Supercapacitors represent one specific class of energy storage devices that bridge the gap between traditional capacitors and batteries.In current work,δ-MnO_(2) nanoflakes arrayed on electrochemically exfoliated gra...Supercapacitors represent one specific class of energy storage devices that bridge the gap between traditional capacitors and batteries.In current work,δ-MnO_(2) nanoflakes arrayed on electrochemically exfoliated graphene(EEG)nanosheets were easily made as one composited electrode material for boosting the charge storage performances of supercapacitors.Coupled with the fluent electron and ion transport from two-dimensional EEG nanosheets,the uniformly anchoredδ-MnO_(2) nanoflake arrays present high reversible capacity,superior cycling stability,and unique rate capability.As expected,the MnO_(2)/EEG-10 electrode delivers high specific capacitance of 190 F·g^(−1) at 0.2 A·g^(−1),and holds 97.3%of its initial capacitance after 10000 cycles at 5 A·g^(−1).Furthermore,an asymmetrical supercapacitor using MnO_(2)/EEG-10 as the positive electrode achieves an energy density of 17.7 W·h·kg^(−1) at a power density of 922.7 W·kg^(−1) with 82.9%capacity retention upon 10000 cycles at 5 A·g^(−1).This work highlights the facile fabrication of high-performance MnO_(2)/graphene composites with excellent structure stability using graphene nanosheets as the conductive matrix.展开更多
We proposed a strategy to address the issue by synthesizing MnO with half-filled 3 d electron orbitals.That is,MnO nanocubes with an edge length of 61.82 nm were successfully prepared through electros-pinning and one-...We proposed a strategy to address the issue by synthesizing MnO with half-filled 3 d electron orbitals.That is,MnO nanocubes with an edge length of 61.82 nm were successfully prepared through electros-pinning and one-step pyrolysis as the cathode electrode for Li-O_(2)batteries.It is observed that the intermediate LiMnO_(4)rather than Li_(2)O_(2)is formed when LiO_(2)interactes with MnO(111)during the discharge process.It is precisely because of LiMnO_(4)that reduces its charge overpotential to 0.29 V.The novel reaction mechanism dominated by LiMnO_(4)further facilitates the lower charge overpotential,thereby enhancing the energy efficiency of the batteries.展开更多
CO_(2)hydrogenation to value-added light olefins(C_(2-4)=)is crucial for the utilization and cycling of global carbon resource.Moderate CO_(2)activation and carbon chain growth ability are key factors for iron-based c...CO_(2)hydrogenation to value-added light olefins(C_(2-4)=)is crucial for the utilization and cycling of global carbon resource.Moderate CO_(2)activation and carbon chain growth ability are key factors for iron-based catalysts for efficient CO_(2)conversion to target C_(2-4)=products.The electronic interaction and confinement effect of electron-deficient graphene inner surface on the active phase are effective to improve surface chemical properties and enhance the catalytic performance.Here,we report a core-shell FeCo alloy catalyst with graphene layers confinement prepared by a simple sol-gel method.The electron transfer from Fe species to curved graphene inner surface modifies the surface electronic structure of the active phaseχ-(Fe_(x)Co_(1-x))_(5)C_(2)and improves CO_(2)adsorption capacity,enhancing the efficient conversion of CO_(2)and moderate C-C coupling.Therefore,the catalyst FeCoK@C exhibits C_(2-4)=selectivity of 33.0%while maintaining high CO_(2)conversion of 52.0%.The high stability without obvious deactivation for over 100 h and unprecedented C_(2-4)=space time yield(STY)up to 52.9 mmolCO_(2)·g^(-1)·h^(-1)demonstrate its potential for practical application.This work provides an efficient strategy for the development of high-performance CO_(2)hydrogenation catalysts.展开更多
Aqueous Zn//MnO2 batteries are emerging as promising large-scale energy storage devices owing to their cost-effectiveness,high safety,high output voltage,and energy density.However,the MnO2 cathode suffers from intrin...Aqueous Zn//MnO2 batteries are emerging as promising large-scale energy storage devices owing to their cost-effectiveness,high safety,high output voltage,and energy density.However,the MnO2 cathode suffers from intrinsically poor rate performance and rapid capacity deterioration.Here,we remove the roadblock by compositing MnO2 nanorods with highly conductive graphene,which remarkably enhances the electrochemical properties of the MnO2 cathode.Benefiting from the boosted electric conductivity and ion diffusion rate as well as the structural protection of graphene,the Zn//MnO2-graphene battery presents an admirable capacity of 301 mAh g^-1 at 0.5 A g^-1,corresponding to a high energy density of 411.6 Wh kg^-1.Even at a high current density of 10 A g^-1,a decent capacity of 95.8 mAh g^-1 is still obtained,manifesting its excellent rate property.Furthermore,an impressive power density of 15 kW kg^-1 is achieved by the Zn//MnO2-graphene battery.展开更多
The unique properties of TiO_(2)-sulfur(TiO_(2)-S)modified graphene nanocomposite electrode(GPE/TiO_(2)-S)in the electrochemical sensing of formaldehyde compound has been evaluated.We prepared TiO_(2)-S by hydrotherma...The unique properties of TiO_(2)-sulfur(TiO_(2)-S)modified graphene nanocomposite electrode(GPE/TiO_(2)-S)in the electrochemical sensing of formaldehyde compound has been evaluated.We prepared TiO_(2)-S by hydrothermal method and modified the graphene nanocomposite electrode by applying electrochemical cyclic voltammetry(CV)approach.The TiO_(2)-S nanocomposite was characterized by X-ray diffraction(XRD),while the GPE/TiO_(2)-S was examined by scanning electron microscopy(FESEM)and X-Ray fluorosense(XRF)techniques.TiO_(2)-S has a grain size of 19.32 nm.The surface morphology of the GPE/TiO_(2)-S nanocomposite shows a good,intact,and tightly porous structure with TiO_(2)-S covers the graphene surface.The content of optimized GPE/TiO_(2)-S electrodes is 41.5%of graphene,37.8%of TiO_(2),and 12.4%of sulfur that was prepared by mixing 1 g of TiO_(2)-S with 0.5 g of graphene and 0.3 mL paraffin.The GPE/TiO_(2)-S electrode produces a high anodic current(I_(pa))of 800μA and a high cathodic current(I_(pc))of-600μA at a scan rate of 0.1 V·s^(-1)using an electrolyte0.01 mol·L^(-1)K_3[Fe(CN)_6]solution containing 150 mg·L^(-1)formaldehyde.The limit of detection can reach as low as 9.7 mg·L^(-1)with stability with Horwitz ratio value as low as 0.397.The composite electrode also exhibits excellent slectivity properties by showing clear formaldehyde sugnal in the presence of high concentration of interfering agent.GPE/TiO_(2)-S electrode should find potential application of formaldehyde detection in food industries.展开更多
Optical polarizers,which allow the transmission of specific polarization states,are essential components in modern optical systems.Here,we experimentally demonstrate integrated photonic polarizers incorporating reduce...Optical polarizers,which allow the transmission of specific polarization states,are essential components in modern optical systems.Here,we experimentally demonstrate integrated photonic polarizers incorporating reduced graphene oxide(rGO)films.2D graphene oxide(GO)films are integrated onto silicon waveguides and microring resonators(MRRs)with precise control over their thicknesses and sizes,followed by GO reduction via two different methods including uniform thermal reduction and localized photothermal reduction.We measure devices with various lengths,thicknesses,and reduction degrees of GO films.The results show that the devices with rGO exhibit better performance than those with GO,achieving a polarization-dependent loss of~47 dB and a polarization extinction ratio of~16 dB for the hybrid waveguides and MRRs with rGO,respectively.By fitting the experimental results with theory,it is found that rGO exhibits more significant anisotropy in loss,with an anisotropy ratio over 4 times that of GO.In addition,rGO shows higher thermal stability and greater robustness to photothermal reduction than GO.These results highlight the strong potential of rGO films for implementing high-performance polarization selective devices in integrated photonic platforms.展开更多
Manipulating catalyst structures to control product selectivity while maintaining high activity presents a considerable challenge in CO_(2)hydrogenation.Combining density functional theory calculations and microkineti...Manipulating catalyst structures to control product selectivity while maintaining high activity presents a considerable challenge in CO_(2)hydrogenation.Combining density functional theory calculations and microkinetic analysis,we proposed that graphene-supported isolated Pt atoms(Pt1/graphene)and Pt_(2)dimers(Pt_(2)/graphene)exhibited distinct selectivity in CO_(2)hydrogenation.Pt_(1)/graphene facilitated the conversion of CO_(2)into formic acid,whereas Pt_(2)/graphene favored methanol generation.The variation in product selectivity arose from the synergistic interaction of Pt_(2)dimers,which facilitated the migration of H atoms between two Pt atoms and promoted the transformation from*COOH intermediates to*C(OH)_(2)intermediates,altering the reaction pathways compared to isolated Pt atoms.Additionally,an analysis of the catalytic activities of three Pt_(1)/graphene and three Pt_(2)/graphene structures revealed that the turnover frequencies for formic acid generation on Pt_(1ii)/graphene and methanol generation on Pt_(2i)/graphene were as high as 744.48 h-1and 789.48 h^(-1),respectively.These values rivaled or even surpassed those previously reported in the literature under identical conditions.This study provides valuable insights into optimizing catalyst structures to achieve desired products in CO_(2)hydrogenation.展开更多
Ultrasound is a powerful tool in materials processing,yet its application in constructing van der Waals(vdW)heterostructures remains under-explored.In this study,MoS_(2)and graphene—two widely studied 2D materials—w...Ultrasound is a powerful tool in materials processing,yet its application in constructing van der Waals(vdW)heterostructures remains under-explored.In this study,MoS_(2)and graphene—two widely studied 2D materials—were successfully assembled into vdW heterostructures via a convenient ultrasound-driven self-assembly approach.The morphology of the heterostructures was characterized by scanning electron microscopy(SEM),while their structural and compositional features were confirmed through x-ray diffraction(XRD),Raman spectroscopy,and x-ray photoelectron spectroscopy(XPS).Red-shifted Raman peaks and decreased binding energies in XPS spectra provided strong evidence of successful heterostructure formation.A three-stage assembly mechanism—comprising dispersion,assembly,and adjustment—is proposed,with acoustic cavitation playing a key role in driving the process.This study not only demonstrates the feasibility of synthesizing 2D heterostructures via an ultrasonic route but also lays a foundation for future scalable,energy-efficient fabrication strategies.展开更多
Charge-neutral method(CNM)is extensively used in investigating the performance of catalysts and the mechanism of N_(2)electrochemical reduction(NRR).However,disparities remain between the predicted potentials required...Charge-neutral method(CNM)is extensively used in investigating the performance of catalysts and the mechanism of N_(2)electrochemical reduction(NRR).However,disparities remain between the predicted potentials required for NRR by the CNM methods and those observed experimentally,as the CNM method neglects the charge effect from the electrode potential.To address this issue,we employed the constant electrode potential(CEP)method to screen atomic transition metal-N-graphene(M_(1)/N-graphene)as NRR electrocatalysts and systematically investigated the underlying catalytic mechanism.Among eight types of M_(1)/N-graphene(M_(1)=Mo,W,Fe,Re,Ni,Co,V,Cr),W_(1)/N-graphene emerges as the most promising NRR electrocatalyst with a limiting potential as low as−0.13 V.Additionally,the W_(1)/N-graphene system consistently maintains a positive charge during the reaction due to its Fermi level being higher than that of the electrode.These results better match with the actual circumstances compared to those calculated by conventional CNM method.Thus,our work not only develops a promising electrocatalyst for NRR but also deepens the understanding of the intrinsic electrocatalytic mechanism.展开更多
Graphene has enormous potential to capture CO_(2)due to its unique properties and cost-effectiveness.However,graphene-based adsorbents have drawbacks of lower CO_(2)adsorption capacity and poor selectivity.This work d...Graphene has enormous potential to capture CO_(2)due to its unique properties and cost-effectiveness.However,graphene-based adsorbents have drawbacks of lower CO_(2)adsorption capacity and poor selectivity.This work demonstrates a one-step rapid and sustainable N_(2)/H_(2)plasma treatment process to prepare graphene-based sorbent material with enhanced CO_(2)adsorption performance.Plasma treatment directly enriches amine species,increases surface area,and improves textural properties.The CO_(2)adsorption capacity increases from 1.6 to 3.3 mmol/g for capturing flue gas,and from 0.14 to 1.3 mmol/g for direct air capture (DAC).Importantly,the electrothermal property of the plasma-modified aerogels has been significantly improved,resulting in faster heating rates and significantly reducing energy consumption compared to conventional external heating for regeneration of sorbents.Modified aerogels display improved selectivity of 42 and 87 after plasma modification for 5 and 10 min,respectively.The plasma-treated aerogels display minimal loss between 17%and 19% in capacity after 40 adsorption/desorption cycles,rendering excellent stability.The N_(2)/H_(2)plasma treatment of adsorbent materials would lower energy expenses and prevent negative effects on the global economy caused by climate change.展开更多
The production of hydrogen peroxide(H_(2)O_(2))via artificial photosynthesis using single-atom semiconductor photocatalysts represents a promising green and sustainable technology.However,its efficiency is still limit...The production of hydrogen peroxide(H_(2)O_(2))via artificial photosynthesis using single-atom semiconductor photocatalysts represents a promising green and sustainable technology.However,its efficiency is still limited by sluggish water oxidation kinetics,poor photogenerated charge separation,and insufficient O_(2)adsorption and activation capabilities.Herein,uniformly dispersed single-atom catalysts(SACs)with a Co-N_(4)coordination structure have been synthesized by thermally transforming cobalt phthalocyanine(CoPc)assemblies pre-anchored on phosphate functionalized reduced graphene oxide(Co@rGO-P),and then used to construct heterojunctions with perylenetetracarboxylic acid(PTA)nanosheets for photocatalytic H_(2)O_(2)production by an in-situ growth method.The optimized Co@rGO-P/PTA achieved an H_(2)O_(2)production rate of 1.4 mmol g^(-1)h^(-1)in pure water,with a 12.9-fold enhancement compared to pristine PTA nanosheets exhibiting competitive photoactivity among reported perylene-based materials.Femtosecond transient absorption spectra,in-situ diffuse reflectance infrared Fourier transform spectra and theoretical calculations reveal that the exceptional performance is attributed to the enhanced electron transfer from PTA to rGO via the phosphate bridge and then to the Co-N_(4),and to the promoted O_(2)adsorption and activation at Co-N_(4)active sites.This work provides a feasible and effective strategy for designing highly efficient single-atom semiconductor heterojunction photocatalysts for H_(2)O_(2)production.展开更多
In this study, a new facile preparation method of nanocomposites consisting of graphene oxide and manganese dioxide nanowires（GO/MnO2 NWs） was developed. The morphology, structure and composition of the resulted pro...In this study, a new facile preparation method of nanocomposites consisting of graphene oxide and manganese dioxide nanowires（GO/MnO2 NWs） was developed. The morphology, structure and composition of the resulted products were characterized by transmission electron microscopy, X-ray diffraction and N2 adsorption and desorption. The GO/MnO2 nanocomposite was used as an electrode material for non-enzymatic determination of hydrogen peroxide. The proposed sensor exhibits excellent electrocatalytic performance for the determination of hydrogen peroxide in phosphate buffer solution（PBS, pH7） at an applied potential of 0.75 V. The non-enzymatic biosensor for determination of hydrogen peroxide displayed a wide linear range of 4.90 mmol L^-1–4.50 mmol L^-1with a correlation coefficient of 0.9992, a low detection limit of 0.48 mmol L^-1 and a high sensitivity of 191.22μA（mmol L^-1）^-1cm^-2（signal/noise, S/N = 3）. Moreover, the non-enzymatic biosensor shows an excellent selectivity.展开更多
Conversion-type anode materials are highly desirable for Na-ion batteries(NIBs)due to their high theoretical capacity.Nevertheless,the active materials undergo severe expansion and pulverization during the sodiation,r...Conversion-type anode materials are highly desirable for Na-ion batteries(NIBs)due to their high theoretical capacity.Nevertheless,the active materials undergo severe expansion and pulverization during the sodiation,resulting in inferior cycling stability.Herein,a self-supporting three-dimensional(3D)graphene sponge decorated with Fe_(2)O_(3)nanocubes(rGO@Fe_(2)O_(3))is constructed.Specifically,the 3D graphene sponge with resilience and high porosity benefits to accommodate the volume expansion of the Fe_(2)O_(3)nanocubes and facilitates the rapid electrons/ions transport,enabling spatial confinement to achieve outstanding results.Besides,the free-standing rGO@Fe_(2)O_(3)can be directly used as an electrode without additional binders and conductive additives,which helps to obtain a higher energy density.Based on the total mass of the rGO@Fe_(2)O_(3)material,the rGO@Fe_(2)O_(3)anode presents a specific capacity of 859 mAh/g at 0.1 A/g.It also delivers an impressive cycling performance(327 mAh/g after 2000 cycles at 1 A/g)and a superior rate capacity(162mAh/g at 20 A/g).The coin-type Na_(3)V_(2)(PO_(4))_(3)@C//rGO@Fe_(2)O_(3)NIB exhibits an energy density of 265.3Wh/kg.This unique 3D ionic/electronic conductive network may provide new strategies to design advanced conversion-type anode materials for high-performance NIBs.展开更多
In this study,the holey graphene was prepared by microwave-assisted chemical etching.The three-dimensional(3D)holey graphene hydrogel was obtained through hydrothermal self-assembly method,followed by the introduction...In this study,the holey graphene was prepared by microwave-assisted chemical etching.The three-dimensional(3D)holey graphene hydrogel was obtained through hydrothermal self-assembly method,followed by the introduction of FeCo_(2)S_(4)particles.The resulting holey graphene hydrogel,characterized by high specific surface area and abundant pores combined with FeCo_(2)S_(4)with high pseudocapacitance by interfacial interaction,shortened the mass transport path and enhanced the specific capacitance.The findings reveal that the holey graphene hydrogel/FeCo_(2)S_(4)(FeCo_(2)S_(4)/HGH)composite exhibits high specific capacitance and impressive rate capability(413.4 F·g^(-1)at 1 A·g^(-1),300.4 F·g^(-1)at 6 A·g^(-1)).The symmetric supercapacitor operated within a stable potential window of 0.1-1.6 V,achieving specific capacitance of 127.5 F·g^(-1)at 1 A·g^(-1),and can deliver 37.1 Wh·kg^(-1)at a power density of 1499 W·kg^(-1).Besides,under the current density of 3 A·g^(-1),the supercapacitor retained 90.8%of its capacitance after 5000 cycles,demonstrating exceptional cycle stability.This study presents an efficient method for fabricating advanced integrated supercapacitors electrodes with enhanced energy density.展开更多
The photo-assisted Fenton-like method is an effective and sustainable way to remove organic pollutants from water.Herein,a series of three-dimensional composites containing MIL-88A(Fe)-derived α-Fe_(2)O_(3)and graphe...The photo-assisted Fenton-like method is an effective and sustainable way to remove organic pollutants from water.Herein,a series of three-dimensional composites containing MIL-88A(Fe)-derived α-Fe_(2)O_(3)and graphene aerogel(GA-Fe-X)were designed and used as catalysts to degrade ciprofloxacin(CIP)by peroxymonosulfate(PMS)activated photo-Fenton-like technology.The as-prepared GA-Fe-1 displayed remarkable enhancement with a CIP degradation rate constant(0.017 min^(-1))higher than that of graphene aerogel(0.0031 min^(-1))and MIL-88A(Fe)(0.0039 min^(-1)).Experimental results demonstrated that the combination of MIL-88A(Fe)-derived α-Fe_(2)O_(3)and graphene aerogel forming GA-Fe-X enhanced the separation efficiency of electron-hole pairs,activating PMS to produce SO_(4)^(·-),^(·)OH and ^(1)O_(2) for enhanced CIP degradation through radical and non-radical pathways.The factors affecting CIP degradation during the photoFenton-like process were thoroughly investigated.The possible CIP degradation pathways and ecotoxicity of the intermediates were also analyzed.This work enhances our understanding of the photo-Fenton-like effect in three-dimensional graphene aerogel composites.展开更多
Low-cost Fe-based disordered rock salt(DRX)Li_(2)FeTiO_(4)is capable of providing high capacity(295 mA h g^(-1))by redox activity of cations(Fe^(2+)/Fe^(4+)and Ti^(3+)/Ti^(4+))and anionic oxygen.However,DRX structures...Low-cost Fe-based disordered rock salt(DRX)Li_(2)FeTiO_(4)is capable of providing high capacity(295 mA h g^(-1))by redox activity of cations(Fe^(2+)/Fe^(4+)and Ti^(3+)/Ti^(4+))and anionic oxygen.However,DRX structures lack transport channels for ions and electrons,resulting in sluggish kinetics,poor electrochemical activity,and cyclability.Herein,graphene conductive carbon network permeated Li_(2)FeTiO_(4)(LFT/C/G)nanofibers are successfully prepared by a facile sol-gel assisted electrospinning method.Ultrafine Li_(2)FeTiO_(4)nanoparticles(2 nm)and one-dimensional(1D)structure provide abu ndant active sites and unobstructed diffu sion channels,accelerating ion diffusion.In addition,introducing graphene reduces the band gap and Li^(+)diffusion barrier and improves the dynamic properties of Li_(2)FeTiO_(4),thus achieving a relatively mild interfacial reaction and reversible redox reaction.As expected,the LFT/C/1.0G cathode delivers a remarkable discharge capacity(238.5 mA h g^(-1)),high energy density(508.8 Wh kg^(-1)),and excellent rate capability(51.2 mA hg^(-1)at 1.0 A g^(-1)).Besides,the LFT/C/1.0G anode also displays a high capacity(514.5 mA h g^(-1)at 500 mA g^(-1))and a remarkable rate capability(243.9 mA h g^(-1)at 8 A g^(-1)).Moreover,the full batteries based on the LFT/C/1.0G symmetric electrode demonstrate a reversible capacity of 117.0 mA h g^(-1)after 100 cycles at 50 mA g^(-1).This study presents useful insights into developing cost-effective DRX cathodes with durable and fast lithium storage.展开更多
Formaldehyde(HCHO)causes increasing concerns due to its ubiquitously found in indoor air and being irritative and carcinogenic to humans.Photothermal-catalysis developed in recent years has been considered as a signif...Formaldehyde(HCHO)causes increasing concerns due to its ubiquitously found in indoor air and being irritative and carcinogenic to humans.Photothermal-catalysis developed in recent years has been considered as a significant strategy for enhancing catalytic activity.Manganese oxides,compared with its strong thermocatalytic activity,generally suffer from much lower photocatalytic activity make its photochemical properties less concerned.Herein,α-MnO_(2)nanowires were composited with the graphene oxide(GO)via mechanical grinding and co-precipitating method,respectively.α-MnO_(2)/GO nanohybrids prepared by co-precipitating method exhibits excellent activity,achieving 100%decomposition of HCHO with the solar-light irradiation at ambient temperature.It is found that,besides the photo-driven thermocatalysis,the photocatalysis mechanism made a major contribution to the decomposition of HCHO.The incorporation of GO,on the one hand,is beneficial to improve the optical absorption capacity and photothermal conversion efficiency;on the other hand,is conductive to electron transfer and effective separation of electrons and holes.These synergistic effects significantly improve the catalytic activity ofα-MnO_(2)/GO nanohybrids.This work proposes a new approach for the utilization of solar energy by combining manganese oxides,and also develops an efficient photothermal-catalyst to control HCHO pollution in indoor air.展开更多
基金supported by Natural Science Foundation of Shandong Province(ZR2023ME155 and ZR2023ME085)the project of“20 Items of University”of Jinan(202228046)the Taishan Scholar Project of Shandong Province(tsqn202306226 and tsqn202211171).
文摘Supercapacitors represent one specific class of energy storage devices that bridge the gap between traditional capacitors and batteries.In current work,δ-MnO_(2) nanoflakes arrayed on electrochemically exfoliated graphene(EEG)nanosheets were easily made as one composited electrode material for boosting the charge storage performances of supercapacitors.Coupled with the fluent electron and ion transport from two-dimensional EEG nanosheets,the uniformly anchoredδ-MnO_(2) nanoflake arrays present high reversible capacity,superior cycling stability,and unique rate capability.As expected,the MnO_(2)/EEG-10 electrode delivers high specific capacitance of 190 F·g^(−1) at 0.2 A·g^(−1),and holds 97.3%of its initial capacitance after 10000 cycles at 5 A·g^(−1).Furthermore,an asymmetrical supercapacitor using MnO_(2)/EEG-10 as the positive electrode achieves an energy density of 17.7 W·h·kg^(−1) at a power density of 922.7 W·kg^(−1) with 82.9%capacity retention upon 10000 cycles at 5 A·g^(−1).This work highlights the facile fabrication of high-performance MnO_(2)/graphene composites with excellent structure stability using graphene nanosheets as the conductive matrix.
基金Funded by the National Natural Science Foundation of China(No.22075035)the Technology Planning Project of Liaoning Province(No.2020JH2/10700008)the Dalian Science and Technology Innovation Fund Project(No.2022JJ11CG005)。
文摘We proposed a strategy to address the issue by synthesizing MnO with half-filled 3 d electron orbitals.That is,MnO nanocubes with an edge length of 61.82 nm were successfully prepared through electros-pinning and one-step pyrolysis as the cathode electrode for Li-O_(2)batteries.It is observed that the intermediate LiMnO_(4)rather than Li_(2)O_(2)is formed when LiO_(2)interactes with MnO(111)during the discharge process.It is precisely because of LiMnO_(4)that reduces its charge overpotential to 0.29 V.The novel reaction mechanism dominated by LiMnO_(4)further facilitates the lower charge overpotential,thereby enhancing the energy efficiency of the batteries.
文摘CO_(2)hydrogenation to value-added light olefins(C_(2-4)=)is crucial for the utilization and cycling of global carbon resource.Moderate CO_(2)activation and carbon chain growth ability are key factors for iron-based catalysts for efficient CO_(2)conversion to target C_(2-4)=products.The electronic interaction and confinement effect of electron-deficient graphene inner surface on the active phase are effective to improve surface chemical properties and enhance the catalytic performance.Here,we report a core-shell FeCo alloy catalyst with graphene layers confinement prepared by a simple sol-gel method.The electron transfer from Fe species to curved graphene inner surface modifies the surface electronic structure of the active phaseχ-(Fe_(x)Co_(1-x))_(5)C_(2)and improves CO_(2)adsorption capacity,enhancing the efficient conversion of CO_(2)and moderate C-C coupling.Therefore,the catalyst FeCoK@C exhibits C_(2-4)=selectivity of 33.0%while maintaining high CO_(2)conversion of 52.0%.The high stability without obvious deactivation for over 100 h and unprecedented C_(2-4)=space time yield(STY)up to 52.9 mmolCO_(2)·g^(-1)·h^(-1)demonstrate its potential for practical application.This work provides an efficient strategy for the development of high-performance CO_(2)hydrogenation catalysts.
基金financially supported by the Guangdong Power Grid Co.,Ltd.(Grant No.GDKJXM20160000)。
文摘Aqueous Zn//MnO2 batteries are emerging as promising large-scale energy storage devices owing to their cost-effectiveness,high safety,high output voltage,and energy density.However,the MnO2 cathode suffers from intrinsically poor rate performance and rapid capacity deterioration.Here,we remove the roadblock by compositing MnO2 nanorods with highly conductive graphene,which remarkably enhances the electrochemical properties of the MnO2 cathode.Benefiting from the boosted electric conductivity and ion diffusion rate as well as the structural protection of graphene,the Zn//MnO2-graphene battery presents an admirable capacity of 301 mAh g^-1 at 0.5 A g^-1,corresponding to a high energy density of 411.6 Wh kg^-1.Even at a high current density of 10 A g^-1,a decent capacity of 95.8 mAh g^-1 is still obtained,manifesting its excellent rate property.Furthermore,an impressive power density of 15 kW kg^-1 is achieved by the Zn//MnO2-graphene battery.
基金the financial support from the Ministry of Education,Culture,Research and Technology of the Republic of Indonesia under the Applied Research award(DIPA023.17.1.690523/2023)the World Class Professor award grant 2023。
文摘The unique properties of TiO_(2)-sulfur(TiO_(2)-S)modified graphene nanocomposite electrode(GPE/TiO_(2)-S)in the electrochemical sensing of formaldehyde compound has been evaluated.We prepared TiO_(2)-S by hydrothermal method and modified the graphene nanocomposite electrode by applying electrochemical cyclic voltammetry(CV)approach.The TiO_(2)-S nanocomposite was characterized by X-ray diffraction(XRD),while the GPE/TiO_(2)-S was examined by scanning electron microscopy(FESEM)and X-Ray fluorosense(XRF)techniques.TiO_(2)-S has a grain size of 19.32 nm.The surface morphology of the GPE/TiO_(2)-S nanocomposite shows a good,intact,and tightly porous structure with TiO_(2)-S covers the graphene surface.The content of optimized GPE/TiO_(2)-S electrodes is 41.5%of graphene,37.8%of TiO_(2),and 12.4%of sulfur that was prepared by mixing 1 g of TiO_(2)-S with 0.5 g of graphene and 0.3 mL paraffin.The GPE/TiO_(2)-S electrode produces a high anodic current(I_(pa))of 800μA and a high cathodic current(I_(pc))of-600μA at a scan rate of 0.1 V·s^(-1)using an electrolyte0.01 mol·L^(-1)K_3[Fe(CN)_6]solution containing 150 mg·L^(-1)formaldehyde.The limit of detection can reach as low as 9.7 mg·L^(-1)with stability with Horwitz ratio value as low as 0.397.The composite electrode also exhibits excellent slectivity properties by showing clear formaldehyde sugnal in the presence of high concentration of interfering agent.GPE/TiO_(2)-S electrode should find potential application of formaldehyde detection in food industries.
基金supported by the Australian Research Council Centre of Excellence Project in Optical Microcombs for Breakthrough Science(No.CE230100006)the Australian Research Council Discovery Projects Programs(Nos.P190103186 and FT210100806)+4 种基金Linkage Program(Nos.LP210200345 and LP210100467)the Swinburne ECR-SUPRA program,the Industrial Transformation Training Centres scheme(No.IC180100005)the National Natural Science Foundation of China(No.12404375)the Beijing Natural Science Foundation(No.Z180007)the Innovation Program for Quantum Science and Technology(No.2021ZD0300703).
文摘Optical polarizers,which allow the transmission of specific polarization states,are essential components in modern optical systems.Here,we experimentally demonstrate integrated photonic polarizers incorporating reduced graphene oxide(rGO)films.2D graphene oxide(GO)films are integrated onto silicon waveguides and microring resonators(MRRs)with precise control over their thicknesses and sizes,followed by GO reduction via two different methods including uniform thermal reduction and localized photothermal reduction.We measure devices with various lengths,thicknesses,and reduction degrees of GO films.The results show that the devices with rGO exhibit better performance than those with GO,achieving a polarization-dependent loss of~47 dB and a polarization extinction ratio of~16 dB for the hybrid waveguides and MRRs with rGO,respectively.By fitting the experimental results with theory,it is found that rGO exhibits more significant anisotropy in loss,with an anisotropy ratio over 4 times that of GO.In addition,rGO shows higher thermal stability and greater robustness to photothermal reduction than GO.These results highlight the strong potential of rGO films for implementing high-performance polarization selective devices in integrated photonic platforms.
基金supported by the National Key Research and Development Program(No.2022YFA1505800)the National Natural Science Foundation of China(No.22373092)+5 种基金CAS Project for Young Scientists in Basic Research(No.YSBR-051)China Association for Science and Technology(No.YESS20200031)the Start-up Funding of Central South University(No.502045005)Industry-University-Research Cooperation Projects with Zhejiang NHU Co.,Ltd.Ningbo Fengcheng Advanced Energy Materials Research Institutesupported by USTC Tang Scholarship。
文摘Manipulating catalyst structures to control product selectivity while maintaining high activity presents a considerable challenge in CO_(2)hydrogenation.Combining density functional theory calculations and microkinetic analysis,we proposed that graphene-supported isolated Pt atoms(Pt1/graphene)and Pt_(2)dimers(Pt_(2)/graphene)exhibited distinct selectivity in CO_(2)hydrogenation.Pt_(1)/graphene facilitated the conversion of CO_(2)into formic acid,whereas Pt_(2)/graphene favored methanol generation.The variation in product selectivity arose from the synergistic interaction of Pt_(2)dimers,which facilitated the migration of H atoms between two Pt atoms and promoted the transformation from*COOH intermediates to*C(OH)_(2)intermediates,altering the reaction pathways compared to isolated Pt atoms.Additionally,an analysis of the catalytic activities of three Pt_(1)/graphene and three Pt_(2)/graphene structures revealed that the turnover frequencies for formic acid generation on Pt_(1ii)/graphene and methanol generation on Pt_(2i)/graphene were as high as 744.48 h-1and 789.48 h^(-1),respectively.These values rivaled or even surpassed those previously reported in the literature under identical conditions.This study provides valuable insights into optimizing catalyst structures to achieve desired products in CO_(2)hydrogenation.
基金supported by the China Inner Mongolia Autonomous Region Directly-Undergraduate Universities Basic Research Business Fund Project:‘Environmental Protection Equipment R&D’Shared Technology and Skills Innovation Platform Construction(Grant No.NJDYWF2301).
文摘Ultrasound is a powerful tool in materials processing,yet its application in constructing van der Waals(vdW)heterostructures remains under-explored.In this study,MoS_(2)and graphene—two widely studied 2D materials—were successfully assembled into vdW heterostructures via a convenient ultrasound-driven self-assembly approach.The morphology of the heterostructures was characterized by scanning electron microscopy(SEM),while their structural and compositional features were confirmed through x-ray diffraction(XRD),Raman spectroscopy,and x-ray photoelectron spectroscopy(XPS).Red-shifted Raman peaks and decreased binding energies in XPS spectra provided strong evidence of successful heterostructure formation.A three-stage assembly mechanism—comprising dispersion,assembly,and adjustment—is proposed,with acoustic cavitation playing a key role in driving the process.This study not only demonstrates the feasibility of synthesizing 2D heterostructures via an ultrasonic route but also lays a foundation for future scalable,energy-efficient fabrication strategies.
基金Natural Science Foundation of Guangdong Province(No.2024A1515011094(C.Q Sun))National Natural Science Foundation of China(Nos.12304243(H.X.Fang),12150100(B.Wang))is gratefully acknowledged。
文摘Charge-neutral method(CNM)is extensively used in investigating the performance of catalysts and the mechanism of N_(2)electrochemical reduction(NRR).However,disparities remain between the predicted potentials required for NRR by the CNM methods and those observed experimentally,as the CNM method neglects the charge effect from the electrode potential.To address this issue,we employed the constant electrode potential(CEP)method to screen atomic transition metal-N-graphene(M_(1)/N-graphene)as NRR electrocatalysts and systematically investigated the underlying catalytic mechanism.Among eight types of M_(1)/N-graphene(M_(1)=Mo,W,Fe,Re,Ni,Co,V,Cr),W_(1)/N-graphene emerges as the most promising NRR electrocatalyst with a limiting potential as low as−0.13 V.Additionally,the W_(1)/N-graphene system consistently maintains a positive charge during the reaction due to its Fermi level being higher than that of the electrode.These results better match with the actual circumstances compared to those calculated by conventional CNM method.Thus,our work not only develops a promising electrocatalyst for NRR but also deepens the understanding of the intrinsic electrocatalytic mechanism.
基金Guangzhou (China) government postdoctoral program for providing financial support to conduct this worksupport from the National Natural Science Foundation of China (No. 72140008)funding from the European Union’s Horizon 2020 Research and Innovation program under grant agreement No. 101022484。
文摘Graphene has enormous potential to capture CO_(2)due to its unique properties and cost-effectiveness.However,graphene-based adsorbents have drawbacks of lower CO_(2)adsorption capacity and poor selectivity.This work demonstrates a one-step rapid and sustainable N_(2)/H_(2)plasma treatment process to prepare graphene-based sorbent material with enhanced CO_(2)adsorption performance.Plasma treatment directly enriches amine species,increases surface area,and improves textural properties.The CO_(2)adsorption capacity increases from 1.6 to 3.3 mmol/g for capturing flue gas,and from 0.14 to 1.3 mmol/g for direct air capture (DAC).Importantly,the electrothermal property of the plasma-modified aerogels has been significantly improved,resulting in faster heating rates and significantly reducing energy consumption compared to conventional external heating for regeneration of sorbents.Modified aerogels display improved selectivity of 42 and 87 after plasma modification for 5 and 10 min,respectively.The plasma-treated aerogels display minimal loss between 17%and 19% in capacity after 40 adsorption/desorption cycles,rendering excellent stability.The N_(2)/H_(2)plasma treatment of adsorbent materials would lower energy expenses and prevent negative effects on the global economy caused by climate change.
文摘The production of hydrogen peroxide(H_(2)O_(2))via artificial photosynthesis using single-atom semiconductor photocatalysts represents a promising green and sustainable technology.However,its efficiency is still limited by sluggish water oxidation kinetics,poor photogenerated charge separation,and insufficient O_(2)adsorption and activation capabilities.Herein,uniformly dispersed single-atom catalysts(SACs)with a Co-N_(4)coordination structure have been synthesized by thermally transforming cobalt phthalocyanine(CoPc)assemblies pre-anchored on phosphate functionalized reduced graphene oxide(Co@rGO-P),and then used to construct heterojunctions with perylenetetracarboxylic acid(PTA)nanosheets for photocatalytic H_(2)O_(2)production by an in-situ growth method.The optimized Co@rGO-P/PTA achieved an H_(2)O_(2)production rate of 1.4 mmol g^(-1)h^(-1)in pure water,with a 12.9-fold enhancement compared to pristine PTA nanosheets exhibiting competitive photoactivity among reported perylene-based materials.Femtosecond transient absorption spectra,in-situ diffuse reflectance infrared Fourier transform spectra and theoretical calculations reveal that the exceptional performance is attributed to the enhanced electron transfer from PTA to rGO via the phosphate bridge and then to the Co-N_(4),and to the promoted O_(2)adsorption and activation at Co-N_(4)active sites.This work provides a feasible and effective strategy for designing highly efficient single-atom semiconductor heterojunction photocatalysts for H_(2)O_(2)production.
基金financially supported by the National Natural Science Foundation of China (No. 21273080)Guangdong Natural Science Foundation (No. 2014A030311039)
文摘In this study, a new facile preparation method of nanocomposites consisting of graphene oxide and manganese dioxide nanowires（GO/MnO2 NWs） was developed. The morphology, structure and composition of the resulted products were characterized by transmission electron microscopy, X-ray diffraction and N2 adsorption and desorption. The GO/MnO2 nanocomposite was used as an electrode material for non-enzymatic determination of hydrogen peroxide. The proposed sensor exhibits excellent electrocatalytic performance for the determination of hydrogen peroxide in phosphate buffer solution（PBS, pH7） at an applied potential of 0.75 V. The non-enzymatic biosensor for determination of hydrogen peroxide displayed a wide linear range of 4.90 mmol L^-1–4.50 mmol L^-1with a correlation coefficient of 0.9992, a low detection limit of 0.48 mmol L^-1 and a high sensitivity of 191.22μA（mmol L^-1）^-1cm^-2（signal/noise, S/N = 3）. Moreover, the non-enzymatic biosensor shows an excellent selectivity.
基金supported by National Natural Science Foundation of China(Nos.52307239,52102300,52207234)the Natural Science Foundation of Hubei Province(Nos.2022CFB1003,2021CFA025).
文摘Conversion-type anode materials are highly desirable for Na-ion batteries(NIBs)due to their high theoretical capacity.Nevertheless,the active materials undergo severe expansion and pulverization during the sodiation,resulting in inferior cycling stability.Herein,a self-supporting three-dimensional(3D)graphene sponge decorated with Fe_(2)O_(3)nanocubes(rGO@Fe_(2)O_(3))is constructed.Specifically,the 3D graphene sponge with resilience and high porosity benefits to accommodate the volume expansion of the Fe_(2)O_(3)nanocubes and facilitates the rapid electrons/ions transport,enabling spatial confinement to achieve outstanding results.Besides,the free-standing rGO@Fe_(2)O_(3)can be directly used as an electrode without additional binders and conductive additives,which helps to obtain a higher energy density.Based on the total mass of the rGO@Fe_(2)O_(3)material,the rGO@Fe_(2)O_(3)anode presents a specific capacity of 859 mAh/g at 0.1 A/g.It also delivers an impressive cycling performance(327 mAh/g after 2000 cycles at 1 A/g)and a superior rate capacity(162mAh/g at 20 A/g).The coin-type Na_(3)V_(2)(PO_(4))_(3)@C//rGO@Fe_(2)O_(3)NIB exhibits an energy density of 265.3Wh/kg.This unique 3D ionic/electronic conductive network may provide new strategies to design advanced conversion-type anode materials for high-performance NIBs.
基金Funded by the National Natural Science Foundation of China(No.51972242)the National College Students'Innovation and Entrepreneurship Training Program(No.202210488020)+2 种基金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(No.KF-20-5)the Research Project of Yingcheng Xinjincheng Environmental Protection Technology Co.,Ltd(No.2023420612000754)the Program(No.BG20210227001)of High-end Foreign Experts of the State of the State Administration of Foreign Experts Affairs(SAFEA)。
文摘In this study,the holey graphene was prepared by microwave-assisted chemical etching.The three-dimensional(3D)holey graphene hydrogel was obtained through hydrothermal self-assembly method,followed by the introduction of FeCo_(2)S_(4)particles.The resulting holey graphene hydrogel,characterized by high specific surface area and abundant pores combined with FeCo_(2)S_(4)with high pseudocapacitance by interfacial interaction,shortened the mass transport path and enhanced the specific capacitance.The findings reveal that the holey graphene hydrogel/FeCo_(2)S_(4)(FeCo_(2)S_(4)/HGH)composite exhibits high specific capacitance and impressive rate capability(413.4 F·g^(-1)at 1 A·g^(-1),300.4 F·g^(-1)at 6 A·g^(-1)).The symmetric supercapacitor operated within a stable potential window of 0.1-1.6 V,achieving specific capacitance of 127.5 F·g^(-1)at 1 A·g^(-1),and can deliver 37.1 Wh·kg^(-1)at a power density of 1499 W·kg^(-1).Besides,under the current density of 3 A·g^(-1),the supercapacitor retained 90.8%of its capacitance after 5000 cycles,demonstrating exceptional cycle stability.This study presents an efficient method for fabricating advanced integrated supercapacitors electrodes with enhanced energy density.
基金National Natural Science Foundation of China(Nos.12075152,42177405,12075147)for the financial support。
文摘The photo-assisted Fenton-like method is an effective and sustainable way to remove organic pollutants from water.Herein,a series of three-dimensional composites containing MIL-88A(Fe)-derived α-Fe_(2)O_(3)and graphene aerogel(GA-Fe-X)were designed and used as catalysts to degrade ciprofloxacin(CIP)by peroxymonosulfate(PMS)activated photo-Fenton-like technology.The as-prepared GA-Fe-1 displayed remarkable enhancement with a CIP degradation rate constant(0.017 min^(-1))higher than that of graphene aerogel(0.0031 min^(-1))and MIL-88A(Fe)(0.0039 min^(-1)).Experimental results demonstrated that the combination of MIL-88A(Fe)-derived α-Fe_(2)O_(3)and graphene aerogel forming GA-Fe-X enhanced the separation efficiency of electron-hole pairs,activating PMS to produce SO_(4)^(·-),^(·)OH and ^(1)O_(2) for enhanced CIP degradation through radical and non-radical pathways.The factors affecting CIP degradation during the photoFenton-like process were thoroughly investigated.The possible CIP degradation pathways and ecotoxicity of the intermediates were also analyzed.This work enhances our understanding of the photo-Fenton-like effect in three-dimensional graphene aerogel composites.
基金supported by the National Natural Science Foundation of China(22278347)the Excellent Doctoral Student Research Innovation Project of Xinjiang University of China(XJU2022BS048)the Postgraduate Innovation Project of Xinjiang Uygur Autonomous Region of China(XJ2023G027).
文摘Low-cost Fe-based disordered rock salt(DRX)Li_(2)FeTiO_(4)is capable of providing high capacity(295 mA h g^(-1))by redox activity of cations(Fe^(2+)/Fe^(4+)and Ti^(3+)/Ti^(4+))and anionic oxygen.However,DRX structures lack transport channels for ions and electrons,resulting in sluggish kinetics,poor electrochemical activity,and cyclability.Herein,graphene conductive carbon network permeated Li_(2)FeTiO_(4)(LFT/C/G)nanofibers are successfully prepared by a facile sol-gel assisted electrospinning method.Ultrafine Li_(2)FeTiO_(4)nanoparticles(2 nm)and one-dimensional(1D)structure provide abu ndant active sites and unobstructed diffu sion channels,accelerating ion diffusion.In addition,introducing graphene reduces the band gap and Li^(+)diffusion barrier and improves the dynamic properties of Li_(2)FeTiO_(4),thus achieving a relatively mild interfacial reaction and reversible redox reaction.As expected,the LFT/C/1.0G cathode delivers a remarkable discharge capacity(238.5 mA h g^(-1)),high energy density(508.8 Wh kg^(-1)),and excellent rate capability(51.2 mA hg^(-1)at 1.0 A g^(-1)).Besides,the LFT/C/1.0G anode also displays a high capacity(514.5 mA h g^(-1)at 500 mA g^(-1))and a remarkable rate capability(243.9 mA h g^(-1)at 8 A g^(-1)).Moreover,the full batteries based on the LFT/C/1.0G symmetric electrode demonstrate a reversible capacity of 117.0 mA h g^(-1)after 100 cycles at 50 mA g^(-1).This study presents useful insights into developing cost-effective DRX cathodes with durable and fast lithium storage.
基金financially supported by National Natural Science Foundation of China(No.21906084)the National Undergraduate Training Program for Innovation and Entrepreneurship(No.202010288026Z)。
文摘Formaldehyde(HCHO)causes increasing concerns due to its ubiquitously found in indoor air and being irritative and carcinogenic to humans.Photothermal-catalysis developed in recent years has been considered as a significant strategy for enhancing catalytic activity.Manganese oxides,compared with its strong thermocatalytic activity,generally suffer from much lower photocatalytic activity make its photochemical properties less concerned.Herein,α-MnO_(2)nanowires were composited with the graphene oxide(GO)via mechanical grinding and co-precipitating method,respectively.α-MnO_(2)/GO nanohybrids prepared by co-precipitating method exhibits excellent activity,achieving 100%decomposition of HCHO with the solar-light irradiation at ambient temperature.It is found that,besides the photo-driven thermocatalysis,the photocatalysis mechanism made a major contribution to the decomposition of HCHO.The incorporation of GO,on the one hand,is beneficial to improve the optical absorption capacity and photothermal conversion efficiency;on the other hand,is conductive to electron transfer and effective separation of electrons and holes.These synergistic effects significantly improve the catalytic activity ofα-MnO_(2)/GO nanohybrids.This work proposes a new approach for the utilization of solar energy by combining manganese oxides,and also develops an efficient photothermal-catalyst to control HCHO pollution in indoor air.
