Photo-assisted Li-O2 batteries(LOBs)have remained a prominent and growing field over the past several years.However,the presence of slow oxygen reduction reaction(ORR)and oxygen evolution reaction(OER),large charging ...Photo-assisted Li-O2 batteries(LOBs)have remained a prominent and growing field over the past several years.However,the presence of slow oxygen reduction reaction(ORR)and oxygen evolution reaction(OER),large charging and discharging overpotentials,and unstable cycle life lead to low energy efficiency,thus limiting their commercial application.The rational design and synthesis of photocathode materials are effective ways to solve the above existing problems of photo-assisted LOB systems.Herein,the recent advances in the design and preparation of photocathode materials for photo-assisted LOBs were summarized in this review.First,we summarize the basic principles and comprehension of the reaction mechanism for photo-assisted LOBs.The second part introduces the latest research progress on photocathode materials.The third section describes the relationship between the structureproperties and electrochemistry of different photocathodes.In addition,attempts to construct efficient photocathode materials for photo-assisted LOBs through vacancy engineering,localized surface plasmon resonance(LSPR),and heterojunction engineering are mainly discussed.Finally,a discussion of attempts to construct efficient photocathode materials using other approaches is also presented.This work will motivate the preparation of stable and efficient photocathode materials for photo-assisted LOBs and aims to promote the commercial application of rechargeable photo-assisted LOBs energy storage.展开更多
Electrocatalysis for nitrate(NO_(3^(–)))removal from wastewater faces the challenge of merging efficient reduction and high selectivity to nitrogen(N2)with economic viability in a durable catalyst.In this study,bimet...Electrocatalysis for nitrate(NO_(3^(–)))removal from wastewater faces the challenge of merging efficient reduction and high selectivity to nitrogen(N2)with economic viability in a durable catalyst.In this study,bimetallic PdCu/TiO_(x)composite catalysts were synthesized with varying Pd and Cu ratios through electrochemical deposition on defective TiOxnanotube arrays.Denitrification experiments demonstrated that the Pd_(1)Cu_(1)/TiO_(x)catalyst exhibited the highest(NO_(3^(–)))removal rate(81.2%)and N_(2)selectivity(67.2%)among all tested catalysts.Leveraging the exceptional light-responsive property of TiO_(x),the introduction of light energy as an assisting factor in electrocatalysis further augmented the(NO_(3^(–)))treatment rate,resulting in a higher(NO_(3^(–)))removal rate of 95.1%and N_(2)selectivity of approximately 90%.Compared to individual electrocatalysis and photocatalysis systems,the overpotential for the catalytic interface active*H formation in the photo-assisted electrocatalysis system was remarkably reduced,thus accelerating electron migration and promoting(NO_(3^(–)))reduction kinetics.Economic analysis revealed an energy consumption of 2.74 k Wh/mol and a corresponding energy consumption per order(EEO)of 0.79 k Wh/m^(3)for the Pd_(1)Cu_(1)/TiOxcatalyst to reduce 25.2 mg/L of(NO_(3^(–)))-N in water to N_(2),showcasing remarkable competitiveness and economic advantages over other water treatment technologies.This study developed the PdCu/TiOxelectrocatalysts with high(NO_(3^(–)))removal rates and N_(2)selectivity,particularly when combined with light energy,the efficiency and selectivity were significantly enhanced,offering a competitive and economically viable solution for wastewater treatment.展开更多
In recent years,photo-powered energy storage devices have attracted considerable research attention due to their potential applications in smart electronics.In this review,we present a comprehensive summary of recent ...In recent years,photo-powered energy storage devices have attracted considerable research attention due to their potential applications in smart electronics.In this review,we present a comprehensive summary of recent developments in two distinct but highly promising energy storage technologies,photo-assisted metal-air batteries and photo-supercapacitors.The section on metal-air batteries primarily describes the electrochemical performance of Zn-air and Li-air systems,innovative photo-electrode designs,and mechanisms that enhance oxygen evolution and reduction reactions.A brief discussion is also provided of other metal-air systems,including Mg,Fe,and Al.In contrast,the section on photo-supercapacitors explores recent advancements in light-driven charge storage,electrode materials,and device architectures,presenting a comparative performance analysis of materials such as metal oxides,sulfides,and perovskites.Various critical challenges,including material stability,efficiency under varying light conditions,and scalability,are also thoroughly examined.Despite their different working principles,both technologies hold great potential to increase energy efficiency and sustainability through the use of photo-assisted processes.The purpose of this review is to bridge existing knowledge gaps and propose future directions for research in these emerging fields.展开更多
In this study,we developed a tandem photo-assisted electrochemical(PA-EC)chemical strategy for both energy-saving ammonia/fertilizer synthesis and comprehensive nitrogen-and phosphorus-rich wastewater treatment,in whi...In this study,we developed a tandem photo-assisted electrochemical(PA-EC)chemical strategy for both energy-saving ammonia/fertilizer synthesis and comprehensive nitrogen-and phosphorus-rich wastewater treatment,in which synchronous hypophosphite ion(H_(2)PO_(2)^(-))oxidation to phosphate ion(PO_(4)^(3–))(POR)and nitrate reduction(NO_(3)RR)to ammonia(NH_(3))occur,followed by cascade chemical precipitation to generate struvite.Herein,a bifunctional Cu_(2)O@NiFe_(2)O_(4)Z-scheme heterojunction with a yolk/shell structure and oxygen vacancies(OVs)was designed and developed to optimize the NO_(3)RR/POR.Serving as a key component,the established PA-EC system consisted of a Janus Cu_(2)O@NiFe_(2)O_(4)/NF self-supporting integrated photocathode and a Cu_(2)O@NiFe_(2)O_(4)/NF photocathode with efficient struvite PA-EC synthesis performance under a low cell voltage of 1.6 V vs NHE.Specifically,Janus Cu_(2)O@NiFe_(2)O_(4)/NF photocathode exhibits superior performance with a high NH3 yield of 38.06 mmol L^(-1)and a faradaic efficiency(FE)of 92.31%at 1.6 V vs.NHE and enables ammonia FE over 60%in a broad NO_(3)–concentration window of 0.005–0.5 mol L^(-1).The photoassisted electrochemical catalytic mechanism and reaction pathway for struvite synthesis on Cu_(2)O@NiFe_(2)O_(4)were investigated through a series of experiments and theoretical calculations.The results demonstrated the critical roles of the interfacial electric field,void confinement,and oxygen vacancies in promoting the overall catalytic efficiency.These encouraging results warrant further studies on combined P and N recovery for efficient production of valuable fertilizers.展开更多
The effective detection of trace methyl mercaptan(CH_(3)SH)with low power consumption is crucial for assessing air quality and facilitating non-invasive diagnosis of diseases such as periodontitis.Herein,we synthesize...The effective detection of trace methyl mercaptan(CH_(3)SH)with low power consumption is crucial for assessing air quality and facilitating non-invasive diagnosis of diseases such as periodontitis.Herein,we synthesized a ternary CeO_(2)-ZnO-Ag nanocomposite by a simple sol-gel one-step method,which shows the capability of monitoring ppb-level CH_(3)SH under room temperature.The incorporation of Ag significantly reduces the particle size and increases the ratio of Ce^(3+)as well as oxygen vacancy.Furthermore,Ag nanoparticles improve light utilization efficiency in CeO_(2)-ZnO composites in favor of the separation of photo-generated charge carriers.The sensor based on the nanocomposites with 2 mol%Ag exhibits an exceptional response of 1.21 towards 50 ppb CH3SH at room temperature under photoassisted excitation(395 nm).Moreover,it shows a stable detection even in an environment with 57.6% humidity and high selectivity towards CH_(3)SH gas.The gas sensing mechanism study indicates that the enhancement in perfo rmance is prima rily attributed to an increased number of oxygen vacancies and the spillover effect of Ag,ultimately leading to an augmented reaction rate of CH_(3)SH on the surface of the sensing material.This work demonstrates that the optimized CeO_(2)-ZnO-Ag nanocomposites hold great promise for highly selective and sensitive detection of trace CH_(3)SH gas under specific humidity conditions.展开更多
Integrating electrocatalytic and photocatalytic functionalities into a single-component system offers a promising strategy for enhancing catalytic activity in photo-assisted electrocatalysis.This synergy is critical f...Integrating electrocatalytic and photocatalytic functionalities into a single-component system offers a promising strategy for enhancing catalytic activity in photo-assisted electrocatalysis.This synergy is critical for advancing energy conversion efficiency,yet significant challenges persist,particularly in optimizing individual layers and minimizing charge recombination.In this work,we present a novel singlecomponent photo-assisted electrocatalytic system based on Ni-or Co-doped CeO_(2),which simultaneously functions as a light absorber and electrocatalyst.We elucidate the critical relationship between bandgap engineering and d-band states,demonstrating that controlled modulation of dopant-derived 3d states within the CeO_(2)bandgap facilitates visible-light harvesting and optimizes the adsorption energetics of key reaction intermediates.Specifically,Ni-doped CeO_(2)introduces additional 3d states near the Fermi level,narrowing the bandgap from 3.0 to 2.7 eV.This modification not only enhances visible-light absorption but also improves charge transfer efficiency at the catalyst-electrolyte interface.Density functional theory(DFT)calculations and spectroscopic analyses reveal that Ni doping significantly enhances performance,achieving a 64 mV reduction in overpotential at 50 mA/cm^(2)under illumination,while Co-doped CeO_(2)exhibits a 35 mV reduction in 1 M NaOH.Our findings demonstrate that a simple doping strategy can tailor 3d states to promote efficient charge carrier separation and intermediate transfer,offering a versatile and scalable approach to designing advanced electrocatalysts for water splitting.展开更多
The lithium-oxygen battery(LOB)is a promising source of green energy due to its energy density.However,the development of this technology is limited by the insoluble discharge product it produces.In this work,a cathod...The lithium-oxygen battery(LOB)is a promising source of green energy due to its energy density.However,the development of this technology is limited by the insoluble discharge product it produces.In this work,a cathode material with a p-n heterostructure of polyaniline(PANI)/ZnS is prepared to trap visible light,utilizing a ZnS quantum dot(ZnS QD)network to form a large number of photogenerated electron–hole pairs,thus promoting the generation and decomposition of Li_(2)O_(2).The prepared PANI/ZnS has an ultra-low overpotential of 0.06 V under illumination.Furthermore,density functional theory theoretical calculation has demonstrated the ability of the heterostructures to adsorb oxygen-containing intermediates,which not only facilitates the growth of Li_(2)O_(2),but also reduces the reaction energy required to decompose Li_(2)O_(2).The present work provides a solution to the problem of insolubility of discharge products in photo-assisted LOB.展开更多
Electrochemical detection is an efficient method for the detection of Bisphenol A(BPA).Herein,a sensitive photo-electrochemical sensor based on two-dimensional(2 D)TiO_(2)(001)nanosheets was fabricated and then used f...Electrochemical detection is an efficient method for the detection of Bisphenol A(BPA).Herein,a sensitive photo-electrochemical sensor based on two-dimensional(2 D)TiO_(2)(001)nanosheets was fabricated and then used for BPA electrochemical detection.Upon light irradiation,the 2 D TiO_(2)(001)nanosheets electrode provided a lower detection limit of BPA detection compared with an ambient electrochemical determination.The low detection limit is^5.37 nmol/L(S/N=3).Furthermore,profiting from the photoelectric characteristics,the 2 D TiO_(2)(001)nanosheets electrode exhibits a nice regeneration prope rty.After 45 min of light irradiation,the electrochemical signal was regenerated from14.7%to 82.9%of the original signal at the 6th cycle.This is attributed to the non-selective·OH mediation produced by the 2 D TiO_(2)(001)nanosheets mineralizing anodic polymeric products and resuming surface reactive sites.This investigation indicates that photo-assistance is an efficient method to improve the electrochemical sensor for detecting BPA in water environments.展开更多
Peroxymonosulfate(PMS)activation and photocatalysis are effective technologies to remove organic pollutants,but the adsorption effect of the catalyst is usually unheeded in degradation process.Herein,a bifunctional ca...Peroxymonosulfate(PMS)activation and photocatalysis are effective technologies to remove organic pollutants,but the adsorption effect of the catalyst is usually unheeded in degradation process.Herein,a bifunctional catalyst of amorphous MoS_(x)(a-MoS_(x))with 3D layer-by-layer superstructure was synthesized by assembling basic active units[Mo_(3)S_(13)]^(2-)of MoS_(2).The large interlayer spacing and high exposure of active sites render a-MoS_(x)to have excellent synergy of adsorption and photo-assisted PMS activation for tetracycline(TC)degradation.Experiments and DFT calculation show that TC can be efficiently enriched on a-MoS_(x)by pore filling,π-πinteraction,hydrogen bonding and high adsorption energy.Subsequently,PMS can be quickly activated through electron transfer with a-MoS_(x),resulting in high TC degradation efficiency of 96.6%within 20 min.In addition,the synergistic mechanism of adsorption and photo-assisted PMS activation was explored,and the degradation pathway of TC was expounded.This work is inspirational for constructing bifunctional catalysts with superior synergistic adsorption and catalytic capabilities to remove refractory organic pollutants in water.展开更多
Solar cells hold a function of photovoltaic conversion,while rechargeable metal batteries have an advantage of high energy storage.The conventional charge mode of batteries is made based on complete utilization of ele...Solar cells hold a function of photovoltaic conversion,while rechargeable metal batteries have an advantage of high energy storage.The conventional charge mode of batteries is made based on complete utilization of electric energy.The combination of solar cells and rechargeable metal batteries brings a new opportunity for the development of photo-assisted rechargeable batteries,in which the solar energy can be utilized to partially achieve photo-charging with or without external electrical bias.This review highlights the working mechanism and structure design of photo-assisted rechargeable metal batteries according to the characteristics of rechargeable metal batteries and advantage of the photovoltaic technology.In particular,the recent advances are introduced for photo-assisted rechargeable batteries based on light-weight metal anodes,including metal lithium,metal sodium,and metal zinc.The working features of the integrated devices are also discussed for energy saving under photo-assisted charging mode.Finally,a future outlook is provided for further improving the performance of photoassisted rechargeable metal batteries.展开更多
Water splitting is important to the conversion and storage of renewable energy,but slow kinetics of the oxygen evolution reaction(OER)greatly limits its utility.Here,under visible light illumination,the p-n WO_(3)/SnS...Water splitting is important to the conversion and storage of renewable energy,but slow kinetics of the oxygen evolution reaction(OER)greatly limits its utility.Here,under visible light illumination,the p-n WO_(3)/SnSe_(2)(WS)heterojunction significantly activates OER catalysis of CoFe-layered double hydroxide(CF)/carbon nanotubes(CNTs).Specifically,the catalyst achieves an overpotential of 224 mV at 10 mA cm^(-2)and a small Tafel slope of 47 mV dec^(-1),superior to RuO_(2)and most previously reported transition metal-based OER catalysts.The p-n WS heterojunction shows strong light absorption to produce photogenerated carriers.The photogenerated holes are trapped by CF to suppresses the charge recombination and facilitate charge transfer,which accelerates OER kinetics and boost the activity for the OER.This work highlights the possibility of using heterojunctions to activate OER catalysis and advances the design of energy-efficient catalysts for water oxidation systems using solar energy.展开更多
ZrO_2 nanodots are successfully prepared on LaAlO_3(LAO)(100) substrates by photo-assisted metal-organic chemical vapor deposition(MOCVD). It is indicated that the sizes and densities of ZrO_2 nanodots are contr...ZrO_2 nanodots are successfully prepared on LaAlO_3(LAO)(100) substrates by photo-assisted metal-organic chemical vapor deposition(MOCVD). It is indicated that the sizes and densities of ZrO_2 nanodots are controllable by modulating the growth temperature, oxygen partial pressure, and growth time. Meanwhile, the microwires are observed on the surfaces of substrates. It is found that there is an obvious competitive relationship between the nanodots and the microwires. In a growth temperature range from 500℃ to 660℃, the microwires turn longest and widest at 600℃, but in contrast, the nanodots grow into the smallest diameter at 600℃. This phenomenon could be illustrated by the energy barrier, decomposition rate of Zr(tmhd)_4, and mobility of atoms. In addition, growth time or oxygen partial pressure also affects the competitive relationship between the nanodots and the microwires. With increasing oxygen partial pressure from 451 Pa to 75_2 Pa,the microwires gradually grow larger while the nanodots become smaller. To further achieve the controllable growth, the coarsening effect of ZrO_2 is modified by varying the growth time, and the experimental results show that the coarsening effect of microwires is higher than that of nanodots by increasing the growth time to quickly minimize ZrO_2 energy density.展开更多
A series of experiments were conducted to systematically study the effects of etching conditions on GaN by a con-venient photo-assisted chemical (PAC) etching method. The solution concentration has an evident influe...A series of experiments were conducted to systematically study the effects of etching conditions on GaN by a con-venient photo-assisted chemical (PAC) etching method. The solution concentration has an evident influence on the surface morphology of GaN and the optimal solution concentrations for GaN hexagonal pyramids have been identified. GaN with hexagonal pyramids have higher crystal quality and tensile strain relaxation compared with as-grown GaN. A detailed anal- ysis about evolution of the size, density and optical property of GaN hexagonal pyramids is described as a function of light intensity. The intensity of photoluminescence spectra of GaN etched with hexagonal pyramids significantly increases compared to that of as-grown GaN due to multiple scattering events, high quality GaN with pyramids and the Bragg effect.展开更多
Photo-assisted rechargeable energy storage devices are a promising strategy to achieve sustainable development by simultaneously integrating solar energy conversion and supercapacitor storage.Herein,we fabricated a li...Photo-assisted rechargeable energy storage devices are a promising strategy to achieve sustainable development by simultaneously integrating solar energy conversion and supercapacitor storage.Herein,we fabricated a light-sensitive macroporous film based on carbon nanotube(CNT),intercalated with Co_(2)V_(2)O_(7),and then modified by black phosphorus quantum dots(BPQD).Physico-chemical characterization and density functional theory are employed to investigate the improved photo-assisted charge storage capability and the underlying mechanism.It is demonstrated that photo-generated carriers can be separated efficiently,and the formed abundant interfaces could modulate the electronic structure of the electrode,effectively im proving the conductivity.Under visible light,the electrode displays an ultra-high capacity of 138.4 mA h g^(-1)(197.9 mA h cm^(-3))at 1 A g^(-1).Besides,the CNT@Co_(2)V_(2)O_(7)/BPQD supercapacitor shows a maximum energy density of 44.4 Wh kg^(-1)(60.0 Wh L^(-1))at a power density of 800 W kg^(-1)(960 W L^(-1))and excellent cyclic stability of 104.8% after 13,000 charge/discharge cycles.The above improvements are attributed to the reactivity and kinetics of electrochemically active components.This study reveals the synergistic effects of multi-interface on“light,photo-generated charge,and energy storage”and provides new possibilities in the controllable design of novel photo-assisted energy storage devices.展开更多
Rechargeable Zn/Sn-air batteries have received considerable attention as promising energy storage devices.However,the electrochemical performance of these batteries is significantly constrained by the sluggish electro...Rechargeable Zn/Sn-air batteries have received considerable attention as promising energy storage devices.However,the electrochemical performance of these batteries is significantly constrained by the sluggish electrocatalytic reaction kinetics at the cathode.The integration of light energy into Zn/Sn-air batteries is a promising strategy for enhancing their performance.However,the photothermal and photoelectric effects generate heat in the battery under prolonged solar irradiation,leading to air cathode instability.This paper presents the first design and synthesis of Ni_(2)-1,5-diamino-4,8-dihydroxyanthraquinone(Ni_(2)DDA),an electronically conductiveπ-d conjugated metal-organic framework(MOF).Ni_(2)DDA exhibits both photoelectric and photothermal effects,with an optical band gap of~1.14 eV.Under illumination,Ni_(2)DDA achieves excellent oxygen evolution reaction performance(with an overpotential of 245 mV vs.reversible hydrogen electrode at 10 mA cm^(−2))and photothermal stability.These properties result from the synergy between the photoelectric and photothermal effects of Ni_(2)DDA.Upon integration into Zn/Sn-air batteries,Ni_(2)DDA ensures excellent cycling stability under light and exhibits remarkable performance in high-temperature environments up to 80℃.This study experimentally confirms the stable operation of photo-assisted Zn/Sn-air batteries under high-temperature conditions for the first time and provides novel insights into the application of electronically conductive MOFs in photoelectrocatalysis and photothermal catalysis.展开更多
Photo-assisted Zn-air batteries(PZABs)hold promise for advancing sustainable energy systems.Herein,to address challenges associated with the cathode charging oxygen evolution reaction(OER),a photo-assisted hybrid Zn-a...Photo-assisted Zn-air batteries(PZABs)hold promise for advancing sustainable energy systems.Herein,to address challenges associated with the cathode charging oxygen evolution reaction(OER),a photo-assisted hybrid Zn-air battery(PHZAB)was constructed by employing photoelectrocatalytic glycerol oxidation reaction(GOR),which is thermodynamically favorable as a replacement for OER during the charging process.Based on element doping and cocatalyst loading strategies,the CoFe-LDH/Mo:BiVO_(4)photoanode was fabricated.Systematic photoelectrochemical tests demonstrate its excellent performance,with a GOR current density of 4.78 mA·cm^(-2) at 1.23 V vs.RHE,2.6 times that of the BiVO_(4),and an applied bias photon-to-current efficiency(ABPE)of 2.21%,3.7 times that of the BiVO_(4).Further analysis proves that these modification strategies enhance bulk carrier density,accelerate surface catalytic reactions,and effectively suppress carrier recombination,thus enhancing the photoelectrochemical(PEC)performance.Benefiting from the excellent performance of the CoFe-LDH/Mo:BiVO_(4)photoanode and the novel hybrid device structure design,the PHZAB exhibits a maximum round-trip efficiency of 206%(at 0.5 mA·cm^(-2))and a 68.7% electricity saving ratio under 1 sun illumination.Even at 2 mA·cm^(-2),a 156% round-trip efficiency and 64.2% electricity saving ratio were maintained.During the photoassisted-charging process,the optimized CoFe-LDH/Mo:BiVO_(4)photoanode yields a high GOR performance of a total production rate of 225 mmol·m^(-2)·h^(-1) and formic acid(FA)production rate of 133 mmol·m^(-2)·h^(-1).This work presents a novel bifunctional system toward the rational design of functional devices and materials for simultaneously converting solar energy into chemical energy and enabling reversible solar power storage for on-demand release.展开更多
The planarization of silicon carbide(SiC),which is crucial for manufacturing power devices resilient to harsh working environments,has garnered significant attention.The utilization of titanium dioxide(TiO_(2))-based ...The planarization of silicon carbide(SiC),which is crucial for manufacturing power devices resilient to harsh working environments,has garnered significant attention.The utilization of titanium dioxide(TiO_(2))-based heterogeneous photocatalysts offers a promising avenue for achieving efficient polishing of SiC surfaces through photo-assisted chemical mechanical polishing(P-CMP)in an environmentally friendly manner.In this study,we employed nanodiamonds(NDs)and graphene oxide(GO)to fabricate a composite of TiO_(2)/ND/GO abrasives.Subsequently,the P-CMP performance of TiO_(2)/NDs/GO on the Si face of SiC was systematically investigated.High-resolution transmission electron microscopy(TEM)revealed the heterostructure between TiO_(2) and the NDs.Furthermore,the P-CMP results indicate that the heterostructure significantly enhances the polishing rate of the composite abrasives on SiC,achieving the highest material removal rate(MRR)of 600 nm/h and reducing the average surface roughness(S_(a))to 1.1705 nm.Additionally,owing to the lubricating and dispersing effects of GO,the occurrence of ND aggregation is avoided,preventing scratching on SiC.The measurement of the·OH concentration indicates that an increase in the·OH concentration is the primary factor contributing to the improvement in the MRR.The results from wetting angle and friction coefficient tests revealed that the polishing slurry containing TiO_(2)/NDs/GO exhibited excellent wettability and provided sufficient frictional force on the SiC surface.X-ray photoelectron spectroscopy(XPS)characterization demonstrated that TiO_(2)/NDs/GO enhanced the degree of oxidation of the SiC surface,leading to the formation of a softer oxide layer.Finally,on the basis of the experimental and characterization results,a comprehensive analysis of TiO_(2)/NDs/GO and P-CMP was conducted.展开更多
Li-O_(2)batteries with an ultrahigh theoretical energy density of up to 3500 W·h/kg have drawn extensive attention as future energy storage technologies.However,large discharge/charge overpotentials(>1 V)and u...Li-O_(2)batteries with an ultrahigh theoretical energy density of up to 3500 W·h/kg have drawn extensive attention as future energy storage technologies.However,large discharge/charge overpotentials(>1 V)and unsatisfactory cycling performance are the main obstacles for practical applications.Recently,integrating photocatalysis into Li-O_(2)batteries has emerged as a promising method to mitigate overpotentials,but the rational design of photocathodes with excellent photoelectrochemical activity and stability remains challenging.This review focuses on recent research progress on the reaction mechanisms in photo-assisted Li-O_(2)batteries and the development of photocathodes.We present several strategies for tailoring catalytic materials from the perspectives of material selection and its catalytic performance optimization,aiming to provide a fundamental understanding and insights into the design of efficient photocathodes.The key challenges in constructing highperformance photocathodes and potential strategies were also discussed,offering insights for the development and application of efficient photocathodes in photo-assisted Li-O_(2)batteries.展开更多
Photo-assisted capacitors are attractive devices for solar energy conversion and storage,while the behavior of photoelectrodes limits their performance.In this work,MoS_(2)photoelectrodes were modified by g-C_(3)N_(4)...Photo-assisted capacitors are attractive devices for solar energy conversion and storage,while the behavior of photoelectrodes limits their performance.In this work,MoS_(2)photoelectrodes were modified by g-C_(3)N_(4),exhibiting enhanced photo-rechargeable properties.Our results show that the introduction of g-C_(3)N_(4)increases the surface area of MoS_(2)photoelectrodes and promotes the transport of charge carriers,which can boost the specific capacity and cycle stability of capacitors.The as-prepared zinc-ion capacitors with g-C_(3)N_(4)/MoS_(2)photoelectrodes show a specific capacity of 380.93 F/g at 1 A/g under AM 1.5 G illumination.Remarkably,after 3000 cycles at 10 A/g,the capacity of the photo-assisted zinc-ion capacitor retains above 99%.展开更多
Establishing supply chains for future ammonia energy systems requires the development of efficient materials and processes for ammonia production under mild conditions.Recent researches disclose unique functionalities...Establishing supply chains for future ammonia energy systems requires the development of efficient materials and processes for ammonia production under mild conditions.Recent researches disclose unique functionalities of binary alkali and alkaline earth metal hydrides in mediating ammonia synthesis.Thanks to the rich compositional and structural properties of the metalhydrogen system,we herein report that LiBaH_(3),as a narrow band gap perovskite hydride,exhibits a strong response to visible light illumination.Specifically,hydridic hydrogen undergoes reductive elimination of producing H_(2)and creates an electron-rich surface.Such an environment favors dinitrogen fixation to form N-H bonds.Based on this chemical property,a chemical looping ammonia synthesis process mediated by LiBaH_(3)and driven by both photo and thermal energies was proposed and evaluated.This work demonstrates that hydride perovskites are promising candidates for mediating photo-assisted nitrogen fixation reactions.展开更多
文摘Photo-assisted Li-O2 batteries(LOBs)have remained a prominent and growing field over the past several years.However,the presence of slow oxygen reduction reaction(ORR)and oxygen evolution reaction(OER),large charging and discharging overpotentials,and unstable cycle life lead to low energy efficiency,thus limiting their commercial application.The rational design and synthesis of photocathode materials are effective ways to solve the above existing problems of photo-assisted LOB systems.Herein,the recent advances in the design and preparation of photocathode materials for photo-assisted LOBs were summarized in this review.First,we summarize the basic principles and comprehension of the reaction mechanism for photo-assisted LOBs.The second part introduces the latest research progress on photocathode materials.The third section describes the relationship between the structureproperties and electrochemistry of different photocathodes.In addition,attempts to construct efficient photocathode materials for photo-assisted LOBs through vacancy engineering,localized surface plasmon resonance(LSPR),and heterojunction engineering are mainly discussed.Finally,a discussion of attempts to construct efficient photocathode materials using other approaches is also presented.This work will motivate the preparation of stable and efficient photocathode materials for photo-assisted LOBs and aims to promote the commercial application of rechargeable photo-assisted LOBs energy storage.
基金the National Natural Science Foundation of China(No.52300084)China Postdoctoral Science Foundation(No.2023M741151)the Fundamental Research Funds for the Central Universities(No.2024MS063)。
文摘Electrocatalysis for nitrate(NO_(3^(–)))removal from wastewater faces the challenge of merging efficient reduction and high selectivity to nitrogen(N2)with economic viability in a durable catalyst.In this study,bimetallic PdCu/TiO_(x)composite catalysts were synthesized with varying Pd and Cu ratios through electrochemical deposition on defective TiOxnanotube arrays.Denitrification experiments demonstrated that the Pd_(1)Cu_(1)/TiO_(x)catalyst exhibited the highest(NO_(3^(–)))removal rate(81.2%)and N_(2)selectivity(67.2%)among all tested catalysts.Leveraging the exceptional light-responsive property of TiO_(x),the introduction of light energy as an assisting factor in electrocatalysis further augmented the(NO_(3^(–)))treatment rate,resulting in a higher(NO_(3^(–)))removal rate of 95.1%and N_(2)selectivity of approximately 90%.Compared to individual electrocatalysis and photocatalysis systems,the overpotential for the catalytic interface active*H formation in the photo-assisted electrocatalysis system was remarkably reduced,thus accelerating electron migration and promoting(NO_(3^(–)))reduction kinetics.Economic analysis revealed an energy consumption of 2.74 k Wh/mol and a corresponding energy consumption per order(EEO)of 0.79 k Wh/m^(3)for the Pd_(1)Cu_(1)/TiOxcatalyst to reduce 25.2 mg/L of(NO_(3^(–)))-N in water to N_(2),showcasing remarkable competitiveness and economic advantages over other water treatment technologies.This study developed the PdCu/TiOxelectrocatalysts with high(NO_(3^(–)))removal rates and N_(2)selectivity,particularly when combined with light energy,the efficiency and selectivity were significantly enhanced,offering a competitive and economically viable solution for wastewater treatment.
基金supported by the National Natural Science Foundation of China(Grant No.52263028)Xingdian Talent Funding Project(Year 2022,Yunnan Province,China).
文摘In recent years,photo-powered energy storage devices have attracted considerable research attention due to their potential applications in smart electronics.In this review,we present a comprehensive summary of recent developments in two distinct but highly promising energy storage technologies,photo-assisted metal-air batteries and photo-supercapacitors.The section on metal-air batteries primarily describes the electrochemical performance of Zn-air and Li-air systems,innovative photo-electrode designs,and mechanisms that enhance oxygen evolution and reduction reactions.A brief discussion is also provided of other metal-air systems,including Mg,Fe,and Al.In contrast,the section on photo-supercapacitors explores recent advancements in light-driven charge storage,electrode materials,and device architectures,presenting a comparative performance analysis of materials such as metal oxides,sulfides,and perovskites.Various critical challenges,including material stability,efficiency under varying light conditions,and scalability,are also thoroughly examined.Despite their different working principles,both technologies hold great potential to increase energy efficiency and sustainability through the use of photo-assisted processes.The purpose of this review is to bridge existing knowledge gaps and propose future directions for research in these emerging fields.
文摘In this study,we developed a tandem photo-assisted electrochemical(PA-EC)chemical strategy for both energy-saving ammonia/fertilizer synthesis and comprehensive nitrogen-and phosphorus-rich wastewater treatment,in which synchronous hypophosphite ion(H_(2)PO_(2)^(-))oxidation to phosphate ion(PO_(4)^(3–))(POR)and nitrate reduction(NO_(3)RR)to ammonia(NH_(3))occur,followed by cascade chemical precipitation to generate struvite.Herein,a bifunctional Cu_(2)O@NiFe_(2)O_(4)Z-scheme heterojunction with a yolk/shell structure and oxygen vacancies(OVs)was designed and developed to optimize the NO_(3)RR/POR.Serving as a key component,the established PA-EC system consisted of a Janus Cu_(2)O@NiFe_(2)O_(4)/NF self-supporting integrated photocathode and a Cu_(2)O@NiFe_(2)O_(4)/NF photocathode with efficient struvite PA-EC synthesis performance under a low cell voltage of 1.6 V vs NHE.Specifically,Janus Cu_(2)O@NiFe_(2)O_(4)/NF photocathode exhibits superior performance with a high NH3 yield of 38.06 mmol L^(-1)and a faradaic efficiency(FE)of 92.31%at 1.6 V vs.NHE and enables ammonia FE over 60%in a broad NO_(3)–concentration window of 0.005–0.5 mol L^(-1).The photoassisted electrochemical catalytic mechanism and reaction pathway for struvite synthesis on Cu_(2)O@NiFe_(2)O_(4)were investigated through a series of experiments and theoretical calculations.The results demonstrated the critical roles of the interfacial electric field,void confinement,and oxygen vacancies in promoting the overall catalytic efficiency.These encouraging results warrant further studies on combined P and N recovery for efficient production of valuable fertilizers.
基金Project supported by China Postdoctoral Science Foundation(2020M673172)National Natural Science Foundation of China(61901401)。
文摘The effective detection of trace methyl mercaptan(CH_(3)SH)with low power consumption is crucial for assessing air quality and facilitating non-invasive diagnosis of diseases such as periodontitis.Herein,we synthesized a ternary CeO_(2)-ZnO-Ag nanocomposite by a simple sol-gel one-step method,which shows the capability of monitoring ppb-level CH_(3)SH under room temperature.The incorporation of Ag significantly reduces the particle size and increases the ratio of Ce^(3+)as well as oxygen vacancy.Furthermore,Ag nanoparticles improve light utilization efficiency in CeO_(2)-ZnO composites in favor of the separation of photo-generated charge carriers.The sensor based on the nanocomposites with 2 mol%Ag exhibits an exceptional response of 1.21 towards 50 ppb CH3SH at room temperature under photoassisted excitation(395 nm).Moreover,it shows a stable detection even in an environment with 57.6% humidity and high selectivity towards CH_(3)SH gas.The gas sensing mechanism study indicates that the enhancement in perfo rmance is prima rily attributed to an increased number of oxygen vacancies and the spillover effect of Ag,ultimately leading to an augmented reaction rate of CH_(3)SH on the surface of the sensing material.This work demonstrates that the optimized CeO_(2)-ZnO-Ag nanocomposites hold great promise for highly selective and sensitive detection of trace CH_(3)SH gas under specific humidity conditions.
基金the support of the Henry Royce Institute for Advanced Materials through the Industrial Collaboration Programme(RICP-R4-100061)and MATcelerateZero(MATZ0)funded from a grant provided by the Engineering and Physical Sciences Research Council EP/X527257/1+6 种基金the Department for Energy Security and Net Zero(Project ID:NEXTCCUS)University College London’s Research,Innovation and Global Engagement,University of Sydney–University College London Partnership Collaboration AwardsUCL-Peking University Strategic Partner FundsCornell-UCL Global Strategic Collaboration Awards and IISc-UCL Joint seed fund for their financial supportthe ACT program(Accelerating CCS Technologies,Horizon2020 Project No.691712)for the financial support of the NEXTCCUS project(project ID:327327)Cambridge Royce facilities grant EP/P024947/1Sir Henry Royce Institute–recurrent grant EP/R00661X/1。
文摘Integrating electrocatalytic and photocatalytic functionalities into a single-component system offers a promising strategy for enhancing catalytic activity in photo-assisted electrocatalysis.This synergy is critical for advancing energy conversion efficiency,yet significant challenges persist,particularly in optimizing individual layers and minimizing charge recombination.In this work,we present a novel singlecomponent photo-assisted electrocatalytic system based on Ni-or Co-doped CeO_(2),which simultaneously functions as a light absorber and electrocatalyst.We elucidate the critical relationship between bandgap engineering and d-band states,demonstrating that controlled modulation of dopant-derived 3d states within the CeO_(2)bandgap facilitates visible-light harvesting and optimizes the adsorption energetics of key reaction intermediates.Specifically,Ni-doped CeO_(2)introduces additional 3d states near the Fermi level,narrowing the bandgap from 3.0 to 2.7 eV.This modification not only enhances visible-light absorption but also improves charge transfer efficiency at the catalyst-electrolyte interface.Density functional theory(DFT)calculations and spectroscopic analyses reveal that Ni doping significantly enhances performance,achieving a 64 mV reduction in overpotential at 50 mA/cm^(2)under illumination,while Co-doped CeO_(2)exhibits a 35 mV reduction in 1 M NaOH.Our findings demonstrate that a simple doping strategy can tailor 3d states to promote efficient charge carrier separation and intermediate transfer,offering a versatile and scalable approach to designing advanced electrocatalysts for water splitting.
基金supported by the National Natural Science Foundation of China(NSFC)(Nos.52171206 and52271209)Key Project of Hebei Natural Science Foundation(Nos.F2024201031 and E20202201030)+4 种基金Beijing-Tianjin-Hebei Collaborative Innovation Community Construction Project(No.21344301D)the Second Batch of Young Talent of Hebei Province(Nos.70280016160250 and 70280011808)Key Fund in Hebei Province Department of Education China(No.ZD2021014)the Central Government Guide Local Funding Projects for Scientific and Technological Development(Nos.216Z4404G and 206Z4402G)Interdisciplinary Research Program of Natural Science of Hebei University(No.DXK202107)。
文摘The lithium-oxygen battery(LOB)is a promising source of green energy due to its energy density.However,the development of this technology is limited by the insoluble discharge product it produces.In this work,a cathode material with a p-n heterostructure of polyaniline(PANI)/ZnS is prepared to trap visible light,utilizing a ZnS quantum dot(ZnS QD)network to form a large number of photogenerated electron–hole pairs,thus promoting the generation and decomposition of Li_(2)O_(2).The prepared PANI/ZnS has an ultra-low overpotential of 0.06 V under illumination.Furthermore,density functional theory theoretical calculation has demonstrated the ability of the heterostructures to adsorb oxygen-containing intermediates,which not only facilitates the growth of Li_(2)O_(2),but also reduces the reaction energy required to decompose Li_(2)O_(2).The present work provides a solution to the problem of insolubility of discharge products in photo-assisted LOB.
基金the Applied Basic Research Programs of Yunnan Science and Technology Department(No.2017FD085)the Program of Introducing Talents of Kunming University(Nos.YJL16003 and YJL18008)+4 种基金National Nature Science Foundation of China(No.61904073)Science Foundation of Yunnan Provincial Education Department(No.2018JS392)Projects of Science and Technology Plans of Kunming(No.20191-C-25318000002189)“Thousand Talents Program”of Yunnan Province for Young TalentsSpring City Plan-Special Program for Young Talents。
文摘Electrochemical detection is an efficient method for the detection of Bisphenol A(BPA).Herein,a sensitive photo-electrochemical sensor based on two-dimensional(2 D)TiO_(2)(001)nanosheets was fabricated and then used for BPA electrochemical detection.Upon light irradiation,the 2 D TiO_(2)(001)nanosheets electrode provided a lower detection limit of BPA detection compared with an ambient electrochemical determination.The low detection limit is^5.37 nmol/L(S/N=3).Furthermore,profiting from the photoelectric characteristics,the 2 D TiO_(2)(001)nanosheets electrode exhibits a nice regeneration prope rty.After 45 min of light irradiation,the electrochemical signal was regenerated from14.7%to 82.9%of the original signal at the 6th cycle.This is attributed to the non-selective·OH mediation produced by the 2 D TiO_(2)(001)nanosheets mineralizing anodic polymeric products and resuming surface reactive sites.This investigation indicates that photo-assistance is an efficient method to improve the electrochemical sensor for detecting BPA in water environments.
基金supported by the National Natural Science Foundation of China(Nos.52370073,12274115)Program for Science and Technology Innovation Team in Universities of Henan Province(No.24IRTSTHN017)+3 种基金Natural Science Foundation of Henan Province(No.212300410336)Program for Science and Technology Innovation Talent in Universities of Henan Province(No.23HASTIT027)Key Scientific and Technological Project of Henan Province(No.222102320188)Key Project of Science and Technology Research of Henan Provincial Department of Education(No.21A430008)。
文摘Peroxymonosulfate(PMS)activation and photocatalysis are effective technologies to remove organic pollutants,but the adsorption effect of the catalyst is usually unheeded in degradation process.Herein,a bifunctional catalyst of amorphous MoS_(x)(a-MoS_(x))with 3D layer-by-layer superstructure was synthesized by assembling basic active units[Mo_(3)S_(13)]^(2-)of MoS_(2).The large interlayer spacing and high exposure of active sites render a-MoS_(x)to have excellent synergy of adsorption and photo-assisted PMS activation for tetracycline(TC)degradation.Experiments and DFT calculation show that TC can be efficiently enriched on a-MoS_(x)by pore filling,π-πinteraction,hydrogen bonding and high adsorption energy.Subsequently,PMS can be quickly activated through electron transfer with a-MoS_(x),resulting in high TC degradation efficiency of 96.6%within 20 min.In addition,the synergistic mechanism of adsorption and photo-assisted PMS activation was explored,and the degradation pathway of TC was expounded.This work is inspirational for constructing bifunctional catalysts with superior synergistic adsorption and catalytic capabilities to remove refractory organic pollutants in water.
基金Financial supports from National Natural Science Foundation(21875123)of Chinathe project of Jiangxi Academy of Sciences(2020-YZD-3)are gratefully acknowledged.
文摘Solar cells hold a function of photovoltaic conversion,while rechargeable metal batteries have an advantage of high energy storage.The conventional charge mode of batteries is made based on complete utilization of electric energy.The combination of solar cells and rechargeable metal batteries brings a new opportunity for the development of photo-assisted rechargeable batteries,in which the solar energy can be utilized to partially achieve photo-charging with or without external electrical bias.This review highlights the working mechanism and structure design of photo-assisted rechargeable metal batteries according to the characteristics of rechargeable metal batteries and advantage of the photovoltaic technology.In particular,the recent advances are introduced for photo-assisted rechargeable batteries based on light-weight metal anodes,including metal lithium,metal sodium,and metal zinc.The working features of the integrated devices are also discussed for energy saving under photo-assisted charging mode.Finally,a future outlook is provided for further improving the performance of photoassisted rechargeable metal batteries.
基金the National Natural Science Foundation of China(No.41807213)the Hydrogeo-logical Survey Project of Huangshui River(No.DD20190331).
文摘Water splitting is important to the conversion and storage of renewable energy,but slow kinetics of the oxygen evolution reaction(OER)greatly limits its utility.Here,under visible light illumination,the p-n WO_(3)/SnSe_(2)(WS)heterojunction significantly activates OER catalysis of CoFe-layered double hydroxide(CF)/carbon nanotubes(CNTs).Specifically,the catalyst achieves an overpotential of 224 mV at 10 mA cm^(-2)and a small Tafel slope of 47 mV dec^(-1),superior to RuO_(2)and most previously reported transition metal-based OER catalysts.The p-n WS heterojunction shows strong light absorption to produce photogenerated carriers.The photogenerated holes are trapped by CF to suppresses the charge recombination and facilitate charge transfer,which accelerates OER kinetics and boost the activity for the OER.This work highlights the possibility of using heterojunctions to activate OER catalysis and advances the design of energy-efficient catalysts for water oxidation systems using solar energy.
基金Project supported by the National Natural Science Foundation of China(Grant No.51002063)the International Science and Technology Cooperation Program of Science and Technology Bureau of Changchun City,China(Grant No.12ZX68)
文摘ZrO_2 nanodots are successfully prepared on LaAlO_3(LAO)(100) substrates by photo-assisted metal-organic chemical vapor deposition(MOCVD). It is indicated that the sizes and densities of ZrO_2 nanodots are controllable by modulating the growth temperature, oxygen partial pressure, and growth time. Meanwhile, the microwires are observed on the surfaces of substrates. It is found that there is an obvious competitive relationship between the nanodots and the microwires. In a growth temperature range from 500℃ to 660℃, the microwires turn longest and widest at 600℃, but in contrast, the nanodots grow into the smallest diameter at 600℃. This phenomenon could be illustrated by the energy barrier, decomposition rate of Zr(tmhd)_4, and mobility of atoms. In addition, growth time or oxygen partial pressure also affects the competitive relationship between the nanodots and the microwires. With increasing oxygen partial pressure from 451 Pa to 75_2 Pa,the microwires gradually grow larger while the nanodots become smaller. To further achieve the controllable growth, the coarsening effect of ZrO_2 is modified by varying the growth time, and the experimental results show that the coarsening effect of microwires is higher than that of nanodots by increasing the growth time to quickly minimize ZrO_2 energy density.
基金Project supported by the National Basic Research Program of China(Grant Nos.2011CB301900,2012CB619304,and 2010CB327504)the National High Technology Research and Development Program of China(Grant No.2011AA03A103)+1 种基金the National Nature Science Foundation of China(Grant Nos.60990311,60906025,60936004,and 61176063)the Natural Science Foundation of Jiangsu Province,China(Grant Nos.BK2011010 and BK2009255)
文摘A series of experiments were conducted to systematically study the effects of etching conditions on GaN by a con-venient photo-assisted chemical (PAC) etching method. The solution concentration has an evident influence on the surface morphology of GaN and the optimal solution concentrations for GaN hexagonal pyramids have been identified. GaN with hexagonal pyramids have higher crystal quality and tensile strain relaxation compared with as-grown GaN. A detailed anal- ysis about evolution of the size, density and optical property of GaN hexagonal pyramids is described as a function of light intensity. The intensity of photoluminescence spectra of GaN etched with hexagonal pyramids significantly increases compared to that of as-grown GaN due to multiple scattering events, high quality GaN with pyramids and the Bragg effect.
基金supported by the National Natural Science Foundation of China(No.22225808)the Industry Prospect and Key Core Technology(Competition Project)of Jiangsu Province(No.BE2019093)the Sino-German Cooperation Group Project(No.GZ1579).
文摘Photo-assisted rechargeable energy storage devices are a promising strategy to achieve sustainable development by simultaneously integrating solar energy conversion and supercapacitor storage.Herein,we fabricated a light-sensitive macroporous film based on carbon nanotube(CNT),intercalated with Co_(2)V_(2)O_(7),and then modified by black phosphorus quantum dots(BPQD).Physico-chemical characterization and density functional theory are employed to investigate the improved photo-assisted charge storage capability and the underlying mechanism.It is demonstrated that photo-generated carriers can be separated efficiently,and the formed abundant interfaces could modulate the electronic structure of the electrode,effectively im proving the conductivity.Under visible light,the electrode displays an ultra-high capacity of 138.4 mA h g^(-1)(197.9 mA h cm^(-3))at 1 A g^(-1).Besides,the CNT@Co_(2)V_(2)O_(7)/BPQD supercapacitor shows a maximum energy density of 44.4 Wh kg^(-1)(60.0 Wh L^(-1))at a power density of 800 W kg^(-1)(960 W L^(-1))and excellent cyclic stability of 104.8% after 13,000 charge/discharge cycles.The above improvements are attributed to the reactivity and kinetics of electrochemically active components.This study reveals the synergistic effects of multi-interface on“light,photo-generated charge,and energy storage”and provides new possibilities in the controllable design of novel photo-assisted energy storage devices.
基金supported by the National Natural Science Foundation of China(No.62464010)Spring City Plan-Special Program for Young Talents(K202005007)+2 种基金Yunnan Talents Support Plan for Young Talents(XDYC-QNRC-2022-0482)Yunnan Local Colleges Applied Basic Research Projects(202101BA070001-138)Frontier Research Team of Kunming University 2023.
文摘Rechargeable Zn/Sn-air batteries have received considerable attention as promising energy storage devices.However,the electrochemical performance of these batteries is significantly constrained by the sluggish electrocatalytic reaction kinetics at the cathode.The integration of light energy into Zn/Sn-air batteries is a promising strategy for enhancing their performance.However,the photothermal and photoelectric effects generate heat in the battery under prolonged solar irradiation,leading to air cathode instability.This paper presents the first design and synthesis of Ni_(2)-1,5-diamino-4,8-dihydroxyanthraquinone(Ni_(2)DDA),an electronically conductiveπ-d conjugated metal-organic framework(MOF).Ni_(2)DDA exhibits both photoelectric and photothermal effects,with an optical band gap of~1.14 eV.Under illumination,Ni_(2)DDA achieves excellent oxygen evolution reaction performance(with an overpotential of 245 mV vs.reversible hydrogen electrode at 10 mA cm^(−2))and photothermal stability.These properties result from the synergy between the photoelectric and photothermal effects of Ni_(2)DDA.Upon integration into Zn/Sn-air batteries,Ni_(2)DDA ensures excellent cycling stability under light and exhibits remarkable performance in high-temperature environments up to 80℃.This study experimentally confirms the stable operation of photo-assisted Zn/Sn-air batteries under high-temperature conditions for the first time and provides novel insights into the application of electronically conductive MOFs in photoelectrocatalysis and photothermal catalysis.
基金the National Key Research and Development Program of China(No.2014CB932101)the National Natural Science Foundation of China,111 Project(No.B07004)+1 种基金Program for Changjiang Scholars and Innovative Research Team in University(No.IRT1205)the Fundamental Research Funds for the Central Universities(No.buctrc201527).
文摘Photo-assisted Zn-air batteries(PZABs)hold promise for advancing sustainable energy systems.Herein,to address challenges associated with the cathode charging oxygen evolution reaction(OER),a photo-assisted hybrid Zn-air battery(PHZAB)was constructed by employing photoelectrocatalytic glycerol oxidation reaction(GOR),which is thermodynamically favorable as a replacement for OER during the charging process.Based on element doping and cocatalyst loading strategies,the CoFe-LDH/Mo:BiVO_(4)photoanode was fabricated.Systematic photoelectrochemical tests demonstrate its excellent performance,with a GOR current density of 4.78 mA·cm^(-2) at 1.23 V vs.RHE,2.6 times that of the BiVO_(4),and an applied bias photon-to-current efficiency(ABPE)of 2.21%,3.7 times that of the BiVO_(4).Further analysis proves that these modification strategies enhance bulk carrier density,accelerate surface catalytic reactions,and effectively suppress carrier recombination,thus enhancing the photoelectrochemical(PEC)performance.Benefiting from the excellent performance of the CoFe-LDH/Mo:BiVO_(4)photoanode and the novel hybrid device structure design,the PHZAB exhibits a maximum round-trip efficiency of 206%(at 0.5 mA·cm^(-2))and a 68.7% electricity saving ratio under 1 sun illumination.Even at 2 mA·cm^(-2),a 156% round-trip efficiency and 64.2% electricity saving ratio were maintained.During the photoassisted-charging process,the optimized CoFe-LDH/Mo:BiVO_(4)photoanode yields a high GOR performance of a total production rate of 225 mmol·m^(-2)·h^(-1) and formic acid(FA)production rate of 133 mmol·m^(-2)·h^(-1).This work presents a novel bifunctional system toward the rational design of functional devices and materials for simultaneously converting solar energy into chemical energy and enabling reversible solar power storage for on-demand release.
基金supported by the National Natural Science Foundation of China(No.52475204)Science and Technology Major Project of Inner Mongolia Autonomous Region in China(No.2021ZD0028)Shanghai Engineering Research Center for Integrated Circuits and Advanced Display Materials.
文摘The planarization of silicon carbide(SiC),which is crucial for manufacturing power devices resilient to harsh working environments,has garnered significant attention.The utilization of titanium dioxide(TiO_(2))-based heterogeneous photocatalysts offers a promising avenue for achieving efficient polishing of SiC surfaces through photo-assisted chemical mechanical polishing(P-CMP)in an environmentally friendly manner.In this study,we employed nanodiamonds(NDs)and graphene oxide(GO)to fabricate a composite of TiO_(2)/ND/GO abrasives.Subsequently,the P-CMP performance of TiO_(2)/NDs/GO on the Si face of SiC was systematically investigated.High-resolution transmission electron microscopy(TEM)revealed the heterostructure between TiO_(2) and the NDs.Furthermore,the P-CMP results indicate that the heterostructure significantly enhances the polishing rate of the composite abrasives on SiC,achieving the highest material removal rate(MRR)of 600 nm/h and reducing the average surface roughness(S_(a))to 1.1705 nm.Additionally,owing to the lubricating and dispersing effects of GO,the occurrence of ND aggregation is avoided,preventing scratching on SiC.The measurement of the·OH concentration indicates that an increase in the·OH concentration is the primary factor contributing to the improvement in the MRR.The results from wetting angle and friction coefficient tests revealed that the polishing slurry containing TiO_(2)/NDs/GO exhibited excellent wettability and provided sufficient frictional force on the SiC surface.X-ray photoelectron spectroscopy(XPS)characterization demonstrated that TiO_(2)/NDs/GO enhanced the degree of oxidation of the SiC surface,leading to the formation of a softer oxide layer.Finally,on the basis of the experimental and characterization results,a comprehensive analysis of TiO_(2)/NDs/GO and P-CMP was conducted.
基金supported by Singapore Ministry of Education under its AcRF Tier 2(MOE-T2EP10123-0001)Singapore National Research Foundation Investigatorship(NRF-NRFI08-2022-0009).
文摘Li-O_(2)batteries with an ultrahigh theoretical energy density of up to 3500 W·h/kg have drawn extensive attention as future energy storage technologies.However,large discharge/charge overpotentials(>1 V)and unsatisfactory cycling performance are the main obstacles for practical applications.Recently,integrating photocatalysis into Li-O_(2)batteries has emerged as a promising method to mitigate overpotentials,but the rational design of photocathodes with excellent photoelectrochemical activity and stability remains challenging.This review focuses on recent research progress on the reaction mechanisms in photo-assisted Li-O_(2)batteries and the development of photocathodes.We present several strategies for tailoring catalytic materials from the perspectives of material selection and its catalytic performance optimization,aiming to provide a fundamental understanding and insights into the design of efficient photocathodes.The key challenges in constructing highperformance photocathodes and potential strategies were also discussed,offering insights for the development and application of efficient photocathodes in photo-assisted Li-O_(2)batteries.
基金upported partially by the National Natural Science Foundation of China(52302250 and 52272200)the Hebei Natural Science Foundation(B2024502013)+4 种基金the State Key Laboratory of Alternate Electrical Power System with Renewable Energy Sources(LAPS21004 and LAPS202114)the Beijing Natural Science Foundation(2222076)the 2022 Strategic Research Key Project of Science and Technology Commission of the Ministry of Education,the China Postdoctoral Science Foundation(2022M721129)the Fundamental Research Funds for the Central Universities(2022MS030 and 2021MS028)the NCEPU"Double First-Class"Program。
文摘Photo-assisted capacitors are attractive devices for solar energy conversion and storage,while the behavior of photoelectrodes limits their performance.In this work,MoS_(2)photoelectrodes were modified by g-C_(3)N_(4),exhibiting enhanced photo-rechargeable properties.Our results show that the introduction of g-C_(3)N_(4)increases the surface area of MoS_(2)photoelectrodes and promotes the transport of charge carriers,which can boost the specific capacity and cycle stability of capacitors.The as-prepared zinc-ion capacitors with g-C_(3)N_(4)/MoS_(2)photoelectrodes show a specific capacity of 380.93 F/g at 1 A/g under AM 1.5 G illumination.Remarkably,after 3000 cycles at 10 A/g,the capacity of the photo-assisted zinc-ion capacitor retains above 99%.
基金supported by the National Key R&D Program of China (2021YFB4000400)the National Natural Science Foundation of China (21988101,22402200)+1 种基金the Youth Innovation Promotion Association CAS (Y2022060)the Liaoning Distinguished Scholars (2024JH3/50100007)。
文摘Establishing supply chains for future ammonia energy systems requires the development of efficient materials and processes for ammonia production under mild conditions.Recent researches disclose unique functionalities of binary alkali and alkaline earth metal hydrides in mediating ammonia synthesis.Thanks to the rich compositional and structural properties of the metalhydrogen system,we herein report that LiBaH_(3),as a narrow band gap perovskite hydride,exhibits a strong response to visible light illumination.Specifically,hydridic hydrogen undergoes reductive elimination of producing H_(2)and creates an electron-rich surface.Such an environment favors dinitrogen fixation to form N-H bonds.Based on this chemical property,a chemical looping ammonia synthesis process mediated by LiBaH_(3)and driven by both photo and thermal energies was proposed and evaluated.This work demonstrates that hydride perovskites are promising candidates for mediating photo-assisted nitrogen fixation reactions.