CO_(2) conversion to CO via the reverse water-gas shift(RWGS)reaction is limited by a low CO_(2) conversion rate and CO selectivity.Herein,an efficient RWGS catalyst is constructed through Enteromorpha prolifera–deri...CO_(2) conversion to CO via the reverse water-gas shift(RWGS)reaction is limited by a low CO_(2) conversion rate and CO selectivity.Herein,an efficient RWGS catalyst is constructed through Enteromorpha prolifera–derived N-rich mesoporous biochar(EPBC)supported atomic-level Cu-Mo_(2)C clusters(Cu-Mo_(2)C/EPBC).Unlike traditional acti-vated carbon(AC)supported Cu-Mo_(2)C particles(Cu-Mo_(2)C/AC),the Cu-Mo_(2)C/EPBC not only presents the better graphitization degree and larger specific surface area,but also uniformly andfirmly anchors atomic-level Cu-Mo_(2)C clusters due to the existence of pyridine nitrogen.Furthermore,the pyridine N of Cu-Mo_(2)C/EPBC strengthens an unblocked electron transfer between Mo_(2)C and Cu clusters,as verified by X-ray absorption spectroscopy.As a result,the synergistic effect between pyridinic N anchoring and the clusters interaction in Cu-Mo_(2)C/EPBC facilitates an improved CO selectivity of 99.95%at 500℃ compared with traditional Cu-Mo_(2)C/AC(99.60%),as well as about 3-fold CO_(2) conversion rate.Density functional theory calculations confirm that pyr-idine N-modified carbon activates the local electronic redistribution at Cu-Mo_(2)C clusters,which contributes to the decreased energy barrier of the transition state of CO^(*)+O^(*)+2H^(*),thereby triggering the transformation of rate-limited step during the redox pathway.This biomass-derived strategy opens perspective on producing sustain-able fuels and building blocks through the RWGS reaction.展开更多
Heterojunctions constructed by traditional methods often result in random stacking of materials, leading to lattice mismatch, which adversely affects the extraction and transfer of photo-generated carriers and, in tur...Heterojunctions constructed by traditional methods often result in random stacking of materials, leading to lattice mismatch, which adversely affects the extraction and transfer of photo-generated carriers and, in turn, hampers light utilization efficiency. In this work, we report a novel heterojunction comprising alternating S-doped g-C_(3)N_(4) (SCN) and N-doped MoS_(2) (NMS), bridged by Mo–N covalent bonds within hierarchical periodic macroporous (HPM) walls. This heterojunction is synthesized by co-pyrolyzing dicyandiamide, thiourea, and ammonium molybdate. Transient reflectance photoluminescence measurements reveal that the Mo–N covalent bonds serve as “fast tracks” for electron transfer from SCN to NMS, significantly enhancing the charge separation efficiency. Additionally, the well-defined spatial separation of photo-induced carriers, coupled with the efficient mass transfer within the HPM structure, promotes superior carrier utilization. Thanks to the synergistic effect of HPM structures and the bridged Mo–N bonds, the optimized HPM NMS/SCN-1.3 sample exhibits a remarkable H_(2) evolution rate of 473.3 µmol g^(−1) h^(−1) under visible light irradiation, which is approximately 163 and 19 times higher than bulk g-C_(3)N_(4) (BCN) and HPM SCN, respectively. This work offers valuable insights into the design of HPM heterojunctions composed of co-catalysts and host catalysts, paving the way for enhanced photocatalytic H₂ evolution.展开更多
The electrochemical reduction of carbon dioxide(CO_(2)RR)is a promising strategy for achieving carbon neutralization.The Ni-N_(4) site is well known as the active site in metal single atoms on N-doped carbon catalysts...The electrochemical reduction of carbon dioxide(CO_(2)RR)is a promising strategy for achieving carbon neutralization.The Ni-N_(4) site is well known as the active site in metal single atoms on N-doped carbon catalysts,while its symmetric charge distribution nature is not favorable for electron transfer and then hindering the efficient CO_(2)RR.Herein,we constructed a Ni SA/CNs single-atom catalyst.Notably,it features unique Ni-N_(4)-O active sites,featuring one axial O atom and four planar N atoms,constituting a broken symmetrical electronic structure of Ni-N_(4) sites.Furthermore,hierarchical pore structures were obtained with the assistance of NaNO_(3) pore-forming agent during thermal treatment process,which promote electronic and mass transfer.And the resulting high specific surface area can host more Ni-N_(4)-O active sites.These specialized active sites promote the key intermediate(∗CO)adsorption/desorption and suppresses hydrogen evolution.Consequently,the Ni SA/CNs catalyst exhibits a high turnover frequency(TOF)value,reaching 34,081 h^(-1) at-0.98 V vs.RHE.Additionally,it achieves an excellent CO Faradaic efficiency,exceeding 90%,over a wide potential range from-0.4 V to-1.0 V vs.RHE.This work not only offers a new method for the rational synthesize single-atom catalysts with unique Ni-N_(4)-O active sites,but also provides in-depth insight into the origin of catalytic activity of porous carbon-base catalysts.展开更多
A visible-light photocatalyst was prepared by calcination of the hydrolysis product of Ti(SO_4)_2 with ammonia as precipitator. The color of this photocatalyst was vivid yellow. It could absorb light under 550 nm wave...A visible-light photocatalyst was prepared by calcination of the hydrolysis product of Ti(SO_4)_2 with ammonia as precipitator. The color of this photocatalyst was vivid yellow. It could absorb light under 550 nm wavelength. The crystal structure of anatase was characterized by XRD. The structure analysis result of X-ray fluorescence(XRF) shows that doped-nitrogen was presented in the sample. The photocatalytic activities were evaluated using methyl orange and phenol as model pollutants. The photocatalytic activities of samples were increasing gradually with calcination temperature from 400℃ to 700℃ under UV irradiation. It can be seen that the degradation of methyl orange follows zero-order kinetics. However, the calcination temperatures have no significant influence on the degradation of phenol under sunlight. The N-doped catalyst shows higher activity than the bare one under solar irradiation.展开更多
We developed a novel approach for the preparation of N-doped TiO2 photocatalysts by calcining ammonium titanium oxalate at different temperatures. The structures of N-TiO2 were characterized by powder X-ray diffractio...We developed a novel approach for the preparation of N-doped TiO2 photocatalysts by calcining ammonium titanium oxalate at different temperatures. The structures of N-TiO2 were characterized by powder X-ray diffraction, infrared spectroscopy, thermogravimetric analysis, N2 adsorption-desorption isotherms, X-ray photoelectron spectroscopy, diffuse reflectance UV-Vis spectroscopy, and scanning electron microscope. The N-doped TiO2 photocatalysts calcined below 700 ℃ are the pure anatase phase but that calcined at 700 ℃ is a mixture of anatase and rutile phases. The doped N locates at the interstitial site of TiO2 which leads to the narrowing of bad gap of pure anatase N-TiO2. Among all photocatalysts, N-TiO2 photocatalysts calcined at 600 and 400 ℃ exhibit the best performance in the photodegradation of methyl orange under the UV light and all-wavelength light illuminations, respectively; however, because of the perfect crystallinity and the existence of anatase-rutile phase junctions, N-TiO2 photocatalyst calcined at 700 ℃ exhibits the highest specific photodegradation rate, i.e., the highest quantum yield, under both the UV light and all-wavelength light illuminations.展开更多
Developing high-performance anodes for potassium ion batteries(KIBs) is of paramount significance but remains challenging.In the normal sense,electrode materials are prepared by ubiquitous wet chemical routes,which ot...Developing high-performance anodes for potassium ion batteries(KIBs) is of paramount significance but remains challenging.In the normal sense,electrode materials are prepared by ubiquitous wet chemical routes,which otherwise might not be versatile enough to create desired heterostructures and/or form clean interfacial areas for fast transport of K-ions and electrons.Along this line,rate capability/cycling stability of resulting KIBs are greatly handicapped.Herein we present an all-chemical vapor deposition approach to harness the direct synthesis of nitrogen-doped graphene(NG)/rhenium diselenide(ReSe_2)hybrids over three-dimensional MXene supports as superior heterostructure anode material for KIBs.In such an innovative design,1 T'-ReSe2 nanoparticles are sandwiched in between the NG coatings and MXene frameworks via strong interfacial interactions,thereby affording facile K~+ diffusion,enhancing overall conductivity,boosting high-power performance and reinforcing structural stability of electrodes.Thus-constructed anode delivers an excellent rate performance of 138 mAh g^(-1) at 10.0 A g^(-1) and a high reversible capacity of 90 mAh g^(-1) at 5 A g^(-1) after 300 cycles.Furthermore,the potassium storage mechanism has been systematically probed by advanced in situlex situ characterization techniques in combination with first principles computations.展开更多
Photocatalysis based on semiconductors has recently been receiving considerable research interest because of its extensive applications in environmental remediation and renewable energy generation.Various semiconducto...Photocatalysis based on semiconductors has recently been receiving considerable research interest because of its extensive applications in environmental remediation and renewable energy generation.Various semiconductor-based materials that are vital to solar energy utilization have been extensively investigated,among which titanium oxide(TiO_(2))has attracted considerable attention because of its exceptional physicochemical characteristics.However,the sluggish responsiveness to visible light in the solar spectrum and the inefficient separation of photoinduced electron-hole pairs hamper the practical application of TiO_(2) materials.To overcome the aforementioned serious drawbacks of TiO_(2),numerous strategies,such as doping with foreign atoms,particularly nitrogen(N),have been improved in the past few decades.This review aims to provide a comprehensive update and description of the recent developments of N-doped TiO_(2) materials for visible lightresponsive photocatalysis,such as(1)the preparation of N-doped/co-doped TiO_(2) photocatalysts and(2)mechanistic studies on the reasons for visible light response.Furthermore,the most recent and significant advances in the field of solar energy applications of modified N-doped TiO_(2) are summarized.The analysis indicated the critical need for further development of these types of materials for the solar-to-energy conversion,particularly for water splitting purposes.展开更多
With great superiorities in energy density,rate capability and structural stability,Na_(3)V_(2)(PO_(4))_(2) F_(3)(NVPF)has attracted much attentions as cathode of sodium ion battery(SIB),but it also faces challenges o...With great superiorities in energy density,rate capability and structural stability,Na_(3)V_(2)(PO_(4))_(2) F_(3)(NVPF)has attracted much attentions as cathode of sodium ion battery(SIB),but it also faces challenges on its poor intrinsic electronic conductivity and the controversial de/sodiation mechanism.Herein,a series of Zr-doped NVPF coated by N-doped carbon layer(~5 nm in thickness,homogenously)materials are fabricated by a sol-gel method,and the optimized heteroatom-doping amounts of Zr and N doping improve intrinsic properties on enlarging lattice distance and enhancing electronic conductivity,respectively.Specifically,among all samples of Na_(3) V_(2-x)Zr_(x)(PO_(4))_(2) F_(3)/NC(NVPF-Zr-x/NC,x=0,0.01,0.02,0.05,and 0.1),the optimized electrode of NVPF-Zr-0.02/NC delivers high reversible capacities(119.2 mAh g^(-1) at0.5 C),superior rate capability(98.1 mA h g^(-1) at 20 C)and excellent cycling performance.The structural evolution of NVPF-Zr-0.02/NC electrode,in-situ monitored by X-ray diffractometer,follows a step-wise Na-extraction/intercalation mechanism with reversible multi-phase changes,not just a solid-solutionreaction one.Full cells of NVPF-Zr-0.02/NC//hard carbon demonstrate high capacity(99.8 mA h g^(-1) at 0.5 C),high out-put voltage(3.5 V)and good cycling stability.This work is favorable to accelerate the development of high-performance cathode materials and explore possible redox reaction mechanisms of SIBs.展开更多
N-doped coaxial CNTs@α-Fe_2O_3@C nanofibers have been successfully synthesized according to a facile solvothermal/hydrothermal method. The obtained CNTs@α-Fe_2O_3@C nanofibers composites exhibited spe- cial three-di...N-doped coaxial CNTs@α-Fe_2O_3@C nanofibers have been successfully synthesized according to a facile solvothermal/hydrothermal method. The obtained CNTs@α-Fe_2O_3@C nanofibers composites exhibited spe- cial three-dimensional （3-D） network structure, which endows they promising candidate for anode ma- terials of lithium ion battery. The coaxial property of CNTs@α-Fe_2O_3@C nanofibers could significantly improve the cycling and rate performance owing to the acceleration of charge/electron transfer, improve- ment of conductivity, maintaining of structural integrity and inhibiting the aggregation. The α-Fe_2O_3 nanoparticles with small size and high percentage of N-doped amount could further improve the elec- trochemical performance. As for the CNTs@α-Fe_2O_3@C nanofibers, the capacity presented a high value of 1255.4 mAh/g at 0.1 C, and retained at 1213.4 mAh/g after 60 cycles. Even at high rate of 5 C, the ca- pacity still exhibited as high as 319 mAh/g. The results indicated that the synthesized N-doped coaxial CNTs@α-Fe_2O_3@C nanofibers exhibited high cvcling and rate oerformance.展开更多
The conversion of carbon dioxide into valuable organic compounds is a highly promising approach to address the energy issues and environmental problems(e.g., global warming). Herein, we presents a facile and efficient...The conversion of carbon dioxide into valuable organic compounds is a highly promising approach to address the energy issues and environmental problems(e.g., global warming). Herein, we presents a facile and efficient method to prepare highly dense and well-dispersed SnO2 nanocrystals on 1 D N-doped carbon nanowires as advanced catalysts for the efficient electroreduction of CO2 to formate. The ultrasmall SnO2 coated on the N-doped carbon nanowires(SnO2@N-CNW) has been synthesized via the simple hydrothermal treatment coupled with a pyrolysis process. The unique structure enables to expose the active tin oxide and also provides the facile pathways for rapid transfer of electron and electrolyte along with the highly porous carbon foam composed with interconnected carbon nanowires. Therefore, SnO2@NCNW electrocatalyst exhibits good durability and high selectivity for formate formation with a Faradaic efficiency of ca. 90%. This work demonstrates a simple method to rationally design high-dense tin oxide nanocrystals on the conductive carbon support as advanced catalysts for CO2 electroreduction.展开更多
Low cost,highly selective and efficient electrocatalysts for CO_(2)reduction reaction(CO_(2)RR)is crucial for lowering the global carbon footprint and mitigating energy shortages.Here,we first report a highly selectiv...Low cost,highly selective and efficient electrocatalysts for CO_(2)reduction reaction(CO_(2)RR)is crucial for lowering the global carbon footprint and mitigating energy shortages.Here,we first report a highly selective and efficient electrocatalyst for CO_(2)RR to CO using a surface-regulated Ni nanoparticles supported on N-doped CMK-3(N,O-Ni/CMK3).Compared with most Ni metal catalysts previously reported with severe competitive hydrogen evolution during the CO_(2)RR,the N,O-Ni/CMK3 catalyst presents a superior CO faradaic efficiency of about 97%,a high CO partial current density(13.01 mA cm^(-1))and turnover frequency(4.25 s^(–1)).The comprehensive characterization provides evidence that the N,O co-regulated Ni acts as the active center.Taking advantage of the N,O co-regulated chemical environment,N,O-Ni/CMK3 also displays a decent stability at negative potentials.Our work paves a novel approach for developing transition metal catalysts for CO_(2)RR with enhanced activity and selectivity via regulating surface chemical environment.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
Electromagnetic wave absorber is critical for reducing increasingly serious electromagnetic wave pollu-tion,however,the development of lightweight and broadband microwave absorbers remains a pressing challenge.We repo...Electromagnetic wave absorber is critical for reducing increasingly serious electromagnetic wave pollu-tion,however,the development of lightweight and broadband microwave absorbers remains a pressing challenge.We report here the rational design and synthesis of N-doped Ni@SiO_(2)/graphene composite con-structed from 3D interconnected porous graphene network and Ni@SiO_(2) core-shell architecture,which fulfills lightweight and broadband requirements while exhibiting highly efficient electromagnetic wave absorption.The porous graphene network,functioning both as lightweight support and dielectric medi-ator,was synthesized via NaCl template-assisted high-temperature calcination method.Upon uniformly attached with core-shell Ni@SiO_(2) on the surface,the resulting abundant heterogeneous interfaces con-structed by graphene-Ni and Ni-SiO_(2) strongly reinforce polarization loss.The presence of low dielectric SiO_(2) allows facile tuning of the complex permittivity of ternary composite by adjusting coating thick-ness to balance the attenuation ability and impedance matching.Moreover,further N-doping of graphene assists in the optimization of dielectric loss ability.Taking account of the advantages arising from the porous hierarchical architecture,multiple absorption centers and diverse interfaces,the lightweight com-posite exhibits an ultra-strong reflection loss(RL)value of-71.13 dB at 13.76 GHz with a thickness of 2.46 mm and broad effective absorption bandwidth of 7.04 GHz at a low filler content of 15 wt.%.More importantly,the effective absorption range covers 13.28 GHz(4.72-18 GHz)with the optimized thickness of 1.6-5 mm,representing 83%of the whole range of frequencies.Our results demonstrate that the novel 3D porous N-doped Ni@SiO_(2)/graphene network with hierarchical architecture is a promising candidate for high-performance electromagnetic wave absorption.展开更多
Orthorhombic-phase Nb_(2)O_(5)(T-Nb_(2)O_(5)) has been widely investigated as an intercalation anode material for Li-ion batteries due to the larger interplanar lattice spacing and high safety.However,its applications...Orthorhombic-phase Nb_(2)O_(5)(T-Nb_(2)O_(5)) has been widely investigated as an intercalation anode material for Li-ion batteries due to the larger interplanar lattice spacing and high safety.However,its applications are limited by the intrinsic low electric conductivity.Herein,an ultrathin N-doped carbon-coating layer was constructed on porous T-Nb_(2)O_(5) microspheres uniformly via a convenient thermal treatment method with ionic liquid as a carbon precursor.The synthesized T-Nb_(2)O_(5)@N-C exhibits significantly enhanced rate capability(155.5 mAh·g^(-1) at 20 C) than initial T-Nb_(2)O_(5)(110.2 mAh·g^(-1) at 20C).Besides,T-Nb_(2)O_(5)@N-C shows ultralong cycle life,with only a 0.02% decrease in the capacity per cycle at a high current density of 10 C.The corresponding electrochemical tests show that the preferable rate capability of T-Nb_(2)O_(5)@N-C electrode is attributed to the increased electronic conductivity and pseudocapacitance contribution induced by ultrathin surface N-doped carbon layer.On the other hand,the mesoporous structure of T-Nb_(2)O_(5)@N-C ensures fast Li+ diffusion dynamics and electrolyte penetration.Furthermore,T-Nb_(2)O_(5)@N-C also performs well in a LiNi_(0.5)Mn_(0.3)Co_(0.2)O_(4) llT-Nb_(2)O_(5)@N-C full cell.This work provides a facile method to construct integrated anode materials for potential applications in lithium-ion batteries.展开更多
Metal organic framework(MOF) has been confirmed as the promising precursor to develop the conve rsion-typed anode mate rials of sodium-ion batteries(SIBs) because of the tunable structure design and simple functional ...Metal organic framework(MOF) has been confirmed as the promising precursor to develop the conve rsion-typed anode mate rials of sodium-ion batteries(SIBs) because of the tunable structure design and simple functional modification.Here,we prepare the ultrasmall Ni_(3)S_(2) nanocrystals embedded into N-doped porous carbon nanoparticles using the scalable Ni-MOF as precursor(denoted as Ni_(3)S_(2)@NPC).The ultrasmall size of Ni_(3)S_(2) can work for accelerated electro n/ion transfer to facilitate the electrochemical reaction kinetics.Moreover,the robust conductivity network originated from N-doped porous carbon nanoparticles can not only improve the electron conductivity,but also enhance the electrode integrity and stability of the electrode/electrolyte interface.In addition,the N heteroatoms provide extra Na storage sites.Accordingly,the electrode delivers the obviously competitive capacities and high-power output with respect to the currently reported Ni_(3)S_(2)/C composites.This study provides a scalable and universal strategy to develop the advanced transition metal sulfides for practically feasible SIBs.展开更多
The exploitation of multifunctional nanocomposites is highly desired in environmental monitoring,biosensors,and medical diagnosis.In this paper,a simple approach has been proposed to fabricate MoS2 decorated N-doped c...The exploitation of multifunctional nanocomposites is highly desired in environmental monitoring,biosensors,and medical diagnosis.In this paper,a simple approach has been proposed to fabricate MoS2 decorated N-doped carbon nanotubes(NCNTs@MoS2)hybrid composites as efficient peroxidase-like mimics.The combination of the MoS2 and N-doped carbon nanotubes(NCNTs)brings about an enhanced synergistic effect,leading to remarkably decent intrinsic peroxidase-mimic activities than that of the single components.Due to the high catalytic efficiency of the resultant NCNTs@MoS2 hybrid nanotubes as peroxidase-like mimics,a co nvenient colorimetric approach for the sensitive determination of H2 O2 and ascorbic acid have been developed with a detection limit of about 0.14μmol/L and 0.12μmol/L,respectively.The work offers a new strategy for the fabrication of peroxidase-like nanomaterials with excellent catalytic activity,which indicates great promising applications in sensitive detections in real samples.展开更多
Photocatalytic CO_(2)conversion efficiency is hampered by the rapid recombination of photogenerated charge carriers.It is effective to suppress the recombination by constructing cocatalysts on photocatalysts with high...Photocatalytic CO_(2)conversion efficiency is hampered by the rapid recombination of photogenerated charge carriers.It is effective to suppress the recombination by constructing cocatalysts on photocatalysts with high-quality interfacial contact.Herein,we develop a novel strategy to in-situ grow ultrathin/V-doped graphene(NG)layer on TiO_(2) hollow spheres(HS) with large area and intimate interfacial contact via a chemical vapor deposition(CVD).The optimized TiO^(2)/NG HS nanocomposite achieves total CO_(2)conversion rates(the sum yield of CO,CH_(3)OH and CH_(4))of 18.11μmol·g^(-1)h^(-1),which is about 4.6 times higher than blank T1O_(2)HS.Experimental results demonstrate that intimate interfacial contact and abundant pyridinic N sites can effectively facilitate photogenerated charge carrier separation and transport,realizing enhanced photocatalytic CO_(2)reduction performance.In addition,this work provides an effective strategy for in-situ construction of graphene-based photocatalysts for highly efficient photocatalytic CO_(2)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 conventional Li–O2 battery(LOB)has hardly been considered as a next-generation flexible electronics thus far,since it is bulk,inflexible and limited by the absence of an adjustable cell configuration.Here,we pres...The conventional Li–O2 battery(LOB)has hardly been considered as a next-generation flexible electronics thus far,since it is bulk,inflexible and limited by the absence of an adjustable cell configuration.Here,we present a flexible Li–O2 cell using N-doped carbon nanocages grown onto the carbon textiles(NCNs/CTs)as a self-standing and binder-free O2 electrode.The highly flexible NCNs/CTs exhibits an excellent mechanic durability,a promising catalytic activity towards the ORR and OER,a considerable cyclability of more than 70 cycles with an overpotential of 0.36 V on the 1 stcycle at a constant current density of 0.2 m A/cm2,a good rate capability,a superior reversibility with formation and decomposition of desired Li2 O2,and a highly electrochemical stability even under stringent bending and twisting conditions.Our work represents a promising progress in the material development and architecture design of O2 electrode for flexible LOBs.展开更多
The development of efficient catalytic electrode toward oxygen reduction reaction(ORR)is still a great challenge for the wide use of zinc–air batteries.Herein,Co_(2)N nanoparticles(NPs)anchored on N-doped carbon from...The development of efficient catalytic electrode toward oxygen reduction reaction(ORR)is still a great challenge for the wide use of zinc–air batteries.Herein,Co_(2)N nanoparticles(NPs)anchored on N-doped carbon from cattail were verified with excellent catalytic performances for ORR.The onset and half-wave potentials over the optimal catalyst reach to 0.96 V and 0.84 V,respectively.Current retention rates of 96.8%after 22-h test and 98.8%after running 1600 s were obtained in 1 M methanol solution.Density functional theory simulation proposes an apparently increased electronic states of Co_(2)N in N-doped carbon layer close to the Fermi level.Higher charge density,favorable adsorption,and charge transfer of intermediates originate from the coexistence of Co_(2)N NPs and N atoms in carbon skeleton.The superior catalytic activity of composites also was confirmed in zinc–air batteries.This novel catalytic property and controllable preparation approach of Co_(2)Ncarbon composites provide a promising avenue to fabricate metal-containing catalytically active carbon from biomass.展开更多
基金support from National Natural Science Foundation of China(32101474 and 42377249)National Key Research and Development Program of China(2023YFD2201605).
文摘CO_(2) conversion to CO via the reverse water-gas shift(RWGS)reaction is limited by a low CO_(2) conversion rate and CO selectivity.Herein,an efficient RWGS catalyst is constructed through Enteromorpha prolifera–derived N-rich mesoporous biochar(EPBC)supported atomic-level Cu-Mo_(2)C clusters(Cu-Mo_(2)C/EPBC).Unlike traditional acti-vated carbon(AC)supported Cu-Mo_(2)C particles(Cu-Mo_(2)C/AC),the Cu-Mo_(2)C/EPBC not only presents the better graphitization degree and larger specific surface area,but also uniformly andfirmly anchors atomic-level Cu-Mo_(2)C clusters due to the existence of pyridine nitrogen.Furthermore,the pyridine N of Cu-Mo_(2)C/EPBC strengthens an unblocked electron transfer between Mo_(2)C and Cu clusters,as verified by X-ray absorption spectroscopy.As a result,the synergistic effect between pyridinic N anchoring and the clusters interaction in Cu-Mo_(2)C/EPBC facilitates an improved CO selectivity of 99.95%at 500℃ compared with traditional Cu-Mo_(2)C/AC(99.60%),as well as about 3-fold CO_(2) conversion rate.Density functional theory calculations confirm that pyr-idine N-modified carbon activates the local electronic redistribution at Cu-Mo_(2)C clusters,which contributes to the decreased energy barrier of the transition state of CO^(*)+O^(*)+2H^(*),thereby triggering the transformation of rate-limited step during the redox pathway.This biomass-derived strategy opens perspective on producing sustain-able fuels and building blocks through the RWGS reaction.
基金support of the National Natural Science Foundation of China(Nos.52174238,22378103,52204307,and 22409128)Natural Science Foundation of Changsha(No.kq2208425)the Research Foundation Bureau of Hunan Province(No.24B0787).
文摘Heterojunctions constructed by traditional methods often result in random stacking of materials, leading to lattice mismatch, which adversely affects the extraction and transfer of photo-generated carriers and, in turn, hampers light utilization efficiency. In this work, we report a novel heterojunction comprising alternating S-doped g-C_(3)N_(4) (SCN) and N-doped MoS_(2) (NMS), bridged by Mo–N covalent bonds within hierarchical periodic macroporous (HPM) walls. This heterojunction is synthesized by co-pyrolyzing dicyandiamide, thiourea, and ammonium molybdate. Transient reflectance photoluminescence measurements reveal that the Mo–N covalent bonds serve as “fast tracks” for electron transfer from SCN to NMS, significantly enhancing the charge separation efficiency. Additionally, the well-defined spatial separation of photo-induced carriers, coupled with the efficient mass transfer within the HPM structure, promotes superior carrier utilization. Thanks to the synergistic effect of HPM structures and the bridged Mo–N bonds, the optimized HPM NMS/SCN-1.3 sample exhibits a remarkable H_(2) evolution rate of 473.3 µmol g^(−1) h^(−1) under visible light irradiation, which is approximately 163 and 19 times higher than bulk g-C_(3)N_(4) (BCN) and HPM SCN, respectively. This work offers valuable insights into the design of HPM heterojunctions composed of co-catalysts and host catalysts, paving the way for enhanced photocatalytic H₂ evolution.
基金financially supported by National High-Level Talent FundNational Natural Science Foundation of China (Nos. 22372138,22461160253,22121001,and 22072118)+3 种基金thank financial support from State Key Laboratory of Physical Chemistry of Solid Surfaces of Xiamen UniversityShenzhen Science and Technology Program (No. JCYJ20220530143401002)supported by Science and Technology Projects of Innovation Laboratory for Sciences and Technologies of Energy Materials of Fujian Province (IKKEM) (No. HRTP-[2022]-3)the Fundamental Research Funds for the Central Universities (No. 20720220008)
文摘The electrochemical reduction of carbon dioxide(CO_(2)RR)is a promising strategy for achieving carbon neutralization.The Ni-N_(4) site is well known as the active site in metal single atoms on N-doped carbon catalysts,while its symmetric charge distribution nature is not favorable for electron transfer and then hindering the efficient CO_(2)RR.Herein,we constructed a Ni SA/CNs single-atom catalyst.Notably,it features unique Ni-N_(4)-O active sites,featuring one axial O atom and four planar N atoms,constituting a broken symmetrical electronic structure of Ni-N_(4) sites.Furthermore,hierarchical pore structures were obtained with the assistance of NaNO_(3) pore-forming agent during thermal treatment process,which promote electronic and mass transfer.And the resulting high specific surface area can host more Ni-N_(4)-O active sites.These specialized active sites promote the key intermediate(∗CO)adsorption/desorption and suppresses hydrogen evolution.Consequently,the Ni SA/CNs catalyst exhibits a high turnover frequency(TOF)value,reaching 34,081 h^(-1) at-0.98 V vs.RHE.Additionally,it achieves an excellent CO Faradaic efficiency,exceeding 90%,over a wide potential range from-0.4 V to-1.0 V vs.RHE.This work not only offers a new method for the rational synthesize single-atom catalysts with unique Ni-N_(4)-O active sites,but also provides in-depth insight into the origin of catalytic activity of porous carbon-base catalysts.
文摘A visible-light photocatalyst was prepared by calcination of the hydrolysis product of Ti(SO_4)_2 with ammonia as precipitator. The color of this photocatalyst was vivid yellow. It could absorb light under 550 nm wavelength. The crystal structure of anatase was characterized by XRD. The structure analysis result of X-ray fluorescence(XRF) shows that doped-nitrogen was presented in the sample. The photocatalytic activities were evaluated using methyl orange and phenol as model pollutants. The photocatalytic activities of samples were increasing gradually with calcination temperature from 400℃ to 700℃ under UV irradiation. It can be seen that the degradation of methyl orange follows zero-order kinetics. However, the calcination temperatures have no significant influence on the degradation of phenol under sunlight. The N-doped catalyst shows higher activity than the bare one under solar irradiation.
基金ACKNOWLEDGMENTS This work was supported by the National Natural Science Foundation of China （No.20773113）, the Solar Energy Project of Chinese Academy of Sciences, the Ministry of Education program for PCSIRT （No.IRT0756）, and the Max Planck Gesellschaft of Chinese Academy of Sciences partner group.
文摘We developed a novel approach for the preparation of N-doped TiO2 photocatalysts by calcining ammonium titanium oxalate at different temperatures. The structures of N-TiO2 were characterized by powder X-ray diffraction, infrared spectroscopy, thermogravimetric analysis, N2 adsorption-desorption isotherms, X-ray photoelectron spectroscopy, diffuse reflectance UV-Vis spectroscopy, and scanning electron microscope. The N-doped TiO2 photocatalysts calcined below 700 ℃ are the pure anatase phase but that calcined at 700 ℃ is a mixture of anatase and rutile phases. The doped N locates at the interstitial site of TiO2 which leads to the narrowing of bad gap of pure anatase N-TiO2. Among all photocatalysts, N-TiO2 photocatalysts calcined at 600 and 400 ℃ exhibit the best performance in the photodegradation of methyl orange under the UV light and all-wavelength light illuminations, respectively; however, because of the perfect crystallinity and the existence of anatase-rutile phase junctions, N-TiO2 photocatalyst calcined at 700 ℃ exhibits the highest specific photodegradation rate, i.e., the highest quantum yield, under both the UV light and all-wavelength light illuminations.
基金supported by the National Natural Science Foundation of China (51702225)the National Key Research and Development Program (2016YFA0200103)+2 种基金the Natural Science Foundation of Jiangsu Province (BK20170336)the support from Suzhou Key Laboratory for Advanced Carbon MaterialsWearable Energy Technologies, Suzhou, China。
文摘Developing high-performance anodes for potassium ion batteries(KIBs) is of paramount significance but remains challenging.In the normal sense,electrode materials are prepared by ubiquitous wet chemical routes,which otherwise might not be versatile enough to create desired heterostructures and/or form clean interfacial areas for fast transport of K-ions and electrons.Along this line,rate capability/cycling stability of resulting KIBs are greatly handicapped.Herein we present an all-chemical vapor deposition approach to harness the direct synthesis of nitrogen-doped graphene(NG)/rhenium diselenide(ReSe_2)hybrids over three-dimensional MXene supports as superior heterostructure anode material for KIBs.In such an innovative design,1 T'-ReSe2 nanoparticles are sandwiched in between the NG coatings and MXene frameworks via strong interfacial interactions,thereby affording facile K~+ diffusion,enhancing overall conductivity,boosting high-power performance and reinforcing structural stability of electrodes.Thus-constructed anode delivers an excellent rate performance of 138 mAh g^(-1) at 10.0 A g^(-1) and a high reversible capacity of 90 mAh g^(-1) at 5 A g^(-1) after 300 cycles.Furthermore,the potassium storage mechanism has been systematically probed by advanced in situlex situ characterization techniques in combination with first principles computations.
基金supported by the National Natural Science Foundation of China(Nos.21633009,21925206,21901240)the National Key Research and Development Program of China(No.2020YFA0406102)。
文摘Photocatalysis based on semiconductors has recently been receiving considerable research interest because of its extensive applications in environmental remediation and renewable energy generation.Various semiconductor-based materials that are vital to solar energy utilization have been extensively investigated,among which titanium oxide(TiO_(2))has attracted considerable attention because of its exceptional physicochemical characteristics.However,the sluggish responsiveness to visible light in the solar spectrum and the inefficient separation of photoinduced electron-hole pairs hamper the practical application of TiO_(2) materials.To overcome the aforementioned serious drawbacks of TiO_(2),numerous strategies,such as doping with foreign atoms,particularly nitrogen(N),have been improved in the past few decades.This review aims to provide a comprehensive update and description of the recent developments of N-doped TiO_(2) materials for visible lightresponsive photocatalysis,such as(1)the preparation of N-doped/co-doped TiO_(2) photocatalysts and(2)mechanistic studies on the reasons for visible light response.Furthermore,the most recent and significant advances in the field of solar energy applications of modified N-doped TiO_(2) are summarized.The analysis indicated the critical need for further development of these types of materials for the solar-to-energy conversion,particularly for water splitting purposes.
基金the National Natural Science Foundation of China(21975154)the Shanghai Municipal Education Commission(Innovation Program(2019-01-07-00-09E00021)+2 种基金Innovative Research Team of High-level Local Universities in Shanghaisupported by The Program for Professor of Special Appointment(Eastern Scholar)at Shanghai Institutions of Higher LearningShanghai Key Laboratory of Materials Protection and Advanced Materials in Electric Power。
文摘With great superiorities in energy density,rate capability and structural stability,Na_(3)V_(2)(PO_(4))_(2) F_(3)(NVPF)has attracted much attentions as cathode of sodium ion battery(SIB),but it also faces challenges on its poor intrinsic electronic conductivity and the controversial de/sodiation mechanism.Herein,a series of Zr-doped NVPF coated by N-doped carbon layer(~5 nm in thickness,homogenously)materials are fabricated by a sol-gel method,and the optimized heteroatom-doping amounts of Zr and N doping improve intrinsic properties on enlarging lattice distance and enhancing electronic conductivity,respectively.Specifically,among all samples of Na_(3) V_(2-x)Zr_(x)(PO_(4))_(2) F_(3)/NC(NVPF-Zr-x/NC,x=0,0.01,0.02,0.05,and 0.1),the optimized electrode of NVPF-Zr-0.02/NC delivers high reversible capacities(119.2 mAh g^(-1) at0.5 C),superior rate capability(98.1 mA h g^(-1) at 20 C)and excellent cycling performance.The structural evolution of NVPF-Zr-0.02/NC electrode,in-situ monitored by X-ray diffractometer,follows a step-wise Na-extraction/intercalation mechanism with reversible multi-phase changes,not just a solid-solutionreaction one.Full cells of NVPF-Zr-0.02/NC//hard carbon demonstrate high capacity(99.8 mA h g^(-1) at 0.5 C),high out-put voltage(3.5 V)and good cycling stability.This work is favorable to accelerate the development of high-performance cathode materials and explore possible redox reaction mechanisms of SIBs.
基金the National Natural Science Foundation of China (No. 91634108, 21376148 and 61503246)National Key Program(2017FYA0205300)
文摘N-doped coaxial CNTs@α-Fe_2O_3@C nanofibers have been successfully synthesized according to a facile solvothermal/hydrothermal method. The obtained CNTs@α-Fe_2O_3@C nanofibers composites exhibited spe- cial three-dimensional （3-D） network structure, which endows they promising candidate for anode ma- terials of lithium ion battery. The coaxial property of CNTs@α-Fe_2O_3@C nanofibers could significantly improve the cycling and rate performance owing to the acceleration of charge/electron transfer, improve- ment of conductivity, maintaining of structural integrity and inhibiting the aggregation. The α-Fe_2O_3 nanoparticles with small size and high percentage of N-doped amount could further improve the elec- trochemical performance. As for the CNTs@α-Fe_2O_3@C nanofibers, the capacity presented a high value of 1255.4 mAh/g at 0.1 C, and retained at 1213.4 mAh/g after 60 cycles. Even at high rate of 5 C, the ca- pacity still exhibited as high as 319 mAh/g. The results indicated that the synthesized N-doped coaxial CNTs@α-Fe_2O_3@C nanofibers exhibited high cvcling and rate oerformance.
基金financially supported by Guangdong Province Science and Technology Plan Project for Public Welfare Fund and Ability Construction Project(JCYJ20180301171324915)the National Natural Science Foundation of China(No.21503116)+1 种基金Taishan Scholars Program of Shandong Province(No.tsqn20161004)the Youth 1000 Talent Program of China。
文摘The conversion of carbon dioxide into valuable organic compounds is a highly promising approach to address the energy issues and environmental problems(e.g., global warming). Herein, we presents a facile and efficient method to prepare highly dense and well-dispersed SnO2 nanocrystals on 1 D N-doped carbon nanowires as advanced catalysts for the efficient electroreduction of CO2 to formate. The ultrasmall SnO2 coated on the N-doped carbon nanowires(SnO2@N-CNW) has been synthesized via the simple hydrothermal treatment coupled with a pyrolysis process. The unique structure enables to expose the active tin oxide and also provides the facile pathways for rapid transfer of electron and electrolyte along with the highly porous carbon foam composed with interconnected carbon nanowires. Therefore, SnO2@NCNW electrocatalyst exhibits good durability and high selectivity for formate formation with a Faradaic efficiency of ca. 90%. This work demonstrates a simple method to rationally design high-dense tin oxide nanocrystals on the conductive carbon support as advanced catalysts for CO2 electroreduction.
文摘Low cost,highly selective and efficient electrocatalysts for CO_(2)reduction reaction(CO_(2)RR)is crucial for lowering the global carbon footprint and mitigating energy shortages.Here,we first report a highly selective and efficient electrocatalyst for CO_(2)RR to CO using a surface-regulated Ni nanoparticles supported on N-doped CMK-3(N,O-Ni/CMK3).Compared with most Ni metal catalysts previously reported with severe competitive hydrogen evolution during the CO_(2)RR,the N,O-Ni/CMK3 catalyst presents a superior CO faradaic efficiency of about 97%,a high CO partial current density(13.01 mA cm^(-1))and turnover frequency(4.25 s^(–1)).The comprehensive characterization provides evidence that the N,O co-regulated Ni acts as the active center.Taking advantage of the N,O co-regulated chemical environment,N,O-Ni/CMK3 also displays a decent stability at negative potentials.Our work paves a novel approach for developing transition metal catalysts for CO_(2)RR with enhanced activity and selectivity via regulating surface chemical environment.
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supported by the National Natural Science Foundation of China (Nos.91963204 and 51871053)Shanghai Pujiang Program (No.19PJ1400200)the Fundamental Research Funds for the Central Universities (Nos.2232019G-07 and 2232020A-02)。
文摘Electromagnetic wave absorber is critical for reducing increasingly serious electromagnetic wave pollu-tion,however,the development of lightweight and broadband microwave absorbers remains a pressing challenge.We report here the rational design and synthesis of N-doped Ni@SiO_(2)/graphene composite con-structed from 3D interconnected porous graphene network and Ni@SiO_(2) core-shell architecture,which fulfills lightweight and broadband requirements while exhibiting highly efficient electromagnetic wave absorption.The porous graphene network,functioning both as lightweight support and dielectric medi-ator,was synthesized via NaCl template-assisted high-temperature calcination method.Upon uniformly attached with core-shell Ni@SiO_(2) on the surface,the resulting abundant heterogeneous interfaces con-structed by graphene-Ni and Ni-SiO_(2) strongly reinforce polarization loss.The presence of low dielectric SiO_(2) allows facile tuning of the complex permittivity of ternary composite by adjusting coating thick-ness to balance the attenuation ability and impedance matching.Moreover,further N-doping of graphene assists in the optimization of dielectric loss ability.Taking account of the advantages arising from the porous hierarchical architecture,multiple absorption centers and diverse interfaces,the lightweight com-posite exhibits an ultra-strong reflection loss(RL)value of-71.13 dB at 13.76 GHz with a thickness of 2.46 mm and broad effective absorption bandwidth of 7.04 GHz at a low filler content of 15 wt.%.More importantly,the effective absorption range covers 13.28 GHz(4.72-18 GHz)with the optimized thickness of 1.6-5 mm,representing 83%of the whole range of frequencies.Our results demonstrate that the novel 3D porous N-doped Ni@SiO_(2)/graphene network with hierarchical architecture is a promising candidate for high-performance electromagnetic wave absorption.
基金financially supported by the National Natural Science Foundation of China(No.21501101)the Natural Science Foundation of Henan Province(No.182300410226)+1 种基金the Technological Project of Henan Province(Nos.172102210426,172102210423 and 182102310068)the Education Department Project of Henan Province(No.16A150038)。
文摘Orthorhombic-phase Nb_(2)O_(5)(T-Nb_(2)O_(5)) has been widely investigated as an intercalation anode material for Li-ion batteries due to the larger interplanar lattice spacing and high safety.However,its applications are limited by the intrinsic low electric conductivity.Herein,an ultrathin N-doped carbon-coating layer was constructed on porous T-Nb_(2)O_(5) microspheres uniformly via a convenient thermal treatment method with ionic liquid as a carbon precursor.The synthesized T-Nb_(2)O_(5)@N-C exhibits significantly enhanced rate capability(155.5 mAh·g^(-1) at 20 C) than initial T-Nb_(2)O_(5)(110.2 mAh·g^(-1) at 20C).Besides,T-Nb_(2)O_(5)@N-C shows ultralong cycle life,with only a 0.02% decrease in the capacity per cycle at a high current density of 10 C.The corresponding electrochemical tests show that the preferable rate capability of T-Nb_(2)O_(5)@N-C electrode is attributed to the increased electronic conductivity and pseudocapacitance contribution induced by ultrathin surface N-doped carbon layer.On the other hand,the mesoporous structure of T-Nb_(2)O_(5)@N-C ensures fast Li+ diffusion dynamics and electrolyte penetration.Furthermore,T-Nb_(2)O_(5)@N-C also performs well in a LiNi_(0.5)Mn_(0.3)Co_(0.2)O_(4) llT-Nb_(2)O_(5)@N-C full cell.This work provides a facile method to construct integrated anode materials for potential applications in lithium-ion batteries.
基金financially supported by the National Natural Science Foundation of China (No.91963118)Fundamental Research Funds for the Central Universities (No.2412019QD013)+1 种基金the 111 Project (No.B13013)the support from China Postdoctoral Science Foundation (No.2019M661191)。
文摘Metal organic framework(MOF) has been confirmed as the promising precursor to develop the conve rsion-typed anode mate rials of sodium-ion batteries(SIBs) because of the tunable structure design and simple functional modification.Here,we prepare the ultrasmall Ni_(3)S_(2) nanocrystals embedded into N-doped porous carbon nanoparticles using the scalable Ni-MOF as precursor(denoted as Ni_(3)S_(2)@NPC).The ultrasmall size of Ni_(3)S_(2) can work for accelerated electro n/ion transfer to facilitate the electrochemical reaction kinetics.Moreover,the robust conductivity network originated from N-doped porous carbon nanoparticles can not only improve the electron conductivity,but also enhance the electrode integrity and stability of the electrode/electrolyte interface.In addition,the N heteroatoms provide extra Na storage sites.Accordingly,the electrode delivers the obviously competitive capacities and high-power output with respect to the currently reported Ni_(3)S_(2)/C composites.This study provides a scalable and universal strategy to develop the advanced transition metal sulfides for practically feasible SIBs.
基金financial support by the Natural Science Foundation of Shanghai City(No.18ZR1416400)the National Natural Science Foundation of China(No.21305086)Science and Technology Development Fund of Shanghai Municipal Public Security Bureau(No.2018003)。
文摘The exploitation of multifunctional nanocomposites is highly desired in environmental monitoring,biosensors,and medical diagnosis.In this paper,a simple approach has been proposed to fabricate MoS2 decorated N-doped carbon nanotubes(NCNTs@MoS2)hybrid composites as efficient peroxidase-like mimics.The combination of the MoS2 and N-doped carbon nanotubes(NCNTs)brings about an enhanced synergistic effect,leading to remarkably decent intrinsic peroxidase-mimic activities than that of the single components.Due to the high catalytic efficiency of the resultant NCNTs@MoS2 hybrid nanotubes as peroxidase-like mimics,a co nvenient colorimetric approach for the sensitive determination of H2 O2 and ascorbic acid have been developed with a detection limit of about 0.14μmol/L and 0.12μmol/L,respectively.The work offers a new strategy for the fabrication of peroxidase-like nanomaterials with excellent catalytic activity,which indicates great promising applications in sensitive detections in real samples.
文摘Photocatalytic CO_(2)conversion efficiency is hampered by the rapid recombination of photogenerated charge carriers.It is effective to suppress the recombination by constructing cocatalysts on photocatalysts with high-quality interfacial contact.Herein,we develop a novel strategy to in-situ grow ultrathin/V-doped graphene(NG)layer on TiO_(2) hollow spheres(HS) with large area and intimate interfacial contact via a chemical vapor deposition(CVD).The optimized TiO^(2)/NG HS nanocomposite achieves total CO_(2)conversion rates(the sum yield of CO,CH_(3)OH and CH_(4))of 18.11μmol·g^(-1)h^(-1),which is about 4.6 times higher than blank T1O_(2)HS.Experimental results demonstrate that intimate interfacial contact and abundant pyridinic N sites can effectively facilitate photogenerated charge carrier separation and transport,realizing enhanced photocatalytic CO_(2)reduction performance.In addition,this work provides an effective strategy for in-situ construction of graphene-based photocatalysts for highly efficient photocatalytic CO_(2)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supported by National Key R&D Program of China(2016YFB0100500)Special fund of key technology research and development projects(20180201097GX)(20180201099GX)(20180201096GX)+5 种基金Jilin Province Science and Technology Department.The R&D Program of power batteries with low temperature and high energy,Science and Technology Bureau of Changchun(19SS013)Key Subject Construction of Physical Chemistry of Northeast Normal UniversityGeneral Financial Grant from the China Postdoctoral Science Foundation(Grant 2016M601363)Fundamental Research Funds for the Central Universities(Grant2412017QD011)Jilin Scientific and Technological Development Program(Grant 20180520143JH)National Natural Science Foundation of China(Grant 21805030)。
文摘The conventional Li–O2 battery(LOB)has hardly been considered as a next-generation flexible electronics thus far,since it is bulk,inflexible and limited by the absence of an adjustable cell configuration.Here,we present a flexible Li–O2 cell using N-doped carbon nanocages grown onto the carbon textiles(NCNs/CTs)as a self-standing and binder-free O2 electrode.The highly flexible NCNs/CTs exhibits an excellent mechanic durability,a promising catalytic activity towards the ORR and OER,a considerable cyclability of more than 70 cycles with an overpotential of 0.36 V on the 1 stcycle at a constant current density of 0.2 m A/cm2,a good rate capability,a superior reversibility with formation and decomposition of desired Li2 O2,and a highly electrochemical stability even under stringent bending and twisting conditions.Our work represents a promising progress in the material development and architecture design of O2 electrode for flexible LOBs.
基金Financial supports from the National Natural Science Foundation of China(no.31901272,no.22075254)the Jiangsu Province Key Laboratory of Biomass Energy and Materials(no.JSBEM-S-201906)。
文摘The development of efficient catalytic electrode toward oxygen reduction reaction(ORR)is still a great challenge for the wide use of zinc–air batteries.Herein,Co_(2)N nanoparticles(NPs)anchored on N-doped carbon from cattail were verified with excellent catalytic performances for ORR.The onset and half-wave potentials over the optimal catalyst reach to 0.96 V and 0.84 V,respectively.Current retention rates of 96.8%after 22-h test and 98.8%after running 1600 s were obtained in 1 M methanol solution.Density functional theory simulation proposes an apparently increased electronic states of Co_(2)N in N-doped carbon layer close to the Fermi level.Higher charge density,favorable adsorption,and charge transfer of intermediates originate from the coexistence of Co_(2)N NPs and N atoms in carbon skeleton.The superior catalytic activity of composites also was confirmed in zinc–air batteries.This novel catalytic property and controllable preparation approach of Co_(2)Ncarbon composites provide a promising avenue to fabricate metal-containing catalytically active carbon from biomass.
