Person recognition in photo collections is a critical yet challenging task in computer vision.Previous studies have used social relationships within photo collections to address this issue.However,these methods often ...Person recognition in photo collections is a critical yet challenging task in computer vision.Previous studies have used social relationships within photo collections to address this issue.However,these methods often fail when performing single-person-in-photos recognition in photo collections,as they cannot rely on social connections for recognition.In this work,we discard social relationships and instead measure the relationships between photos to solve this problem.We designed a new model that includes a multi-parameter attention network for adaptively fusing visual features and a unified formula for measuring photo intimacy.This model effectively recognizes individuals in single photo within the collection.Due to outdated annotations and missing photos in the existing PIPA(Person in Photo Album)dataset,wemanually re-annotated it and added approximately ten thousand photos of Asian individuals to address the underrepresentation issue.Our results on the re-annotated PIPA dataset are superior to previous studies in most cases,and experiments on the supplemented dataset further demonstrate the effectiveness of our method.We have made the PIPA dataset publicly available on Zenodo,with the DOI:10.5281/zenodo.12508096(accessed on 15 October 2025).展开更多
Electrochemical CO_(2) reduction reaction(CO_(2)RR) into valuable formate provides a strategy for carbon neutrality.Bismuth(Bi) catalysts,attributed to their appropriate energy barrier of OCHO*intermediate,have demons...Electrochemical CO_(2) reduction reaction(CO_(2)RR) into valuable formate provides a strategy for carbon neutrality.Bismuth(Bi) catalysts,attributed to their appropriate energy barrier of OCHO*intermediate,have demonstrated substantial potential for the advancement of electrocatalytic CO_(2) reduction to formate.However,due to the weak bonding of protons(H^(*)) of Bi,the available protonate of CO_(2) on Bi is insufficient,which limits the formation of OCHO^(*).Prediction by theoretical calculation,chlorine doping can effectively promote the dissociation of H_(2)O and thus achieve effective proton supply.We prepare chlorine-doped Bi(Cl-Bi) via an electrochemical conversion strategy for electroreduction of CO_(2) .An obvious improvement of faradaic efficiency(FE) of formate(96.7% at-0.95 V vs.RHE) can be achieved on Cl-Bi,higher than that of Bi(89.4%).Meanwhile,Cl-Bi has the highest formate production rate of 275 μmol h^(-1)cm^(-2)at-0.95 V vs.RHE,which is 1.2 times higher than that of Bi(224 μmol h^(-1)cm^(-2)).In situ characterizations and kinetic analysis reveal that chlorine doping promotes the activation of H_(2)O and supply sufficient protons to promote the protonation of CO_(2) to OCHO^(*),which is consistent with theoretical calculation.The study presents an effective strategy for rational design of highly efficient electrocatalysts to promote green chemical production.展开更多
To alleviate the global warming by removing excess CO_(2) and converting them into value-added chemicals,(photo)electrochemical reduction has been recognized as a promising strategy.As the CO_(2) reduction reaction(CO...To alleviate the global warming by removing excess CO_(2) and converting them into value-added chemicals,(photo)electrochemical reduction has been recognized as a promising strategy.As the CO_(2) reduction reaction(CO_(2) RR) is involved with multiple electrons and multiple products,plus the complexity of the surface chemical environment of the catalyst,it is extremely challenging to establish the structure/function relationship.Atomically precise metal nanoclusters(NCs),with crystallographically resolved structure,molecule-like characters and strong quantum confinement effects,have been emerging as a new type of catalyst for CO_(2) RR,and more importantly,they can provide an ideal platform to unravel the comprehensive mechanistic insights and establish the structure/function relationship eventually.In this review,the recent advances regarding employing molecular metal NCs with well-defined structure including Au NCs,Au-based alloy NCs,Ag NCs,Cu NCs for CO_(2) RR and relevant mechanistic studies are discussed,and the opportunities and challenges are proposed at the end for paving the development of CO_(2) RR by using atomically precise metal NCs.展开更多
Metallene has been widely considered as an advanced electrocatalytic material due to its large specific surface area and highly active reaction sites.Herein,we design and synthesize ultrathin rhodium metallene(Rh ML)w...Metallene has been widely considered as an advanced electrocatalytic material due to its large specific surface area and highly active reaction sites.Herein,we design and synthesize ultrathin rhodium metallene(Rh ML)with abundant wrinkles to supply surface-strained Rh sites for driving acetonitrile electroreduction to ethylamine(AER).The electrochemical tests indicate that Rh ML shows an ethylamine yield rate of 137.1 mmol gcat^(-1) h^(-1) in an acidic solution,with stability lasting up to 200 h.Theoretical calculations reveal that Rh ML with wrinkle-induced compressive strain not only shows a lower energy barrier in the rate-determining step but also facilitates the ethylamine desorption process compared to wrinkle-free Rh ML and commercial Rh black.The assembled electrolyzer with bifunctional Rh ML shows an electrolysis voltage of 0.41 V at 10 mA cm^(-2),enabling simultaneous ethylamine production and hydrazine waste treatment.Furthermore,the voltage of an assembled hybrid zinc-acetonitrile battery can effectively drive this electrolyzer to achieve the dual AER process.This study provides guidance for improving the catalytic efficiency of surface atoms in two-dimensional materials,as well as the electrochemical synthesis technology for series-connected battery-electrolyzer systems.展开更多
Are you tred of regular selfies?Try a self-photo studio!The lights and camera are ready for you.At the studio,you can fix your hair.There are clothes and props.You can use those and take fun photos.Bring your friends ...Are you tred of regular selfies?Try a self-photo studio!The lights and camera are ready for you.At the studio,you can fix your hair.There are clothes and props.You can use those and take fun photos.Bring your friends with you.Then you can take photos together.Pose in silly ways and have fun!You can take the photos home and remember your good time.展开更多
Photoelectrocatalysis(PEC)is extensively applied in diverse redox reactions.However,the traditional oxygen evolution reaction(OER)occurring at the(photo)anode is hindered by high thermodynamic demands and sluggish kin...Photoelectrocatalysis(PEC)is extensively applied in diverse redox reactions.However,the traditional oxygen evolution reaction(OER)occurring at the(photo)anode is hindered by high thermodynamic demands and sluggish kinetics,resulting in excessive energy consumption and limited economic value of the O2 produced,thereby impeding the practical application of PEC reactions.To overcome these limitations,advanced anodic-cathodic coupling systems,as an emerging energy conversion technology,have garnered significant research interest.These systems substitute OER with lower potential,valuable oxidation reactions,significantly enhancing energy conversion efficiency,yielding high-value chemicals,while reducing energy consumption and environmental pollution.More importantly,by designing and optimizing photoelectrodes to generate sufficient photovoltage under illumination,meeting the thermodynamic and kinetic potential requirements of the reactions,and by tuning the voltage to match the current densities of the cathode and anode,coupling reactions can be achieved under bias-free conditions.In this review,we provide an overview of the mechanisms of PEC coupling reactions and summarize photoelectrode catalysts along with their synthesis methods.We further explore advanced catalyst modification strategies and highlight the latest development in advanced PEC coupling systems,including photocathodic CO_(2)reduction,nitrate reduction,oxygen reduction,enzyme activation,coupled with photoanodic organic oxidation,biomass oxidation,and pollutant degradation.Additionally,advanced in situ characterization techniques for elucidating reaction mechanisms are discussed.Finally,we propose the challenges in catalyst design,reaction systems,and large-scale applications,while offering future perspectives for PEC coupling system.This work underscores the tremendous potential of PEC coupling systems in energy conversion and environmental remediation,and provides valuable insights for the future design of such coupling systems.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
The pervasive use of photo editing applications such as Photoshop and FaceTune has significantly altered societal beauty standards, particularly for individuals with skin of color, often leading to unrealistic expecta...The pervasive use of photo editing applications such as Photoshop and FaceTune has significantly altered societal beauty standards, particularly for individuals with skin of color, often leading to unrealistic expectations regarding skin appearance and health. These tools allow users to smooth skin textures, lighten skin tones, and erase imperfections, perpetuating Eurocentric beauty ideals that frequently marginalize the natural diversity of skin tones and textures. Consequently, individuals with skin of color may seek dermatological interventions—such as skin lightening treatments, aggressive acne scar revisions, and other cosmetic procedures—aimed at achieving appearances that align more closely with digitally manipulated images. This pursuit of an unattainable aesthetic can result in increased dissatisfaction with common skin conditions like hyperpigmentation and keloids, which are often misrepresented in edited photos. Additionally, the psychological impact of these alterations can exacerbate feelings of inadequacy, contributing to conditions such as anxiety and body dysmorphic disorder. Dermatologists face the dual challenge of addressing patients’ clinical needs while also managing their expectations shaped by digital enhancements. To combat this, it is essential for dermatologists to integrate patient education that emphasizes the beauty of diverse skin tones and the discrepancies between digital images and authentic skin health. By fostering an understanding of realistic outcomes and promoting the acceptance of natural skin characteristics, dermatologists can empower individuals with skin of color to prioritize authentic skin health over digitally influenced ideals, ultimately leading to more satisfying dermatological care and improved self-image.展开更多
Developing Sn,nitrogen-doped carbon catalysts(Sn-NC)for efficient CO_(2) electroreduction(CO_(2)RR)to CO remains a great challenge.Here,we employed a defective hierarchical porous graphene nanomesh to anchor the singl...Developing Sn,nitrogen-doped carbon catalysts(Sn-NC)for efficient CO_(2) electroreduction(CO_(2)RR)to CO remains a great challenge.Here,we employed a defective hierarchical porous graphene nanomesh to anchor the single atomic tin-nitrogen sites(A-Sn-NGM)for effective CO_(2) electroreduction.The synthesized A-Sn-NGM typically showed remarkable CO_(2)RR activity towards CO production,which achieved a maximum CO Faradaic efficiency(FECO)of 98.7%and a turnover frequency of 5117.4 h^(−1) at a potential of−0.6 V(vs.RHE).Further analysis proves that the increased activity to CO production of A-Sn-NGM derives from the enlarged roughness and enhanced intrinsic activity.Density-functional theory(DFT)calculations indicate that the adjacent carbon defects anchored Sn-Nx coordination sites can markedly inhibit the competing hydrogen evolution reaction(HER)and lower the energy barrier for the formation of *COOH intermediates as compared to bulk Sn-Nx sites without carbon defects.This work provides a reliable method by engineering the carbon support to improve the CO_(2)RR performance for single-atom catalysts.展开更多
Electrochemical CO_(2) reduction is a sustainable method for producing fuels and chemicals using renewable energy sources.Sn is a widely employed catalyst for formate production,with its performance closely influenced...Electrochemical CO_(2) reduction is a sustainable method for producing fuels and chemicals using renewable energy sources.Sn is a widely employed catalyst for formate production,with its performance closely influenced by the catalyst ink formulations and reac-tion conditions.The present study explores the influence of catalyst loading,current density,and binder choice on Sn-based CO_(2) reduc-tion systems.Decreasing catalyst loading from 10 to 1.685 mg·cm^(-2) and increasing current density in highly concentrated bicarbonate solutions significantly enhances formate selectivity,achieving 88%faradaic efficiency(FE)at a current density of−30 mA·cm^(-2) with a cathodic potential of−1.22 V vs.reversible hydrogen electrode(RHE)and a catalyst loading of 1.685 mg·cm^(-2).This low-loading strategy not only reduces catalyst costs but also enhances surface utilization and suppresses the hydrogen evolution reaction.Nafion enhances formate production when applied as a surface coating rather than pre-mixed in the ink,as evidenced by improved faradaic efficiency and lower cathodic potentials.However,this performance still does not match that of binder-free systems because Sn-based catalysts intrinsic-ally exhibit high catalytic activity,making the binder contribution less significant.Although modifying the electrode surface with binders leads to blocked active sites and increased resistance,polyvinylidene fluoride(PVDF)remains promising because of its stability,strength,and conductivity,achieving up to 72%FE to formate at−30 mA·cm^(-2) and−1.66 V vs.RHE.The findings of this research reveal method-ologies for optimizing the catalyst ink formulations and binder utilization to enhance the conversion of CO_(2) to formate,thereby offering crucial insights for the development of a cost-efficient catalyst for high-current-density operations.展开更多
This paper presents the design and implementation of a Python-based conversion tool for Apple Live Photo files(.livp).The tool converts.livp files into standard image formats(JPEG/HEIC/PNG)by renaming them to.zip and ...This paper presents the design and implementation of a Python-based conversion tool for Apple Live Photo files(.livp).The tool converts.livp files into standard image formats(JPEG/HEIC/PNG)by renaming them to.zip and extracting the static images while optionally removing the embedded short video(.mov).It supports one-click batch processing of all.livp files within a folder.The software adopts a modular design,consisting of file renaming,batch decompression,temporary file cleaning,and a Tkinter-based graphical user interface(GUI).A multithreading mechanism ensures a smooth user experience without interface freezing.With a compact size of approximately 10.7 MB,the software is easy to deploy and suitable for users who need to batch-convert Live Photos into static images.This paper introduces the system design,key implementation details,performance analysis,and potential improvements,providing references for developing lightweight format conversion applications.展开更多
The generation of economically valuable chemicals through electrocatalytic CO_(2)reduction reaction(CO_(2)RR)is a highly attractive strategy for achieving the carbon cycle.Bismuth(Bi)is a prospective element due to th...The generation of economically valuable chemicals through electrocatalytic CO_(2)reduction reaction(CO_(2)RR)is a highly attractive strategy for achieving the carbon cycle.Bismuth(Bi)is a prospective element due to the high selectivity for formate.Researches demonstrate the Bi–O bonds have a significant effect on the key*OCHO intermediate.Herein,we report a F-doped catalyst that displays remarkable performance in generating formate in pH-universal electrolytes.Specifically,the as-prepared F-Bi/BOC@GO achieves formate Faradaic efficiencies(FEformate)around 95%in a wide range of pH from 1 to 13.6.Furthermore,at an industrial level,current density of 200 mA cm^(-2),the F-Bi/BOC@GO catalyst shows a much more stable FE_(formate)than the catalyst without introducing F.In situ Raman reveals that the doped F can greatly improve the stability of Bi–O bonds during the electroreduction process.DFT calculations further demonstrate that fluorine doping raises the energy barrier for oxygen desorption from Bi–O motifs,thus enhancing the stability of active sites.Combined with X-ray photoelectron spectroscopy(XPS),the doped F acts as an electron trapping,which may direct electrons towards Bi–Bi bonds,thus protecting the key Bi–O motif.This work reveals the critical role of fluorine in stabilizing Bi–O active centers across a wide pH range,maintaining high formate Faradaic efficiency for a longer time than the catalyst without fluorine introduction.展开更多
The efficient production of acetate through electrochemical CO_(2)reduction reaction(eCO_(2)RR)with low energy consumption has consistently been a challenging yet extremely significant task.Current catalysts suffered ...The efficient production of acetate through electrochemical CO_(2)reduction reaction(eCO_(2)RR)with low energy consumption has consistently been a challenging yet extremely significant task.Current catalysts suffered from high energy consumption and low relative purity of acetate product.Herein,we report ultrasmall Cu_(2)O nanoparticles with an average size of 2.5±0.09 nm immobilized on a conductive copper-based metal-organic framework(Cu-THQ)(denoted as Cu_(2)O@Cu-THQ),which attained a Faradaic efficiency of 65(3)%for acetate at a very low potential of-0.3 V vs.RHE with a current density of 10.5 m A/cm^(2).Importantly,as there are no other liquid phase products such as formate,methanol or ethanol,the relative purity of the obtained acetate product was as high as 100%.Taking into account the relative purity of the liquid product,current density,and energy consumption,the performance for electroreduction of CO_(2)to acetate of Cu_(2)O@Cu-THQ is not only much higher than that of the commercial Cu_(2)O nanoparticles,but also higher than those of all reported catalysts.Operando infrared spectroscopy and theoretical calculations indicated that the synergy effect between Cu-THQ and Cu_(2)O promoted the e CO_(2)RR to yield acetate.Specifically,the hydroxyl group on the organic ligand THQ in the Cu-THQ formed hydrogen bond interactions with the key C_(2)intermediates(*CH_(2)COOH and*HOCCOH)adsorbed on Cu_(2)O,which played a crucial role in stabilizing the key C_(2)intermediates and thus reduced the formation energy of the key C_(2) intermediates.展开更多
The steps of NO_(3)^(-)adsorption,deoxygenation,nitrogen species hydrogenation and ammonia desorption are vital for electrocatalytic nitrate reduction(NO_(3)^(-)RR)to ammonia,and lowering their Gibbs free energy chan...The steps of NO_(3)^(-)adsorption,deoxygenation,nitrogen species hydrogenation and ammonia desorption are vital for electrocatalytic nitrate reduction(NO_(3)^(-)RR)to ammonia,and lowering their Gibbs free energy change(ΔG)is the essential approach for improving NO_(3)^(-)RR.The copper-based alloys are considered as the outstanding catalysts thanks to the tunable d-band center,reconstruction and synergistic effect of multiple metal atoms in the past decades.Here,we synthesized a single-phase coppernickel alloy by electrodeposition and optimized itsΔG during NO_(3)^(-)RR through tuning the electrodeposition potential to regulate the metal component ratio.The atomic ratio of Ni/Cu in CuNi alloys is gradually increased as the negative shift of deposition potential from-1.0 to-1.2 V versus SCE,thus achieving the fast modulation of intermediate adsorption energy for NO_(3)^(-)RR.According to density functional theory,profited by a strong NO_(3)^(-)adsorption and a weak NH_(3)desorption energy barrier,the optimized CuNi alloy(Cu_(3)Ni_(1)/CF)exhibits an ideal ammonia yield of 364.1μmol cm^(-2)h^(-1)and Faradaic efficiency of 92.25%at-0.23 V versus RHE.Further applying Cu_(3)Ni_(1)/CF as the cathode material,a novel Znnitrate battery exhibits a maximum power density of5.85 mW cm^(-2)with a NH_(3)yield of 92.50μmol cm^(-2)h^(-1)and Faradaic efficiency of 99.15%at 20 mA cm^(-2)for NH_(3)production.This work not only offers a rational design concept with clear guidance for efficient modulation of intermediate adsorption free energy on alloy catalysts prepared by electrodeposition,but also provides the further understanding for efficient developments of NO_(3)^(-)RR and Zn-based batteries.展开更多
Electrochemical reduction of carbon dioxide(CO_(2)RR)is a promising approach to complete the carbon cycle and potentially convert CO_(2)into valuable chemicals and fuels.Cu is unique among transition metals in its abi...Electrochemical reduction of carbon dioxide(CO_(2)RR)is a promising approach to complete the carbon cycle and potentially convert CO_(2)into valuable chemicals and fuels.Cu is unique among transition metals in its ability to catalyze the CO_(2)RR and produce multi-carbon products.However,achieving high selectivity for C2+products is challenging for copper-based catalysts,as C–C coupling reactions proceed slowly.Herein,a surface modification strategy involving grafting long alkyl chains onto copper nanowires(Cu NWs)has been proposed to regulate the electronic structure of Cu surface,which facilitates*CO-*CO coupling in the CO_(2)RR.The hydrophobicity of the catalysts increases greatly after the introduction of long alkyl chains,therefore the hydrogen evolution reaction(HER)has been inhibited effectively.Such surface modification approach proves to be highly efficient and universal,with the Faradaic efficiency(FE)of C_(2)H_(4) up to 53%for the optimized Cu–SH catalyst,representing a significant enhancement compared to the pristine Cu NWs(30%).In-situ characterizations and theoretical calculations demonstrate that the different terminal groups of the grafted octadecyl chains can effectively regulate the charge density of Cu NWs interface and change the adsorption configuration of*CO intermediate.The top-adsorbed*CO intermediates(*COtop)on Cu–SH catalytic interface endow Cu–SH with the highest charge density,which effectively lowers the reaction energy barrier for*CO-*CO coupling,promoting the formation of the*OCCO intermediate,thereby enhancing the selectivity towards C_(2)H_(4).This study provides a promising method for designing efficient Cu-based catalysts with high catalytic activity and selectivity towards C2H4.展开更多
The atomic-level exploration of structure-property correlations poses significant challenges in establishing precise design principles for electrocatalysts targeting efficient CO_(2)conversion.This study demonstrates ...The atomic-level exploration of structure-property correlations poses significant challenges in establishing precise design principles for electrocatalysts targeting efficient CO_(2)conversion.This study demonstrates how controlled exposure of metal sites governs CO_(2)electroreduction performance through two octanuclear bismuth-oxo clusters with distinct architectures.The Bi_(8)-DMF cluster,constructed using tert–butylthiacalix[4]arene(TC4A)as the sole ligand,features two surface-exposed Bi active sites,while the dual-ligand Bi_(8)-Fc(with TC4A/ferrocene carboxylate)forms a fully encapsulated structure.Electrocatalytic tests reveal Bi_(8)-DMF achieves exceptional formate selectivity(>90%Faradaic efficiency)across a broad potential window(-0.9 V to-1.6 V vs.RHE)with 20 h stability,outperforming Bi_(8)-Fc(60%efficiency at-1.5 V).Theoretical calculations attribute Bi_(8)-DMF's superiority to exposed Bi sites that stabilize the critical*OCHO intermediate via optimized orbital interactions.This work provides crucial guidance for polynuclear catalyst design:moderate exposure of metal active sites significantly enhances CO_(2)reduction performance.展开更多
基金supported by“the Fundamental Research Funds for the Central Universities”(GrantNos.:3282025045,3282024008)“Science and Technology Project of the State ArchivesAdministration ofChina”(Grant No.:2025-Z-009).
文摘Person recognition in photo collections is a critical yet challenging task in computer vision.Previous studies have used social relationships within photo collections to address this issue.However,these methods often fail when performing single-person-in-photos recognition in photo collections,as they cannot rely on social connections for recognition.In this work,we discard social relationships and instead measure the relationships between photos to solve this problem.We designed a new model that includes a multi-parameter attention network for adaptively fusing visual features and a unified formula for measuring photo intimacy.This model effectively recognizes individuals in single photo within the collection.Due to outdated annotations and missing photos in the existing PIPA(Person in Photo Album)dataset,wemanually re-annotated it and added approximately ten thousand photos of Asian individuals to address the underrepresentation issue.Our results on the re-annotated PIPA dataset are superior to previous studies in most cases,and experiments on the supplemented dataset further demonstrate the effectiveness of our method.We have made the PIPA dataset publicly available on Zenodo,with the DOI:10.5281/zenodo.12508096(accessed on 15 October 2025).
基金financially supported by the Natural Science Foundation of Shandong Province (No.ZR2022QE076)the National Natural Science Foundation of China (No.52202092)the Science and Technology Support Plan for Youth Innovation of Colleges and Universities of Shandong Province of China (No.2023KJ104)。
文摘Electrochemical CO_(2) reduction reaction(CO_(2)RR) into valuable formate provides a strategy for carbon neutrality.Bismuth(Bi) catalysts,attributed to their appropriate energy barrier of OCHO*intermediate,have demonstrated substantial potential for the advancement of electrocatalytic CO_(2) reduction to formate.However,due to the weak bonding of protons(H^(*)) of Bi,the available protonate of CO_(2) on Bi is insufficient,which limits the formation of OCHO^(*).Prediction by theoretical calculation,chlorine doping can effectively promote the dissociation of H_(2)O and thus achieve effective proton supply.We prepare chlorine-doped Bi(Cl-Bi) via an electrochemical conversion strategy for electroreduction of CO_(2) .An obvious improvement of faradaic efficiency(FE) of formate(96.7% at-0.95 V vs.RHE) can be achieved on Cl-Bi,higher than that of Bi(89.4%).Meanwhile,Cl-Bi has the highest formate production rate of 275 μmol h^(-1)cm^(-2)at-0.95 V vs.RHE,which is 1.2 times higher than that of Bi(224 μmol h^(-1)cm^(-2)).In situ characterizations and kinetic analysis reveal that chlorine doping promotes the activation of H_(2)O and supply sufficient protons to promote the protonation of CO_(2) to OCHO^(*),which is consistent with theoretical calculation.The study presents an effective strategy for rational design of highly efficient electrocatalysts to promote green chemical production.
基金the grant from the National Natural Science Foundation of China(No.21805170)financial support from Guangdong Natural Science Funds for Distinguished Young Scholars(No.2015A030306006)+1 种基金Guangzhou Science and Technology Plan Projects(No.201804010323)the fundamental funds for central universities(SCUT No.2018ZD022)。
文摘To alleviate the global warming by removing excess CO_(2) and converting them into value-added chemicals,(photo)electrochemical reduction has been recognized as a promising strategy.As the CO_(2) reduction reaction(CO_(2) RR) is involved with multiple electrons and multiple products,plus the complexity of the surface chemical environment of the catalyst,it is extremely challenging to establish the structure/function relationship.Atomically precise metal nanoclusters(NCs),with crystallographically resolved structure,molecule-like characters and strong quantum confinement effects,have been emerging as a new type of catalyst for CO_(2) RR,and more importantly,they can provide an ideal platform to unravel the comprehensive mechanistic insights and establish the structure/function relationship eventually.In this review,the recent advances regarding employing molecular metal NCs with well-defined structure including Au NCs,Au-based alloy NCs,Ag NCs,Cu NCs for CO_(2) RR and relevant mechanistic studies are discussed,and the opportunities and challenges are proposed at the end for paving the development of CO_(2) RR by using atomically precise metal NCs.
基金supported by the National Natural Science Foundation of China(22272103)the National Natural Science Foundation of China for the Youth(22309108,22202076)+3 种基金the Science and Technology Innovation Team of Shaanxi Province(2023-CX-TD-27)the China Postdoctoral Science Foundation(2023TQ0204)the Young Scientist Initiative Project of School of Materials Science and Engineering at Shaanxi Normal University(2024YSIP-MSE-SNNU008)Sanqin Scholars Innovation Teams in Shaanxi Province in China.
文摘Metallene has been widely considered as an advanced electrocatalytic material due to its large specific surface area and highly active reaction sites.Herein,we design and synthesize ultrathin rhodium metallene(Rh ML)with abundant wrinkles to supply surface-strained Rh sites for driving acetonitrile electroreduction to ethylamine(AER).The electrochemical tests indicate that Rh ML shows an ethylamine yield rate of 137.1 mmol gcat^(-1) h^(-1) in an acidic solution,with stability lasting up to 200 h.Theoretical calculations reveal that Rh ML with wrinkle-induced compressive strain not only shows a lower energy barrier in the rate-determining step but also facilitates the ethylamine desorption process compared to wrinkle-free Rh ML and commercial Rh black.The assembled electrolyzer with bifunctional Rh ML shows an electrolysis voltage of 0.41 V at 10 mA cm^(-2),enabling simultaneous ethylamine production and hydrazine waste treatment.Furthermore,the voltage of an assembled hybrid zinc-acetonitrile battery can effectively drive this electrolyzer to achieve the dual AER process.This study provides guidance for improving the catalytic efficiency of surface atoms in two-dimensional materials,as well as the electrochemical synthesis technology for series-connected battery-electrolyzer systems.
文摘Are you tred of regular selfies?Try a self-photo studio!The lights and camera are ready for you.At the studio,you can fix your hair.There are clothes and props.You can use those and take fun photos.Bring your friends with you.Then you can take photos together.Pose in silly ways and have fun!You can take the photos home and remember your good time.
文摘Photoelectrocatalysis(PEC)is extensively applied in diverse redox reactions.However,the traditional oxygen evolution reaction(OER)occurring at the(photo)anode is hindered by high thermodynamic demands and sluggish kinetics,resulting in excessive energy consumption and limited economic value of the O2 produced,thereby impeding the practical application of PEC reactions.To overcome these limitations,advanced anodic-cathodic coupling systems,as an emerging energy conversion technology,have garnered significant research interest.These systems substitute OER with lower potential,valuable oxidation reactions,significantly enhancing energy conversion efficiency,yielding high-value chemicals,while reducing energy consumption and environmental pollution.More importantly,by designing and optimizing photoelectrodes to generate sufficient photovoltage under illumination,meeting the thermodynamic and kinetic potential requirements of the reactions,and by tuning the voltage to match the current densities of the cathode and anode,coupling reactions can be achieved under bias-free conditions.In this review,we provide an overview of the mechanisms of PEC coupling reactions and summarize photoelectrode catalysts along with their synthesis methods.We further explore advanced catalyst modification strategies and highlight the latest development in advanced PEC coupling systems,including photocathodic CO_(2)reduction,nitrate reduction,oxygen reduction,enzyme activation,coupled with photoanodic organic oxidation,biomass oxidation,and pollutant degradation.Additionally,advanced in situ characterization techniques for elucidating reaction mechanisms are discussed.Finally,we propose the challenges in catalyst design,reaction systems,and large-scale applications,while offering future perspectives for PEC coupling system.This work underscores the tremendous potential of PEC coupling systems in energy conversion and environmental remediation,and provides valuable insights for the future design of such coupling systems.
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The pervasive use of photo editing applications such as Photoshop and FaceTune has significantly altered societal beauty standards, particularly for individuals with skin of color, often leading to unrealistic expectations regarding skin appearance and health. These tools allow users to smooth skin textures, lighten skin tones, and erase imperfections, perpetuating Eurocentric beauty ideals that frequently marginalize the natural diversity of skin tones and textures. Consequently, individuals with skin of color may seek dermatological interventions—such as skin lightening treatments, aggressive acne scar revisions, and other cosmetic procedures—aimed at achieving appearances that align more closely with digitally manipulated images. This pursuit of an unattainable aesthetic can result in increased dissatisfaction with common skin conditions like hyperpigmentation and keloids, which are often misrepresented in edited photos. Additionally, the psychological impact of these alterations can exacerbate feelings of inadequacy, contributing to conditions such as anxiety and body dysmorphic disorder. Dermatologists face the dual challenge of addressing patients’ clinical needs while also managing their expectations shaped by digital enhancements. To combat this, it is essential for dermatologists to integrate patient education that emphasizes the beauty of diverse skin tones and the discrepancies between digital images and authentic skin health. By fostering an understanding of realistic outcomes and promoting the acceptance of natural skin characteristics, dermatologists can empower individuals with skin of color to prioritize authentic skin health over digitally influenced ideals, ultimately leading to more satisfying dermatological care and improved self-image.
基金supported by the National Natural Science Foundation of China(Nos.22208021 and 52225003)the 5·5 Engineering Research&Innovation Team Project of Beijing Forestry University(No.BLRC2023B04).
文摘Developing Sn,nitrogen-doped carbon catalysts(Sn-NC)for efficient CO_(2) electroreduction(CO_(2)RR)to CO remains a great challenge.Here,we employed a defective hierarchical porous graphene nanomesh to anchor the single atomic tin-nitrogen sites(A-Sn-NGM)for effective CO_(2) electroreduction.The synthesized A-Sn-NGM typically showed remarkable CO_(2)RR activity towards CO production,which achieved a maximum CO Faradaic efficiency(FECO)of 98.7%and a turnover frequency of 5117.4 h^(−1) at a potential of−0.6 V(vs.RHE).Further analysis proves that the increased activity to CO production of A-Sn-NGM derives from the enlarged roughness and enhanced intrinsic activity.Density-functional theory(DFT)calculations indicate that the adjacent carbon defects anchored Sn-Nx coordination sites can markedly inhibit the competing hydrogen evolution reaction(HER)and lower the energy barrier for the formation of *COOH intermediates as compared to bulk Sn-Nx sites without carbon defects.This work provides a reliable method by engineering the carbon support to improve the CO_(2)RR performance for single-atom catalysts.
基金financially supported by a PhD Grant from VITO’s Strategic Research Funds(No.2310345).
文摘Electrochemical CO_(2) reduction is a sustainable method for producing fuels and chemicals using renewable energy sources.Sn is a widely employed catalyst for formate production,with its performance closely influenced by the catalyst ink formulations and reac-tion conditions.The present study explores the influence of catalyst loading,current density,and binder choice on Sn-based CO_(2) reduc-tion systems.Decreasing catalyst loading from 10 to 1.685 mg·cm^(-2) and increasing current density in highly concentrated bicarbonate solutions significantly enhances formate selectivity,achieving 88%faradaic efficiency(FE)at a current density of−30 mA·cm^(-2) with a cathodic potential of−1.22 V vs.reversible hydrogen electrode(RHE)and a catalyst loading of 1.685 mg·cm^(-2).This low-loading strategy not only reduces catalyst costs but also enhances surface utilization and suppresses the hydrogen evolution reaction.Nafion enhances formate production when applied as a surface coating rather than pre-mixed in the ink,as evidenced by improved faradaic efficiency and lower cathodic potentials.However,this performance still does not match that of binder-free systems because Sn-based catalysts intrinsic-ally exhibit high catalytic activity,making the binder contribution less significant.Although modifying the electrode surface with binders leads to blocked active sites and increased resistance,polyvinylidene fluoride(PVDF)remains promising because of its stability,strength,and conductivity,achieving up to 72%FE to formate at−30 mA·cm^(-2) and−1.66 V vs.RHE.The findings of this research reveal method-ologies for optimizing the catalyst ink formulations and binder utilization to enhance the conversion of CO_(2) to formate,thereby offering crucial insights for the development of a cost-efficient catalyst for high-current-density operations.
基金The 2025 Beijing College Students’Innovation and Entrepreneurship Training Program(Project No.:S202510009001)。
文摘This paper presents the design and implementation of a Python-based conversion tool for Apple Live Photo files(.livp).The tool converts.livp files into standard image formats(JPEG/HEIC/PNG)by renaming them to.zip and extracting the static images while optionally removing the embedded short video(.mov).It supports one-click batch processing of all.livp files within a folder.The software adopts a modular design,consisting of file renaming,batch decompression,temporary file cleaning,and a Tkinter-based graphical user interface(GUI).A multithreading mechanism ensures a smooth user experience without interface freezing.With a compact size of approximately 10.7 MB,the software is easy to deploy and suitable for users who need to batch-convert Live Photos into static images.This paper introduces the system design,key implementation details,performance analysis,and potential improvements,providing references for developing lightweight format conversion applications.
基金supported by the National Natural Science Foundation of China(22322805,22178104,U22B20143,U24A20546)Shanghai Municipal Science and Technology Major Project+1 种基金the Shanghai Scientific and Technological Innovation Project(22dz1205900)the Fundamental Research Funds for the Central Universities,and Shanghai Rising-Star Program(23QA1402200)。
文摘The generation of economically valuable chemicals through electrocatalytic CO_(2)reduction reaction(CO_(2)RR)is a highly attractive strategy for achieving the carbon cycle.Bismuth(Bi)is a prospective element due to the high selectivity for formate.Researches demonstrate the Bi–O bonds have a significant effect on the key*OCHO intermediate.Herein,we report a F-doped catalyst that displays remarkable performance in generating formate in pH-universal electrolytes.Specifically,the as-prepared F-Bi/BOC@GO achieves formate Faradaic efficiencies(FEformate)around 95%in a wide range of pH from 1 to 13.6.Furthermore,at an industrial level,current density of 200 mA cm^(-2),the F-Bi/BOC@GO catalyst shows a much more stable FE_(formate)than the catalyst without introducing F.In situ Raman reveals that the doped F can greatly improve the stability of Bi–O bonds during the electroreduction process.DFT calculations further demonstrate that fluorine doping raises the energy barrier for oxygen desorption from Bi–O motifs,thus enhancing the stability of active sites.Combined with X-ray photoelectron spectroscopy(XPS),the doped F acts as an electron trapping,which may direct electrons towards Bi–Bi bonds,thus protecting the key Bi–O motif.This work reveals the critical role of fluorine in stabilizing Bi–O active centers across a wide pH range,maintaining high formate Faradaic efficiency for a longer time than the catalyst without fluorine introduction.
基金supported by the National Key Research and Development Program of China(No.2021YFA1500401)National Natural Science Foundation of China(NSFC,Nos.21821003,22371304+3 种基金223B2123)Fundamental Research Funds for the Central Universities,Sun Yat-Sen University(No.24lgzy006)Science and Technology Innovation Special Support Project of Guangdong Province,China(No.STKJ2023078)the Guangzhou Science and Technology Program(No.SL2023A04J01767)。
文摘The efficient production of acetate through electrochemical CO_(2)reduction reaction(eCO_(2)RR)with low energy consumption has consistently been a challenging yet extremely significant task.Current catalysts suffered from high energy consumption and low relative purity of acetate product.Herein,we report ultrasmall Cu_(2)O nanoparticles with an average size of 2.5±0.09 nm immobilized on a conductive copper-based metal-organic framework(Cu-THQ)(denoted as Cu_(2)O@Cu-THQ),which attained a Faradaic efficiency of 65(3)%for acetate at a very low potential of-0.3 V vs.RHE with a current density of 10.5 m A/cm^(2).Importantly,as there are no other liquid phase products such as formate,methanol or ethanol,the relative purity of the obtained acetate product was as high as 100%.Taking into account the relative purity of the liquid product,current density,and energy consumption,the performance for electroreduction of CO_(2)to acetate of Cu_(2)O@Cu-THQ is not only much higher than that of the commercial Cu_(2)O nanoparticles,but also higher than those of all reported catalysts.Operando infrared spectroscopy and theoretical calculations indicated that the synergy effect between Cu-THQ and Cu_(2)O promoted the e CO_(2)RR to yield acetate.Specifically,the hydroxyl group on the organic ligand THQ in the Cu-THQ formed hydrogen bond interactions with the key C_(2)intermediates(*CH_(2)COOH and*HOCCOH)adsorbed on Cu_(2)O,which played a crucial role in stabilizing the key C_(2)intermediates and thus reduced the formation energy of the key C_(2) intermediates.
基金financially supported by the National Natural Science Foundation of China(No.U22A20253)High-level Talent Doctoral Scientific Research Foundation of Zhoukou Normal University(No.ZKNUC2023027)Young and Middle-Aged Backbone Teachers of Zhoukou Normal University
文摘The steps of NO_(3)^(-)adsorption,deoxygenation,nitrogen species hydrogenation and ammonia desorption are vital for electrocatalytic nitrate reduction(NO_(3)^(-)RR)to ammonia,and lowering their Gibbs free energy change(ΔG)is the essential approach for improving NO_(3)^(-)RR.The copper-based alloys are considered as the outstanding catalysts thanks to the tunable d-band center,reconstruction and synergistic effect of multiple metal atoms in the past decades.Here,we synthesized a single-phase coppernickel alloy by electrodeposition and optimized itsΔG during NO_(3)^(-)RR through tuning the electrodeposition potential to regulate the metal component ratio.The atomic ratio of Ni/Cu in CuNi alloys is gradually increased as the negative shift of deposition potential from-1.0 to-1.2 V versus SCE,thus achieving the fast modulation of intermediate adsorption energy for NO_(3)^(-)RR.According to density functional theory,profited by a strong NO_(3)^(-)adsorption and a weak NH_(3)desorption energy barrier,the optimized CuNi alloy(Cu_(3)Ni_(1)/CF)exhibits an ideal ammonia yield of 364.1μmol cm^(-2)h^(-1)and Faradaic efficiency of 92.25%at-0.23 V versus RHE.Further applying Cu_(3)Ni_(1)/CF as the cathode material,a novel Znnitrate battery exhibits a maximum power density of5.85 mW cm^(-2)with a NH_(3)yield of 92.50μmol cm^(-2)h^(-1)and Faradaic efficiency of 99.15%at 20 mA cm^(-2)for NH_(3)production.This work not only offers a rational design concept with clear guidance for efficient modulation of intermediate adsorption free energy on alloy catalysts prepared by electrodeposition,but also provides the further understanding for efficient developments of NO_(3)^(-)RR and Zn-based batteries.
文摘Electrochemical reduction of carbon dioxide(CO_(2)RR)is a promising approach to complete the carbon cycle and potentially convert CO_(2)into valuable chemicals and fuels.Cu is unique among transition metals in its ability to catalyze the CO_(2)RR and produce multi-carbon products.However,achieving high selectivity for C2+products is challenging for copper-based catalysts,as C–C coupling reactions proceed slowly.Herein,a surface modification strategy involving grafting long alkyl chains onto copper nanowires(Cu NWs)has been proposed to regulate the electronic structure of Cu surface,which facilitates*CO-*CO coupling in the CO_(2)RR.The hydrophobicity of the catalysts increases greatly after the introduction of long alkyl chains,therefore the hydrogen evolution reaction(HER)has been inhibited effectively.Such surface modification approach proves to be highly efficient and universal,with the Faradaic efficiency(FE)of C_(2)H_(4) up to 53%for the optimized Cu–SH catalyst,representing a significant enhancement compared to the pristine Cu NWs(30%).In-situ characterizations and theoretical calculations demonstrate that the different terminal groups of the grafted octadecyl chains can effectively regulate the charge density of Cu NWs interface and change the adsorption configuration of*CO intermediate.The top-adsorbed*CO intermediates(*COtop)on Cu–SH catalytic interface endow Cu–SH with the highest charge density,which effectively lowers the reaction energy barrier for*CO-*CO coupling,promoting the formation of the*OCCO intermediate,thereby enhancing the selectivity towards C_(2)H_(4).This study provides a promising method for designing efficient Cu-based catalysts with high catalytic activity and selectivity towards C2H4.
基金supported by the Natural Science Foundation of Hunan Province(No.2023JJ30650)the Central South University Innovation-Driven Research Programme(No.2023CXQD061)。
文摘The atomic-level exploration of structure-property correlations poses significant challenges in establishing precise design principles for electrocatalysts targeting efficient CO_(2)conversion.This study demonstrates how controlled exposure of metal sites governs CO_(2)electroreduction performance through two octanuclear bismuth-oxo clusters with distinct architectures.The Bi_(8)-DMF cluster,constructed using tert–butylthiacalix[4]arene(TC4A)as the sole ligand,features two surface-exposed Bi active sites,while the dual-ligand Bi_(8)-Fc(with TC4A/ferrocene carboxylate)forms a fully encapsulated structure.Electrocatalytic tests reveal Bi_(8)-DMF achieves exceptional formate selectivity(>90%Faradaic efficiency)across a broad potential window(-0.9 V to-1.6 V vs.RHE)with 20 h stability,outperforming Bi_(8)-Fc(60%efficiency at-1.5 V).Theoretical calculations attribute Bi_(8)-DMF's superiority to exposed Bi sites that stabilize the critical*OCHO intermediate via optimized orbital interactions.This work provides crucial guidance for polynuclear catalyst design:moderate exposure of metal active sites significantly enhances CO_(2)reduction performance.
