates.Consequently,our findings reveal that this synergy substantially enhances the photocatalytic performance of ZnO slabs,providing deeper insights into the role of defect engineering and morphology control on photocatalysis.
基金financially supported by the National Natural Science Foundation of China(Nos.52100032 and 52350005)the Basic and Applied Basic Research Project of Guangzhou(Nos.2024A04J3679 and 2024A03J0088)+2 种基金the Introduced Innovative Research and Development Team Project under the“The Pearl River Talent Recruitment Program”of Guangdong Province(No.2019ZT08L387)the Opening Project of Shanxi Province Key Laboratory of Chemical Process Intensification,North University of China(No.2023-HOCE10)the National College Students’Innovation and Entrepreneurship Training Program(No.202211078135)
文摘The introduction of metal single atoms(SAs)into semiconductors can effectively optimize their electronic configuration and enhance their photocatalytic properties.Therefore,it is crucial to clarify the corresponding principles and photocatalytic mechanisms for efficient and sustainable photocatalytic water remediation systems.Herein,a promising Fe single-atom photocatalyst(Fe_(SA)-CN)is obtained by anchoring Fe SAs in graphitic carbon nitride using a simple calcination strategy.Characterization and experimental results indicate that the modification of Fe SAs not only introduces a doping energy level,but also changes the valence band position,which expands the light absorption range,enhances the reduction ability of photogenerated electrons,and improves the separation and transfer of photogenerated charge carriers.Subsequently,contaminants adsorbed on the FeSA-CN surface trigger their oxidation removal by h^(+),and the H_(2)O_(2)generated via two-electron direct reductions is converted in situ into OH by self-Fenton reaction for the synergistic contaminant degradation.In summary,FeSA-CN offers a promising pathway for single-atom photocatalysts in water remediation because of outstanding contamination removal efficiency,adaptability,and stability.
文摘Covalent organic frameworks(COFs)based photocatalysts utilizing infrared light remains unexplored due to the limitation of electronic absorption.Herein,two novel two-dimensional(2D)polyimide-linked phthalocyanine COFs,namely MPc-DPA-COFs(M=Zn/Cu),were prepared from the imidization reaction of metal tetraanhydrides of 2,3,9,10,16,17,23,24-octacarboxyphthalocyaninato(M(TAPc))with 9,10-diphenyl anthracene(DPA).Both COFs possess highly crystalline eclipsed AA stacking structure with neighboring layer distance of 0.33 nm on the basis of powder X-ray diffraction analysis and high-resolution transmission electron microscopy.Effective π–π interaction between phthalocyanine chromophores in neighboring layers of 2D COFs leads to significant bathochromic-shift of narrow Q band from 697 nm for M(TAPc)to the infrared light absorption range of 760–1000 nm for MPc-DPA-COFs according to solid UV-vis diffuse reflectance spectra.This endows them in particular ZnPc-DPA-COF with excellent reactive oxygen species of•O_(2)^(–)and 1O_(2) generation activity under infrared light radiation(λ>760 nm)based on the electron spin resonance spectroscopy measurement,in turn resulting in the excellent photocatalytic capacity towards oxidation of sulfides under infrared light radiation.Corresponding quenching experiments reveal the contribution of both•O_(2)^(–)and 1O_(2) to the oxidation of sulfides,but the former•O_(2)^(–)species plays a leading role in this photocatalytic process.The present result not only provides a new efficient infrared light photocatalyst but also unveils the good potentials of phthalocyanine-based COFs in photocatalysis.
基金supported by National Natural Science Foundation of China(22171041,22071020,52130101)National Key R&D Program of China(2023YFB3003001)+2 种基金Natural Science Foundation of Jilin Province Science and Technology Department(discipline layout project)(grant no.20230508094RC)the Fundamental Research Funds for the Central Universities(grant no.2412021QD008)the Fundamental Research Funds for the Central Universities-Excellent Youth Team Program(2412023YQ001).
文摘In conjugated polymers(CPs)photocatalytic system,the generation of reactive oxygen species(ROS)is regulated by cross-scale factors involving active site,excitonic behavior,and O_(2)activation process on the surface.However,research on exploring the domino effect of“structure→excitonic behavior→O_(2)activation→photocatalytic reaction”through structural modification at the atomic scale remains at its early stages.Herein,two heptazine-based CPs,CP-DPA,and CP-CZ were successfully prepared by polymerization of precursors formed by reacting diphenylamine(DPA)and carbazole(CZ)with cyameluric chloride,respectively.The minute difference in single bond between DPA and CZ endows the polymers with distinct physicochemical properties.Owing to the rotation between benzene rings,CP-DPA exhibits relatively lower conjugation,resulting in increased exciton binding energy(Eb)and inhibited exciton dissociation.Meanwhile,its more triplet state excitons facilitate energy transfer to generate singlet oxygen.Therefore,CP-DPA shows excellent activity for phenylboronic acid oxidation.Conversely,CP-CZ possesses relatively higher conjugation,minimal Eb and intensified exciton dissociation,which promotes charge transfer to produce superoxide radical.Consequently,CP-CZ displays optimal activity for phe-nylacetylene oxidation and[3+2]cycloaddition.This work provides new insights into regulating ROS gener-ation by modulating the composition and structure of photocatalysts at the atomic scale.
基金financially supported by the National Natural Science Foundation of China(No.51302061)Natural Science Foundation of Hebei Province(No.E2020201021 and E2023201019)+4 种基金Industry-University-Research Cooperation Major Projects of Shijiazhuang(No.241130477A)Research Innovation Team of College of Chemistry and Environmental Science of Hebei University(No.hxkytd2102)Industry-University-research Cooperation Project of Colleges and Universities in Hebei Province(No.CXZX2025016)Hebei Province Innovation Capability Enhancement Plan Project(No.22567620H)Bintuan Science and Technology Program(Nos.2020DB002 and 2022DB009)。
文摘Peroxymonosulfate(PMS)is commonly used in advanced oxidation processes to degrade organic pollutants in wastewater.In this work,to obtain better PMS activation efficiency,Bi_(4)O_(5)Br_(2)/BCZT(BBT)piezoelectric photocatalyst was designed.Abundant active radicals produced by BBT under visible light irradiation and ultrasonic vibration were used to activate PMS,thereby achieving rapid degradation of high concentration pollutants.With the introduction of BCZT,the catalyst has a strong internal electric field and three-dimensional lamellar structure,which promotes the separation and transfer of electrons and holes.It is worth noting that under optimal reaction conditions,the degradation rate of ARB reached 93%by BBT15 within 10 min.The catalytic experiment combined with the piezoelectric performance test results revealed the key role of piezoelectric photocatalytic reaction in PMS activation.This provides an important prospect for PMS to effectively deal with the degradation of high concentrations of organic pollutants.
文摘Reactive oxygen species(ROS),including singlet oxygen(^(1)O_(2)),hydroxyl radicals(·OH),and superoxide anions(O_(2)^(·-)),are highly reactive molecules that play central roles in many chemical,biological,and environmental processes due to their strong oxidative power[1].Generating ROS in a controlled manner under mild conditions is essential for achieving selective oxidation reactions.Light-driven methods are especially appealing for this purpose,as they offer precise control over where and when ROS are produced.
基金supported by the National Natural Science Foundation of China(No.22271090)。
文摘Herein,a simple and effective outer-surface interactions assisted supramolecular hierarchical assembly has been first exploited to uniformly distribute tungstosilicic acid(TSA)inside the porous structure of cucurbit[10]uril-based single-layer 2D supramolecular-organic-frameworks(Q[10]-SOFs)in water.Importantly,the 2D Q[10]-SOFs can further serve as light harvesting antenna,achieving fast energy transfer to the embedded redox-active TSA upon photoexcitation,resulting in efficient visible light-driven selective oxidation of benzyl alcohols into the corresponding aldehydes in high yield at room temperature.Further studies revealed that the integrated of 2D Q[10]-SOFs and TSA played a key role in the catalytic process,due to the presence of a novel stepwise electron transfer route in the single-layer hybrid 2D structures.
基金Project supported by the National Natural Science Foundation of China(22106074)Tianjin Science and Technology Program(23YDTPJC00540,22YJDSS00060)。
文摘Ce-β-Bi_(2)O_(3)/AgI was prepared using solvothermal calcination and in-situ deposition methods.The introduction of Ce can inhibit the conversion of Bi_(2)O_(3)fromβtoαphase at high temperatures,promoting the formation of oxygen vacancies(OVs)in the photocatalyst.OVs can adsorb more dissolved oxygen to promote the formation rate of·O^(-)_(2).Moreover,the interaction between Ce-Bi_(2)O_(3)and AgI results in the formation of Z-scheme heterojunctions,which can broaden the light absorption region,facilitate photogenerated carrier separation and transfer and enhance the ability to produce more active oxygen species(ROS).The morphology,crystal,element distribution and photo-electric chemical properties of the Ce-Bi_(2)O_(3)/AgI were analyzed,and the result shows that the optimal ratio of Ce-Bi_(2)O_(3)/AgI photocatalyst achieves a removal rate of 88.63%(180 min)of tetracycline(TC)(20 mg/L)and 100%(120 min)of methyl orange(MO)(20 mg/L).This work clarified the photocatalytic degradation mechanism,providing a promising avenue for developing photocatalytic composites by rare earth metal doping in environme ntal remediation applications.
基金financially supported by the National Natural Science Foundation of China (No.52071146)Guangdong Provincial Natural Science Foundation (No.2023A1515010989)the Science and Technology Projects in Guangzhou (No.202201000008)。
文摘Water purification systems based on transition metal dichalcogenides face significant challenges,including lack of reactivity under dark conditions,scarcity of catalytically active sites,and rapid recombination of photogenerated charge carriers.Simultaneously increasing the number of active sites and improving charge separation efficiency has proven difficult.In this study,we present a novel approach combining molybdenum(Mo) monoatomic doping and size engineering to produce a series of Mo-ReS_(2) quantum dots(MR QDs) with controllable dimensions.High-resolution structural characterization,first-principle calculations,and piezo force microscopy reveal that Mo monoatomic doping enhances the lattice asymmetry,thereby improving the piezoelectric properties.The resulting piezoelectric polarization and the generated built-in electric field significantly improve charge separation efficiency,leading to optimized photocatalytic performance.Additionally,the doping strategy increases the number of active sites and improves the adsorption of intermediate radicals,substantially boosting photo-sterilization efficiency.Our results demonstrate the elimination of 99.95% of Escherichia coli and 100.00% of Staphylococcus aureus within 30 min.Furthermore,we developed a self-purification system simulating water drainage,utilizing low-frequency water streams to trigger the piezoelectric behavior of MR QDs,achieving piezoelectric synergistic photodegradation.This innovative approach provides a more environmentally friendly and economical method for water self-purification,paving the way for advanced water treatment technologies.
文摘This work reports a soft chemistry approach for the synthesis of magnesium oxide nanoparticles(MgO)incorporated in a polyaniline(PANI)matrix to give PANI/MgO nanocomposite.Using spin coating method,three different percentages of MgO/PVC(1,2,and 3%in wt.%)were deposited on glass substrates.These films of PANI/MgO nanocomposite were characterized by X-ray diffraction(XRD),atomic force microscopy(AFM),and UV-visible spectroscopy.The results of the XRD pattern revealed the embedding of MgO nanoparticles in the PANI matrix with cubic phase,with the average size of nanoparticles varying from 35.12 to 59.55 nm.The AFM images displayed a significant change in the morphology of the PANI/MgO NPs composite films as MgO concentration was increased.The optical transmittance analysis revealed that at very low concentrations of MgO in PANI/MgO nanocomposite films,there is a high transparency,reaching close to 90%.However,this transmittance decreases significantly as the concentration of MgO increases.The photocatalytic activity of the nanocomposite film was then evaluated for the degradation of methylene blue(MB)dye under UV light irradiation.The results indicated a strong potential for PANI/MgO nanocomposite films in effectively degrading MB,supported by a proposed mechanism for the photocatalytic reaction.Compared with other composites such as PVC/MgO,PANI/MgO nanocomposite presented better MB degradation efficiency.
基金financially supported by Guangdong Basic and Applied Basic Research Foundation(No.2024A1515010976)Shenzhen Peacock Plan(No.20210802524B)+3 种基金the Postdoctoral Research Foundation of China(Nos.GZC20241085,GZC20230562,GZC20230564)China Postdoctoral Science Foundation(No.2024M760583)the National Natural Science Foundation of China(No.52402234)Shenzhen Key Laboratory of 2D Metamaterials for Information Technology
文摘This article systematically reviewed the applications of single-atom catalysts(SACs)in the domain of photocatalytic reactions,with a particular emphasis on the indispensable role of H_(2)O in these processes.SACs,due to their distinct active sites and superior catalytic efficacy,found their applications in the fields of energy conversion and environmental protection.The review elaborated on the potential carriers,preparation methods,and characterization techniques for single-atom photocatalysts.Subsequently,the article provided an in-depth explanation of the crucial role of H_(2)O in photocatalytic reactions,serving as an important green solvent and an oxygen/proton source.The adsorption of water could also change the surface energy structure and charge distribution of the photocatalyst.Conversely,the presence of H_(2)O might also inhibit the target reaction.Additionally,the distinct roles of water in both liquid and gas phases were discussed.Furthermore,the review systematically summarized the applications of single-atom photocatalysts in H_(2)generation,CO_(2)reduction,N2fixation,H_(2)O_(2)production,and environmentalremediation.It delved into the mechanisms by which water molecules participated in photocatalytic processes and their interactions with competing pathways,thereby revealing the complexity and critical importance of water in photocatalytic reactions.Finally,the article discusses the opportunities and challenges of SACs in photocatalytic reactions with H_(2)O.This article provides a comprehensive perspective for understanding the role of SACs in waterinvolved photocatalytic reactions.
基金financially supported by the National Natural Science Foundation of China(Nos.22350410391 and 22001094)the Research Initiation Fund Project from Zhejiang Sci-Tech University(No.23212072-Y).
文摘Photocatalysis,harnessing abundant solar energy,presents a sustainable strategy to address the dual chal-lenges of fossil fuel depletion and environmental degradation.Among the emerging materials for photo-catalytic applications,reticular framework materials,including metal-organic frameworks(MOFs),cova-lent organic frameworks(COFs),and hydrogen-bonded organic frameworks(HOFs),have attracted signif-icant attention due to their high surface area,tunable architectures,and versatile chemical compositions.These properties enable efficient light harvesting and charge separation,making them promising candi-dates for various photocatalytic processes.This review systematically explores recent advancements in the synthesis and structural properties of MOFs,COFs,and HOFs,elucidating the complex mechanisms governing solar-driven photocatalysis and comparing their performance with a particular focus on their applications in CO_(2)reduction,H_(2)generation,H_(2)O_(2)production,N_(2)fixation,and pollutant degradation.Key strategies for enhancing photocatalytic performance,including structural modifications,bandgap en-gineering,defect engineering,hybridization,and heterojunction formation,are critically analyzed.A com-parative evaluation of reticular framework materials against traditional semiconductors is provided,con-sidering factors such as efficiency,cost,and long-term stability.Furthermore,this review highlights the challenges related to stability and scalability,along with key achievements and barriers to practical im-plementation.This work offers possible insights to overcome existing limitations and improve efficiency.Ultimately,this comprehensive assessment highlights the pivotal role of reticular frameworks in advanc-ing sustainable energy solutions and provides a roadmap for future research and innovation in this rapidly evolving field.
