The development of flexible zinc-ion batteries(ZIBs)faces a threeway trade-off among the ionic conductivity,Zn^(2+)mobility,and the electrochemical stability of hydrogel electrolytes.To address this challenge,we desig...The development of flexible zinc-ion batteries(ZIBs)faces a threeway trade-off among the ionic conductivity,Zn^(2+)mobility,and the electrochemical stability of hydrogel electrolytes.To address this challenge,we designed a cationic hydrogel named PAPTMA to holistically improve the reversibility of ZIBs.The long cationic branch chains in the polymeric matrix construct express pathways for rapid Zn^(2+)transport through an ionic repulsion mechanism,achieving simultaneously high Zn^(2+)transference number(0.79)and high ionic conductivity(28.7 mS cm−1).Additionally,the reactivity of water in the PAPTMA hydrogels is significantly inhibited,thus possessing a strong resistance to parasitic reactions.Mechanical characterization further reveals the superior tensile and adhesion strength of PAPTMA.Leveraging these properties,symmetric batteries employing PAPTMA hydrogel deliver exceeding 6000 h of reversible cycling at 1 mA cm^(−2) and maintain stable operation for 1000 h with a discharge of depth of 71%.When applied in 4×4 cm2 pouch cells with MnO_(2) as the cathode material,the device demonstrates remarkable operational stability and mechanical robustness through 150 cycles.This work presents an eclectic strategy for designing advanced hydrogels that combine high ionic conductivity,enhanced Zn^(2+)mobility,and strong resistance to parasitic reactions,paving the way for long-lasting flexible ZIBs.展开更多
Practical Zn metal batteries have been hindered by several challenges,including Zn dendrite growth,undesirable side reactions,and unstable electrode/electrolyte interface.These issues are particularly more serious in ...Practical Zn metal batteries have been hindered by several challenges,including Zn dendrite growth,undesirable side reactions,and unstable electrode/electrolyte interface.These issues are particularly more serious in low-concentration electrolytes.Herein,we design a Zn salt-mediated electrolyte with in situ ring-opening polymerization of the small molecule organic solvent.The Zn(TFSI)_(2)salt catalyzes the ring-opening polymerization of(1,3-dioxolane(DOL)),generating oxidation-resistant and non-combustible long-chain polymer(poly(1,3-dioxolane)(pDOL)).The pDOL reduces the active H_(2)O molecules in electrolyte and assists in forming stable organic–inorganic gradient solid electrolyte interphase with rich organic constituents,ZnO and ZnF_(2).The introduction of pDOL endows the electrolyte with several advantages:excellent Zn dendrite inhibition,improved corrosion resistance,widened electrochemical window(2.6 V),and enhanced low-temperature performance(freezing point=-34.9°C).Zn plating/stripping in pDOL-enhanced electrolyte lasts for 4200 cycles at 99.02%Coulomb efficiency and maintains a lifetime of 8200 h.Moreover,Zn metal anodes deliver stable cycling for 2500 h with a high Zn utilization of 60%.A Zn//VO_(2)pouch cell assembled with lean electrolyte(electrolyte/capacity(E/C=41 mL(Ah)^(-1))also demonstrates a capacity retention ratio of 92%after 600 cycles.These results highlight the promising application prospects of practical Zn metal batteries enabled by the Zn(TFSI)2-mediated electrolyte engineering.展开更多
With the merits of the high energy density of batteries and power density of supercapacitors,the aqueous Zn-ion hybrid supercapacitors emerge as a promising candidate for applications where both rapid energy delivery ...With the merits of the high energy density of batteries and power density of supercapacitors,the aqueous Zn-ion hybrid supercapacitors emerge as a promising candidate for applications where both rapid energy delivery and moderate energy storage are required.However,the narrow electrochemical window of aqueous electrolytes induces severe side reactions on the Zn metal anode and shortens its lifespan.It also limits the operation voltage and energy density of the Zn-ion hybrid supercapacitors.Using'water in salt'electrolytes can effectively broaden their electrochemical windows,but this is at the expense of high cost,low ionic conductivity,and narrow temperature compatibility,compromising the electrochemical performance of the Zn-ion hybrid supercapacitors.Thus,designing a new electrolyte to balance these factors towards high-performance Zn-ion hybrid supercapacitors is urgent and necessary.We developed a dilute water/acetonitrile electrolyte(0.5 m Zn(CF_(3)SO_(3))_(2)+1 m LiTFSI-H_(2)O/AN)for Zn-ion hybrid supercapacitors,which simultaneously exhibited expanded electrochemical window,decent ionic conductivity,and broad temperature compatibility.In this electrolyte,the hydration shells and hydrogen bonds are significantly modulated by the acetonitrile and TFSI-anions.As a result,a Zn-ion hybrid supercapacitor with such an electrolyte demonstrates a high operating voltage up to 2.2 V and long lifespan beyond 120,000 cycles.展开更多
A considerable efficiency gap exists between large-area perovskite solar modules and small-area perovskite solar cells.The control of forming uniform and large-area film and perovskite crystallization is still the mai...A considerable efficiency gap exists between large-area perovskite solar modules and small-area perovskite solar cells.The control of forming uniform and large-area film and perovskite crystallization is still the main obstacle restricting the efficiency of PSMs.In this work,we adopted a solid-liquid two-step film formation technique,which involved the evaporation of a lead iodide film and blade coating of an organic ammonium halide solution to prepare perovskite films.This method possesses the advantages of integrating vapor deposition and solution methods,which could apply to substrates with different roughness and avoid using toxic solvents to achieve a more uniform,large-area perovskite film.Furthermore,modification of the NiO_(x)/perovskite buried interface and introduction of Urea additives were utilized to reduce interface recombination and regulate perovskite crystallization.As a result,a large-area perovskite film possessing larger grains,fewer pinholes,and reduced defects could be achieved.The inverted PSM with an active area of 61.56 cm^(2)(10×10 cm^(2)substrate)achieved a champion power conversion efficiency of 20.56%and significantly improved stability.This method suggests an innovative approach to resolving the uniformity issue associated with large-area film fabrication.展开更多
Suppression of uncontrollable dendrite growth and water-induced side reactions of Zn metal anodes is crucial for achieving long-lasting cycling stability and facilitating the practical implementations of aqueous Zn-me...Suppression of uncontrollable dendrite growth and water-induced side reactions of Zn metal anodes is crucial for achieving long-lasting cycling stability and facilitating the practical implementations of aqueous Zn-metal batteries.To address these challenges,we report in this study a functional nitro-cellulose interfacial layer(NCIL)on the surface of Zn anodes enlightened by a nitro-coordination chemistry strategy.The NCIL exhibits strong zincophilicity and superior coordination capability with Zn^(2+)due to the highly electronegative and highly nucleophilic nature of the nitro functional group.This characteristic facilitates a rapid Zn-ion desolvation process and homogeneous Zn plating,effectively preventing H_(2) evolution and dendrite formation.Additionally,the negatively charged surface of NCIL acts as a shield,repelling SO_(4)^(2-)anions and inhibiting corrosive reactions on the Zn surface.Remarkably,reversible and stable Zn plating/stripping is achieved for over 5100 h at a current density of 1 mA cm^(-2),which is nearly 30 times longer than that of bare Zn anodes.Furthermore,the Zn/V_(2)O_(5) full cells with the functional interface layer deliver a high-capacity retention of 80.3%for over 10,000 cycles at 5 A g^(-1).This research offers valuable insights for the rational development of advanced protective interface layers in order to achieve ultra-long-lifeZnmetal batteries.展开更多
The electrochemical carbon dioxide reduction reaction(eCO_(2)RR),which converts CO_(2)into various hydrocarbons or alcohols,has been extensively researched because it promises a sustainable energy economy.However,only...The electrochemical carbon dioxide reduction reaction(eCO_(2)RR),which converts CO_(2)into various hydrocarbons or alcohols,has been extensively researched because it promises a sustainable energy economy.However,only copper(Cu)can currently achieve stable and efficient hydrocarbon conversion in the eCO_(2)RR.Therefore,understanding the catalytic mechanisms and summarizing the research progress on synthesis strategies of Cu catalysts are essential for the eCO_(2)RR.This paper reviews Cu catalysts with different surface states of Cu catalysts:oxide-derived Cu,Cu nanoparticles,Cu single atoms,and Cu nanoclusters.It then reviews the development and progress of different Cu-catalyst preparation methods in recent years,focusing on the activity and selectivity of materials.Besides revealing the tendencies of catalytic selection and deep reactive mechanisms of Cu catalysts with four different surface states,this review can guide the subsequent construction of catalysts and provides an understanding of catalytic mechanisms.展开更多
Electrocatalytic CO_(2) reduction reaction (eCO_(2)RR) presents a promising approach for harnessing renewable energy and converting greenhouse gas (CO_(2)) into high value-added CO products.N-doped single atom (SA) an...Electrocatalytic CO_(2) reduction reaction (eCO_(2)RR) presents a promising approach for harnessing renewable energy and converting greenhouse gas (CO_(2)) into high value-added CO products.N-doped single atom (SA) and atomic-level metal nanocluster (MN) tandem catalysts with rich defects for eCO_(2)RR are reported,which achieved a maximum CO Faraday efficiency (FE_(CO)) of 97.7%(-0.7 V vs.RHE) in the H-type cell and maintained over 95% FE_(CO)at potentials from -0.18 to -0.73 V vs.RHE in the flow cell.Furthermore,the catalyst in the flow cell demonstrated a remarkably low onset potential of-0.14 V vs.RHE and the current density was approximately three times that of the H-type cell.Interestingly,XPS analysis indicates that carbon substrates containing defects have more pyridine-N content.DFT calculations and in-situ attenuated total reflection Fourier transform infrared support this finding by showing that the Ni-(N-C_(2))_(3) active sites with defect favors preferentially convert CO_(2)-to-CO.展开更多
Atypical polypoid adenomyoma(APA)is an uncommon type of polypoid characterized by fibroid stroma and endometrial glands.It occurs mostly in premenopausal women and rarely in postmenopausal women with irregular vaginal...Atypical polypoid adenomyoma(APA)is an uncommon type of polypoid characterized by fibroid stroma and endometrial glands.It occurs mostly in premenopausal women and rarely in postmenopausal women with irregular vaginal bleeding.In our current case,a 76-year-old woman presented with irregular vaginal bleeding.The final pathological diagnosis of the mass was APA.APA is not easy to diagnose before surgery.On the one hand,there was no obvious particularity in imaging features and clinical features,especially for uncomfortably identifying endometrial cancer.On the other hand,APA has a pedicle,attaching to any part of the uterine cavity,which can cause pseudocoel between the mass with the uterine cavity wall.So,when it comes to getting the pathological tissue in the absence of hysteroscopy,it is easy to access to the pseudocoel and obtain endometrial tissue rather than the pathological tissue of the mass.Therefore,preoperative imaging examination is of great significance diagnosis way of thinking to clinicians for APA.In the meantime,pathological tissue of APA can be obtained by hysteroscopy in visual conditions.展开更多
Over the last decade,remarkable progress has been made in metal halide perovskite solar cells(PSCs),which have been a focus of emerging photovoltaic techniques and show great potential for commercialization.However,th...Over the last decade,remarkable progress has been made in metal halide perovskite solar cells(PSCs),which have been a focus of emerging photovoltaic techniques and show great potential for commercialization.However,the upscaling of small-area PSCs to large-area solar modules to meet the demands of practical applications remains a significant challenge.The scalable production of high-quality perovskite films by a simple,reproducible process is crucial for resolving this issue.Furthermore,the crystallization behavior in the solution-processed fabrication of perovskite films can be strongly influenced by the physicochemical properties of the precursor inks,which are significantly affected by the employed solvents and their interactions with the solutes.Thus,a comprehensive understanding of solvent engineering for fabricating perovskite films over large areas is urgently required.In this paper,we first analyze the role of solvents in the solution-processed fabrication of large-area perovskite films based on the classical crystal nucleation and growth mechanism.Recent efforts in solvent engineering to improve the quality of perovskite films for solar modules are discussed.Finally,the basic principles and future challenges of solvent system design for scalable fabrication of high-quality perovskite films for efficient solar modules are proposed.展开更多
Efficient bifunctional oxygen electrocatalysts for ORR and OER are fundamental to the development of high performance metal-air batteries.Herein,a facile cost-efficient two-step pyrolysis strategy for the fabrication ...Efficient bifunctional oxygen electrocatalysts for ORR and OER are fundamental to the development of high performance metal-air batteries.Herein,a facile cost-efficient two-step pyrolysis strategy for the fabrication of a bifunctional oxygen electrocatalyst has been proposed.The efficient non-preciousmetal-based electrocatalyst,Fe/Fe_(3)C@Fe-N_(x)-C consists of highly curved onion-like carbon shells that encapsulate Fe/Fe_(3)C nanoparticles,distributed on an extensively porous graphitic carbon aerogel.The obtained Fe/Fe_(3)C@Fe-N_(x)-C aerogel exhibited superb electrochemical activity,excellent durability,and high methanol tolerance.The experimental results indicated that the assembly of onion-like carbon shells with encapsulated Fe/Fe_(3)C yielded highly curved carbon surfaces with abundant Fe-Nxactive sites,a porous structure,and enhanced electrocatalytic activity towards ORR and OER,hence displaying promising potential for application as an air cathode in rechargeable Zn-air batteries.The constructed Zn-air battery possessed an exceptional peak power density of~147 mW cm^(-2),outstanding cycling stability(200 cycles,1 h per cycle),and a small voltage gap of 0.87 V.This study offers valuable insights regarding the construction of low-cost and highly active bifunctional oxygen electrocatalysts for efficient air batteries.展开更多
Non-noble-metal-based electrocatalysts with superior oxygen reduction reaction(ORR)activity to platinum(Pt)are highly desirable but their fabrications are challenging and thus impeding their applications in metal-air ...Non-noble-metal-based electrocatalysts with superior oxygen reduction reaction(ORR)activity to platinum(Pt)are highly desirable but their fabrications are challenging and thus impeding their applications in metal-air batteries and fuel cells.Here,we report a facile molten salt assisted two-step pyrolysis strategy to construct carbon nanosheets matrix with uniformly dispersed Fe_(3) N/Fe nanoparticles and abundant nitrogen-coordinated Fe single atom moieties(Fe@Fe_(SA)-N-C).Thermal exfoliation and etching effect of molten salt contribute to the formation of carbon nanosheets with high porosity,large surface area and abundant uniformly immobilized active sites.Aberration-corrected high-angle annular dark-field scanning transmission electron microscopy(HAADF-STEM)image,X-ray absorption fine spectroscopy,and X-ray photoelectron spectroscopy indicate the generation of Fe(mainly Fe_(3) N/Fe)and Fe_(SA)-N-C moieties,which account for the catalytic activity for ORR.Further study on modulating the crystal structure and composition of Fe_(3) N/Fe nanoparticles reveals that proper chemical environment of Fe in Fe_(3) N/Fe notably optimizes the ORR activity.Consequently,the presence of abundant Fe_(SA)-N-C moieties,and potential synergies of Fe_(3) N/Fe nanoparticles and carbon shells,markedly promote the reaction kinetics.The as-developed Fe@Fe_(SA)-N-C-900 electrocatalyst displays superior ORR performance with a half-wave potential(E_(1/2))of 0.83 V versus reversible hydrogen electrode(RHE)and a diffusion limited current density of 5.6 mA cm^(-2).In addition,a rechargeable Zn-air battery device assembled by the Fe@Fe_(SA)-N-C-900 possesses remarkably stable performance with a small voltage gap without obvious voltage loss after500 h of operation.The facile synthesis strategy for the high-performance composites represents another viable avenue to stable and low-cost electrocatalysts for ORR catalysis.展开更多
In a pulsed vacuum discharge,the ejection performance of a metal plasma jet can be effectively improved by preventing charged particles from moving to the anode.In this paper,the effects of resistance and capacitance ...In a pulsed vacuum discharge,the ejection performance of a metal plasma jet can be effectively improved by preventing charged particles from moving to the anode.In this paper,the effects of resistance and capacitance on the anode side on the discharge characteristics and the generation characteristics of plasma jet are investigated.Results show that the existence of a resistor on the anode side can increase the anode potential,thereby preventing charged particles from entering the anode and promoting the ejection of charged particles along the axis of the insulating sleeve nozzle.The application of a capacitor on the anode side can not only absorb electrons at the initial stage of discharge,increasing the peak value of the cathode hump potential,but also prevent charged particles from moving to the anode,thereby improving the ejection performance of the plasma jet.In addition,the use of a larger resistance and a smaller capacitance can improve the blocking effect on charged particles and further improve the ejection performance of the plasma jet.Results of this study will provide a reference for the improvement of the ejection performance of plasma jets and their applications.展开更多
Silicon suboxide(SiO_(x),0<x<2)is an appealing anode material to replace traditional graphite owing to its much higher theoretical specific capacity enabling higher-energy-density lithium batteries.Nevertheless,...Silicon suboxide(SiO_(x),0<x<2)is an appealing anode material to replace traditional graphite owing to its much higher theoretical specific capacity enabling higher-energy-density lithium batteries.Nevertheless,the huge volume change and rapid capacity decay of SiO_(x)electrodes during cycling pose huge challenges to their large-scale practical applications.To eliminate this bottleneck,a dragonfly wing microstructure-inspired polymer electrolyte(denoted as PPM-PE)is developed based on in-situ polymerization of bicyclic phosphate ester-and urethane motif-containing monomer and methyl methacrylate in traditional liquid electrolyte.PPM-PE delivers excellent mechanical properties,highly correlated with the formation of a micro-phase separation structure similar with dragonfly wings.By virtue of superior mechanical properties and the in-situ solidified preparation method,PPM-PE can form a 3D polymer network buffer against stress within the electrode particles gap,enabling much suppressed electrode volume expansion and more stabilized solid electrolyte interface along with evidently decreased electrolyte decomposition.Resultantly,PPM-PE shows significant improvements in both cycling and rate performance in button and soft package batteries with SiO_(x)-based electrodes,compared with the liquid electrolyte counterpart.Such a dragonfly wing microstructure-inspired design philosophy of in-situ solidified polymer electrolytes helps facilitate the practical implementation of high-energy lithium batteries with SiO_(x)-based anodes.展开更多
基金financially supported by the General Research Fund(CityU 11315622 and CityU 11310123)National Natural Science Foundation(NSFC 52372229 and NSFC 52172241)+3 种基金Green Tech Fund(GTF202220105)Guangdong Basic and Applied Basic Research Foundation(2024A1515011008)City University of Hong Kong(No.9020002)the Shenzhen Research Institute of City University of Hong Kong.
文摘The development of flexible zinc-ion batteries(ZIBs)faces a threeway trade-off among the ionic conductivity,Zn^(2+)mobility,and the electrochemical stability of hydrogel electrolytes.To address this challenge,we designed a cationic hydrogel named PAPTMA to holistically improve the reversibility of ZIBs.The long cationic branch chains in the polymeric matrix construct express pathways for rapid Zn^(2+)transport through an ionic repulsion mechanism,achieving simultaneously high Zn^(2+)transference number(0.79)and high ionic conductivity(28.7 mS cm−1).Additionally,the reactivity of water in the PAPTMA hydrogels is significantly inhibited,thus possessing a strong resistance to parasitic reactions.Mechanical characterization further reveals the superior tensile and adhesion strength of PAPTMA.Leveraging these properties,symmetric batteries employing PAPTMA hydrogel deliver exceeding 6000 h of reversible cycling at 1 mA cm^(−2) and maintain stable operation for 1000 h with a discharge of depth of 71%.When applied in 4×4 cm2 pouch cells with MnO_(2) as the cathode material,the device demonstrates remarkable operational stability and mechanical robustness through 150 cycles.This work presents an eclectic strategy for designing advanced hydrogels that combine high ionic conductivity,enhanced Zn^(2+)mobility,and strong resistance to parasitic reactions,paving the way for long-lasting flexible ZIBs.
基金financially supported by the National Natural Science Foundation of China(52162036 and 22378342)Key Project of Nature Science Foundation of Xinjiang(2021D01D08)+2 种基金Major Projects of Xinjiang(2022A01005-4 and 2021A01001-1)Key Research and Development Project of Xinjiang(2023B01025-1)the support from the Doctoral Student Special Program of the Young Talents Support Project of the China Association for Science and Technology in 2024。
文摘Practical Zn metal batteries have been hindered by several challenges,including Zn dendrite growth,undesirable side reactions,and unstable electrode/electrolyte interface.These issues are particularly more serious in low-concentration electrolytes.Herein,we design a Zn salt-mediated electrolyte with in situ ring-opening polymerization of the small molecule organic solvent.The Zn(TFSI)_(2)salt catalyzes the ring-opening polymerization of(1,3-dioxolane(DOL)),generating oxidation-resistant and non-combustible long-chain polymer(poly(1,3-dioxolane)(pDOL)).The pDOL reduces the active H_(2)O molecules in electrolyte and assists in forming stable organic–inorganic gradient solid electrolyte interphase with rich organic constituents,ZnO and ZnF_(2).The introduction of pDOL endows the electrolyte with several advantages:excellent Zn dendrite inhibition,improved corrosion resistance,widened electrochemical window(2.6 V),and enhanced low-temperature performance(freezing point=-34.9°C).Zn plating/stripping in pDOL-enhanced electrolyte lasts for 4200 cycles at 99.02%Coulomb efficiency and maintains a lifetime of 8200 h.Moreover,Zn metal anodes deliver stable cycling for 2500 h with a high Zn utilization of 60%.A Zn//VO_(2)pouch cell assembled with lean electrolyte(electrolyte/capacity(E/C=41 mL(Ah)^(-1))also demonstrates a capacity retention ratio of 92%after 600 cycles.These results highlight the promising application prospects of practical Zn metal batteries enabled by the Zn(TFSI)2-mediated electrolyte engineering.
基金supported by the National Nature Science Foundation of China(22209211 and 52172241)Hong Kong Research Grants Council(CityU 11315622)+1 种基金the research funds from South-Central Minzu University(YZZ22001)the National Key R&D Program of China(2021YFA1501101).
文摘With the merits of the high energy density of batteries and power density of supercapacitors,the aqueous Zn-ion hybrid supercapacitors emerge as a promising candidate for applications where both rapid energy delivery and moderate energy storage are required.However,the narrow electrochemical window of aqueous electrolytes induces severe side reactions on the Zn metal anode and shortens its lifespan.It also limits the operation voltage and energy density of the Zn-ion hybrid supercapacitors.Using'water in salt'electrolytes can effectively broaden their electrochemical windows,but this is at the expense of high cost,low ionic conductivity,and narrow temperature compatibility,compromising the electrochemical performance of the Zn-ion hybrid supercapacitors.Thus,designing a new electrolyte to balance these factors towards high-performance Zn-ion hybrid supercapacitors is urgent and necessary.We developed a dilute water/acetonitrile electrolyte(0.5 m Zn(CF_(3)SO_(3))_(2)+1 m LiTFSI-H_(2)O/AN)for Zn-ion hybrid supercapacitors,which simultaneously exhibited expanded electrochemical window,decent ionic conductivity,and broad temperature compatibility.In this electrolyte,the hydration shells and hydrogen bonds are significantly modulated by the acetonitrile and TFSI-anions.As a result,a Zn-ion hybrid supercapacitor with such an electrolyte demonstrates a high operating voltage up to 2.2 V and long lifespan beyond 120,000 cycles.
基金the financial support from Shanxi Province Science and Technology Department(20201101012,202101060301016)the support from the APRC Grant of the City University of Hong Kong(9380086)+5 种基金the TCFS Grant(GHP/018/20SZ)MRP Grant(MRP/040/21X)from the Innovation and Technology Commission of Hong Kongthe Green Tech Fund(202020164)from the Environment and Ecology Bureau of Hong Kongthe GRF grants(11307621,11316422)from the Research Grants Council of Hong KongGuangdong Major Project of Basic and Applied Basic Research(2019B030302007)Guangdong-Hong Kong-Macao Joint Laboratory of Optoelectronic and Magnetic Functional Materials(2019B121205002).
文摘A considerable efficiency gap exists between large-area perovskite solar modules and small-area perovskite solar cells.The control of forming uniform and large-area film and perovskite crystallization is still the main obstacle restricting the efficiency of PSMs.In this work,we adopted a solid-liquid two-step film formation technique,which involved the evaporation of a lead iodide film and blade coating of an organic ammonium halide solution to prepare perovskite films.This method possesses the advantages of integrating vapor deposition and solution methods,which could apply to substrates with different roughness and avoid using toxic solvents to achieve a more uniform,large-area perovskite film.Furthermore,modification of the NiO_(x)/perovskite buried interface and introduction of Urea additives were utilized to reduce interface recombination and regulate perovskite crystallization.As a result,a large-area perovskite film possessing larger grains,fewer pinholes,and reduced defects could be achieved.The inverted PSM with an active area of 61.56 cm^(2)(10×10 cm^(2)substrate)achieved a champion power conversion efficiency of 20.56%and significantly improved stability.This method suggests an innovative approach to resolving the uniformity issue associated with large-area film fabrication.
基金supported by the National Natural Science Foundation of China (No. 22005216 and 52172241)the General Research Fund of Hong Kong (No. CityU 11308321)Tianjin Research Innovation Project for Postgraduate Students (No.2022BKY130)
文摘Suppression of uncontrollable dendrite growth and water-induced side reactions of Zn metal anodes is crucial for achieving long-lasting cycling stability and facilitating the practical implementations of aqueous Zn-metal batteries.To address these challenges,we report in this study a functional nitro-cellulose interfacial layer(NCIL)on the surface of Zn anodes enlightened by a nitro-coordination chemistry strategy.The NCIL exhibits strong zincophilicity and superior coordination capability with Zn^(2+)due to the highly electronegative and highly nucleophilic nature of the nitro functional group.This characteristic facilitates a rapid Zn-ion desolvation process and homogeneous Zn plating,effectively preventing H_(2) evolution and dendrite formation.Additionally,the negatively charged surface of NCIL acts as a shield,repelling SO_(4)^(2-)anions and inhibiting corrosive reactions on the Zn surface.Remarkably,reversible and stable Zn plating/stripping is achieved for over 5100 h at a current density of 1 mA cm^(-2),which is nearly 30 times longer than that of bare Zn anodes.Furthermore,the Zn/V_(2)O_(5) full cells with the functional interface layer deliver a high-capacity retention of 80.3%for over 10,000 cycles at 5 A g^(-1).This research offers valuable insights for the rational development of advanced protective interface layers in order to achieve ultra-long-lifeZnmetal batteries.
基金supported by the Tianjin Science and Technology support key projects (20JCYBJC01420)。
文摘The electrochemical carbon dioxide reduction reaction(eCO_(2)RR),which converts CO_(2)into various hydrocarbons or alcohols,has been extensively researched because it promises a sustainable energy economy.However,only copper(Cu)can currently achieve stable and efficient hydrocarbon conversion in the eCO_(2)RR.Therefore,understanding the catalytic mechanisms and summarizing the research progress on synthesis strategies of Cu catalysts are essential for the eCO_(2)RR.This paper reviews Cu catalysts with different surface states of Cu catalysts:oxide-derived Cu,Cu nanoparticles,Cu single atoms,and Cu nanoclusters.It then reviews the development and progress of different Cu-catalyst preparation methods in recent years,focusing on the activity and selectivity of materials.Besides revealing the tendencies of catalytic selection and deep reactive mechanisms of Cu catalysts with four different surface states,this review can guide the subsequent construction of catalysts and provides an understanding of catalytic mechanisms.
基金supported by the Tianjin Science and Technology support key projects (20JCYBJC01420)。
文摘Electrocatalytic CO_(2) reduction reaction (eCO_(2)RR) presents a promising approach for harnessing renewable energy and converting greenhouse gas (CO_(2)) into high value-added CO products.N-doped single atom (SA) and atomic-level metal nanocluster (MN) tandem catalysts with rich defects for eCO_(2)RR are reported,which achieved a maximum CO Faraday efficiency (FE_(CO)) of 97.7%(-0.7 V vs.RHE) in the H-type cell and maintained over 95% FE_(CO)at potentials from -0.18 to -0.73 V vs.RHE in the flow cell.Furthermore,the catalyst in the flow cell demonstrated a remarkably low onset potential of-0.14 V vs.RHE and the current density was approximately three times that of the H-type cell.Interestingly,XPS analysis indicates that carbon substrates containing defects have more pyridine-N content.DFT calculations and in-situ attenuated total reflection Fourier transform infrared support this finding by showing that the Ni-(N-C_(2))_(3) active sites with defect favors preferentially convert CO_(2)-to-CO.
文摘Atypical polypoid adenomyoma(APA)is an uncommon type of polypoid characterized by fibroid stroma and endometrial glands.It occurs mostly in premenopausal women and rarely in postmenopausal women with irregular vaginal bleeding.In our current case,a 76-year-old woman presented with irregular vaginal bleeding.The final pathological diagnosis of the mass was APA.APA is not easy to diagnose before surgery.On the one hand,there was no obvious particularity in imaging features and clinical features,especially for uncomfortably identifying endometrial cancer.On the other hand,APA has a pedicle,attaching to any part of the uterine cavity,which can cause pseudocoel between the mass with the uterine cavity wall.So,when it comes to getting the pathological tissue in the absence of hysteroscopy,it is easy to access to the pseudocoel and obtain endometrial tissue rather than the pathological tissue of the mass.Therefore,preoperative imaging examination is of great significance diagnosis way of thinking to clinicians for APA.In the meantime,pathological tissue of APA can be obtained by hysteroscopy in visual conditions.
基金financially supported by the National Key Research and Development Project funding from the Ministry of Science and Technology of China(2021YFB3800104)the National Natural Science Foundation of China(51822203,52002140,U20A20252,51861145404,62105293,62205187)+4 种基金the Young Elite Scientists Sponsorship Program by CAST,the Self-determined and Innovative Research Funds of HUST(2020KFYXJJS008)the Natural Science Foundation of Hubei Province(ZRJQ2022000408)the Shenzhen Science and Technology Innovation Committee(JCYJ20180507182257563)Fundamental Research Program of Shanxi Province(202103021223032)the Innovation Project of Optics Valley Laboratory of China(OVL2021BG008)。
文摘Over the last decade,remarkable progress has been made in metal halide perovskite solar cells(PSCs),which have been a focus of emerging photovoltaic techniques and show great potential for commercialization.However,the upscaling of small-area PSCs to large-area solar modules to meet the demands of practical applications remains a significant challenge.The scalable production of high-quality perovskite films by a simple,reproducible process is crucial for resolving this issue.Furthermore,the crystallization behavior in the solution-processed fabrication of perovskite films can be strongly influenced by the physicochemical properties of the precursor inks,which are significantly affected by the employed solvents and their interactions with the solutes.Thus,a comprehensive understanding of solvent engineering for fabricating perovskite films over large areas is urgently required.In this paper,we first analyze the role of solvents in the solution-processed fabrication of large-area perovskite films based on the classical crystal nucleation and growth mechanism.Recent efforts in solvent engineering to improve the quality of perovskite films for solar modules are discussed.Finally,the basic principles and future challenges of solvent system design for scalable fabrication of high-quality perovskite films for efficient solar modules are proposed.
基金supported financially by the National Natural Science Foundation of China,China(Grant No.51702180,51572136,91963113,21703116,51372127,51873096)The Scientific and Technical Development Project of Qingdao,China(Grant No.18-2-2-52-jch)+1 种基金The Taishan Scholar Advantage and Characteristic Discipline Team of Eco Chemical Process and TechnologyThe Natural Science Foundation of Hebei Province(B2019204009)。
文摘Efficient bifunctional oxygen electrocatalysts for ORR and OER are fundamental to the development of high performance metal-air batteries.Herein,a facile cost-efficient two-step pyrolysis strategy for the fabrication of a bifunctional oxygen electrocatalyst has been proposed.The efficient non-preciousmetal-based electrocatalyst,Fe/Fe_(3)C@Fe-N_(x)-C consists of highly curved onion-like carbon shells that encapsulate Fe/Fe_(3)C nanoparticles,distributed on an extensively porous graphitic carbon aerogel.The obtained Fe/Fe_(3)C@Fe-N_(x)-C aerogel exhibited superb electrochemical activity,excellent durability,and high methanol tolerance.The experimental results indicated that the assembly of onion-like carbon shells with encapsulated Fe/Fe_(3)C yielded highly curved carbon surfaces with abundant Fe-Nxactive sites,a porous structure,and enhanced electrocatalytic activity towards ORR and OER,hence displaying promising potential for application as an air cathode in rechargeable Zn-air batteries.The constructed Zn-air battery possessed an exceptional peak power density of~147 mW cm^(-2),outstanding cycling stability(200 cycles,1 h per cycle),and a small voltage gap of 0.87 V.This study offers valuable insights regarding the construction of low-cost and highly active bifunctional oxygen electrocatalysts for efficient air batteries.
基金supported financially by the National Natural Science Foundation of China,China(Grant No.51702180,51772162)the Taishan Scholar Advantage and Characteristic Discipline Team of Eco Chemical Process and Technologythe Scientific and Technical Development Project of Qingdao,China(Grant No.18-2-2-52-jch)。
文摘Non-noble-metal-based electrocatalysts with superior oxygen reduction reaction(ORR)activity to platinum(Pt)are highly desirable but their fabrications are challenging and thus impeding their applications in metal-air batteries and fuel cells.Here,we report a facile molten salt assisted two-step pyrolysis strategy to construct carbon nanosheets matrix with uniformly dispersed Fe_(3) N/Fe nanoparticles and abundant nitrogen-coordinated Fe single atom moieties(Fe@Fe_(SA)-N-C).Thermal exfoliation and etching effect of molten salt contribute to the formation of carbon nanosheets with high porosity,large surface area and abundant uniformly immobilized active sites.Aberration-corrected high-angle annular dark-field scanning transmission electron microscopy(HAADF-STEM)image,X-ray absorption fine spectroscopy,and X-ray photoelectron spectroscopy indicate the generation of Fe(mainly Fe_(3) N/Fe)and Fe_(SA)-N-C moieties,which account for the catalytic activity for ORR.Further study on modulating the crystal structure and composition of Fe_(3) N/Fe nanoparticles reveals that proper chemical environment of Fe in Fe_(3) N/Fe notably optimizes the ORR activity.Consequently,the presence of abundant Fe_(SA)-N-C moieties,and potential synergies of Fe_(3) N/Fe nanoparticles and carbon shells,markedly promote the reaction kinetics.The as-developed Fe@Fe_(SA)-N-C-900 electrocatalyst displays superior ORR performance with a half-wave potential(E_(1/2))of 0.83 V versus reversible hydrogen electrode(RHE)and a diffusion limited current density of 5.6 mA cm^(-2).In addition,a rechargeable Zn-air battery device assembled by the Fe@Fe_(SA)-N-C-900 possesses remarkably stable performance with a small voltage gap without obvious voltage loss after500 h of operation.The facile synthesis strategy for the high-performance composites represents another viable avenue to stable and low-cost electrocatalysts for ORR catalysis.
基金supported by the Fundamental Research Funds for the Central Universities(No.2019YJS187)National Natural Science Foundation of China(No.51577011)。
文摘In a pulsed vacuum discharge,the ejection performance of a metal plasma jet can be effectively improved by preventing charged particles from moving to the anode.In this paper,the effects of resistance and capacitance on the anode side on the discharge characteristics and the generation characteristics of plasma jet are investigated.Results show that the existence of a resistor on the anode side can increase the anode potential,thereby preventing charged particles from entering the anode and promoting the ejection of charged particles along the axis of the insulating sleeve nozzle.The application of a capacitor on the anode side can not only absorb electrons at the initial stage of discharge,increasing the peak value of the cathode hump potential,but also prevent charged particles from moving to the anode,thereby improving the ejection performance of the plasma jet.In addition,the use of a larger resistance and a smaller capacitance can improve the blocking effect on charged particles and further improve the ejection performance of the plasma jet.Results of this study will provide a reference for the improvement of the ejection performance of plasma jets and their applications.
基金financially supported by the National Key R&D Program of China(2023YFC2812700)the Key Scientific and Technological Innovation Project of Shandong(2022CXGC020301)+6 种基金the National Natural Science Foundation of China(22279153,U22A2044,22479154,52303287)the Taishan Scholars of Shandong Province(No.ts201511063)the Shandong Energy Institute(Grant No.SEI I202108)the Postdoctoral Fellowship Program of CPSF(E31Z3F04)China Postdoctoral Science Foundation(2024 M753350)the Natural Science Foundation of Shandong Province(ZR2023QB208)Qingdao Natural Science Foundation(23-2-1-77-zyyd-jch)。
文摘Silicon suboxide(SiO_(x),0<x<2)is an appealing anode material to replace traditional graphite owing to its much higher theoretical specific capacity enabling higher-energy-density lithium batteries.Nevertheless,the huge volume change and rapid capacity decay of SiO_(x)electrodes during cycling pose huge challenges to their large-scale practical applications.To eliminate this bottleneck,a dragonfly wing microstructure-inspired polymer electrolyte(denoted as PPM-PE)is developed based on in-situ polymerization of bicyclic phosphate ester-and urethane motif-containing monomer and methyl methacrylate in traditional liquid electrolyte.PPM-PE delivers excellent mechanical properties,highly correlated with the formation of a micro-phase separation structure similar with dragonfly wings.By virtue of superior mechanical properties and the in-situ solidified preparation method,PPM-PE can form a 3D polymer network buffer against stress within the electrode particles gap,enabling much suppressed electrode volume expansion and more stabilized solid electrolyte interface along with evidently decreased electrolyte decomposition.Resultantly,PPM-PE shows significant improvements in both cycling and rate performance in button and soft package batteries with SiO_(x)-based electrodes,compared with the liquid electrolyte counterpart.Such a dragonfly wing microstructure-inspired design philosophy of in-situ solidified polymer electrolytes helps facilitate the practical implementation of high-energy lithium batteries with SiO_(x)-based anodes.
