Bio based nitrogen doped carbon dots(N-CDs)were obtained from empty fruit bunch carboxymethylcellulose and ethylenediamine(EDA)through one-pot hydrothermal carbonization route.The optimum as-formed NCDs were thoroughl...Bio based nitrogen doped carbon dots(N-CDs)were obtained from empty fruit bunch carboxymethylcellulose and ethylenediamine(EDA)through one-pot hydrothermal carbonization route.The optimum as-formed NCDs were thoroughly characterized via Transmission electron microscopy(TEM),high-resolution TEM(HRTEM),Fourier transform infrared(FTIR),X-ray photoelectron spectra(XPS),UV–vis spectra(UV–Vis)and Fluorescence spectra(PL).Response surface methodology was statistically used to assess three independent variables that have major influence on the fluorescence quantum yield(QY),including temperature(230–270℃),time(2–6 h)and EDA mass(10%–23.3%).Based on analysis of variance(ANOVA)results,synthesis temperature was found to be the most influential factor on the QY,followed by time and EDA mass.Higher temperature,long synthesis time and high amount of EDA were satisfactorily enough for efficient carbonization conversion rate and obtaining highest QY of N-CDs.The obtained quadratic model(R^2=0.9991)shows a good correlation between the experimental data and predicted values.The optimum synthetic parameters are of 270℃temperature,6 h reaction time and 23.3%of EDA mass.The optimized as-made N-CDs exhibited blue photoluminescence with both excitation dependent/independent phenomena and high nitrogen content.The maximum emission intensity was 426 nm at a maximum excitation wavelength of 320 nm,with a QY of up to 22.9%.XPS and FTIR data confirmed the existence of polar containing groups,such as carbonyl,carboxyl,hydroxyl and amino groups over the surface of N-CDs whereas nitrogen species in the form of(pyridinic and graphitic-N)were introduced in the aromatic carbon domains,which imparts the hydrophilic and photostability of N-CDs.Taking into account the low-cost and sustainable production of N-CDs,this method considered a feasible route for converting low quality waste into value-added nanomaterials and utilizing for different functionalization processes and analytical applications.展开更多
The nitrogen-doped carbon dots(N-CDs)were prepared by using coke powder as carbon source and one-step hydrothermal method.The N-CDs were studied as a fluorescent chemosensor for determining Cr(Ⅵ)in water.The selectiv...The nitrogen-doped carbon dots(N-CDs)were prepared by using coke powder as carbon source and one-step hydrothermal method.The N-CDs were studied as a fluorescent chemosensor for determining Cr(Ⅵ)in water.The selective,sensitive,reproducibility and stability of as-prepared N-CDs were investigated.The morphology,composition and properties of N-CDs were characterized by a series of methods.The fluorescence quenching of N-CDs by Cr(Ⅵ)was explored.The experimental results reveal that the obtained N-CDs have great hydrophilicity and strong luminescence properties,which demonstrates the successful doping of nitrogen into the CDs.The surface-active groups and emission wavelength range of CDs increase due to the electronegativity and electron donor effect of doping N atom.Furthermore,the N-CDs exhibit good photochemical properties for the detection of Cr(Ⅵ),including a wide linear range from 0.3 to 200μM(R^(2)=0.9935)and a low detection limit of 0.10μM at the signal-to-noise ratio of 3(S/N=3).Moreover,the N-CDs as a sensor was used successfully for Cr(Ⅵ)detection in real water samples with recovery rates of 99.9%-110.6%.This sensor also shows highly reproducibility and stability.The N-CDs fluorescent chemical sensor may be a potential candidate for applying in the field of other fluorescent chemical sensing,catalysis,photoelectric devices and other fields.展开更多
Highly dispersed Pd/N-doped carbon dots(Pd/NCDs)were successfully immobilized in the mesoporous channels of amino-functionalized dendritic mesoporous silica nanospheres(NMS).The synthesized Pd/NCDs@NMS catalyst exhibi...Highly dispersed Pd/N-doped carbon dots(Pd/NCDs)were successfully immobilized in the mesoporous channels of amino-functionalized dendritic mesoporous silica nanospheres(NMS).The synthesized Pd/NCDs@NMS catalyst exhibits outstanding performance in the catalytic reduction of 4-nitrophenol(4-NP),achieving a turnover frequency of 1461.8 mol·molPd^(-1)·h^(-1),with the conversion rate remaining above 80%after 11 cycles.Experiments and density functional theory calculations reveal that the NCDs significantly affect the electronic structure of Pd nanoparticles,leading to changes in the energy barriers for the adsorption of 4-NP at the Pd sites and the conversion of 4-NP reaction intermediates,which is a key factor contributing to the catalytic performance.This study offers a new strategy for synthesizing carbon-dot-modified metal-based catalysts.展开更多
Due to their superior fluorescence,phosphorescence,and catalytic capabilities,carbon dots(CDs),an emerging class of fluorescent carbon nanomaterials,have a wide range of potential applications.The properties of CDs ha...Due to their superior fluorescence,phosphorescence,and catalytic capabilities,carbon dots(CDs),an emerging class of fluorescent carbon nanomaterials,have a wide range of potential applications.The properties of CDs have recently been controlled extensively by heteroatom doping.Boron atoms have been effectively doped into the structure of CDs due to their similar size to carbon atoms and excellent electron-absorbing ability to further improve the performance of CDs.In this review,we summarize the research progress of boron-doped CDs in recent years from the aspects of doping strategies,effects of boron doping on different performances of CDs and applications.Starting from the two aspects of single boron doping and boron and other atom co-doping,from different precursor materials to different synthesis methods,the doping strategies of boron-doped CDs are reviewed in detail.Then,the effects of boron doping on the fluorescence,phosphorescence and catalytic performance of CDs and applications of boron-doped CDs in optical sensors,information encryption and anti-counterfeiting are discussed.Finally,we further provide a prospect towards the future development of boron-doped CDs.展开更多
Prussian blue(PB),as a promising inorganic electrochromic material(ECM),has been widely used in smart windows,displays,sensors,etc.However,there are still many challenges for PB to achieve high electrochromic performa...Prussian blue(PB),as a promising inorganic electrochromic material(ECM),has been widely used in smart windows,displays,sensors,etc.However,there are still many challenges for PB to achieve high electrochromic performance.Herein,we synthesized nitrogen-doped carbon dots-modified PB film(defined as PB@N-CDs)with a sandwich-like structure by a simple stepwise electrodeposition method.The carbon dots show an obvious advantage in ultrafast electron transfer ability,which can reduce charge loss during the transfer process,improve the electrochemical activity on both sides of PB,and thus facilitate a rapid electrochromic response.Furthermore,the surface of nitrogen-doped carbon dots contains multiple organic functional groups,which widen the movement path of K+ions under electrostatic adsorption.Impressively,the PB@N-CDs film exhibits a short bleaching/coloring time(0.5/0.9 s)and a superior optical modulation range(78.6%).Particularly,the coloring efficiency has been significantly improved to 137.71 cm^(2)/C(at 700 nm).All of these results open up new avenues for developing highperformance PB-based ECMs and promoting their applications in corresponding electrochromic devices(ECDs)and smart windows.展开更多
Regulating the doping of carbon dots(CDs)and the generation of reactive oxygen species(ROS)is essential to selectively control their application in photocatalytic organic reactions.This study successfully synthesized ...Regulating the doping of carbon dots(CDs)and the generation of reactive oxygen species(ROS)is essential to selectively control their application in photocatalytic organic reactions.This study successfully synthesized five newly developed nitrogen-doped carbon dots(CDs 1-5)with varying nitrogen content,which have the ability to generate ROS when exposed to light radiation,specifically superoxide anion radicals(O_(2)•-)and singlet oxygen(^(1)O_(2)).The utilization of the aforementioned nitrogen-doped CDs as photocatalysts enables the realization of their potential in facilitating efficient photocatalytic organic conversion.Simultaneously,it was observed that the photocatalytic efficiency exhibited a gradual decrease when the nitrogen content in the CDs increased.In order to provide more evidence for this claim,we employed a set of five CDs in the context of photocatalytic dehalogenation ofα-bromoacetophenone,photocatalytic oxidative coupling reaction of amines to imines,photooxidation reaction of sulfides to sulfoxides,and cross-dehydrogenation coupling(CDC)reaction,in which it was further observed that there was a steady decrease in the yields of photocatalytic organic reactions as the nitrogen content in CDs increased.Notably,CDs 1 exhibited the best photocatalytic efficiency,thereby reinforcing the hypothesis that a higher nitrogen content corresponds to a decreased catalytic efficiency.This study not only investigates the impact of the nitrogen content on the catalytic performance of CDs,but also offers valuable insights for the future utilization of CDs for photocatalytic organic reactions in water.展开更多
Exclusive responsiveness to ultraviolet light (~3.2 eV) and high photogenerated charge recombination rate are the two primary drawbacks of pure TiO_(2). We combined N-doped graphene quantum dots (N-GQDs), morphology r...Exclusive responsiveness to ultraviolet light (~3.2 eV) and high photogenerated charge recombination rate are the two primary drawbacks of pure TiO_(2). We combined N-doped graphene quantum dots (N-GQDs), morphology regulation, and heterojunction construction strategies to synthesize N-GQD/N-doped TiO_(2)/P-doped porous hollow g-C_(3)N_(4) nanotube (PCN) composite photocatalysts (denoted as G-TPCN). The optimal sample (G-TPCN doped with 0.1wt% N-GQD, denoted as 0.1% G-TPCN) exhibits significantly enhanced photoabsorption, which is attributed to the change in bandgap caused by elemental doping (P and N), the improved light-harvesting resulting from the tube structure, and the upconversion effect of N-GQDs. In addition, the internal charge separation and transfer capability of0.1% G-TPCN are dramatically boosted, and its carrier concentration is 3.7, 2.3, and 1.9 times that of N-TiO_(2), PCN, and N-TiO_(2)/PCN(TPCN-1), respectively. This phenomenon is attributed to the formation of Z-scheme heterojunction between N-TiO_(2) and PCNs, the excellent electron conduction ability of N-GQDs, and the short transfer distance caused by the porous nanotube structure. Compared with those of N-TiO_(2), PCNs, and TPCN-1, the H2 production activity of 0.1%G-TPCN under visible light is enhanced by 12.4, 2.3, and 1.4times, respectively, and its ciprofloxacin (CIP) degradation rate is increased by 7.9, 5.7, and 2.9 times, respectively. The optimized performance benefits from excellent photoresponsiveness and improved carrier separation and migration efficiencies. Finally, the photocatalytic mechanism of 0.1% G-TPCN and five possible degradation pathways of CIP are proposed. This study clarifies the mechanism of multiple modification strategies to synergistically improve the photocatalytic performance of 0.1% G-TPCN and provides a potential strategy for rationally designing novel photocatalysts for environmental remediation and solar energy conversion.展开更多
With the advantage of fast charge transfer,heterojunction engineering is identified as a viable method to reinforce the anodes'sodium storage performance.Also,vacancies can effectively strengthen the Na+adsorption...With the advantage of fast charge transfer,heterojunction engineering is identified as a viable method to reinforce the anodes'sodium storage performance.Also,vacancies can effectively strengthen the Na+adsorption ability and provide extra active sites for Na+adsorption.However,their synchronous engineering is rarely reported.Herein,a hybrid of Co_(0.85)Se/WSe_(2) heterostructure with Se vacancies and N-doped carbon polyhedron(CoWSe/NCP)has been fabricated for the first time via a hydrothermal and subsequent selenization strategy.Spherical aberration-corrected transmission electron microscopy confirms the phase interface of the Co_(0.85)Se/WSe_(2) heterostructure and the existence of Se vacancies.Density functional theory simulations reveal the accelerated charge transfer and enhanced Na+adsorption ability,which are contributed by the Co_(0.85)Se/WSe_(2) heterostructure and Se vacancies,respectively.As expected,the CoWSe/NCP anode in sodium-ion battery achieves outstanding rate capability(339.6 mAh g^(−1) at 20 A g^(−1)),outperforming almost all Co/W-based selenides.展开更多
The synergistic reaction of photocatalysis and advanced oxidation is a valid strategy for the degradation of harmful antibiotic wastewater.Herein,carbon dots(CDs)modified MIL-101(Fe)octahedrons to form CDs/MIL-101(Fe)...The synergistic reaction of photocatalysis and advanced oxidation is a valid strategy for the degradation of harmful antibiotic wastewater.Herein,carbon dots(CDs)modified MIL-101(Fe)octahedrons to form CDs/MIL-101(Fe)composite photocatalyst was synthesized for visible light-driven photocatalytic/persulfate(PS)-activated tetracycline(TC)degradation.The electron spin resonance(ESR)spectra,scavenging experiment and electrochemical analysis were carried out to reveal that the high visible light-driven photocatalytic degradation activity of TC over CDs/MIL-101(Fe)photocatalysts is not only ascribed to the production of free active radicals in the CDs/MIL-101(Fe)/PS system(·OH,·SO_(4-),^(1)O_(2),h^(+)and·O_(2)^(-))but also attributed to the consumption of electrons caused by the PS,which can suppress the recombination of photo-generated carriers as well as strong light scattering and electron trapping effects of CDs.Finally,the possible degradation pathways were proposed by analyzing intermediates via liquid chromatography-mass spectrometry technique.This research presents a rational design conception to construct a CDs/PS-based photocatalysis/advanced oxidation technology with high-efficient degradation activity for the remediation of organic antibiotic pollutant wastewater and for the improvement of carrier transport kinetics of photocatalysts.展开更多
Defect engineering by heteroatom doping gives carbon materials some new characteristics such as a different electronic structure and a high electrochemical activity,making them suitable for high-performance applicatio...Defect engineering by heteroatom doping gives carbon materials some new characteristics such as a different electronic structure and a high electrochemical activity,making them suitable for high-performance applications.N-doping has been widely investigated because of its similar atom radius to carbon,high electronegativity as well as many different configurations.We summarize the preparation methods and properties of N-doped carbon materials,and discuss their possible use in sodium ion storage.The relationships between N content/configuration and crystallinity,electronic conductivity,wettability,chemical reactivity as well as sodium ion storage performance are discussed.展开更多
Enhancing the stability of supported noble metal catalysts emerges is a major challenge in both science and industry.Herein,a heterogeneous Pd catalyst(Pd/NCF)was prepared by supporting Pd ultrafine metal nanoparticle...Enhancing the stability of supported noble metal catalysts emerges is a major challenge in both science and industry.Herein,a heterogeneous Pd catalyst(Pd/NCF)was prepared by supporting Pd ultrafine metal nanoparticles(NPs)on nitrogen-doped carbon;synthesized by using F127 as a stabilizer,as well as chitosan as a carbon and nitrogen source.The Pd/NCF catalyst was efficient and recyclable for oxidative carbonylation of phenol to diphenyl carbonate,exhibiting higher stability than Pd/NC prepared without F127 addition.The hydrogen bond between chitosan(CTS)and F127 was enhanced by F127,which anchored the N in the free amino group,increasing the N content of the carbon material and ensuring that the support could provide sufficient N sites for the deposition of Pd NPs.This process helped to improve metal dispersion.The increased metal-support interaction,which limits the leaching and coarsening of Pd NPs,improves the stability of the Pd/NCF catalyst.Furthermore,density functional theory calculations indicated that pyridine N stabilized the Pd^(2+)species,significantly inhibiting the loss of Pd^(2+)in Pd/NCF during the reaction process.This work provides a promising avenue towards enhancing the stability of nitrogen-doped carbon-supported metal catalysts.展开更多
Soil salinity seriously affects the utilization of farmland and threatens the crop production.Here,a selenium-nitrogen-co-doped carbon dots was developed,which increased rice seedling growth and alleviated its inhibit...Soil salinity seriously affects the utilization of farmland and threatens the crop production.Here,a selenium-nitrogen-co-doped carbon dots was developed,which increased rice seedling growth and alleviated its inhibition by salt stress by foliar spraying.The treatment activated Ca^(2+)and jasmonic acid signaling pathways and increased iron homeostasis,antioxidant defense,and cell wall development of rice seedlings.It could be used to increase crop resistance to environmental stress.展开更多
Over the past few decades,photocatalysis technology has received extensive attention because of its potential to mitigate or solve energy and environmental pollution problems.Designing novel materials with outstanding...Over the past few decades,photocatalysis technology has received extensive attention because of its potential to mitigate or solve energy and environmental pollution problems.Designing novel materials with outstanding photocatalytic activities has become a research hotspot in this field.In this study,we prepared a series of photocatalysts in which BiOCl nanosheets were modified with carbon quantum dots(CQDs)to form CQDs/BiOCl composites by using a simple solvothermal method.The photocatalytic performance of the resulting CQDs/BiOCl composite photocatalysts was assessed by rhodamine B and tetracycline degradation under visible-light irradiation.Compared with bare BiOCl,the photocatalytic activity of the CQDs/BiOCl composites was significantly enhanced,and the 5 wt%CQDs/BiOCl composite exhibited the highest photocatalytic activity with a degradation efficiency of 94.5%after 30 min of irradiation.Moreover,photocatalytic N_(2)reduction performance was significantly improved after introducing CQDs.The 5 wt%CQDs/BiOCl composite displayed the highest photocatalytic N_(2)reduction performance to yield NH_3(346.25μmol/(g h)),which is significantly higher than those of 3 wt%CQDs/BiOCl(256.04μmol/(g h)),7 wt%CQDs/BiOCl(254.07μmol/(g h)),and bare BiOCl(240.19μmol/(g h)).Our systematic characterizations revealed that the key role of CQDs in improving photocatalytic performance is due to their increased light harvesting capacity,remarkable electron transfer ability,and higher photocatalytic activity sites.展开更多
N-doped carbon materials,with their applications as electrocatalysts for the oxygen reduction reaction(ORR),have been extensively studied.However,a negletcted fact is that the operating potential of the ORR is higher ...N-doped carbon materials,with their applications as electrocatalysts for the oxygen reduction reaction(ORR),have been extensively studied.However,a negletcted fact is that the operating potential of the ORR is higher than the theoretical oxida-tion potential of carbon,possibly leading to the oxidation of carbon materials.Consequently,the infl uence of the structural oxidation evolution on ORR performance and the real active sites are not clear.In this study,we discover a two-step oxida-tion process of N-doped carbon during the ORR.The fi rst oxidation process is caused by the applied potential and bubbling oxygen during the ORR,leading to the oxidative dissolution of N and the formation of abundant oxygen-containing functional groups.This oxidation process also converts the reaction path from the four-electron(4e)ORR to the two-electron(2e)ORR.Subsequently,the enhanced 2e ORR generates oxidative H_(2)O_(2),which initiates the second stage of oxidation to some newly formed oxygen-containing functional groups,such as quinones to dicarboxyls,further diversifying the oxygen-containing functional groups and making carboxyl groups as the dominant species.We also reveal the synergistic eff ect of multiple oxygen-containing functional groups by providing additional opportunities to access active sites with optimized adsorption of OOH*,thus leading to high effi ciency and durability in electrocatalytic H_(2)O_(2) production.展开更多
Precision engineering of catalytic sites to guide more favorable pathways for Li_(2)O_(2) nucleation and decom-position represents an enticing kinetic strategy for mitigating overpotential,enhancing discharge capac-it...Precision engineering of catalytic sites to guide more favorable pathways for Li_(2)O_(2) nucleation and decom-position represents an enticing kinetic strategy for mitigating overpotential,enhancing discharge capac-ity,and improving recycling stability of Li-O_(2) batteries.In this work,we employ metal-organic frameworks(MOFs)derivation and ion substitution strategies to construct atomically dispersed Mn-N_(4) moieties on hierarchical porous nitrogen-doped carbon(Mn SAs-NC)with the aim of reducing the over-potential and improving the cycling stability of Li-O_(2) batteries.The porous structure provides more chan-nels for mass transfer and exposes more highly active sites for electrocatalytic reactions,thus promoting the formation and decomposition of Li_(2)O_(2).The Li-O_(2) batteries with Mn SAs-NC cathode achieve lower overpotential,higher specific capacity(14290 mA h g^(-1) at 100 mAg^(-1)),and superior cycle stability(>100 cycles at 200 mA g^(-1))compared with the Mn NPs-NC and NC.Density functional theory(DFT)cal-culations reveal that the construction of Mn-N_(4) moiety tunes the charge distribution of the pyridinic N-rich vacancy and balances the affinity of the intermediates(LiO_(2) and Li_(2)O_(2)).The initial nucleation of Li_(2)O_(2) on Mn SAs-NC favors the O_(2)-→LiO_(2)→Li_(2)O_(2) surface-adsorption pathway,which mitigates the overpoten-tials of the oxygen reduction(ORR)and oxygen evolution reaction(OER).As a result,Mn SAs-NC with Mn-N_(4) moiety effectively facilitates the Li_(2)O_(2) nucleation and enables its reversible decomposition.This work establishes a methodology for constructing carbon-based electrocatalysts with high activity and selectivity for Li-O_(2)batteries.展开更多
In this work,p⁃phenylenediamine and L⁃cysteine were used as raw materials,and water⁃soluble N,S co⁃doped carbon dots(N,S⁃CDs)with excellent performance were prepared through a one⁃step solvothermal method.The morpholo...In this work,p⁃phenylenediamine and L⁃cysteine were used as raw materials,and water⁃soluble N,S co⁃doped carbon dots(N,S⁃CDs)with excellent performance were prepared through a one⁃step solvothermal method.The morphology and structure of N,S⁃CDs were characterized by transmission electron microscope,X⁃ray diffrac⁃tion,Fourier transform infrared spectroscopy,and X⁃ray photoelectron spectroscopy,and the basic photophysical properties were investigated via UV⁃Vis absorption spectra and fluorescence spectra.Meanwhile,the N,S⁃CDs have excellent luminescence stability with pH,ionic strength,radiation time,and storage time.Experimental results illus⁃trated the present sensor platform exhibited high sensitivity and selectivity in response to baicalein with a detection limit of 85 nmol·L-1.The quenching mechanism is proved to be the inner filter effect.In addition,this sensor can also detect baicalein in biofluids(serum and urine)with good accuracy and reproducibility.展开更多
Liquid metal(LM)and liquid metal alloys(LMs)possess unique physicochemical features,which have become emerging and functionalized materials that are attractive applicants in various fields.Herein,uniform LM nanodrople...Liquid metal(LM)and liquid metal alloys(LMs)possess unique physicochemical features,which have become emerging and functionalized materials that are attractive applicants in various fields.Herein,uniform LM nanodroplets armored by carbon dots(LMD@CDs)were prepared and exhibited high colloidal stability in various solvents,as well as water.After optimization,LMD@CDs can be applied as functional additives for the 3D/4D printing of hydrogel and cross-linked resin through digital light processing(DLP).The light absorption of LMD@CDs not only improved the printing accuracy,but also led to the cross-linking density differential during the post-curing process.Base on the cross-linking density differential of soft hydrogel and photothermal performance of the LM,the 3D printed objects can exhibit stimulus responses to both water and laser irradiation.Additionally,the CDs shell and LM core of LMD@CDs provide the printed objects interesting photoluminescence and electric conductivity capabilities,respectively.We deduce this versatile 3D/4D printing system would provide a new platform for the preparation of multi-functional and stimuli-responsive advance materials.展开更多
SnO_(2) has been extensively investigated as an anode material for sodium-ion batteries(SIBs)and potassium-ion batteries(PIBs)due to its high Na/K storage capacity,high abundance,and low toxicity.However,the sluggish ...SnO_(2) has been extensively investigated as an anode material for sodium-ion batteries(SIBs)and potassium-ion batteries(PIBs)due to its high Na/K storage capacity,high abundance,and low toxicity.However,the sluggish reaction kinetics,low electronic conductivity,and large volume changes during charge and discharge hinder the practical applications of SnO_(2)-based electrodes for SIBs and PIBs.Engineering rational structures with fast charge/ion transfer and robust stability is important to overcoming these challenges.Herein,S-doped SnO_(2)(S-SnO_(2))quantum dots(QDs)(≈3 nm)encapsulated in an N,S codoped carbon fiber networks(S-SnO_(2)-CFN)are rationally fabricated using a sequential freeze-drying,calcination,and S-doping strategy.Experimental analysis and density functional theory calculations reveal that the integration of S-SnO_(2) QDs with N,S codoped carbon fiber network remarkably decreases the adsorption energies of Na/K atoms in the interlayer of SnO_(2)-CFN,and the S doping can increase the conductivity of SnO_(2),thereby enhancing the ion transfer kinetics.The synergistic interaction between S-SnO_(2) QDs and N,S codoped carbon fiber network results in a composite with fast Na+/K+storage and extraordinary long-term cyclability.Specifically,the S-SnO_(2)-CFN delivers high rate capacities of 141.0 mAh g^(−1) at 20 A g^(−1) in SIBs and 102.8 mAh g^(−1) at 10 A g^(−1) in PIBs.Impressively,it delivers ultra-stable sodium storage up to 10,000 cycles at 5 A g^(−1) and potassium storage up to 5000 cycles at 2 A g^(−1).This study provides insights into constructing metal oxide-based carbon fiber network structures for high-performance electrochemical energy storage and conversion devices.展开更多
Molybdenum carbide(Mo_(2)C)is a promising non-noble metal electrocatalyst with electronic structures similar to Pt for hydrogen evolution reaction(HER).However,strong H^(*)adsorption at the Mo sites hinders the improv...Molybdenum carbide(Mo_(2)C)is a promising non-noble metal electrocatalyst with electronic structures similar to Pt for hydrogen evolution reaction(HER).However,strong H^(*)adsorption at the Mo sites hinders the improvement of HER performance.Here,we synthesized monodisperse hollow Mo_(2)C nanoreactors,in which the carbon dots(CD)were in situ formed onto the surface of Mo_(2)C through carburization reactions.According to finite element simulation and analysis,the CD@Mo_(2)C possesses better mesoscale diffusion properties than Mo_(2)C alone.The optimized CD@Mo_(2)C nanoreactor demonstrates superior HER performance in alkaline electrolyte with a low overpotential of 57 mV at 10 mA cm^(−2),which is better than most Mo_(2)C-based electrocatalysts.Moreover,CD@Mo_(2)C exhibits excellent electrochemical stability during 240 h,confirmed by operando Raman and X-ray diffraction(XRD).Density functional theory(DFT)calculations show that carbon dots cause the d-band center of CD@Mo_(2)C to shift away from Fermi level,promoting water dissociation and the desorption of H^(*).This study provides a reasonable strategy towards high-activity Mo-based HER eletrocatalysts by modulating the strength of Mo–H bonds.展开更多
Electrolysis of seawater offers a highly promising and sustainable route to attain carbon-neutral hydrogen energy without demanding on high-purity water resource.However,it is severely limited by the undesirable chlor...Electrolysis of seawater offers a highly promising and sustainable route to attain carbon-neutral hydrogen energy without demanding on high-purity water resource.However,it is severely limited by the undesirable chlorine oxidation reaction(ClOR)on the anode and the releasing toxic chlorine species,inducing anode corrosion and multiple pollutions to reduce the efficiency and sustainability of this technology.The effective way is to limit the overpotential of oxygen evolution reaction(OER)below 480 mV and thus suppress the ClOR.Herein,we demonstrate that nitrogen-doped carbon dots strongly coupled NiFe layered double hydroxide nanosheet arrays on Ni foam(N-CDs/NiFe-LDH/NF)can efficiently facilitate OER with an ultralow overpotential of 260 mV to deliver the geometric current density of 100 mA·cm^(−2)and a Tafel slope of as low as 43.4 mV·dec−1 in 1.0 M KOH.More importantly,the N-CDs/NiFe-LDH/NF electrode at 100 mA·cm^(−2)shows overpotentials of 285 and 273 mV,respectively,by utilizing 1.0 M KOH with 0.5 M NaCl and 1.0 M KOH with 1.0 M NaCl as the simulated seawater,well avoid triggering ClOR.Notably,despite the complex environment of real seawater,N-CDs/NiFe-LDH/NF still effectively promotes alkaline seawater(1.0 M KOH+seawater)electrolysis with a lifetime longer than 50 and 20 h,respectively,in 1.0 M KOH and alkaline seawater electrolytes.The investigation result reveals that M–N–C bonding generated between N-CDs and NiFe-LDH intrinsically optimizes the charge transfer efficiency,further promoting the OER kinetics.展开更多
基金Universiti Putra Malaysia for funding this project(GP-IPS/2017/9556800).
文摘Bio based nitrogen doped carbon dots(N-CDs)were obtained from empty fruit bunch carboxymethylcellulose and ethylenediamine(EDA)through one-pot hydrothermal carbonization route.The optimum as-formed NCDs were thoroughly characterized via Transmission electron microscopy(TEM),high-resolution TEM(HRTEM),Fourier transform infrared(FTIR),X-ray photoelectron spectra(XPS),UV–vis spectra(UV–Vis)and Fluorescence spectra(PL).Response surface methodology was statistically used to assess three independent variables that have major influence on the fluorescence quantum yield(QY),including temperature(230–270℃),time(2–6 h)and EDA mass(10%–23.3%).Based on analysis of variance(ANOVA)results,synthesis temperature was found to be the most influential factor on the QY,followed by time and EDA mass.Higher temperature,long synthesis time and high amount of EDA were satisfactorily enough for efficient carbonization conversion rate and obtaining highest QY of N-CDs.The obtained quadratic model(R^2=0.9991)shows a good correlation between the experimental data and predicted values.The optimum synthetic parameters are of 270℃temperature,6 h reaction time and 23.3%of EDA mass.The optimized as-made N-CDs exhibited blue photoluminescence with both excitation dependent/independent phenomena and high nitrogen content.The maximum emission intensity was 426 nm at a maximum excitation wavelength of 320 nm,with a QY of up to 22.9%.XPS and FTIR data confirmed the existence of polar containing groups,such as carbonyl,carboxyl,hydroxyl and amino groups over the surface of N-CDs whereas nitrogen species in the form of(pyridinic and graphitic-N)were introduced in the aromatic carbon domains,which imparts the hydrophilic and photostability of N-CDs.Taking into account the low-cost and sustainable production of N-CDs,this method considered a feasible route for converting low quality waste into value-added nanomaterials and utilizing for different functionalization processes and analytical applications.
基金by the National Nature Science Foundation of China(61904130)the Open Fund of the Fujian Universities and Colleges Engineering Research Center of Modern Facility Agriculture of Fujian University(G2-KF2002)+4 种基金the Opening Project of Key Laboratory of Optoelectronic Chemical Materials and Devices,Ministry of Education,Jianghan University(JDGD202017)the Open Fund of the Hubei Provincial Key Laboratory for New Processes of Ironmaking and Steel Making(Wuhan University of Science and Technology)of China(KF-20-5)the Fund of Hangzhou Meishi Technology Co.,Ltd of China(2021420112000081)the Key Research and Development Program of Hubei Province(2020BAB084)the Program(BG20190227001)of High-end Foreign Experts of the State of the State Administration of Foreign Experts Affairs(SAFEA)。
文摘The nitrogen-doped carbon dots(N-CDs)were prepared by using coke powder as carbon source and one-step hydrothermal method.The N-CDs were studied as a fluorescent chemosensor for determining Cr(Ⅵ)in water.The selective,sensitive,reproducibility and stability of as-prepared N-CDs were investigated.The morphology,composition and properties of N-CDs were characterized by a series of methods.The fluorescence quenching of N-CDs by Cr(Ⅵ)was explored.The experimental results reveal that the obtained N-CDs have great hydrophilicity and strong luminescence properties,which demonstrates the successful doping of nitrogen into the CDs.The surface-active groups and emission wavelength range of CDs increase due to the electronegativity and electron donor effect of doping N atom.Furthermore,the N-CDs exhibit good photochemical properties for the detection of Cr(Ⅵ),including a wide linear range from 0.3 to 200μM(R^(2)=0.9935)and a low detection limit of 0.10μM at the signal-to-noise ratio of 3(S/N=3).Moreover,the N-CDs as a sensor was used successfully for Cr(Ⅵ)detection in real water samples with recovery rates of 99.9%-110.6%.This sensor also shows highly reproducibility and stability.The N-CDs fluorescent chemical sensor may be a potential candidate for applying in the field of other fluorescent chemical sensing,catalysis,photoelectric devices and other fields.
基金supported by the National Key R&D Program of China(No.2022YFA1503501)the National Natural Science Foundation of China(Nos.22088101 and U21A20329)+2 种基金Program of Shanghai Academic Research Leader(No.21XD1420800)Shanghai Pilot Program for Basic Research-FuDan University 21TQ1400100(21TQ008)“Shuguang Program”supported by Shanghai Education Development Foundation and Shanghai Municipal Education Commission(No.22SG02).
文摘Highly dispersed Pd/N-doped carbon dots(Pd/NCDs)were successfully immobilized in the mesoporous channels of amino-functionalized dendritic mesoporous silica nanospheres(NMS).The synthesized Pd/NCDs@NMS catalyst exhibits outstanding performance in the catalytic reduction of 4-nitrophenol(4-NP),achieving a turnover frequency of 1461.8 mol·molPd^(-1)·h^(-1),with the conversion rate remaining above 80%after 11 cycles.Experiments and density functional theory calculations reveal that the NCDs significantly affect the electronic structure of Pd nanoparticles,leading to changes in the energy barriers for the adsorption of 4-NP at the Pd sites and the conversion of 4-NP reaction intermediates,which is a key factor contributing to the catalytic performance.This study offers a new strategy for synthesizing carbon-dot-modified metal-based catalysts.
基金the Youth Talent Program Startup Foundation of Qufu Normal University(No.602601)the Natural Science Foundation of Rizhao(No.RZ2021ZR37)。
文摘Due to their superior fluorescence,phosphorescence,and catalytic capabilities,carbon dots(CDs),an emerging class of fluorescent carbon nanomaterials,have a wide range of potential applications.The properties of CDs have recently been controlled extensively by heteroatom doping.Boron atoms have been effectively doped into the structure of CDs due to their similar size to carbon atoms and excellent electron-absorbing ability to further improve the performance of CDs.In this review,we summarize the research progress of boron-doped CDs in recent years from the aspects of doping strategies,effects of boron doping on different performances of CDs and applications.Starting from the two aspects of single boron doping and boron and other atom co-doping,from different precursor materials to different synthesis methods,the doping strategies of boron-doped CDs are reviewed in detail.Then,the effects of boron doping on the fluorescence,phosphorescence and catalytic performance of CDs and applications of boron-doped CDs in optical sensors,information encryption and anti-counterfeiting are discussed.Finally,we further provide a prospect towards the future development of boron-doped CDs.
基金supported by Jiangsu Specially Appointed Professor programthe Tsinghua-Toyota Joint Research Fundthe National Key Research and Development Program of China(Nos.2020YFC2201103 and 2020YFA0210702).
文摘Prussian blue(PB),as a promising inorganic electrochromic material(ECM),has been widely used in smart windows,displays,sensors,etc.However,there are still many challenges for PB to achieve high electrochromic performance.Herein,we synthesized nitrogen-doped carbon dots-modified PB film(defined as PB@N-CDs)with a sandwich-like structure by a simple stepwise electrodeposition method.The carbon dots show an obvious advantage in ultrafast electron transfer ability,which can reduce charge loss during the transfer process,improve the electrochemical activity on both sides of PB,and thus facilitate a rapid electrochromic response.Furthermore,the surface of nitrogen-doped carbon dots contains multiple organic functional groups,which widen the movement path of K+ions under electrostatic adsorption.Impressively,the PB@N-CDs film exhibits a short bleaching/coloring time(0.5/0.9 s)and a superior optical modulation range(78.6%).Particularly,the coloring efficiency has been significantly improved to 137.71 cm^(2)/C(at 700 nm).All of these results open up new avenues for developing highperformance PB-based ECMs and promoting their applications in corresponding electrochromic devices(ECDs)and smart windows.
基金the National Natural Science Foundation of China(No.52205210)the Natural Science Foundation of Shandong Province(Nos.ZR2020MB018,ZR2022QE033,and ZR2021QB049).
文摘Regulating the doping of carbon dots(CDs)and the generation of reactive oxygen species(ROS)is essential to selectively control their application in photocatalytic organic reactions.This study successfully synthesized five newly developed nitrogen-doped carbon dots(CDs 1-5)with varying nitrogen content,which have the ability to generate ROS when exposed to light radiation,specifically superoxide anion radicals(O_(2)•-)and singlet oxygen(^(1)O_(2)).The utilization of the aforementioned nitrogen-doped CDs as photocatalysts enables the realization of their potential in facilitating efficient photocatalytic organic conversion.Simultaneously,it was observed that the photocatalytic efficiency exhibited a gradual decrease when the nitrogen content in the CDs increased.In order to provide more evidence for this claim,we employed a set of five CDs in the context of photocatalytic dehalogenation ofα-bromoacetophenone,photocatalytic oxidative coupling reaction of amines to imines,photooxidation reaction of sulfides to sulfoxides,and cross-dehydrogenation coupling(CDC)reaction,in which it was further observed that there was a steady decrease in the yields of photocatalytic organic reactions as the nitrogen content in CDs increased.Notably,CDs 1 exhibited the best photocatalytic efficiency,thereby reinforcing the hypothesis that a higher nitrogen content corresponds to a decreased catalytic efficiency.This study not only investigates the impact of the nitrogen content on the catalytic performance of CDs,but also offers valuable insights for the future utilization of CDs for photocatalytic organic reactions in water.
基金financially supported by the National Natural Science Foundation of China (Nos.U2002212,52102058,52204414,52204413,and 52204412)the National Key R&D Program of China (Nos.2021YFC1910504,2019YFC1907101,2019YFC1907103,and 2017YFB0702304)+7 种基金the Key R&D Program of Ningxia Hui Autonomous Region,China (Nos.2021BEG01003 and2020BCE01001)the Xijiang Innovation and Entrepreneurship Team,China (No.2017A0109004)the Macao Young Scholars Program (No.AM2022024),Chinathe Beijing Natural Science Foundation (Nos.L212020 and 2214073),Chinathe Guangdong Basic and Applied Basic Research Foundation,China (Nos.2021A1515110998 and 2020A1515110408)the China Postdoctoral Science Foundation (No.2022M710349)the Fundamental Research Funds for the Central Universities,China (Nos.FRF-BD-20-24A,FRF-TP-20-031A1,FRF-IC-19-017Z,and 06500141)the Integration of Green Key Process Systems MIIT and Scientific and Technological Innovation Foundation of Foshan,China(Nos.BK22BE001 and BK21BE002)。
文摘Exclusive responsiveness to ultraviolet light (~3.2 eV) and high photogenerated charge recombination rate are the two primary drawbacks of pure TiO_(2). We combined N-doped graphene quantum dots (N-GQDs), morphology regulation, and heterojunction construction strategies to synthesize N-GQD/N-doped TiO_(2)/P-doped porous hollow g-C_(3)N_(4) nanotube (PCN) composite photocatalysts (denoted as G-TPCN). The optimal sample (G-TPCN doped with 0.1wt% N-GQD, denoted as 0.1% G-TPCN) exhibits significantly enhanced photoabsorption, which is attributed to the change in bandgap caused by elemental doping (P and N), the improved light-harvesting resulting from the tube structure, and the upconversion effect of N-GQDs. In addition, the internal charge separation and transfer capability of0.1% G-TPCN are dramatically boosted, and its carrier concentration is 3.7, 2.3, and 1.9 times that of N-TiO_(2), PCN, and N-TiO_(2)/PCN(TPCN-1), respectively. This phenomenon is attributed to the formation of Z-scheme heterojunction between N-TiO_(2) and PCNs, the excellent electron conduction ability of N-GQDs, and the short transfer distance caused by the porous nanotube structure. Compared with those of N-TiO_(2), PCNs, and TPCN-1, the H2 production activity of 0.1%G-TPCN under visible light is enhanced by 12.4, 2.3, and 1.4times, respectively, and its ciprofloxacin (CIP) degradation rate is increased by 7.9, 5.7, and 2.9 times, respectively. The optimized performance benefits from excellent photoresponsiveness and improved carrier separation and migration efficiencies. Finally, the photocatalytic mechanism of 0.1% G-TPCN and five possible degradation pathways of CIP are proposed. This study clarifies the mechanism of multiple modification strategies to synergistically improve the photocatalytic performance of 0.1% G-TPCN and provides a potential strategy for rationally designing novel photocatalysts for environmental remediation and solar energy conversion.
基金support from the Natural Science Foundation of Jilin Province(Grant No.20200201073JC)the National Natural Science Foundation of China(Grant No.52130101)+1 种基金Interdisciplinary Integration and Innovation Project of JLU(Grant No.JLUXKJC2021ZY01)the Fundamental Research Funds for the Central Universities.
文摘With the advantage of fast charge transfer,heterojunction engineering is identified as a viable method to reinforce the anodes'sodium storage performance.Also,vacancies can effectively strengthen the Na+adsorption ability and provide extra active sites for Na+adsorption.However,their synchronous engineering is rarely reported.Herein,a hybrid of Co_(0.85)Se/WSe_(2) heterostructure with Se vacancies and N-doped carbon polyhedron(CoWSe/NCP)has been fabricated for the first time via a hydrothermal and subsequent selenization strategy.Spherical aberration-corrected transmission electron microscopy confirms the phase interface of the Co_(0.85)Se/WSe_(2) heterostructure and the existence of Se vacancies.Density functional theory simulations reveal the accelerated charge transfer and enhanced Na+adsorption ability,which are contributed by the Co_(0.85)Se/WSe_(2) heterostructure and Se vacancies,respectively.As expected,the CoWSe/NCP anode in sodium-ion battery achieves outstanding rate capability(339.6 mAh g^(−1) at 20 A g^(−1)),outperforming almost all Co/W-based selenides.
基金the funding support from the National Natural Science Foundation of China(21906072,22006057)the Natural Science Foundation of Jiangsu Province(BK20190982)“Doctor of Mass entrepreneurship and innovation”Project in Jiangsu Province。
文摘The synergistic reaction of photocatalysis and advanced oxidation is a valid strategy for the degradation of harmful antibiotic wastewater.Herein,carbon dots(CDs)modified MIL-101(Fe)octahedrons to form CDs/MIL-101(Fe)composite photocatalyst was synthesized for visible light-driven photocatalytic/persulfate(PS)-activated tetracycline(TC)degradation.The electron spin resonance(ESR)spectra,scavenging experiment and electrochemical analysis were carried out to reveal that the high visible light-driven photocatalytic degradation activity of TC over CDs/MIL-101(Fe)photocatalysts is not only ascribed to the production of free active radicals in the CDs/MIL-101(Fe)/PS system(·OH,·SO_(4-),^(1)O_(2),h^(+)and·O_(2)^(-))but also attributed to the consumption of electrons caused by the PS,which can suppress the recombination of photo-generated carriers as well as strong light scattering and electron trapping effects of CDs.Finally,the possible degradation pathways were proposed by analyzing intermediates via liquid chromatography-mass spectrometry technique.This research presents a rational design conception to construct a CDs/PS-based photocatalysis/advanced oxidation technology with high-efficient degradation activity for the remediation of organic antibiotic pollutant wastewater and for the improvement of carrier transport kinetics of photocatalysts.
文摘Defect engineering by heteroatom doping gives carbon materials some new characteristics such as a different electronic structure and a high electrochemical activity,making them suitable for high-performance applications.N-doping has been widely investigated because of its similar atom radius to carbon,high electronegativity as well as many different configurations.We summarize the preparation methods and properties of N-doped carbon materials,and discuss their possible use in sodium ion storage.The relationships between N content/configuration and crystallinity,electronic conductivity,wettability,chemical reactivity as well as sodium ion storage performance are discussed.
基金support by the National Natural Science Foundation of China(U21A20306,U20A20152)Natural Science Foundation of Hebei Province(B2022202077).
文摘Enhancing the stability of supported noble metal catalysts emerges is a major challenge in both science and industry.Herein,a heterogeneous Pd catalyst(Pd/NCF)was prepared by supporting Pd ultrafine metal nanoparticles(NPs)on nitrogen-doped carbon;synthesized by using F127 as a stabilizer,as well as chitosan as a carbon and nitrogen source.The Pd/NCF catalyst was efficient and recyclable for oxidative carbonylation of phenol to diphenyl carbonate,exhibiting higher stability than Pd/NC prepared without F127 addition.The hydrogen bond between chitosan(CTS)and F127 was enhanced by F127,which anchored the N in the free amino group,increasing the N content of the carbon material and ensuring that the support could provide sufficient N sites for the deposition of Pd NPs.This process helped to improve metal dispersion.The increased metal-support interaction,which limits the leaching and coarsening of Pd NPs,improves the stability of the Pd/NCF catalyst.Furthermore,density functional theory calculations indicated that pyridine N stabilized the Pd^(2+)species,significantly inhibiting the loss of Pd^(2+)in Pd/NCF during the reaction process.This work provides a promising avenue towards enhancing the stability of nitrogen-doped carbon-supported metal catalysts.
基金financially supported by the National Natural Science Foundation of China (42207032,52070064)the Key Project of National Natural Science Foundation of China (42330705)+2 种基金Key R&D Project of Hebei Province (21373601D)Advanced Talents Incubation Program of the Hebei University (521100222012)economic support from Collaborative Innovation Center for Baiyangdian Basin Ecological Protection and Beijing-Tianjin-Hebei Sustainable Development and Institute of Life Sciences and Green Development of Hebei University。
文摘Soil salinity seriously affects the utilization of farmland and threatens the crop production.Here,a selenium-nitrogen-co-doped carbon dots was developed,which increased rice seedling growth and alleviated its inhibition by salt stress by foliar spraying.The treatment activated Ca^(2+)and jasmonic acid signaling pathways and increased iron homeostasis,antioxidant defense,and cell wall development of rice seedlings.It could be used to increase crop resistance to environmental stress.
基金financially suppor ted by Key Research and Development Project of Anhui Province(No.2023h11020002)Natural Science Research Project for Universities in Anhui Province(No.KJ2021ZD0006)+3 种基金Natural Science Foundation of Anhui Province(No.2208085MB21)Fundamental Research Funds for the Central Universities of China(No.PA2022GDSK0056)Anhui Laboratory of Molecule-Based Materials(No.fzj22009)National Natural Science Foundation of China(Nos.21725102,22205108)。
文摘Over the past few decades,photocatalysis technology has received extensive attention because of its potential to mitigate or solve energy and environmental pollution problems.Designing novel materials with outstanding photocatalytic activities has become a research hotspot in this field.In this study,we prepared a series of photocatalysts in which BiOCl nanosheets were modified with carbon quantum dots(CQDs)to form CQDs/BiOCl composites by using a simple solvothermal method.The photocatalytic performance of the resulting CQDs/BiOCl composite photocatalysts was assessed by rhodamine B and tetracycline degradation under visible-light irradiation.Compared with bare BiOCl,the photocatalytic activity of the CQDs/BiOCl composites was significantly enhanced,and the 5 wt%CQDs/BiOCl composite exhibited the highest photocatalytic activity with a degradation efficiency of 94.5%after 30 min of irradiation.Moreover,photocatalytic N_(2)reduction performance was significantly improved after introducing CQDs.The 5 wt%CQDs/BiOCl composite displayed the highest photocatalytic N_(2)reduction performance to yield NH_3(346.25μmol/(g h)),which is significantly higher than those of 3 wt%CQDs/BiOCl(256.04μmol/(g h)),7 wt%CQDs/BiOCl(254.07μmol/(g h)),and bare BiOCl(240.19μmol/(g h)).Our systematic characterizations revealed that the key role of CQDs in improving photocatalytic performance is due to their increased light harvesting capacity,remarkable electron transfer ability,and higher photocatalytic activity sites.
基金We acknowledge the National Natural Science Foundation of China(No.22275134)for fi nancial support.
文摘N-doped carbon materials,with their applications as electrocatalysts for the oxygen reduction reaction(ORR),have been extensively studied.However,a negletcted fact is that the operating potential of the ORR is higher than the theoretical oxida-tion potential of carbon,possibly leading to the oxidation of carbon materials.Consequently,the infl uence of the structural oxidation evolution on ORR performance and the real active sites are not clear.In this study,we discover a two-step oxida-tion process of N-doped carbon during the ORR.The fi rst oxidation process is caused by the applied potential and bubbling oxygen during the ORR,leading to the oxidative dissolution of N and the formation of abundant oxygen-containing functional groups.This oxidation process also converts the reaction path from the four-electron(4e)ORR to the two-electron(2e)ORR.Subsequently,the enhanced 2e ORR generates oxidative H_(2)O_(2),which initiates the second stage of oxidation to some newly formed oxygen-containing functional groups,such as quinones to dicarboxyls,further diversifying the oxygen-containing functional groups and making carboxyl groups as the dominant species.We also reveal the synergistic eff ect of multiple oxygen-containing functional groups by providing additional opportunities to access active sites with optimized adsorption of OOH*,thus leading to high effi ciency and durability in electrocatalytic H_(2)O_(2) production.
基金supported by the National Natural Science Foundation of China (21878340)supported in part by the High-Performance Computing Center of Central South University
文摘Precision engineering of catalytic sites to guide more favorable pathways for Li_(2)O_(2) nucleation and decom-position represents an enticing kinetic strategy for mitigating overpotential,enhancing discharge capac-ity,and improving recycling stability of Li-O_(2) batteries.In this work,we employ metal-organic frameworks(MOFs)derivation and ion substitution strategies to construct atomically dispersed Mn-N_(4) moieties on hierarchical porous nitrogen-doped carbon(Mn SAs-NC)with the aim of reducing the over-potential and improving the cycling stability of Li-O_(2) batteries.The porous structure provides more chan-nels for mass transfer and exposes more highly active sites for electrocatalytic reactions,thus promoting the formation and decomposition of Li_(2)O_(2).The Li-O_(2) batteries with Mn SAs-NC cathode achieve lower overpotential,higher specific capacity(14290 mA h g^(-1) at 100 mAg^(-1)),and superior cycle stability(>100 cycles at 200 mA g^(-1))compared with the Mn NPs-NC and NC.Density functional theory(DFT)cal-culations reveal that the construction of Mn-N_(4) moiety tunes the charge distribution of the pyridinic N-rich vacancy and balances the affinity of the intermediates(LiO_(2) and Li_(2)O_(2)).The initial nucleation of Li_(2)O_(2) on Mn SAs-NC favors the O_(2)-→LiO_(2)→Li_(2)O_(2) surface-adsorption pathway,which mitigates the overpoten-tials of the oxygen reduction(ORR)and oxygen evolution reaction(OER).As a result,Mn SAs-NC with Mn-N_(4) moiety effectively facilitates the Li_(2)O_(2) nucleation and enables its reversible decomposition.This work establishes a methodology for constructing carbon-based electrocatalysts with high activity and selectivity for Li-O_(2)batteries.
文摘In this work,p⁃phenylenediamine and L⁃cysteine were used as raw materials,and water⁃soluble N,S co⁃doped carbon dots(N,S⁃CDs)with excellent performance were prepared through a one⁃step solvothermal method.The morphology and structure of N,S⁃CDs were characterized by transmission electron microscope,X⁃ray diffrac⁃tion,Fourier transform infrared spectroscopy,and X⁃ray photoelectron spectroscopy,and the basic photophysical properties were investigated via UV⁃Vis absorption spectra and fluorescence spectra.Meanwhile,the N,S⁃CDs have excellent luminescence stability with pH,ionic strength,radiation time,and storage time.Experimental results illus⁃trated the present sensor platform exhibited high sensitivity and selectivity in response to baicalein with a detection limit of 85 nmol·L-1.The quenching mechanism is proved to be the inner filter effect.In addition,this sensor can also detect baicalein in biofluids(serum and urine)with good accuracy and reproducibility.
基金The financial support from the National Natural Science Foundation of China(Grant No.51973201,U1804128,to X.P.Grant No.52173209,to Y.H.)+4 种基金the 111 Project(D18023,to X.P.)the National Science Foundation for Young Scientists of China(Grant No.22105179,to G.S.)the National Key R&D Program of China(2017YFB0307600,to M.L)China Postdoctoral Science Foundation(2020M682317,to X.Z)Scientific&technological research projects in Henan Province(222102520009,to X.Q.)
文摘Liquid metal(LM)and liquid metal alloys(LMs)possess unique physicochemical features,which have become emerging and functionalized materials that are attractive applicants in various fields.Herein,uniform LM nanodroplets armored by carbon dots(LMD@CDs)were prepared and exhibited high colloidal stability in various solvents,as well as water.After optimization,LMD@CDs can be applied as functional additives for the 3D/4D printing of hydrogel and cross-linked resin through digital light processing(DLP).The light absorption of LMD@CDs not only improved the printing accuracy,but also led to the cross-linking density differential during the post-curing process.Base on the cross-linking density differential of soft hydrogel and photothermal performance of the LM,the 3D printed objects can exhibit stimulus responses to both water and laser irradiation.Additionally,the CDs shell and LM core of LMD@CDs provide the printed objects interesting photoluminescence and electric conductivity capabilities,respectively.We deduce this versatile 3D/4D printing system would provide a new platform for the preparation of multi-functional and stimuli-responsive advance materials.
基金National Natural Science Foundation of China,Grant/Award Number:51971065Innovation Program of Shanghai Municipal Education Commission,Grant/Award Number:2019-01-07-00-07-E00028。
文摘SnO_(2) has been extensively investigated as an anode material for sodium-ion batteries(SIBs)and potassium-ion batteries(PIBs)due to its high Na/K storage capacity,high abundance,and low toxicity.However,the sluggish reaction kinetics,low electronic conductivity,and large volume changes during charge and discharge hinder the practical applications of SnO_(2)-based electrodes for SIBs and PIBs.Engineering rational structures with fast charge/ion transfer and robust stability is important to overcoming these challenges.Herein,S-doped SnO_(2)(S-SnO_(2))quantum dots(QDs)(≈3 nm)encapsulated in an N,S codoped carbon fiber networks(S-SnO_(2)-CFN)are rationally fabricated using a sequential freeze-drying,calcination,and S-doping strategy.Experimental analysis and density functional theory calculations reveal that the integration of S-SnO_(2) QDs with N,S codoped carbon fiber network remarkably decreases the adsorption energies of Na/K atoms in the interlayer of SnO_(2)-CFN,and the S doping can increase the conductivity of SnO_(2),thereby enhancing the ion transfer kinetics.The synergistic interaction between S-SnO_(2) QDs and N,S codoped carbon fiber network results in a composite with fast Na+/K+storage and extraordinary long-term cyclability.Specifically,the S-SnO_(2)-CFN delivers high rate capacities of 141.0 mAh g^(−1) at 20 A g^(−1) in SIBs and 102.8 mAh g^(−1) at 10 A g^(−1) in PIBs.Impressively,it delivers ultra-stable sodium storage up to 10,000 cycles at 5 A g^(−1) and potassium storage up to 5000 cycles at 2 A g^(−1).This study provides insights into constructing metal oxide-based carbon fiber network structures for high-performance electrochemical energy storage and conversion devices.
基金financially supported by the National Natural Science Foundation of China (22372001)Starting Fund for Scientific Research of High-Level Talents, Anhui Agricultural University (rc382108)+1 种基金Anhui Provincial Key Research and Development Plan (2022e07020037)Innovation and Entrepreneurship Training Program for College Students (X202310364204, S202210364046, X202310364209)
文摘Molybdenum carbide(Mo_(2)C)is a promising non-noble metal electrocatalyst with electronic structures similar to Pt for hydrogen evolution reaction(HER).However,strong H^(*)adsorption at the Mo sites hinders the improvement of HER performance.Here,we synthesized monodisperse hollow Mo_(2)C nanoreactors,in which the carbon dots(CD)were in situ formed onto the surface of Mo_(2)C through carburization reactions.According to finite element simulation and analysis,the CD@Mo_(2)C possesses better mesoscale diffusion properties than Mo_(2)C alone.The optimized CD@Mo_(2)C nanoreactor demonstrates superior HER performance in alkaline electrolyte with a low overpotential of 57 mV at 10 mA cm^(−2),which is better than most Mo_(2)C-based electrocatalysts.Moreover,CD@Mo_(2)C exhibits excellent electrochemical stability during 240 h,confirmed by operando Raman and X-ray diffraction(XRD).Density functional theory(DFT)calculations show that carbon dots cause the d-band center of CD@Mo_(2)C to shift away from Fermi level,promoting water dissociation and the desorption of H^(*).This study provides a reasonable strategy towards high-activity Mo-based HER eletrocatalysts by modulating the strength of Mo–H bonds.
基金the National Natural Science Foundation of China(Nos.52122308,21905253,and 51973200)the Natural Science Foundation of Henan(No.202300410372).
文摘Electrolysis of seawater offers a highly promising and sustainable route to attain carbon-neutral hydrogen energy without demanding on high-purity water resource.However,it is severely limited by the undesirable chlorine oxidation reaction(ClOR)on the anode and the releasing toxic chlorine species,inducing anode corrosion and multiple pollutions to reduce the efficiency and sustainability of this technology.The effective way is to limit the overpotential of oxygen evolution reaction(OER)below 480 mV and thus suppress the ClOR.Herein,we demonstrate that nitrogen-doped carbon dots strongly coupled NiFe layered double hydroxide nanosheet arrays on Ni foam(N-CDs/NiFe-LDH/NF)can efficiently facilitate OER with an ultralow overpotential of 260 mV to deliver the geometric current density of 100 mA·cm^(−2)and a Tafel slope of as low as 43.4 mV·dec−1 in 1.0 M KOH.More importantly,the N-CDs/NiFe-LDH/NF electrode at 100 mA·cm^(−2)shows overpotentials of 285 and 273 mV,respectively,by utilizing 1.0 M KOH with 0.5 M NaCl and 1.0 M KOH with 1.0 M NaCl as the simulated seawater,well avoid triggering ClOR.Notably,despite the complex environment of real seawater,N-CDs/NiFe-LDH/NF still effectively promotes alkaline seawater(1.0 M KOH+seawater)electrolysis with a lifetime longer than 50 and 20 h,respectively,in 1.0 M KOH and alkaline seawater electrolytes.The investigation result reveals that M–N–C bonding generated between N-CDs and NiFe-LDH intrinsically optimizes the charge transfer efficiency,further promoting the OER kinetics.