Effectively separating bastnaesite from calcium-bearing gangue minerals(particularly calcite)presents a formidable challenge,making the development of efficient collectors crucial.To achieve this,we have designed and ...Effectively separating bastnaesite from calcium-bearing gangue minerals(particularly calcite)presents a formidable challenge,making the development of efficient collectors crucial.To achieve this,we have designed and synthesized a novel,highly efficient,water-soluble cationic collector,N-dodecylisopropanolamine(NDIA),for use in the bastnaesite-calcite flotation process.Density functional theory(DFT)calculations identified the amine nitrogen atom in NDIA as the site most susceptible to electrophilic attack and electron loss.By introducing an OH group into the traditional collector dodecylamine(DDA)structure,NDIA provided additional adsorption sites,enabling synergistic adsorption on the surface of bastnaesite,thereby significantly enhancing both the floatability and selectivity of these minerals.The recovery of bastnaesite was 76.02%,while the calcite was 1.26%.The NDIA markedly affected the zeta potential of bastnaesite,while its impact on calcite was relatively minor.Detailed Fourier-transform infrared spectroscopy(FTIR)and X-ray photoelectron spectroscopy(XPS)results elucidated that the―NH―and―OH groups in NDIA anchored onto the bastnaesite surface through robust electrostatic and hydrogen bonding interactions,thereby enhancing bastnaesite's affinity for NDIA.Furthermore,in situ atomic force microscopy(AFM)provided conclusive evidence of NDIA aggregation on the bastnaesite surface,improving contact angle and hydrophobicity,and significantly boosting the flotation recovery of bastnaesite.展开更多
The electrochemical interaction between galena and monoclinic pyrrhotite was investigated to examine its impact on the physical and chemical properties of the mineral micro-surface.This investigation employed techniqu...The electrochemical interaction between galena and monoclinic pyrrhotite was investigated to examine its impact on the physical and chemical properties of the mineral micro-surface.This investigation employed techniques such as electrochemistry,metal ion stripping,X-ray photoelectron spectroscopy,and quantum chemistry.The electrochemical test results demonstrate that the galena surface in the electro-couple system exhibits a lower electrostatic potential and higher electrochemical activity compared to the monoclinic pyrrhotite surface,rendering it more susceptible to oxidation dissolution.Monoclinic pyrrhotite significantly amplifies the corrosion rate of the galena surface.Mulliken charge population calculations indicate that electrons are consistently transferred from galena to monoclinic pyrrhotite,with the number of electron transfers on the mineral surface increasing as the interaction distance decreases.The analysis of state density revealed a shift in the surface state density of galena towards lower energy levels,resulting in decreased reactivity and increased difficulty for the reagent to adsorb onto the mineral surface.Conversely,monoclinic pyrrhotite exhibited an opposite trend.The X-ray photoelectron spectroscopy(XPS)test results indicate that galvanic interaction leads to the formation of hydrophilic substances,PbS_(x)O_(y) and Pb(OH)_(2),on the surface of galena.Additionally,the surface of monoclinic pyrrhotite not only adsorbs Pb^(2+)but also undergoes S^(0) formation,thereby augmenting its hydrophobic nature.展开更多
Cancer metastasis is the leading cause of death in cancer patients worldwide and one of the major challenges in treating cancer.Circulating tumor cells(CTCs)play a pivotal role in cancer metastasis.However,the content...Cancer metastasis is the leading cause of death in cancer patients worldwide and one of the major challenges in treating cancer.Circulating tumor cells(CTCs)play a pivotal role in cancer metastasis.However,the content of CTCs in peripheral blood is minimal,so the detection of CTCs in real samples is extremely challenging.Therefore,efficient enrichment and early detection of CTCs are essential to achieve timely diagnosis of diseases.In this work,we constructed an innovative and sensitive single-nanoparticle collision electrochemistry(SNCE)biosensor for the detection of MCF-7 cells(human breast cancer cells)by immunomagnetic separation technique and liposome signal amplification strategy.Liposomes embedded with platinum nanoparticles(Pt NPs)were used as signal probes,and homemade gold ultramicroelectrodes(Au UME)were used as the working electrodes.The effective collision between Pt NPs and UME would produce distinguishable step-type current.MCF-7 cells were accurately quantified according to the relationship between cell concentration and collision frequency(the number of step-type currents generated per unit time),realizing highly sensitive and specific detection of MCF-7 cells.The SNCE biosensor has a linear range of 10 cells·mL^(-1)to 10^(5) cells·mL^(-1)with a detection limit as low as 5 cells·mL^(-1).In addition,the successful detection of MCF-7 cells in complex samples showed that the SNCE biosensors have great potential for patient sample detection.展开更多
Single-entity collisional electrochemistry(SECE)is a branch of single-entity electrochemistry.It can directly characterize entities/particles with single particle resolution through random collisions between particles...Single-entity collisional electrochemistry(SECE)is a branch of single-entity electrochemistry.It can directly characterize entities/particles with single particle resolution through random collisions between particles and electrodes in a solution,and obtain rich physicochemical information,thus becoming one of the frontiers of electroanalytical chemistry in the past two decades.Interestingly,the(micro/nanoscale)sensing electrodes have evolved from a polarizable liquid/liquid(mercury/liquid)interface to a solid/liquid interface and then to a liquid/liquid interface(i.e.,an interface between twoimmiscible electrolyte solutions,ITIES),as if they have completed a cycle(but in fact they have not).ITIES has become the latest sensing electrode in the booming SECE due to its polarizability(up to 1.1 V at the water/a,a,a-trifluorotoluene interface)and high reproducibility.The four measurement modes(direct electrolysis,mediated electrolysis,current blockade,and charge displacement)developed in the realm of SECE at solid/liquid interfaces have also been fully realized at the miniature ITIES.This article will discuss these four modes at the ITIES from the perspectives of basic concepts,operating mechanisms,and latest developments(e.g.,discovery of ionosomes,blockade effect of Faradaic ion transfer,etc.),and look forward to the future development and direction of this emerging field.展开更多
Chloropcroxidase （CPO） was immobilized by konjac glucomannan （KGM） on the 1-butyl-3-methyl imidazolium tetrafluoroborate [BMIM][BF4]/Nafion modified glassy carbon eloctrode. The electrochemical behaviors of the im...Chloropcroxidase （CPO） was immobilized by konjac glucomannan （KGM） on the 1-butyl-3-methyl imidazolium tetrafluoroborate [BMIM][BF4]/Nafion modified glassy carbon eloctrode. The electrochemical behaviors of the immobilized CPO were investigated by cyclic voltammetry. The results showed that CPO was successfully immobilized on the GCE and underwent fast direct electron transfer reactions with the formal potential at -0.3 V vs. SCE. The modified electrode showed a good catalytic activity for elcctrocatalytical reduction of O2 and H2O2.展开更多
For designing batteries with high-rate and long-life, electronic/ionic transport and reaction must be unified for metal oxide electrodes. However, it remains challenging for effectively integrating the whole substrate...For designing batteries with high-rate and long-life, electronic/ionic transport and reaction must be unified for metal oxide electrodes. However, it remains challenging for effectively integrating the whole substrate/active materials/electrolyte interfaces. Herein by taking Li ion battery as example, we propose a semiconductor-electrochemistry model by which a general but novel insight has been gained into interfacial effect in batteries. Different from those traditional viewpoints, this derived model lies across from physics to electrochemistry. A reaction driving force can be expressed in terms of Fermi energy change,based on the tradeoff between electronic and ionic concentration at the reaction interfacial region. Therefore, at thermodynamic-controlled interface I of substrate/electrode, increasing contact areas can afford higher activity for active materials. Whereas at kinetically-governed interface II of electrode/electrolyte or inside active materials, it is crucial to guarantee high-reaction Li ionic concentration, with which some sufficient reaction degrees can reach.展开更多
In the thermodynamics, for flotation separation of the SbAs bulk concentrate system there is no potential extent using butyl xanthate as collector. However in the kinetics, there exists 150 mV in reducing potential of...In the thermodynamics, for flotation separation of the SbAs bulk concentrate system there is no potential extent using butyl xanthate as collector. However in the kinetics, there exists 150 mV in reducing potential of butyl dixanthogen on the surface of stibnite and arsenopyrite. In this paper, their reducing kinetic difference of electrochemistry was confirmed by pure mineral flotation under controlled potential, the artificial SbAs bulk concentrate flotation separation and UVspectrophotometic analysis. The electrochemical separation of SbAs bulk concentrate has been carried out. qualified concentrate has been obtained. Sbconcentrate contains Sb 4944 %, As 044 %, Sbrecovery is 8783 % and Asconcentrate contains As 1096 %, Asrecovery is 9466 %.展开更多
The development of highly safe and low-cost aqueous batteries is of great significance in the background of carbon neutrality.However,the practical deployment of aqueous batteries has been plagued due to their relativ...The development of highly safe and low-cost aqueous batteries is of great significance in the background of carbon neutrality.However,the practical deployment of aqueous batteries has been plagued due to their relatively low capacity and poor cycling stability.Herein,we propose unique conversion electrochemistry of copper selenides for robust and energetic aqueous charge storage.In situ X-ray diffraction and operando Raman techniques reveal a reversible transformation from CuSe to Cu_(2)Se through the intermediates of Cu_(3)Se_(2) and Cu_(1.8)Se.Such a conversion process activates the redox carrier of Cu^(2+)ion and delivers a remarkable rate capability of 285 mAh g^(-1) at 20 A g^(-1) and electrochemical durability up to 30,000 cycles.Furthermore,Cu^(2+)and H+coinsertion chemistry is proposed to facilitate the conversion process.As a proof-of-concept,a hybrid aqueous pouch cell coupling CuSe//Zn is capable of affording maximum energy and power densities of 190 Wh kg^(-1) and 1366W kg^(-1),respectively.展开更多
Metal-organic frameworks(MOFs)with high porosity and variable structure have attracted extensive attention in the field of electrochemistry,but their poor conductivity and stability have limited their development.Mate...Metal-organic frameworks(MOFs)with high porosity and variable structure have attracted extensive attention in the field of electrochemistry,but their poor conductivity and stability have limited their development.Materials derived from MOFs can maintain the structural diversity and porosity characteristics of MOFs while improving their electrical conductivity and stability.Metal phosphides play an important role in electrochemistry because they possess rich active sites,unique physicochemical properties,and a porous structure.Published results show that MOF-derived metal-phosphides materials have great promise in the field of electrochemistry due to their controllable structure,high specific surface area,high stability and excellent electrical conductivity.MOF-derived metal-phosphides with significant electrochemical properties can be obtained by simply,economical and scalable synthetic methods.This work reviews the application of MOF-derived metal phosphides in electrochemistry.Specifically,the synthesis methodology and morphological characterization of MOFs derived metal-phosphides and their application in electrochemistry are described.Based on recent scientific advances,we discuss the challenges and opportunities for future research on MOF-derived metal-phosphides materials.展开更多
Layered two-dimensional(2 D)materials have received tremendous attention due to their unique physical and chemical properties when downsized to single or few layers.Several types of layered materials,especially transi...Layered two-dimensional(2 D)materials have received tremendous attention due to their unique physical and chemical properties when downsized to single or few layers.Several types of layered materials,especially transition metal dichalcogenides(TMDs)have been demonstrated to be good electrode materials due to their interesting physical and chemical properties.Apart from TMDs,post-transition metal chalcogenides(PTMCs)recently have emerged as a family of important semiconducting materials for electrochemical studies.PTMCs are layered materials which are composed of post-transition metals raging from main group IIIA to group VA(Ga,In,Ge,Sn,Sb and Bi)and group VI chalcogen atoms(S,selenium(Se)and tellurium(Te)).Although a large number of literatures have reviewed the electrochemical and electrocatalytic applications of TMDs,less attention has been focused on PTMCs.In this review,we focus our attention on PTMCs with the aim to provide a summary to describe their fundamental electrochemical properties and electrocatalytic activity towards hydrogen evolution reaction(HER).The characteristic chemical compositions and crystal structures of PTMCs are firstly discussed,which are different from TMDs.Then,inherent electrochemistry of PTMCs is discussed to unveil the well-defined redox behaviors of PTMCs,which could potentially affect their efficiency when applied as electrode materials.Following,we focus our attention on electrocatalytic activity of PTMCs towards HER including novel synthetic strategies developed for the optimization of their HER activity.This review ends with the perspectives for the future research direction in the field of PTMC based electrocatalysts.展开更多
Exploring novel versatile electrode materials with outstanding electrochemical performance is the key to the development of advanced energy conversion and storage devices.In this work,we aim to construct new-fangled o...Exploring novel versatile electrode materials with outstanding electrochemical performance is the key to the development of advanced energy conversion and storage devices.In this work,we aim to construct new-fangled one-dimensional(1D)quasi-layered patronite vanadium tetrasulfide(VS_(4))nanostructures by using different sulfur sources,namely thiourea,thioacetamide,and L-cysteine through an ethyleneaminetetraacetic-acid(EDTA)-mediated solvothermal process.The as-prepared VS4exhibits several unique morphologies such as urchin,fluffy nanoflower,and polyhedron with appropriate surface areas.Among the prepared nanostructures,the VS_(4)-1@NF nanostructure exhibited excellent electrochemical properties in 6 M KOH solution,and we explored its redox electrochemistry in detail.The asprepared VS_(4)-1@NF electrode exhibited battery-type redox characteristics with the highest capacity of280 C g^(-1)in a three-electrode assembly.Moreover,it offered a capacity of 123 F g^(-1)in a hybrid twoelectrode set-up at 1 A g^(-1)with the highest specific energy and specific power of 38.5 W h kg^(-1)and750 W kg^(-1),respectively.Furthermore,to ensure the practical applicability and real-world performance of the prepared hybrid AC@NF//VS_(4)-1@NF cell,we performed a cycling stability test with more than 5,000galvanostatic charge–discharge cycles at 2 A g^(-1),and the cell retained around 84.7%of its capacitance even after 5,000 cycles with a CE of 96.1%.展开更多
In the past decade, the aprotic lithium-oxygen(Li-O_2) battery has generated a great deal of interest because theoretically it can store more energy than today's lithium-ion batteries. Although considerable resear...In the past decade, the aprotic lithium-oxygen(Li-O_2) battery has generated a great deal of interest because theoretically it can store more energy than today's lithium-ion batteries. Although considerable research efforts have been devoted to the R&D of this potentially disruptive technology, many scientific and engineering obstacles still remain to be addressed before a practical device could be realized. In this review, we summarize recent advances in the fundamental understanding of the O_2 electrochemistry in Li-O_2 batteries, including the O_2 reduction to Li_2O_2 on discharge and the reverse Li_2 O_2 oxidation on recharge and factors that exert strong influences on the redox of O_2/Li_2O_2. In addition,challenges and perspectives are also provided for the future study of Li—O_2 batteries.展开更多
Techniques are developed for studying the mechanism of localized corrosion and protectivemeasures against such corrosion are suggested.The pH values and composition of the occluded sol-ution at different propagation s...Techniques are developed for studying the mechanism of localized corrosion and protectivemeasures against such corrosion are suggested.The pH values and composition of the occluded sol-ution at different propagation stages are determined.Measurements of the critical pH value and cor-rosion rate inside the occluded cells are conducted.Potential-pH diagrams depicting kinetic andthermodynamic behaviors of occluded cell corrosion are being established.The mechanism of inhibi-tion of pitting and stress corrosion cracking have also been investigated.展开更多
Stable adsorption and direct electrochemistry of glucose oxidase （COx） occurred on nitric acid （HNO3）-treated multi-walled carbon nanotubcs （MWNTs） instead of as-received MWNTs, demonstrating the critical roles ...Stable adsorption and direct electrochemistry of glucose oxidase （COx） occurred on nitric acid （HNO3）-treated multi-walled carbon nanotubcs （MWNTs） instead of as-received MWNTs, demonstrating the critical roles of oxygen-containing groups in stable adsorption and direct electrochemistry of GOx on carbon nanotubcs （CNTs）.展开更多
The direct electron transfer of hemoglobin at the PAMAM-MWNTs-AuNPs composite film modified glassy carbon electrode was studied. In a phosphate buffer solution（PBS, pH=7.0）, the formal potential（E^0） of Hb was -0....The direct electron transfer of hemoglobin at the PAMAM-MWNTs-AuNPs composite film modified glassy carbon electrode was studied. In a phosphate buffer solution（PBS, pH=7.0）, the formal potential（E^0） of Hb was -0.105 V versus SCE, the electron transfer rate constant was 4.66 s-1. E^0＇ of Hb at the modified electrode was linearly varied in a pH range of 5.0-8.0 with a slope of-49.2 mV/pH. The Hb/PAMAM-MWNTs-AuNPs/GCE gave an excellent electrocatalytic response to the reduction of hydrogen peroxide. The catalytic current increased linearly with H2O2 concentration in a range of 1.0× 10^-6 to 2.2× 10^-3 mol/L. The detection limit was 2.0× 10^-7 mol/L at a signal to noise ratio of 3. The Michaelis-Menten constant（Km^app） was 2.95 mmol/L.展开更多
Nanotube-based mixed-dimensional or one-dimensional heterostructures have attracted great attention recently because of their unique physical properties and therefore potential for novel devices. Their chemical proper...Nanotube-based mixed-dimensional or one-dimensional heterostructures have attracted great attention recently because of their unique physical properties and therefore potential for novel devices. Their chemical properties, however, were less explored but can be utilized for energy storage and conversion.In this review, we summarize the recent progress of nanotube-based low dimensional materials for electrochemistry, in particular, lithium storage and hydrogen evolution. First, we describe the atomic structure of low-dimensional heterostructures and briefly touch previous work on planar van der Waals heterostructures(2D+2D) in electrochemistry applications. Then we focus this review on the more recently developed nanotube-based, i.e., 1D+2D and 1D + 1D heterostructures, and discuss their various preparation approaches and electrochemical performances. Finally, we outline the challenges and opportunities in this direction and particularly emphasize the possibility of building high-performance electrodes using a single-walled carbon nanotube-based ultra-thin 1D heterostructure, and the importance of understanding the fundamental mechanism at atomic precision.展开更多
Room temperature ionic liquid （RTILs） [BMIM]PF6 was used as a new kind of binder to construct a chemical modified carbon paste electrode （CPE） and the direct electrochemistry of hemoglobin （Hb）, which was immobi...Room temperature ionic liquid （RTILs） [BMIM]PF6 was used as a new kind of binder to construct a chemical modified carbon paste electrode （CPE） and the direct electrochemistry of hemoglobin （Hb）, which was immobilized on the surface of RTIL/CPE with the film of sodium alginate hydrogel, was studied by cyclic voltammetry. The presence of RTILs improved the direct electron transfer of Hb and a pair of well-defined quasi-revesible redox peaks appeared in pH 7.0 B-R buffer solution. The cathodic and anodic peak potentials were located at -0.383 V and -0.305 V with the formal potential （E^0） at -0.344 V （vs. SCE）. In addition the immobilized Hb showed good electrocatalytic activity to the reduction of H2O2.展开更多
The difference in the electrochemical behavior of hydroquinone and pyrocatechol at platinum and gold surfaces was analyzed using voltammetry and attenuated total reflection Fourier transform infrared spectroscopy. The...The difference in the electrochemical behavior of hydroquinone and pyrocatechol at platinum and gold surfaces was analyzed using voltammetry and attenuated total reflection Fourier transform infrared spectroscopy. The results show that the hydroquinone derivatives are adsorbed on a gold surface with vertical orientation, which makes the electron transfer between the bulk species and the electrode surface easier than that in the case of flat adsorption of hydroquinone derivatives that occurs at a platinum electrode. The formation of the vertical conformation and the rapid process of electron transfer were also confirmed by quantum chemistry calculations. In addition, the pre-adsorbed iodine on the electrodes played a key role on the adsorbed configuration and electron transfer of redox species.展开更多
The recent development on flotation electrochemistry of sulphide minerals at Central South University of Technology is briefly summarized. General behavior of natural floatability, self and sulphur induced, and collec...The recent development on flotation electrochemistry of sulphide minerals at Central South University of Technology is briefly summarized. General behavior of natural floatability, self and sulphur induced, and collector induced floatability of sulphide minerals are described. The mechanism is discussed based on Eh pH diagrams, voltammograms, energy band theory and molecular orbital theory.展开更多
基金supported by the the National Key R&D Program of China(No.2021YFC2900800)National Natural Science Foundation of China(Nos.52425406,51874247,51922091,and 52204285)+4 种基金the Open Research Fund of State Key Laboratory of Complex Nonferrous Metal Resources Clean Utilization(No.CNMRCUKF2001)Science and Technology Major Project of Ordos City-Iconic Innovation Team and “Rejuvenating Inner Mongolia through Science and Technology”(No.202204/2023)Yueqi Outstanding Scholar Award of CUMTB(No.202022)Funded by Open Foundation of State Key Laboratory of Mineral Processing(No.BGRIMM-KJSKL-2023-05)Fundamental Research Funds for the Central Universities(Ph.D.Top Innovative Talents Fund of CUMT BBJ2024048)。
文摘Effectively separating bastnaesite from calcium-bearing gangue minerals(particularly calcite)presents a formidable challenge,making the development of efficient collectors crucial.To achieve this,we have designed and synthesized a novel,highly efficient,water-soluble cationic collector,N-dodecylisopropanolamine(NDIA),for use in the bastnaesite-calcite flotation process.Density functional theory(DFT)calculations identified the amine nitrogen atom in NDIA as the site most susceptible to electrophilic attack and electron loss.By introducing an OH group into the traditional collector dodecylamine(DDA)structure,NDIA provided additional adsorption sites,enabling synergistic adsorption on the surface of bastnaesite,thereby significantly enhancing both the floatability and selectivity of these minerals.The recovery of bastnaesite was 76.02%,while the calcite was 1.26%.The NDIA markedly affected the zeta potential of bastnaesite,while its impact on calcite was relatively minor.Detailed Fourier-transform infrared spectroscopy(FTIR)and X-ray photoelectron spectroscopy(XPS)results elucidated that the―NH―and―OH groups in NDIA anchored onto the bastnaesite surface through robust electrostatic and hydrogen bonding interactions,thereby enhancing bastnaesite's affinity for NDIA.Furthermore,in situ atomic force microscopy(AFM)provided conclusive evidence of NDIA aggregation on the bastnaesite surface,improving contact angle and hydrophobicity,and significantly boosting the flotation recovery of bastnaesite.
基金supported by the National Key Research and Development Program Project(No.2022YFC2904504).
文摘The electrochemical interaction between galena and monoclinic pyrrhotite was investigated to examine its impact on the physical and chemical properties of the mineral micro-surface.This investigation employed techniques such as electrochemistry,metal ion stripping,X-ray photoelectron spectroscopy,and quantum chemistry.The electrochemical test results demonstrate that the galena surface in the electro-couple system exhibits a lower electrostatic potential and higher electrochemical activity compared to the monoclinic pyrrhotite surface,rendering it more susceptible to oxidation dissolution.Monoclinic pyrrhotite significantly amplifies the corrosion rate of the galena surface.Mulliken charge population calculations indicate that electrons are consistently transferred from galena to monoclinic pyrrhotite,with the number of electron transfers on the mineral surface increasing as the interaction distance decreases.The analysis of state density revealed a shift in the surface state density of galena towards lower energy levels,resulting in decreased reactivity and increased difficulty for the reagent to adsorb onto the mineral surface.Conversely,monoclinic pyrrhotite exhibited an opposite trend.The X-ray photoelectron spectroscopy(XPS)test results indicate that galvanic interaction leads to the formation of hydrophilic substances,PbS_(x)O_(y) and Pb(OH)_(2),on the surface of galena.Additionally,the surface of monoclinic pyrrhotite not only adsorbs Pb^(2+)but also undergoes S^(0) formation,thereby augmenting its hydrophobic nature.
基金supported by the National Natural Science Foundation of China(Nos.22274037,22376055 and 21904032)the Natural Science Foundation of Hubei Province(2022CFB383)。
文摘Cancer metastasis is the leading cause of death in cancer patients worldwide and one of the major challenges in treating cancer.Circulating tumor cells(CTCs)play a pivotal role in cancer metastasis.However,the content of CTCs in peripheral blood is minimal,so the detection of CTCs in real samples is extremely challenging.Therefore,efficient enrichment and early detection of CTCs are essential to achieve timely diagnosis of diseases.In this work,we constructed an innovative and sensitive single-nanoparticle collision electrochemistry(SNCE)biosensor for the detection of MCF-7 cells(human breast cancer cells)by immunomagnetic separation technique and liposome signal amplification strategy.Liposomes embedded with platinum nanoparticles(Pt NPs)were used as signal probes,and homemade gold ultramicroelectrodes(Au UME)were used as the working electrodes.The effective collision between Pt NPs and UME would produce distinguishable step-type current.MCF-7 cells were accurately quantified according to the relationship between cell concentration and collision frequency(the number of step-type currents generated per unit time),realizing highly sensitive and specific detection of MCF-7 cells.The SNCE biosensor has a linear range of 10 cells·mL^(-1)to 10^(5) cells·mL^(-1)with a detection limit as low as 5 cells·mL^(-1).In addition,the successful detection of MCF-7 cells in complex samples showed that the SNCE biosensors have great potential for patient sample detection.
基金supported by the National Natural Science Foundation of China(No.21904143).
文摘Single-entity collisional electrochemistry(SECE)is a branch of single-entity electrochemistry.It can directly characterize entities/particles with single particle resolution through random collisions between particles and electrodes in a solution,and obtain rich physicochemical information,thus becoming one of the frontiers of electroanalytical chemistry in the past two decades.Interestingly,the(micro/nanoscale)sensing electrodes have evolved from a polarizable liquid/liquid(mercury/liquid)interface to a solid/liquid interface and then to a liquid/liquid interface(i.e.,an interface between twoimmiscible electrolyte solutions,ITIES),as if they have completed a cycle(but in fact they have not).ITIES has become the latest sensing electrode in the booming SECE due to its polarizability(up to 1.1 V at the water/a,a,a-trifluorotoluene interface)and high reproducibility.The four measurement modes(direct electrolysis,mediated electrolysis,current blockade,and charge displacement)developed in the realm of SECE at solid/liquid interfaces have also been fully realized at the miniature ITIES.This article will discuss these four modes at the ITIES from the perspectives of basic concepts,operating mechanisms,and latest developments(e.g.,discovery of ionosomes,blockade effect of Faradaic ion transfer,etc.),and look forward to the future development and direction of this emerging field.
基金supported by grants from National Natural Science Foundation of China (No.20503016,20775049).
文摘Chloropcroxidase （CPO） was immobilized by konjac glucomannan （KGM） on the 1-butyl-3-methyl imidazolium tetrafluoroborate [BMIM][BF4]/Nafion modified glassy carbon eloctrode. The electrochemical behaviors of the immobilized CPO were investigated by cyclic voltammetry. The results showed that CPO was successfully immobilized on the GCE and underwent fast direct electron transfer reactions with the formal potential at -0.3 V vs. SCE. The modified electrode showed a good catalytic activity for elcctrocatalytical reduction of O2 and H2O2.
基金the National Natural Science Foundation of China(51872115)Program for the Development of Science and Technology of Jilin Province(20190201309JC)+5 种基金the Fundamental Research Funds for the Central Universities(Grant no.531107051230)The Open Project Program of Wuhan National Laboratory for Optoelectronicsthe Jilin Province/Jilin University co-Construction Project-Funds for New Materials(SXGJSF2017-3,Branch-2/440050316A36)Program for JLU Science and Technology Innovative Research Team(JLUSTIRT,2017TD-09)the Fundamental Research Funds for the Central Universities,JLU“Double-First Class”Discipline for Materials Science&Engineering。
文摘For designing batteries with high-rate and long-life, electronic/ionic transport and reaction must be unified for metal oxide electrodes. However, it remains challenging for effectively integrating the whole substrate/active materials/electrolyte interfaces. Herein by taking Li ion battery as example, we propose a semiconductor-electrochemistry model by which a general but novel insight has been gained into interfacial effect in batteries. Different from those traditional viewpoints, this derived model lies across from physics to electrochemistry. A reaction driving force can be expressed in terms of Fermi energy change,based on the tradeoff between electronic and ionic concentration at the reaction interfacial region. Therefore, at thermodynamic-controlled interface I of substrate/electrode, increasing contact areas can afford higher activity for active materials. Whereas at kinetically-governed interface II of electrode/electrolyte or inside active materials, it is crucial to guarantee high-reaction Li ionic concentration, with which some sufficient reaction degrees can reach.
文摘In the thermodynamics, for flotation separation of the SbAs bulk concentrate system there is no potential extent using butyl xanthate as collector. However in the kinetics, there exists 150 mV in reducing potential of butyl dixanthogen on the surface of stibnite and arsenopyrite. In this paper, their reducing kinetic difference of electrochemistry was confirmed by pure mineral flotation under controlled potential, the artificial SbAs bulk concentrate flotation separation and UVspectrophotometic analysis. The electrochemical separation of SbAs bulk concentrate has been carried out. qualified concentrate has been obtained. Sbconcentrate contains Sb 4944 %, As 044 %, Sbrecovery is 8783 % and Asconcentrate contains As 1096 %, Asrecovery is 9466 %.
基金Natural Science Foundation of Shanghai,Grant/Award Number:22ZR1403600Natural Science Foundation of Jiangsu Province,Grant/Award Number:BK20180002+1 种基金National Natural Science Foundation of China,Grant/Award Numbers:22109029,51772197,51872192,52025028,52172219Natural Science Foundation of the Jiangsu Higher Education Institutions of China,Grant/Award Number:19KJA170001。
文摘The development of highly safe and low-cost aqueous batteries is of great significance in the background of carbon neutrality.However,the practical deployment of aqueous batteries has been plagued due to their relatively low capacity and poor cycling stability.Herein,we propose unique conversion electrochemistry of copper selenides for robust and energetic aqueous charge storage.In situ X-ray diffraction and operando Raman techniques reveal a reversible transformation from CuSe to Cu_(2)Se through the intermediates of Cu_(3)Se_(2) and Cu_(1.8)Se.Such a conversion process activates the redox carrier of Cu^(2+)ion and delivers a remarkable rate capability of 285 mAh g^(-1) at 20 A g^(-1) and electrochemical durability up to 30,000 cycles.Furthermore,Cu^(2+)and H+coinsertion chemistry is proposed to facilitate the conversion process.As a proof-of-concept,a hybrid aqueous pouch cell coupling CuSe//Zn is capable of affording maximum energy and power densities of 190 Wh kg^(-1) and 1366W kg^(-1),respectively.
基金supported by the National Natural Science Foundation of China(U1904215)Natural Science Foundation of Jiangsu Province(BK20200044)Changjiang scholars program of the Ministry of Education(Q2018270)。
文摘Metal-organic frameworks(MOFs)with high porosity and variable structure have attracted extensive attention in the field of electrochemistry,but their poor conductivity and stability have limited their development.Materials derived from MOFs can maintain the structural diversity and porosity characteristics of MOFs while improving their electrical conductivity and stability.Metal phosphides play an important role in electrochemistry because they possess rich active sites,unique physicochemical properties,and a porous structure.Published results show that MOF-derived metal-phosphides materials have great promise in the field of electrochemistry due to their controllable structure,high specific surface area,high stability and excellent electrical conductivity.MOF-derived metal-phosphides with significant electrochemical properties can be obtained by simply,economical and scalable synthetic methods.This work reviews the application of MOF-derived metal phosphides in electrochemistry.Specifically,the synthesis methodology and morphological characterization of MOFs derived metal-phosphides and their application in electrochemistry are described.Based on recent scientific advances,we discuss the challenges and opportunities for future research on MOF-derived metal-phosphides materials.
基金financial support from the National Natural Science Foundation of China(Grant No.11774044)。
文摘Layered two-dimensional(2 D)materials have received tremendous attention due to their unique physical and chemical properties when downsized to single or few layers.Several types of layered materials,especially transition metal dichalcogenides(TMDs)have been demonstrated to be good electrode materials due to their interesting physical and chemical properties.Apart from TMDs,post-transition metal chalcogenides(PTMCs)recently have emerged as a family of important semiconducting materials for electrochemical studies.PTMCs are layered materials which are composed of post-transition metals raging from main group IIIA to group VA(Ga,In,Ge,Sn,Sb and Bi)and group VI chalcogen atoms(S,selenium(Se)and tellurium(Te)).Although a large number of literatures have reviewed the electrochemical and electrocatalytic applications of TMDs,less attention has been focused on PTMCs.In this review,we focus our attention on PTMCs with the aim to provide a summary to describe their fundamental electrochemical properties and electrocatalytic activity towards hydrogen evolution reaction(HER).The characteristic chemical compositions and crystal structures of PTMCs are firstly discussed,which are different from TMDs.Then,inherent electrochemistry of PTMCs is discussed to unveil the well-defined redox behaviors of PTMCs,which could potentially affect their efficiency when applied as electrode materials.Following,we focus our attention on electrocatalytic activity of PTMCs towards HER including novel synthetic strategies developed for the optimization of their HER activity.This review ends with the perspectives for the future research direction in the field of PTMC based electrocatalysts.
基金supported by the Research Program of Dongguk University in 2022(No.S-2022-G0001-00016)。
文摘Exploring novel versatile electrode materials with outstanding electrochemical performance is the key to the development of advanced energy conversion and storage devices.In this work,we aim to construct new-fangled one-dimensional(1D)quasi-layered patronite vanadium tetrasulfide(VS_(4))nanostructures by using different sulfur sources,namely thiourea,thioacetamide,and L-cysteine through an ethyleneaminetetraacetic-acid(EDTA)-mediated solvothermal process.The as-prepared VS4exhibits several unique morphologies such as urchin,fluffy nanoflower,and polyhedron with appropriate surface areas.Among the prepared nanostructures,the VS_(4)-1@NF nanostructure exhibited excellent electrochemical properties in 6 M KOH solution,and we explored its redox electrochemistry in detail.The asprepared VS_(4)-1@NF electrode exhibited battery-type redox characteristics with the highest capacity of280 C g^(-1)in a three-electrode assembly.Moreover,it offered a capacity of 123 F g^(-1)in a hybrid twoelectrode set-up at 1 A g^(-1)with the highest specific energy and specific power of 38.5 W h kg^(-1)and750 W kg^(-1),respectively.Furthermore,to ensure the practical applicability and real-world performance of the prepared hybrid AC@NF//VS_(4)-1@NF cell,we performed a cycling stability test with more than 5,000galvanostatic charge–discharge cycles at 2 A g^(-1),and the cell retained around 84.7%of its capacitance even after 5,000 cycles with a CE of 96.1%.
基金supported by the National Foundation of China (Grant No. 91545129, 21575135 and 21605136)the "Strategic Priority Research Program" of the CAS (Grant No. XDA09010401)+1 种基金the National Key R&D Program of China (Grant No. 2016YBF0100100)the Science and Technology Development Program of the Jilin Province (Grant No. 20150623002TC and 20160414034GH)
文摘In the past decade, the aprotic lithium-oxygen(Li-O_2) battery has generated a great deal of interest because theoretically it can store more energy than today's lithium-ion batteries. Although considerable research efforts have been devoted to the R&D of this potentially disruptive technology, many scientific and engineering obstacles still remain to be addressed before a practical device could be realized. In this review, we summarize recent advances in the fundamental understanding of the O_2 electrochemistry in Li-O_2 batteries, including the O_2 reduction to Li_2O_2 on discharge and the reverse Li_2 O_2 oxidation on recharge and factors that exert strong influences on the redox of O_2/Li_2O_2. In addition,challenges and perspectives are also provided for the future study of Li—O_2 batteries.
文摘Techniques are developed for studying the mechanism of localized corrosion and protectivemeasures against such corrosion are suggested.The pH values and composition of the occluded sol-ution at different propagation stages are determined.Measurements of the critical pH value and cor-rosion rate inside the occluded cells are conducted.Potential-pH diagrams depicting kinetic andthermodynamic behaviors of occluded cell corrosion are being established.The mechanism of inhibi-tion of pitting and stress corrosion cracking have also been investigated.
基金This research is supported by the National Natural Science Foundation of China(Nos.30370397 and 60571042).
文摘Stable adsorption and direct electrochemistry of glucose oxidase （COx） occurred on nitric acid （HNO3）-treated multi-walled carbon nanotubcs （MWNTs） instead of as-received MWNTs, demonstrating the critical roles of oxygen-containing groups in stable adsorption and direct electrochemistry of GOx on carbon nanotubcs （CNTs）.
基金Supported by the National Natural Science Foundation of China(No.20605009)
文摘The direct electron transfer of hemoglobin at the PAMAM-MWNTs-AuNPs composite film modified glassy carbon electrode was studied. In a phosphate buffer solution（PBS, pH=7.0）, the formal potential（E^0） of Hb was -0.105 V versus SCE, the electron transfer rate constant was 4.66 s-1. E^0＇ of Hb at the modified electrode was linearly varied in a pH range of 5.0-8.0 with a slope of-49.2 mV/pH. The Hb/PAMAM-MWNTs-AuNPs/GCE gave an excellent electrocatalytic response to the reduction of hydrogen peroxide. The catalytic current increased linearly with H2O2 concentration in a range of 1.0× 10^-6 to 2.2× 10^-3 mol/L. The detection limit was 2.0× 10^-7 mol/L at a signal to noise ratio of 3. The Michaelis-Menten constant（Km^app） was 2.95 mmol/L.
基金supported by JSPS KAKENHI(JP18H05329,JP19H02543,JP20H00220,JP20KK0114)by JST,CREST(JPMJCR20B5),Japan+2 种基金conducted at the Advanced Characterization Nanotechnology Platform of the University of Tokyosupported by the “Nanotechnology Platform”of the MEXT,Japan(JPMXP09A20UT0063 and JPMXP09A21UT0050)。
文摘Nanotube-based mixed-dimensional or one-dimensional heterostructures have attracted great attention recently because of their unique physical properties and therefore potential for novel devices. Their chemical properties, however, were less explored but can be utilized for energy storage and conversion.In this review, we summarize the recent progress of nanotube-based low dimensional materials for electrochemistry, in particular, lithium storage and hydrogen evolution. First, we describe the atomic structure of low-dimensional heterostructures and briefly touch previous work on planar van der Waals heterostructures(2D+2D) in electrochemistry applications. Then we focus this review on the more recently developed nanotube-based, i.e., 1D+2D and 1D + 1D heterostructures, and discuss their various preparation approaches and electrochemical performances. Finally, we outline the challenges and opportunities in this direction and particularly emphasize the possibility of building high-performance electrodes using a single-walled carbon nanotube-based ultra-thin 1D heterostructure, and the importance of understanding the fundamental mechanism at atomic precision.
基金supported by the National Natural.Science Foundation of China(No.20405008,20635020).
文摘Room temperature ionic liquid （RTILs） [BMIM]PF6 was used as a new kind of binder to construct a chemical modified carbon paste electrode （CPE） and the direct electrochemistry of hemoglobin （Hb）, which was immobilized on the surface of RTIL/CPE with the film of sodium alginate hydrogel, was studied by cyclic voltammetry. The presence of RTILs improved the direct electron transfer of Hb and a pair of well-defined quasi-revesible redox peaks appeared in pH 7.0 B-R buffer solution. The cathodic and anodic peak potentials were located at -0.383 V and -0.305 V with the formal potential （E^0） at -0.344 V （vs. SCE）. In addition the immobilized Hb showed good electrocatalytic activity to the reduction of H2O2.
基金Supported by the National Natural Science Foundation of China(No. 20475053) and Department of Science and Technology ofJilin Province(No.20050102)
文摘The difference in the electrochemical behavior of hydroquinone and pyrocatechol at platinum and gold surfaces was analyzed using voltammetry and attenuated total reflection Fourier transform infrared spectroscopy. The results show that the hydroquinone derivatives are adsorbed on a gold surface with vertical orientation, which makes the electron transfer between the bulk species and the electrode surface easier than that in the case of flat adsorption of hydroquinone derivatives that occurs at a platinum electrode. The formation of the vertical conformation and the rapid process of electron transfer were also confirmed by quantum chemistry calculations. In addition, the pre-adsorbed iodine on the electrodes played a key role on the adsorbed configuration and electron transfer of redox species.
文摘The recent development on flotation electrochemistry of sulphide minerals at Central South University of Technology is briefly summarized. General behavior of natural floatability, self and sulphur induced, and collector induced floatability of sulphide minerals are described. The mechanism is discussed based on Eh pH diagrams, voltammograms, energy band theory and molecular orbital theory.
