Fast and high-throughput determination of drugs is a key trend in clinical medicine.Single particles have increasingly been adopted in a variety of photoanalytical and electroanalytical applications,and microscopic an...Fast and high-throughput determination of drugs is a key trend in clinical medicine.Single particles have increasingly been adopted in a variety of photoanalytical and electroanalytical applications,and microscopic analysis has been a hot topic in recent years,especially for electrochemiluminescence(ECL).This paper describes a simple ECL method based on single gold microbeads to image lecithin.Lecithin reacts to produce hydrogen peroxide under the successive enzymatic reaction of phospholipase D and choline oxidase.ECL was generated by the electrochemical reaction between a luminol analog and hydrogen peroxide,and ECL signals were imaged by a camera.Despite the heterogeneity of single gold microbeads,their luminescence obeyed statistical regularity.The average luminescence of 30 gold microbeads is correlated with the lecithin concentration,and thus,a visualization method for analyzing lecithin was established.Calibration curves were constructed for ECL intensity and lecithin concentration,achieving detection limits of 0.05 m M lecithin.This ECL imaging platform based on single gold microbeads exhibits outstanding advantages,such as high throughput,versatility and low cost,and holds great potential in disease diagnostics,environmental monitoring and food safety.展开更多
Polyferrocene macrocycles hold immense potential in the fields of molecular electronics and electrochemistry,primarily due to their multiple metal centers.However,developing highly efficient synthetic strategies for c...Polyferrocene macrocycles hold immense potential in the fields of molecular electronics and electrochemistry,primarily due to their multiple metal centers.However,developing highly efficient synthetic strategies for constructing these rings remains a significant challenge.In this study,we successfully synthesized triferrocenyl macrocycles using Pt-mediated coupling strategy and determined their configuration using single-crystal X-ray diffraction analysis,revealing a structure reminiscent of the Penrose Stair.We comprehensively investigated the macrocycle’s structure,photophysical properties,and employed density functional theory(DFT)calculations to gain further insights.Notably,this macrocycle exhibits several advantageous features,including a flexible structure,good solubility,and a highly efficient synthetic pathway.展开更多
Chemodynamic therapy(CDT)is considered as a promising modality for selective cancer therapy,which is realized via Fenton reaction-mediated decomposition of endogenous H_(2)O_(2) to produce toxic hydroxyl radical(•OH)f...Chemodynamic therapy(CDT)is considered as a promising modality for selective cancer therapy,which is realized via Fenton reaction-mediated decomposition of endogenous H_(2)O_(2) to produce toxic hydroxyl radical(•OH)for tumor ablation.While extensive efforts have been made to develop CDT-based therapeutics,their in vivo efficacy is usually unsatisfactory due to poor catalytic activity limited by tumor microenvironment,such as anti-oxidative systems,insufficient H_(2)O_(2),and mild acidity.To mitigate these issues,we have witnessed a surge in the development of CDT-based combinatorial nanomedicines with complementary or synergistic mechanisms for enhanced tumor therapy.By virtue of their bio-imaging capabilities,Fenton metal nanomedicines(FMNs)are equipped with intrinsic properties of imaging-guided tumor therapies.In this critical review,we summarize recent progress of this field,focusing on FMNs for imaging-guided combinatorial tumor therapy.First,various Fenton metals with inherent catalytic performances and imaging properties,including Fe,Cu and Mn,were introduced to illustrate their possible applications for tumor theranostics.Then,CDT-based combinatorial systems were reviewed by incorporating many other treatment means,including chemotherapy,photodynamic therapy(PDT),sonodynamic therapy(SDT),photothermal therapy(PTT),starvation therapy and immunotherapy.Next,various imaging approaches based on Fenton metals were presented in detail.Finally,challenges are discussed,and future prospects are speculated in the field to pave way for future developments.展开更多
The utilization of non-noble metal catalysts with robust and highly efficient electrocatalytic activity for hydrogen evolution reaction(HER)and oxygen evolution reaction(OER)are extremely important for the large-scale...The utilization of non-noble metal catalysts with robust and highly efficient electrocatalytic activity for hydrogen evolution reaction(HER)and oxygen evolution reaction(OER)are extremely important for the large-scale implementation of renewable energy devices.Integration of bifunctional electrocatalysts on both anode and cathode electrodes remains a significant challenge.Herein,we report on a novel and facile strategy to construct the ordered and aligned MoS_(2)nanosheet-encapsulated metal–organic frameworks(MOFs)derived hollow CoS polyhedron,in-situ grown on a nickel foam(NF).The starfish-like MoS_(2)/CoS/NF heterojunctions were formed due to the ordered growth of the material caused by NF substrate.The optimized 2-MoS_(2)/CoS/NF heterojunction exhibits robust bifunctional electrocatalytic activity with a low overpotential of 67 and 207 m V toward the HER and OER at 10 mA cm^(-2),and the long-term stability,which exceeds most of the reported bifunctional electrocatalysts.Such high electrocatalytic performance arises due to the synergistic effect between the MoS_(2)and CoS phases across the interface,the abundant active sites,as well as the hierarchical pore framework,which collectively enhance the mass and electron transfer during the reactions.The work provides a promising approach to fabricating bifunctional catalysts with custom-designed heterojunctions and remarkable performance for applications in electrochemical energy devices and related areas.展开更多
Electrocatalysis is a surface-sensitive process,in which the catalytic activity of electrocatalyst highly re-lates to the surface adsorption/desorption behaviors of the reactants/intermediates/products on the cat-alyt...Electrocatalysis is a surface-sensitive process,in which the catalytic activity of electrocatalyst highly re-lates to the surface adsorption/desorption behaviors of the reactants/intermediates/products on the cat-alytically active sites.Surface chemical microenvironment engineering via organic molecules functional-ization is a promising strategy to tune the electrocatalytic activity since it can well modify the elec-trode/electrolyte interface and alter the reaction pathways.In this review,we summarize the recent progress of surface microenvironment engineering of electrocatalysts induced by organic molecules func-tionalization,with the special focus on the organic molecule-assisted growth mechanism and unique electronic effect.More importantly,the applications of organic molecule functionalized catalysts in var-ious electrocatalytic reactions are also systematically summarized,along with a deep discussion on the conclusion and perspective.This work will open a new avenue for the construction and modification of advanced electrocatalysts based on organic molecule-mediated interface engineering.展开更多
A double magnetic separation-assisted fluorescence method was developed to rapidly detect ochratoxin A(OTA). The OTA aptamer functionalized magnetic nanomaterial(Fe3O4-Aptanier) and complementary DNA conjugated nitrog...A double magnetic separation-assisted fluorescence method was developed to rapidly detect ochratoxin A(OTA). The OTA aptamer functionalized magnetic nanomaterial(Fe3O4-Aptanier) and complementary DNA conjugated nitrogen-doped graphene quantum dots(NGQDs-cDNA) were used in this assay. Aptamer could hybridize with cDNA, which induced tlie NGQDs-cDNA to bind onto Fe3O4-Aptamer, and resulted in the fluorescence quenching of NGQDs. After the addition of OTA, the NGQDs-cDNA could release into the solution, and resulted in the recovery of fluorescence signal of NGQDs consequently. By utilizing the magnetic separation, the unbonded NGQDs-cDNA and residual Fe3O4-Aptamer were removed, which significantly increased the fluorescence signal intensity. OTA could be detected in the linear range of 10 nmol/L to 2000 nmol/L, with a limit of detection as 0.66 mnol/L. The advantages of this method include simple operation, good selectivity and high sensitivity, and this method can be used for the rapid detection of ochratoxin A in wheat and com.展开更多
Silver-catalyzed decarboxylative C–H alkylation of cyclic aldimines with abundant aliphatic carboxylic acids has been realized under mild reaction conditions generating the corresponding products in moderate to good ...Silver-catalyzed decarboxylative C–H alkylation of cyclic aldimines with abundant aliphatic carboxylic acids has been realized under mild reaction conditions generating the corresponding products in moderate to good yields(32%–91%).In addition,a gram-scale reaction,late-stage modification of drug,synthetic transformation of the product,and further application of the catalytic strategy were also performed.Preliminary studies indicate that the reaction undergoes a radical process.展开更多
Accurate detection of hydrogen sulfide(H_(2)S)is of great significance for environmental monitoring and protection.We propose a colorimetric method for the detection of H_(2)S by the use of mixed-node Cu-Fe metal orga...Accurate detection of hydrogen sulfide(H_(2)S)is of great significance for environmental monitoring and protection.We propose a colorimetric method for the detection of H_(2)S by the use of mixed-node Cu-Fe metal organic frameworks(Cu-Fe MOFs)as highly efficient mimic enzymes for target-induced deactivation.The Cu-Fe MOFs were synthesized by a simple solvothermal method and could catalyze the H_(2)O_(2)mediated oxidation of 3,30,5,50-tetramethylbenzidine(TMB)to oxTMB with a blue color.The presence of dissolved H_(2)S would deactivate the mimic enzymes,and then the blue color disappeared.The mechanism of the sensor was discussed by steady-state kinetic analysis.The designed assay was highly sensitive for H_(2)S detection with a linear range of 0à80 mmol/L and a detection limit of 1.6 mmol/L.Moreover,some potential substances in the water samples had no interference.This method with the advantages of low cost,high sensitivity,selectivity,and visual readout with the naked eye was successfully applied to the determination of H_(2)S in industrial wastewater samples.展开更多
The interfacial proton transfer(PT)reaction on the metal oxide surface is an important step in many chemical processes including photoelectrocatalytic water splitting,dehydrogenation,and hydrogen storage.The investiga...The interfacial proton transfer(PT)reaction on the metal oxide surface is an important step in many chemical processes including photoelectrocatalytic water splitting,dehydrogenation,and hydrogen storage.The investigation of the PT process,in terms of thermodynamics and kinetics,has received considerable attention,but the individual free energy barriers and solvent effects for different PT pathways on rutile oxide are still lacking.Here,by applying a combination of ab initio and deep potential molecular dynamics methods,we have studied interfacial PT mechanisms by selecting the rutile SnO_(2)(110)/H_(2)O interface as an example of an oxide with the characteristic of frequently interfacial PT processes.Three types of PT pathways among the interfacial groups are found,i.e.,proton transfer from terminal adsorbed water to bridge oxygen directly(surface-PT)or via a solvent water(mediated-PT),and proton hopping between two terminal groups(adlayer PT).Our simulations reveal that the terminal water in mediated-PT prefers to point toward the solution and forms a shorter H-bond with the assisted solvent water,leading to the lowest energy barrier and the fastest relative PT rate.In particular,it is found that the full solvation environment plays a crucial role in water-mediated proton conduction,while having little effect on direct PT reactions.The PT mechanisms on aqueous rutile oxide interfaces are also discussed by comparing an oxide series composed of SnO_(2),TiO_(2),and IrO_(2).Consequently,this work provides valuable insights into the ability of a deep neural network to reproduce the ab initio potential energy surface,as well as the PT mechanisms at such oxide/liquid interfaces,which can help understand the important chemical processes in electrochemistry,photoelectrocatalysis,colloid science,and geochemistry.展开更多
Transition metal sulfides are demonstrated to play an increasingly important role in boosting the deployment of ecofriendly electrocatalytic energy conversion technologies.It is also widely recognized that the introdu...Transition metal sulfides are demonstrated to play an increasingly important role in boosting the deployment of ecofriendly electrocatalytic energy conversion technologies.It is also widely recognized that the introduction of vacancies is now becoming an important and valid approach to promote the electrocatalytic performance.In this review,the significance of sulfur vacancies on the enhancement of catalytic performance via four main functionalities,including tuning the electronic structure,tailoring the active sites,improving the electrical conductivity,and regulating surface reconstruction,is comprehensively summarized.Many effective strategies for the sulfur vacancy engineering,such as plasma treatment,heteroatom doping,and chemical reduction are also comprehensively provided.Subsequently,recent achievements in sulfur vacancy fabrication on various hotspot electrocatalytic reactions are also systematically discussed.Finally,a summary of the recent progress and challenges of this interesting field are organized,which hopes to guide the future development of more efficient metal sulfide electrocatalysts.展开更多
In this study,we developed an eff ective method to detect hypochlorite acid(HClO)by using methylene blue(MB)derivative(BPY1).BPY1 was selectively oxidized through HClO,and the solution color changed from colorless to ...In this study,we developed an eff ective method to detect hypochlorite acid(HClO)by using methylene blue(MB)derivative(BPY1).BPY1 was selectively oxidized through HClO,and the solution color changed from colorless to blue.In the presence of HClO,the ultraviolet–visible(UV–vis)spectra and concentration of HClO had a linear relationship with a detection limit of 0.5μM.Furthermore,a test paper for HClO monitoring was successfully prepared using the BPY1 probe,and the observed detection limit by the naked eye was estimated at 5μM.Additionally,using the BPY1 probe,HClO could also be detected through smartphone colorimetry,and the method showed a good recovery ranging from 98.7 to 104.0%for HClO detection in an actual water sample.Especially for developing countries,such a low-cost and highly sensitive detection method provides a simple and practical method for monitoring HClO in water.展开更多
1 Introduction As environmental pollution continues to worsen,governments are increasing their efforts to develop green transport vehicles,such as electric vehicles and hybrid cars.
In this work,via a facile solvothermal route,we synthesized an anode material for lithium ion batteries（LIBs）—SnS2 nanoparticle/graphene（SnS2 NP/GNs） nanocomposite.The nanocomposite consists of SnS2nanoparticles ...In this work,via a facile solvothermal route,we synthesized an anode material for lithium ion batteries（LIBs）—SnS2 nanoparticle/graphene（SnS2 NP/GNs） nanocomposite.The nanocomposite consists of SnS2nanoparticles with an average diameter of 4 nm and graphene nanosheets without restacking.The SnS2 nanoparticles are firmly anchored on the graphene nanosheets.As an anode material for LIBs,the nanocomposite exhibits good Li storage performance especially high rate performance.At the high current rate of 5,10,and 20 A/g,the nanocomposite delivered high capacities of 525,443,and 378 mAh/g,respectively.The good conductivity of the graphene nanosheets and the small particle size of SnS2contribute to the electrochemical performance of SnS2 NP/GNs.展开更多
基金supported by Anhui Provincial Natural Science Foundation(Grant Nos.2008085QB68 and 1808085QB29)Key Project of Provincial Natural Science Research Foundation of Anhui Universities(Grant Nos.KJ2018A0675 and KJ2018A0389)+1 种基金Foundation of State Key Laboratory of Analytical Chemistry for Life Science(Grant No.SKLACLS2003)Foundation of Henan Key Laboratory of Biomolecular Recognition and Sensing(Grant No.HKLBRSK1905)。
文摘Fast and high-throughput determination of drugs is a key trend in clinical medicine.Single particles have increasingly been adopted in a variety of photoanalytical and electroanalytical applications,and microscopic analysis has been a hot topic in recent years,especially for electrochemiluminescence(ECL).This paper describes a simple ECL method based on single gold microbeads to image lecithin.Lecithin reacts to produce hydrogen peroxide under the successive enzymatic reaction of phospholipase D and choline oxidase.ECL was generated by the electrochemical reaction between a luminol analog and hydrogen peroxide,and ECL signals were imaged by a camera.Despite the heterogeneity of single gold microbeads,their luminescence obeyed statistical regularity.The average luminescence of 30 gold microbeads is correlated with the lecithin concentration,and thus,a visualization method for analyzing lecithin was established.Calibration curves were constructed for ECL intensity and lecithin concentration,achieving detection limits of 0.05 m M lecithin.This ECL imaging platform based on single gold microbeads exhibits outstanding advantages,such as high throughput,versatility and low cost,and holds great potential in disease diagnostics,environmental monitoring and food safety.
基金supported by the National Natural Science Foundation of China(Nos.22071025 and 22373019)the Key Research and Development and Promotion Projects in Henan Province,China(No.222102520032).
文摘Polyferrocene macrocycles hold immense potential in the fields of molecular electronics and electrochemistry,primarily due to their multiple metal centers.However,developing highly efficient synthetic strategies for constructing these rings remains a significant challenge.In this study,we successfully synthesized triferrocenyl macrocycles using Pt-mediated coupling strategy and determined their configuration using single-crystal X-ray diffraction analysis,revealing a structure reminiscent of the Penrose Stair.We comprehensively investigated the macrocycle’s structure,photophysical properties,and employed density functional theory(DFT)calculations to gain further insights.Notably,this macrocycle exhibits several advantageous features,including a flexible structure,good solubility,and a highly efficient synthetic pathway.
基金supported by Innovation-Driven Project of Central South University (No. 20170030010004)National Natural Science Foundation of China (Nos. 21804144, U1903125, 82073799)
文摘Chemodynamic therapy(CDT)is considered as a promising modality for selective cancer therapy,which is realized via Fenton reaction-mediated decomposition of endogenous H_(2)O_(2) to produce toxic hydroxyl radical(•OH)for tumor ablation.While extensive efforts have been made to develop CDT-based therapeutics,their in vivo efficacy is usually unsatisfactory due to poor catalytic activity limited by tumor microenvironment,such as anti-oxidative systems,insufficient H_(2)O_(2),and mild acidity.To mitigate these issues,we have witnessed a surge in the development of CDT-based combinatorial nanomedicines with complementary or synergistic mechanisms for enhanced tumor therapy.By virtue of their bio-imaging capabilities,Fenton metal nanomedicines(FMNs)are equipped with intrinsic properties of imaging-guided tumor therapies.In this critical review,we summarize recent progress of this field,focusing on FMNs for imaging-guided combinatorial tumor therapy.First,various Fenton metals with inherent catalytic performances and imaging properties,including Fe,Cu and Mn,were introduced to illustrate their possible applications for tumor theranostics.Then,CDT-based combinatorial systems were reviewed by incorporating many other treatment means,including chemotherapy,photodynamic therapy(PDT),sonodynamic therapy(SDT),photothermal therapy(PTT),starvation therapy and immunotherapy.Next,various imaging approaches based on Fenton metals were presented in detail.Finally,challenges are discussed,and future prospects are speculated in the field to pave way for future developments.
基金the financial support from the National Natural Science Foundation of China(22005273,21825106 and 21671175)the Natural Science Foundation of Henan Province(222300420258)+3 种基金the Scientific and Technological Research Project in Henan Province(222102240065 and 212102210647)the Key scientific research projects of colleges and universities in Henan Province(No.22A530006)the Natural Science Foundation of Jiangsu Province(BK20220598)the Program for Science&Technology Innovative Research Team in University of Henan Province(20IRTSTHN007)。
文摘The utilization of non-noble metal catalysts with robust and highly efficient electrocatalytic activity for hydrogen evolution reaction(HER)and oxygen evolution reaction(OER)are extremely important for the large-scale implementation of renewable energy devices.Integration of bifunctional electrocatalysts on both anode and cathode electrodes remains a significant challenge.Herein,we report on a novel and facile strategy to construct the ordered and aligned MoS_(2)nanosheet-encapsulated metal–organic frameworks(MOFs)derived hollow CoS polyhedron,in-situ grown on a nickel foam(NF).The starfish-like MoS_(2)/CoS/NF heterojunctions were formed due to the ordered growth of the material caused by NF substrate.The optimized 2-MoS_(2)/CoS/NF heterojunction exhibits robust bifunctional electrocatalytic activity with a low overpotential of 67 and 207 m V toward the HER and OER at 10 mA cm^(-2),and the long-term stability,which exceeds most of the reported bifunctional electrocatalysts.Such high electrocatalytic performance arises due to the synergistic effect between the MoS_(2)and CoS phases across the interface,the abundant active sites,as well as the hierarchical pore framework,which collectively enhance the mass and electron transfer during the reactions.The work provides a promising approach to fabricating bifunctional catalysts with custom-designed heterojunctions and remarkable performance for applications in electrochemical energy devices and related areas.
基金supported by the Key Research&Development and Promotion Projects in Henan Province(No.232102230079).
文摘Electrocatalysis is a surface-sensitive process,in which the catalytic activity of electrocatalyst highly re-lates to the surface adsorption/desorption behaviors of the reactants/intermediates/products on the cat-alytically active sites.Surface chemical microenvironment engineering via organic molecules functional-ization is a promising strategy to tune the electrocatalytic activity since it can well modify the elec-trode/electrolyte interface and alter the reaction pathways.In this review,we summarize the recent progress of surface microenvironment engineering of electrocatalysts induced by organic molecules func-tionalization,with the special focus on the organic molecule-assisted growth mechanism and unique electronic effect.More importantly,the applications of organic molecule functionalized catalysts in var-ious electrocatalytic reactions are also systematically summarized,along with a deep discussion on the conclusion and perspective.This work will open a new avenue for the construction and modification of advanced electrocatalysts based on organic molecule-mediated interface engineering.
基金the National Natural Science Foundation of China(No.21305032)the China Postdoctoral Science Foundation (No.2014M551522)+2 种基金the Postdoctoral Science Foundation of Jiangsu Province, China(No.1402073B)the Henan Key Laboratory of Biomolecular Recognition and Sensing(Shangqiu Normal University), China(No.HKLBRSKl803)the Hong Kong Scholar Program, China (No. XJ2017008).
文摘A double magnetic separation-assisted fluorescence method was developed to rapidly detect ochratoxin A(OTA). The OTA aptamer functionalized magnetic nanomaterial(Fe3O4-Aptanier) and complementary DNA conjugated nitrogen-doped graphene quantum dots(NGQDs-cDNA) were used in this assay. Aptamer could hybridize with cDNA, which induced tlie NGQDs-cDNA to bind onto Fe3O4-Aptamer, and resulted in the fluorescence quenching of NGQDs. After the addition of OTA, the NGQDs-cDNA could release into the solution, and resulted in the recovery of fluorescence signal of NGQDs consequently. By utilizing the magnetic separation, the unbonded NGQDs-cDNA and residual Fe3O4-Aptamer were removed, which significantly increased the fluorescence signal intensity. OTA could be detected in the linear range of 10 nmol/L to 2000 nmol/L, with a limit of detection as 0.66 mnol/L. The advantages of this method include simple operation, good selectivity and high sensitivity, and this method can be used for the rapid detection of ochratoxin A in wheat and com.
基金financially supported by the National Natural Science Foundation of China(Nos.21402116,21502111,21572126)the Science and Technology Innovation Talents of Henan Province(No.2018JQ0011)the Key Science Research of Education Committee in Henan Province(No.21A150044)。
文摘Silver-catalyzed decarboxylative C–H alkylation of cyclic aldimines with abundant aliphatic carboxylic acids has been realized under mild reaction conditions generating the corresponding products in moderate to good yields(32%–91%).In addition,a gram-scale reaction,late-stage modification of drug,synthetic transformation of the product,and further application of the catalytic strategy were also performed.Preliminary studies indicate that the reaction undergoes a radical process.
基金the financial support from the National Natural Science Foundation of China(Nos.21675109,22074089)Central Thousand Talents Plan(No.ZYQR201810151)Henan Joint International Research Laboratory of Chemo/Biosensing and Early Diagnosis of Major Diseases。
文摘Accurate detection of hydrogen sulfide(H_(2)S)is of great significance for environmental monitoring and protection.We propose a colorimetric method for the detection of H_(2)S by the use of mixed-node Cu-Fe metal organic frameworks(Cu-Fe MOFs)as highly efficient mimic enzymes for target-induced deactivation.The Cu-Fe MOFs were synthesized by a simple solvothermal method and could catalyze the H_(2)O_(2)mediated oxidation of 3,30,5,50-tetramethylbenzidine(TMB)to oxTMB with a blue color.The presence of dissolved H_(2)S would deactivate the mimic enzymes,and then the blue color disappeared.The mechanism of the sensor was discussed by steady-state kinetic analysis.The designed assay was highly sensitive for H_(2)S detection with a linear range of 0à80 mmol/L and a detection limit of 1.6 mmol/L.Moreover,some potential substances in the water samples had no interference.This method with the advantages of low cost,high sensitivity,selectivity,and visual readout with the naked eye was successfully applied to the determination of H_(2)S in industrial wastewater samples.
基金funding from the National Science Fund for Distinguished Young Scholars(Grant No.22225302)the National Natural Science Foundation of China(Grant Nos.92161113,21991151,21991150,and 22021001)+5 种基金the Fundamental Research Funds for the Central Universities(Grant Nos.20720220008,20720220009,20720220010)Laboratory of AI for Electrochemistry(AI4EC)IKKEM(Grant Nos.RD2023100101 and RD2022070501)M.J.greatly appreciates the financial support from the Natural Science Foundation of Henan Province(Grant No.242300420420570)the Key Scientific Research Projects of Colleges and Universities in Henan Province(No.24A150031)the International Scientific and Technological Cooperation Projects in Henan Province(No.232102520020)。
文摘The interfacial proton transfer(PT)reaction on the metal oxide surface is an important step in many chemical processes including photoelectrocatalytic water splitting,dehydrogenation,and hydrogen storage.The investigation of the PT process,in terms of thermodynamics and kinetics,has received considerable attention,but the individual free energy barriers and solvent effects for different PT pathways on rutile oxide are still lacking.Here,by applying a combination of ab initio and deep potential molecular dynamics methods,we have studied interfacial PT mechanisms by selecting the rutile SnO_(2)(110)/H_(2)O interface as an example of an oxide with the characteristic of frequently interfacial PT processes.Three types of PT pathways among the interfacial groups are found,i.e.,proton transfer from terminal adsorbed water to bridge oxygen directly(surface-PT)or via a solvent water(mediated-PT),and proton hopping between two terminal groups(adlayer PT).Our simulations reveal that the terminal water in mediated-PT prefers to point toward the solution and forms a shorter H-bond with the assisted solvent water,leading to the lowest energy barrier and the fastest relative PT rate.In particular,it is found that the full solvation environment plays a crucial role in water-mediated proton conduction,while having little effect on direct PT reactions.The PT mechanisms on aqueous rutile oxide interfaces are also discussed by comparing an oxide series composed of SnO_(2),TiO_(2),and IrO_(2).Consequently,this work provides valuable insights into the ability of a deep neural network to reproduce the ab initio potential energy surface,as well as the PT mechanisms at such oxide/liquid interfaces,which can help understand the important chemical processes in electrochemistry,photoelectrocatalysis,colloid science,and geochemistry.
基金supported by the start-up funding to H.Xu by Changzhou University(No.ZMF22020055)Advanced Catalysis and Green Manufacturing Collaborative Innovation Center,Changzhou University for financial support。
文摘Transition metal sulfides are demonstrated to play an increasingly important role in boosting the deployment of ecofriendly electrocatalytic energy conversion technologies.It is also widely recognized that the introduction of vacancies is now becoming an important and valid approach to promote the electrocatalytic performance.In this review,the significance of sulfur vacancies on the enhancement of catalytic performance via four main functionalities,including tuning the electronic structure,tailoring the active sites,improving the electrical conductivity,and regulating surface reconstruction,is comprehensively summarized.Many effective strategies for the sulfur vacancy engineering,such as plasma treatment,heteroatom doping,and chemical reduction are also comprehensively provided.Subsequently,recent achievements in sulfur vacancy fabrication on various hotspot electrocatalytic reactions are also systematically discussed.Finally,a summary of the recent progress and challenges of this interesting field are organized,which hopes to guide the future development of more efficient metal sulfide electrocatalysts.
基金the National Natural Science Foundation of China(Nos.U1404215,22074089,21804085,21675109)Innovation Scientists and Technicians Troop Construction Projects of Henan Province(No:41)Key Scientific Research Projects of Colleges and Universities in Henan Province(No:21A150043)for support。
文摘In this study,we developed an eff ective method to detect hypochlorite acid(HClO)by using methylene blue(MB)derivative(BPY1).BPY1 was selectively oxidized through HClO,and the solution color changed from colorless to blue.In the presence of HClO,the ultraviolet–visible(UV–vis)spectra and concentration of HClO had a linear relationship with a detection limit of 0.5μM.Furthermore,a test paper for HClO monitoring was successfully prepared using the BPY1 probe,and the observed detection limit by the naked eye was estimated at 5μM.Additionally,using the BPY1 probe,HClO could also be detected through smartphone colorimetry,and the method showed a good recovery ranging from 98.7 to 104.0%for HClO detection in an actual water sample.Especially for developing countries,such a low-cost and highly sensitive detection method provides a simple and practical method for monitoring HClO in water.
基金supported by the National Science Foundation of China(51502009,51532001,21675109)the National Key Basic Research Program of China(2014CB31802)the Science Foundation of Henan province(162300410209)
文摘1 Introduction As environmental pollution continues to worsen,governments are increasing their efforts to develop green transport vehicles,such as electric vehicles and hybrid cars.
基金financially supported by the National Natural Science Foundation of China (No. 21475085)the key scientific research project of high schools in Henan Province (Nos. 16A430025 & 17A480009)
文摘In this work,via a facile solvothermal route,we synthesized an anode material for lithium ion batteries（LIBs）—SnS2 nanoparticle/graphene（SnS2 NP/GNs） nanocomposite.The nanocomposite consists of SnS2nanoparticles with an average diameter of 4 nm and graphene nanosheets without restacking.The SnS2 nanoparticles are firmly anchored on the graphene nanosheets.As an anode material for LIBs,the nanocomposite exhibits good Li storage performance especially high rate performance.At the high current rate of 5,10,and 20 A/g,the nanocomposite delivered high capacities of 525,443,and 378 mAh/g,respectively.The good conductivity of the graphene nanosheets and the small particle size of SnS2contribute to the electrochemical performance of SnS2 NP/GNs.
