Organic–inorganic single-crystalline perovskites have attracted significant attentions due to their exceptional progress in intrinsic properties＇ investigation and applications in photovoltaics and optoelectronics. ...Organic–inorganic single-crystalline perovskites have attracted significant attentions due to their exceptional progress in intrinsic properties＇ investigation and applications in photovoltaics and optoelectronics. In this study, the large perovskite CH3NH3PbI3 single crystal with the largest length of 80 mm was prepared through the method of inverse-temperature crystallization. Meanwhile, the mass production of integrate photodetectors have been fabricated on the single-crystalline wafer and the photoresponse performances were investigated. The results show that the single-crystalline photodetectors have broad spectrum response to 900 nm, rapid response speed（〈40 μs） and excellent stability. These findings are of great importance for future promising perovskite single crystalline for integrated photoelectronic application.展开更多
Developing single-crystalline Ni-rich cathodes is an effective strategy to improve the safety and cycle life of Li-ion batteries(LIBs).However,the easy-to-loss of Li and O in high-temperature lithiation results in uns...Developing single-crystalline Ni-rich cathodes is an effective strategy to improve the safety and cycle life of Li-ion batteries(LIBs).However,the easy-to-loss of Li and O in high-temperature lithiation results in unsatisfactory ordered layered structure and stoichiometry.Herein,we demonstrate the synthesis of highly-ordered and fully-stoichiometric single-crystalline LiNi_(0.83)Co_(0.12)Mn_(0.05)O_(2)(SC-NCM83)cathodes by the regulation of pre-lithiation kinetics.The well-balanced pre-lithiation kinetics have been proved to greatly improve the proportion of layered phase in the intermediate by inhibiting the formation of metastable spinel phase,which promoted the rapid transformation of the intermediate into highly-ordered layered SC-NCM83 in the subsequent lithiation process.After coating a layer of Li_(2)O–B_(2)O_(3),the resultant cathodes deliver superior cycling stability with 90.9%capacity retention at 1C after 300 cycles in pouch-type full batteries.The enhancement mechanism has also been clarified.These findings exhibit fundamental insights into the pre-lithiation kinetics process for guiding the synthesis of high-quality singlecrystalline Ni-rich cathodes.展开更多
Single-crystalline hierarchical ZSM-5 zeolites with different particle sizes(namely 100,140,and 200 nm)were successfully prepared by adjusting the amount of tetrapropylammonium hydroxide(TPAOH),and investigated in n-h...Single-crystalline hierarchical ZSM-5 zeolites with different particle sizes(namely 100,140,and 200 nm)were successfully prepared by adjusting the amount of tetrapropylammonium hydroxide(TPAOH),and investigated in n-heptane catalytic cracking reaction.Diffusional measurements by zero-length column(ZLC)method showed that the apparent diffusivities of n-heptane decreased with the reduction of particle size,indicating the existence of surface barriers.Moreover,with the decrease of particle size,the additional diffusion path length increased,which meant the influence of surface barriers became more apparent.Despite the change of surface barriers,the intracrystalline diffusion still dominated the overall diffusion.Catalytic performance showed that the zeolite with smaller particle size had better stability.展开更多
Higher nickel content endows Ni-rich cathode materials LiNi_(x)Co_yMn_(1-x-y)O_(2)(x>0.6)with higher specific capacity and high energy density,which is regarded as the most promising cathode materials for Li-ion ba...Higher nickel content endows Ni-rich cathode materials LiNi_(x)Co_yMn_(1-x-y)O_(2)(x>0.6)with higher specific capacity and high energy density,which is regarded as the most promising cathode materials for Li-ion batteries.However,the deterioration of structural stability hinders its practical application,especially under harsh working conditions such as high-temperature cycling.Given these circumstances,it becomes particularly critical to clarify the impact of the crystal morphology on the structure and high-temperature performance as for the ultrahigh-nickel cathodes.Herein,we conducted a comprehensive comparison in terms of microstructure,high-temperature long-cycle phase evolution,and high-temperature electrochemical stability,revealing the differences and the working mechanisms among polycrystalline(PC),single-crystalline(SC)and Al doped SC ultrahigh-nickel materials.The results show that the PC sample suffers a severe irreversible phase transition along with the appearance of microcracks,resulting a serious decay of both average voltage and the energy density.While the Al doped SC sample exhibits superior cycling stability with intact layered structure.In-situ XRD and intraparticle structural evolution characterization reveal that Al doping can significantly alleviate the irreversible phase transition,thus inhibiting microcracks generation and enabling enhanced structure.Specifically,it exhibits excellent cycling performance in pouch-type full-cell with a high capacity retention of 91.8%after 500 cycles at 55℃.This work promotes the fundamental understanding on the correlation between the crystalline morphology and high-temperature electrochemical stability and provides a guide for optimization the Ni-rich cathode materials.展开更多
The rapid growth in global electric vehicles(EVs)sales has promoted the development of Co-free,Ni-rich layered cathodes for state-of-the-art high energy-density,inexpensive lithium-ion batteries(LIBs).However,progress...The rapid growth in global electric vehicles(EVs)sales has promoted the development of Co-free,Ni-rich layered cathodes for state-of-the-art high energy-density,inexpensive lithium-ion batteries(LIBs).However,progress in their commercial use has been seriously hampered by exasperating performance deterioration and safety concerns.Herein,a robust single-crystalline,Co-free,Ni-rich LiNi_(0.95)Mn_(0.05)O_(2)(SC-NM95)cathode is successfully designed using a molten salt-assisted method,and it exhibits better structural stability and cycling durability than those of polycrystalline LiNi_(0.95)Mn_(0.05)O_(2) (PC-NM95).Notably,the SC-NM95 cathode achieves a high discharge capacity of 218.2 mAh g^(-1),together with a high energy density of 837.3 Wh kg^(-1) at 0.1 C,mainly due to abundant Ni^(2+)/Ni^(3+) redox.It also presents an outstanding capacity retention(84.4%)after 200 cycles at 1 C,because its integrated single-crystalline structure effectively inhibits particle microcracking and surface phase transformation.In contrast,the PC-NM95 cathode suffers from rapid capacity fading owing to the nucleation and propagation of intergranular microcracking during cycling,facilitating aggravated parasitic reactions and rocksalt phase accumulation.This work provides a fundamental strategy for designing high-performance singlecrystalline,Co-free,Ni-rich cathode materials and also represents an important breakthrough in developing high-safe,low-cost,and high-energy LIBs.展开更多
A fundamental understanding of the electrochemical reaction process and mechanism of electrodes is very crucial for developing high-performance electrode materials.In this study,we report the sodium ion storage behavi...A fundamental understanding of the electrochemical reaction process and mechanism of electrodes is very crucial for developing high-performance electrode materials.In this study,we report the sodium ion storage behavior and mechanism of orthorhombic V_(2)O_(5) single-crystalline nanowires in the voltage window of 1.0–4.0 V(vs.Na/Na+).The single-crystalline nanowires exhibit a large irreversible capacity loss during the first discharge/charge cycle,and then show excellent cycling stability in the following cycles.At a current density of 100 mA g^(−1),the nanowires electrode delivers initial discharge/charge capacity of 217/88 mA h g^(−1),corresponding to a Coulombic efficiency of only 40.5%;after 100 cycles,the electrode remains a reversible discharge capacity of 78 mA h g^(−1) with a fading rate of only 0.09%per cycle compared with the 2nd cycle discharge capacity.The sodium ion storage mechanism was investigated,illustrating that the large irreversible capacity loss in the first cycle can be attributed to the initially formed single-crystalline α′-Nax V_(2)O_(5)(0.02<x<0.88),in which sodium ions cannot be electrochemically extracted and the α′-Na0.88 V_(2)O_(5) can reversibly host and release sodium ions via a single-phase(solid solution)reaction,leading to excellent cycling stability.The Na^(+) diffusion coefficient in α′-Nax V_(2)O_(5) ranges from 10^(−12) to 10^(−11.5) cm^(2) s^(−1) as evaluated by galvanostatic intermittent titration technique(GITT).展开更多
Electrocatalytic synthesis of value-added chemicals is attracting significant research attention owing to its mild reaction conditions, environmental benignity, and potentially scalable application to organic syntheti...Electrocatalytic synthesis of value-added chemicals is attracting significant research attention owing to its mild reaction conditions, environmental benignity, and potentially scalable application to organic synthetic chemistry. Herein, we report the preparation of a single-crystalline NiS2 nanostructure film of N 50 nm thickness grown directly on a carbon fiber doth （NiSJCFC） by a facile vapor-phase hydrothermal （VPH） method. NiSJCFC as an electrocatalyst exhibits activity for both the oxygen evolution reaction （OER） and the hydrogen evolution reaction （HER） in alkaline media. Furthermore, a series of alcohols （2-propanol, 2-butanol, 2-pentanol, and cyclohexanol） were electrocatalytically converted to the corresponding ketones with high selectivity, efficienc and durability using the NiSJCFC electrode in alkaline media. In the presence of 0.45 M alcohol, a remarkably decreased overpotential （- 150 mV, vs. RHE） at the NiS2/CFC anode compared with that for water oxidation to generate O2, i.e., the OER, in alkaline media leads to significantly improved H2 generation. For instance, the H2 generation rate in the presence of 0.45 M 2-propanol is almost 1.2-times of that obtained for pure water splitting, but in a system that employs an applied voltage at least 280 mV lower than that required for water splitting to achieve the same current density （20 mA-crn-2）. Thus, our results demonstrate the applicability of our bifunctional non-precious-metal electrocatalyst for organic synthesis and simultaneous H2 production.展开更多
The fast growth of large single-crystalline graphene by chemical vapor deposition on Cu foil remains a challenge for industrial-scale applications. To achieve the fast growth of large single-crystalline graphene, unde...The fast growth of large single-crystalline graphene by chemical vapor deposition on Cu foil remains a challenge for industrial-scale applications. To achieve the fast growth of large single-crystalline graphene, understanding the detailed dynamics governing the entire growth process--including nucleation, growth, and coalescence is important; however, these remain unexplored. In this study, by using a pulsed carbon isotope labeling technique in conjunction with micro-Raman spectroscopy identification, we visualized the growth dynamics, such as nucleation, growth, and coalescence, during the fast growth of large single- crystalline graphene domains. By tuning the supply of the carbon source, a growth rate of 320 μm/min and the growth of centimeter-sized graphene single crystals were achieved on Cu foil.展开更多
Various and critical electrocatalytic processes are involved during the redox reactions in the Li-S batteries,which extremely depend on the surface structure and chemical state.Recently,single-atom concept unlocks a r...Various and critical electrocatalytic processes are involved during the redox reactions in the Li-S batteries,which extremely depend on the surface structure and chemical state.Recently,single-atom concept unlocks a route to maximize the use of surface-active atoms,however,further increasing the density of active site is still strictly limited by the inherent structure that single-atoms are only highly-dispersed on substrate.Herein,we provide a viewpoint that an elaborate facet design with singlecrystalline structure engineering can harvest high-density surface active sites,which can significantly boost the electrocatalyst performance for excellent Li-S batteries.Specifically,the single-crystal CoSe_(2)(scCS)exhibits three-types of terminated(011)facet,efficiently obtaining the surface with a high-rich Co^(3+)–Se bond termination,in contrast with lots of surface grain boundaries and dangling bonds in polycrystalline CoSe_(2).Surprisingly,the surface active sites concentration can reach more than 69%.As anticipated,it can provide high-density and high-efficient active sites,enormously suppressing the shuttle effect and improving the reaction kinetics via accelerating the conversion and deposition of polysulfides and Li2S.This surface lattice strategy with element terminated mode is a promising approach for designing electrocatalyst effect-based energy system,not merely for Li-S batteries.展开更多
Mesoporous single crystals have unique potential in catalysis,but remain unexplored owing to the enormous synthetic challenge that they pose.Herein,we report a facile soft-template method to prepare palladium(Pd)and P...Mesoporous single crystals have unique potential in catalysis,but remain unexplored owing to the enormous synthetic challenge that they pose.Herein,we report a facile soft-template method to prepare palladium(Pd)and Pd alloy nanocubes with single-crystallinity and abundant mesoporosity.The successful formation of these exotic nanostructures essentially relies on the cointroduction of cetyltrimethylammonium chloride as the surfactant template and extra Cl^(−) ions as the facet-selective capping agent under well controlled experimental conditions.Thanks to their large surface areas and penetrating mesoporous channels,our products exhibit a great performance for electrochemical CO_(2) reduction.The best sample from alloying palladium with copper enables the efficient formate production with high selectivity(90∼100%)over a broad potential range,and great stability even under the working potential as cathodic as −0.5 V versus a reversible hydrogen electrode.These performance metrics are far superior to previous Pd-based materials,and underscore the structural advantages of our products.展开更多
Organic field-effect transistors(OFETs) based on organic micro-/nanocrystals have been widely reported with charge carrier mobility exceeding 1.0 cm^2V^(-1)s^(-1), demonstrating great potential for high-performance, l...Organic field-effect transistors(OFETs) based on organic micro-/nanocrystals have been widely reported with charge carrier mobility exceeding 1.0 cm^2V^(-1)s^(-1), demonstrating great potential for high-performance, low-cost organic electronic applications. However, fabrication of large-area organic micro-/nanocrystal arrays with consistent crystal growth direction has posed a significant technical challenge. Here, we describe a solution-processed dip-coating technique to grow large-area, aligned 9,10-bis(phenylethynyl) anthracene(BPEA) and 6,13-bis(triisopropylsilylethynyl) pentacene(TIPSPEN) single-crystalline nanoribbon arrays. The method is scalable to a 5 9 10 cm^2 wafer substrate, with around 60% of the wafer surface covered by aligned crystals. The quality of crystals can be easily controlled by tuning the dip-coating speed. Furthermore, OFETs based on well-aligned BPEA and TIPS-PEN single-crystalline nanoribbons were constructed.By optimizing channel lengths and using appropriate metallic electrodes, the BPEA and TIPS-PEN-based OFETs showed hole mobility exceeding 2.0 cm^2V^(-1)s^(-1)(average mobility 1.2 cm^2V^(-1)s^(-1)) and 3.0 cm^2V^(-1)s^(-1)(average mobility2.0 cm^2V^(-1)s^(-1)), respectively. They both have a high on/off ratio(I_(on)/I_(off))>10~9. The performance can well satisfy the requirements for light-emitting diodes driving.展开更多
We report on the successful fabrication of highly branched Cu S nanocrystals by laser-induced photochemical reaction.Surprisingly, the single-crystalline nature with preferential alignment of the（107） orientation ca...We report on the successful fabrication of highly branched Cu S nanocrystals by laser-induced photochemical reaction.Surprisingly, the single-crystalline nature with preferential alignment of the（107） orientation can be well improved during the moderate growth process. The branch length drastically increases from about 5 nm to 6 μm with an increase of photochemical reaction time（0-40 min）. The absorption spectra of as-prepared Cu S nanodendrites show that localized surface plasmon resonance（LSPR） peaks can be modulated from about 1037 nm to 1700 nm with an increase of branch length. Our results have a promising potential for photodynamic therapy and biological imaging application.展开更多
Rare-earth doped titania single-crystalline hollow nanoparticles of 20 nm are constructed via a simple sol-gel process. Amphiphilic ABA tri-block copolymers played a key role in assisting the formation of hollow struc...Rare-earth doped titania single-crystalline hollow nanoparticles of 20 nm are constructed via a simple sol-gel process. Amphiphilic ABA tri-block copolymers played a key role in assisting the formation of hollow structure, for which a hollow nanostructure growth mechanism is proposed. By introducing rare earth into the synthesis process, the as-prepared nanoparticles exhibit near-infrared light absorption properties. Photo-decomposition efficiency of Orange II azo dye can be successfully evaluated when using Yb3+-doped Ti O2 hollow nanoparticles as photocatalysts; it is more than two times higher than the pure Ti O2 hollow nanoparticles. The hollow nanostructured Yb3+-doped Ti O2 samples are exploited as photoanodes in N719- sensitized solar cells and prove able to improve the photoelectric conversion efficiency by measuring the solar cell parameters of dye-sensitized solar cells(DSSCs) under simulative sunlight.展开更多
基金support from the National Key Research and Development Program of China(no.2016YFA0202403)National Natural Science Foundation of China(nos.61604091/61674098)+3 种基金the 111 Project(B14041)the National University Research Fund(grant nos.GK261001009,GK201603107)Changjiang Scholar and Innovative Research Team(IRT_14R33)the Chinese National 1000-talent-plan program(1110010341)
文摘Organic–inorganic single-crystalline perovskites have attracted significant attentions due to their exceptional progress in intrinsic properties＇ investigation and applications in photovoltaics and optoelectronics. In this study, the large perovskite CH3NH3PbI3 single crystal with the largest length of 80 mm was prepared through the method of inverse-temperature crystallization. Meanwhile, the mass production of integrate photodetectors have been fabricated on the single-crystalline wafer and the photoresponse performances were investigated. The results show that the single-crystalline photodetectors have broad spectrum response to 900 nm, rapid response speed（〈40 μs） and excellent stability. These findings are of great importance for future promising perovskite single crystalline for integrated photoelectronic application.
基金supported by the National Natural Science Foundation of China(21975074,91834301)the Innovation Program of Shanghai Municipal Education Commissionthe Fundamental Research Funds for the Central Universities.
文摘Developing single-crystalline Ni-rich cathodes is an effective strategy to improve the safety and cycle life of Li-ion batteries(LIBs).However,the easy-to-loss of Li and O in high-temperature lithiation results in unsatisfactory ordered layered structure and stoichiometry.Herein,we demonstrate the synthesis of highly-ordered and fully-stoichiometric single-crystalline LiNi_(0.83)Co_(0.12)Mn_(0.05)O_(2)(SC-NCM83)cathodes by the regulation of pre-lithiation kinetics.The well-balanced pre-lithiation kinetics have been proved to greatly improve the proportion of layered phase in the intermediate by inhibiting the formation of metastable spinel phase,which promoted the rapid transformation of the intermediate into highly-ordered layered SC-NCM83 in the subsequent lithiation process.After coating a layer of Li_(2)O–B_(2)O_(3),the resultant cathodes deliver superior cycling stability with 90.9%capacity retention at 1C after 300 cycles in pouch-type full batteries.The enhancement mechanism has also been clarified.These findings exhibit fundamental insights into the pre-lithiation kinetics process for guiding the synthesis of high-quality singlecrystalline Ni-rich cathodes.
基金The support from the National Natural Science Foundation of China(22278353)is greatly appreciated。
文摘Single-crystalline hierarchical ZSM-5 zeolites with different particle sizes(namely 100,140,and 200 nm)were successfully prepared by adjusting the amount of tetrapropylammonium hydroxide(TPAOH),and investigated in n-heptane catalytic cracking reaction.Diffusional measurements by zero-length column(ZLC)method showed that the apparent diffusivities of n-heptane decreased with the reduction of particle size,indicating the existence of surface barriers.Moreover,with the decrease of particle size,the additional diffusion path length increased,which meant the influence of surface barriers became more apparent.Despite the change of surface barriers,the intracrystalline diffusion still dominated the overall diffusion.Catalytic performance showed that the zeolite with smaller particle size had better stability.
基金supported by the Natural Science Foundation of Jiangsu Province (BK20210887)the Jiangsu Provincial Double Innovation Program (JSSCB20210984)+1 种基金the Natural Science Fund for Colleges and Universities of Jiangsu Province (21KJB450003)the Jiangsu University of Science and Technology Doctoral Research Start-up Fund (120200012)。
文摘Higher nickel content endows Ni-rich cathode materials LiNi_(x)Co_yMn_(1-x-y)O_(2)(x>0.6)with higher specific capacity and high energy density,which is regarded as the most promising cathode materials for Li-ion batteries.However,the deterioration of structural stability hinders its practical application,especially under harsh working conditions such as high-temperature cycling.Given these circumstances,it becomes particularly critical to clarify the impact of the crystal morphology on the structure and high-temperature performance as for the ultrahigh-nickel cathodes.Herein,we conducted a comprehensive comparison in terms of microstructure,high-temperature long-cycle phase evolution,and high-temperature electrochemical stability,revealing the differences and the working mechanisms among polycrystalline(PC),single-crystalline(SC)and Al doped SC ultrahigh-nickel materials.The results show that the PC sample suffers a severe irreversible phase transition along with the appearance of microcracks,resulting a serious decay of both average voltage and the energy density.While the Al doped SC sample exhibits superior cycling stability with intact layered structure.In-situ XRD and intraparticle structural evolution characterization reveal that Al doping can significantly alleviate the irreversible phase transition,thus inhibiting microcracks generation and enabling enhanced structure.Specifically,it exhibits excellent cycling performance in pouch-type full-cell with a high capacity retention of 91.8%after 500 cycles at 55℃.This work promotes the fundamental understanding on the correlation between the crystalline morphology and high-temperature electrochemical stability and provides a guide for optimization the Ni-rich cathode materials.
基金This work was financially supported by National Key Research and Development Program of China(2019YFC1907805)Fundamental Research Funds for the Central Universities of Central South University(2021zzts0072).
文摘The rapid growth in global electric vehicles(EVs)sales has promoted the development of Co-free,Ni-rich layered cathodes for state-of-the-art high energy-density,inexpensive lithium-ion batteries(LIBs).However,progress in their commercial use has been seriously hampered by exasperating performance deterioration and safety concerns.Herein,a robust single-crystalline,Co-free,Ni-rich LiNi_(0.95)Mn_(0.05)O_(2)(SC-NM95)cathode is successfully designed using a molten salt-assisted method,and it exhibits better structural stability and cycling durability than those of polycrystalline LiNi_(0.95)Mn_(0.05)O_(2) (PC-NM95).Notably,the SC-NM95 cathode achieves a high discharge capacity of 218.2 mAh g^(-1),together with a high energy density of 837.3 Wh kg^(-1) at 0.1 C,mainly due to abundant Ni^(2+)/Ni^(3+) redox.It also presents an outstanding capacity retention(84.4%)after 200 cycles at 1 C,because its integrated single-crystalline structure effectively inhibits particle microcracking and surface phase transformation.In contrast,the PC-NM95 cathode suffers from rapid capacity fading owing to the nucleation and propagation of intergranular microcracking during cycling,facilitating aggravated parasitic reactions and rocksalt phase accumulation.This work provides a fundamental strategy for designing high-performance singlecrystalline,Co-free,Ni-rich cathode materials and also represents an important breakthrough in developing high-safe,low-cost,and high-energy LIBs.
基金financially supported by the National Natural Science Foundation of China (51664012)Guangxi Natural Science Foundation (2017GXNSFAA198117 and2015GXNSFGA139006)the Technology Major Project of Guangxi(AA19046001)
文摘A fundamental understanding of the electrochemical reaction process and mechanism of electrodes is very crucial for developing high-performance electrode materials.In this study,we report the sodium ion storage behavior and mechanism of orthorhombic V_(2)O_(5) single-crystalline nanowires in the voltage window of 1.0–4.0 V(vs.Na/Na+).The single-crystalline nanowires exhibit a large irreversible capacity loss during the first discharge/charge cycle,and then show excellent cycling stability in the following cycles.At a current density of 100 mA g^(−1),the nanowires electrode delivers initial discharge/charge capacity of 217/88 mA h g^(−1),corresponding to a Coulombic efficiency of only 40.5%;after 100 cycles,the electrode remains a reversible discharge capacity of 78 mA h g^(−1) with a fading rate of only 0.09%per cycle compared with the 2nd cycle discharge capacity.The sodium ion storage mechanism was investigated,illustrating that the large irreversible capacity loss in the first cycle can be attributed to the initially formed single-crystalline α′-Nax V_(2)O_(5)(0.02<x<0.88),in which sodium ions cannot be electrochemically extracted and the α′-Na0.88 V_(2)O_(5) can reversibly host and release sodium ions via a single-phase(solid solution)reaction,leading to excellent cycling stability.The Na^(+) diffusion coefficient in α′-Nax V_(2)O_(5) ranges from 10^(−12) to 10^(−11.5) cm^(2) s^(−1) as evaluated by galvanostatic intermittent titration technique(GITT).
文摘Electrocatalytic synthesis of value-added chemicals is attracting significant research attention owing to its mild reaction conditions, environmental benignity, and potentially scalable application to organic synthetic chemistry. Herein, we report the preparation of a single-crystalline NiS2 nanostructure film of N 50 nm thickness grown directly on a carbon fiber doth （NiSJCFC） by a facile vapor-phase hydrothermal （VPH） method. NiSJCFC as an electrocatalyst exhibits activity for both the oxygen evolution reaction （OER） and the hydrogen evolution reaction （HER） in alkaline media. Furthermore, a series of alcohols （2-propanol, 2-butanol, 2-pentanol, and cyclohexanol） were electrocatalytically converted to the corresponding ketones with high selectivity, efficienc and durability using the NiSJCFC electrode in alkaline media. In the presence of 0.45 M alcohol, a remarkably decreased overpotential （- 150 mV, vs. RHE） at the NiS2/CFC anode compared with that for water oxidation to generate O2, i.e., the OER, in alkaline media leads to significantly improved H2 generation. For instance, the H2 generation rate in the presence of 0.45 M 2-propanol is almost 1.2-times of that obtained for pure water splitting, but in a system that employs an applied voltage at least 280 mV lower than that required for water splitting to achieve the same current density （20 mA-crn-2）. Thus, our results demonstrate the applicability of our bifunctional non-precious-metal electrocatalyst for organic synthesis and simultaneous H2 production.
文摘The fast growth of large single-crystalline graphene by chemical vapor deposition on Cu foil remains a challenge for industrial-scale applications. To achieve the fast growth of large single-crystalline graphene, understanding the detailed dynamics governing the entire growth process--including nucleation, growth, and coalescence is important; however, these remain unexplored. In this study, by using a pulsed carbon isotope labeling technique in conjunction with micro-Raman spectroscopy identification, we visualized the growth dynamics, such as nucleation, growth, and coalescence, during the fast growth of large single- crystalline graphene domains. By tuning the supply of the carbon source, a growth rate of 320 μm/min and the growth of centimeter-sized graphene single crystals were achieved on Cu foil.
基金National Natural Science Foundation of China(Nos.52070194,52073309,51902347,51932003,51872115,and 22109135)Science and Technology Development Project of Jilin Province(Nos.YDZJ202101ZYTS165,20210506034ZP,and 20210509051RQ).
文摘Various and critical electrocatalytic processes are involved during the redox reactions in the Li-S batteries,which extremely depend on the surface structure and chemical state.Recently,single-atom concept unlocks a route to maximize the use of surface-active atoms,however,further increasing the density of active site is still strictly limited by the inherent structure that single-atoms are only highly-dispersed on substrate.Herein,we provide a viewpoint that an elaborate facet design with singlecrystalline structure engineering can harvest high-density surface active sites,which can significantly boost the electrocatalyst performance for excellent Li-S batteries.Specifically,the single-crystal CoSe_(2)(scCS)exhibits three-types of terminated(011)facet,efficiently obtaining the surface with a high-rich Co^(3+)–Se bond termination,in contrast with lots of surface grain boundaries and dangling bonds in polycrystalline CoSe_(2).Surprisingly,the surface active sites concentration can reach more than 69%.As anticipated,it can provide high-density and high-efficient active sites,enormously suppressing the shuttle effect and improving the reaction kinetics via accelerating the conversion and deposition of polysulfides and Li2S.This surface lattice strategy with element terminated mode is a promising approach for designing electrocatalyst effect-based energy system,not merely for Li-S batteries.
基金the Natural Science Foundation of Jiangsu Province(no.BK20180723)the Open Project of State Key Laboratory of Supramolecular Structure and Materials(no.sklssm2021011)+3 种基金the program of Jiangsu Province Innovation Team for financial supportthe Collaborative Innovation Center of Suzhou Nano Science and Technology for their supportthe Natural Science Foundation of Jiangsu Province(no.BK20191366)for its supportthe National Natural Science Foundation of China(no.21902114)for its support.
文摘Mesoporous single crystals have unique potential in catalysis,but remain unexplored owing to the enormous synthetic challenge that they pose.Herein,we report a facile soft-template method to prepare palladium(Pd)and Pd alloy nanocubes with single-crystallinity and abundant mesoporosity.The successful formation of these exotic nanostructures essentially relies on the cointroduction of cetyltrimethylammonium chloride as the surfactant template and extra Cl^(−) ions as the facet-selective capping agent under well controlled experimental conditions.Thanks to their large surface areas and penetrating mesoporous channels,our products exhibit a great performance for electrochemical CO_(2) reduction.The best sample from alloying palladium with copper enables the efficient formate production with high selectivity(90∼100%)over a broad potential range,and great stability even under the working potential as cathodic as −0.5 V versus a reversible hydrogen electrode.These performance metrics are far superior to previous Pd-based materials,and underscore the structural advantages of our products.
基金supported by the National Basic Research Program of China(2013CB933500)National Natural Science Foundation of China(Grant Nos.61422403,51672180,51622306,21673151)+2 种基金Qing Lan ProjectCollaborative Innovation Center of Suzhou Nano Science and Technology(NANO-CIC)the Priority Academic Program Development of Jiangsu Higher Education Institutions(PAPD)
文摘Organic field-effect transistors(OFETs) based on organic micro-/nanocrystals have been widely reported with charge carrier mobility exceeding 1.0 cm^2V^(-1)s^(-1), demonstrating great potential for high-performance, low-cost organic electronic applications. However, fabrication of large-area organic micro-/nanocrystal arrays with consistent crystal growth direction has posed a significant technical challenge. Here, we describe a solution-processed dip-coating technique to grow large-area, aligned 9,10-bis(phenylethynyl) anthracene(BPEA) and 6,13-bis(triisopropylsilylethynyl) pentacene(TIPSPEN) single-crystalline nanoribbon arrays. The method is scalable to a 5 9 10 cm^2 wafer substrate, with around 60% of the wafer surface covered by aligned crystals. The quality of crystals can be easily controlled by tuning the dip-coating speed. Furthermore, OFETs based on well-aligned BPEA and TIPS-PEN single-crystalline nanoribbons were constructed.By optimizing channel lengths and using appropriate metallic electrodes, the BPEA and TIPS-PEN-based OFETs showed hole mobility exceeding 2.0 cm^2V^(-1)s^(-1)(average mobility 1.2 cm^2V^(-1)s^(-1)) and 3.0 cm^2V^(-1)s^(-1)(average mobility2.0 cm^2V^(-1)s^(-1)), respectively. They both have a high on/off ratio(I_(on)/I_(off))>10~9. The performance can well satisfy the requirements for light-emitting diodes driving.
基金Project supported by National Natural Science Foundation of China(Grant Nos.11575102,11105085,11405098,and 11375108)the Fundamental Research Funds of Shandong University,China(Grant No.2015JC007)
文摘We report on the successful fabrication of highly branched Cu S nanocrystals by laser-induced photochemical reaction.Surprisingly, the single-crystalline nature with preferential alignment of the（107） orientation can be well improved during the moderate growth process. The branch length drastically increases from about 5 nm to 6 μm with an increase of photochemical reaction time（0-40 min）. The absorption spectra of as-prepared Cu S nanodendrites show that localized surface plasmon resonance（LSPR） peaks can be modulated from about 1037 nm to 1700 nm with an increase of branch length. Our results have a promising potential for photodynamic therapy and biological imaging application.
基金financially supported by the National Natural Science Foundation of China(21201133,51272186)
文摘Rare-earth doped titania single-crystalline hollow nanoparticles of 20 nm are constructed via a simple sol-gel process. Amphiphilic ABA tri-block copolymers played a key role in assisting the formation of hollow structure, for which a hollow nanostructure growth mechanism is proposed. By introducing rare earth into the synthesis process, the as-prepared nanoparticles exhibit near-infrared light absorption properties. Photo-decomposition efficiency of Orange II azo dye can be successfully evaluated when using Yb3+-doped Ti O2 hollow nanoparticles as photocatalysts; it is more than two times higher than the pure Ti O2 hollow nanoparticles. The hollow nanostructured Yb3+-doped Ti O2 samples are exploited as photoanodes in N719- sensitized solar cells and prove able to improve the photoelectric conversion efficiency by measuring the solar cell parameters of dye-sensitized solar cells(DSSCs) under simulative sunlight.
