A series of spinel-type Mg_(0.25-x)Al_(2.57)O_(3.79)N_(0.21):xMn^(2+)(MgAlON:xMn^(2+))phosphors were synthesized by the solid-state reaction route.The transparent ceramic phosphors were fabricated by pressureless sint...A series of spinel-type Mg_(0.25-x)Al_(2.57)O_(3.79)N_(0.21):xMn^(2+)(MgAlON:xMn^(2+))phosphors were synthesized by the solid-state reaction route.The transparent ceramic phosphors were fabricated by pressureless sintering followed by hot-isostatic pressing(HIP).The crystal structure,luminescence and mechanical properties of the samples were systematically investigated.The transparent ceramic phosphors with tetrahedrally coordinated Mn^(2+)show strong green emission centered around 515 nm under blue light excitation.As the Mn^(2+)concentration increases,the crystal lattice expands slightly,resulting in a variation of crystal field and a slight red-shift of green emission peak.Six weak absorption peaks in the transmittance spectra originate from the spin-forbidden ^(4)T_(1)(^(4)G)→^(6)A_(1) transition of Mn^(2+).The decay time was found to decrease from 5.66 to 5.16 ms with the Mn^(2+)concentration.The present study contributes to the systematic understanding of crystal structure and properties of MgAlON:xMn^(2+)green-emitting transparent ceramic phosphor which has a potential application in high-power light-emitting diodes.展开更多
Graphene's large theoretical surface area and high conductivity make it an attractive anode material for potassium-ion batteries(PIBs).However,its practical application is hindered by small interlayer distance and...Graphene's large theoretical surface area and high conductivity make it an attractive anode material for potassium-ion batteries(PIBs).However,its practical application is hindered by small interlayer distance and long ion transfer distance.Herein,this paper aims to address the issue by introducing MXene through a simple and scalable method for assembling graphene and realizing ultrahigh P doping content.The findings reveal that MXene and P-C bonds have a "pillar effect" on the structure of graphene,and the P-C bond plays a primary role.In addition,N/P co-doping introduces abundant defects,providing more active sites for K^(+) storage and facilitating K^(+) adsorption.As expected,the developed ultrahigh phosphorous/nitrogen co-doped flexible reduced graphene oxide/MXene(NPrGM) electrode exhibits remarkable reversible discharge capacity(554 mA hg^(-1) at 0.05 A g^(-1)),impressive rate capability(178 mA h g^(-1) at 2 A g^(-1)),and robust cyclic stability(0.0005% decay per cycle after 10,000 cycles at 2 A g^(-1)).Furthermore,the assembled activated carbon‖NPrGM potassium-ion hybrid capacitor(PIHC) can deliver an impressive energy density of 131 W h kg^(-1) and stable cycling performance with 98.1% capacitance retention after5000 cycles at 1 A g^(-1).Such a new strategy will effectively promote the practical application of graphene materials in PIBs/PIHCs and open new avenues for the scalable development of flexible films based on two-dimensional materials for potential applications in energy storage,thermal interface,and electromagnetic shielding.展开更多
In this study,a single-doped phosphors yttrium aluminum garnet(Y_(3)Al_(5)O_(12),YAG):Ce^(3+),single-doped YAG:Sc^(3+),and double-doped phosphors YAG:Ce^(3+),Sc^(3+) were prepared by spark plasma sintering(SPS)(lower ...In this study,a single-doped phosphors yttrium aluminum garnet(Y_(3)Al_(5)O_(12),YAG):Ce^(3+),single-doped YAG:Sc^(3+),and double-doped phosphors YAG:Ce^(3+),Sc^(3+) were prepared by spark plasma sintering(SPS)(lower than 1 200℃).The characteristics of synthesized phosphors were determined using scanning electron microscopy(SEM),X-ray diffraction(XRD),and fluorescence spectroscopy.During SPS,the lattice structure of YAG was maintained by the added Ce^(3+) and Sc^(3+).The emission wavelength of YAG:Ce^(3+) prepared from SPS(425-700 nm) was wider compared to that of YAG:Ce^(3+) prepared from high-temperature solid-state reaction(HSSR)(500-700 nm).The incorporation of low-dose Sc^(3+) in YAG:Ce^(3+) moved the emission peak towards the short wavelength.展开更多
Phase engineering is an efficient strategy for enhancing the kinetics of electrocatalytic reactions.Herein,phase engineering was employed to prepare high‐performance phosphorous‐doped biphase(1T/2H)MoS_(2)(P‐BMS)na...Phase engineering is an efficient strategy for enhancing the kinetics of electrocatalytic reactions.Herein,phase engineering was employed to prepare high‐performance phosphorous‐doped biphase(1T/2H)MoS_(2)(P‐BMS)nanoflakes for hydrogen evolution reaction(HER).The doping of MoS_(2)with P atoms modifies its electronic structure and optimizes its electrocatalytic reaction kinetics,which significantly enhances its electrical conductivity and structural stability,which are verified by various characterization tools,including X‐ray photoelectron spectroscopy,high‐resolution transmission electron microscopy,X‐ray absorption near‐edge spectroscopy,and extended X‐ray absorption fine structure.Moreover,the hierarchically formed flakes of P‐BMS provide numerous catalytic surface‐active sites,which remarkably enhance its HER activity.The optimized P‐BMS electrocatalysts exhibit low overpotentials(60 and 72 mV at 10 mA cm^(−2))in H_(2)SO_(4)(0.5 M)and KOH(1.0 M),respectively.The mechanism of improving the HER activity of the material was systematically studied using density functional theory calculations and various electrochemical characterization techniques.This study has shown that phase engineering is a promising strategy for enhancing the H*adsorption of metal sulfides.展开更多
Magnesium hydride has been seen as a potential material for solid state hydrogen storage,but the kinetics and thermodynamics obstacles have hindered its development and application.Three-dimensional flower-like TiO2@C...Magnesium hydride has been seen as a potential material for solid state hydrogen storage,but the kinetics and thermodynamics obstacles have hindered its development and application.Three-dimensional flower-like TiO2@C and TiO2 were synthesized as the catalyst for MgH2 system and great catalytic activities are acquired in the hydrogen sorption properties.Experiments also show that the flower-like TiO2@C is superior to flower-like TiO2 in improving the hydrogen storage properties of MgH2.The hydrogen desorption onset and peak temperatures of flower-like TiO2 doped MgH2 is reduced to 199.2℃and 245.4℃,while the primitive MgH2 starts to release hydrogen at 294.6℃and the rapid dehydrogenation temperature is even as high as 362.6℃.The onset and peak temperatures of flower-like TiO2@C doped MgH2 are further reduced to 180.3℃and 233.0℃.The flower-like TiO2@C doped MgH2 composite can release6.0 wt%hydrogen at 250℃within 7 min,and 4.86 wt%hydrogen at 225℃within 60 min,while flowerlike TiO2 doped MgH2 can release 6.0 wt%hydrogen at 250℃within 8 min,and 3.89 wt%hydrogen at225℃within 60 min.Hydrogen absorption kinetics is also improved dramatically.Moreover,compared with primitive MgH2 and the flower-like TiO2 doped MgH2,the activation energy of flower-like TiO2@C doped MgH2 is significantly decreased to 67.10 kJ/mol.All the improvement of hydrogen sorption properties can be ascribed to the flower-like structure and the two-phase coexistence of TiO2 and amorphous carbon.Such phase composition and unique structure are proved to be the critical factor to improve the hydrogen sorption properties of MgH2,which can be considered as the new prospect for improving the kinetics of light-metal hydrogen storage materials.展开更多
Flower-like ZnO microstructures were successfully produced using a hydrothermal method employing ZnSO_(4)/(NH_(4))_(2)SO_(4) as a raw material.The effect of the operating parameters of the hydrothermal temperature, OH...Flower-like ZnO microstructures were successfully produced using a hydrothermal method employing ZnSO_(4)/(NH_(4))_(2)SO_(4) as a raw material.The effect of the operating parameters of the hydrothermal temperature, OH^(-)/Zn^(2+) molar ratio, time, and amount of dispersant on the phase structure and micromorphology of the ZnO particles were investigated.The synthesis conditions of the flower-like ZnO microstructures were: hydrothermal temperature of 160℃, OH^(-)/Zn^(2+) molar ratio of 5:1, reaction time of 4 h, and 4 mL of dispersant.The flower-like ZnO microstructures were comprised of hexagon-shaped ZnO rods arranged in a radiatively.Degradation experiments of Rhodamine B with the flower-like ZnO microstructures demonstrated a degradation efficiency of 97.6% after 4 h of exposure to sunshine, indicating excellent photocatalytic capacity.The growth mechanism of the flower-like ZnO microstructures was presented.展开更多
Calcium carbonate with three-dimensional chrysanthemun flower-like structure was successfully prepared from calcium chloride and sodium carbonate ethanol/water mixed solution by a simple precipitation method,using tri...Calcium carbonate with three-dimensional chrysanthemun flower-like structure was successfully prepared from calcium chloride and sodium carbonate ethanol/water mixed solution by a simple precipitation method,using trisodium citrate as crystal modifier.The experimental results show that the three-dimensional structure of chrysanthemun flower-like calcium carbonate is built up with several symmetrical micrometer multi-layer petals arranged around the multi-layer pancake-liked center,and the micrometer center and petals are assemblied by a large number of nanometer spherical particles with size 10-20 nm.It is found that the amount of trisodium citrate,the ethanol volume content has an important influence on the formation of this morphology.A possible mechanism is proposed to explain the formation of three-dimensional chrysanthemun flower-like calcium carbonate according the results.Scanning electron microscopy(SEM),X-ray powder diffraction(XRD),flourier transform infrared spectroscopy(FT-IR),thermogravimety analysis(TG),transmission electron microscopy(TEM) equipped with energy-dispersive X-ray(EDX),and selected area electron diffraction(SAED) were used to characterize the crystals.展开更多
Finding easy-to-operate strategy to obtain anode material with well-designed structure and excellent electrochemical performance is necessary to promote the development of the future potassium-ion batteries(PIBs).In t...Finding easy-to-operate strategy to obtain anode material with well-designed structure and excellent electrochemical performance is necessary to promote the development of the future potassium-ion batteries(PIBs).In this work,we synthesized reduced graphene oxide doping flower-like Fe_(7)S_(8) nanosheets electrode materials using one-step hydrothermal strategy.The rGO@Fe_(7)S_(8) composite is composed of homogeneous Fe_(7)S_(8) and reduced graphene oxide thin nanosheets.This unique structure not only promotes the penetration of electrolyte and increases the conductive of the pure Fe_(7)S_(8) electrode materials,but also relieves the volume expansion of K^(+) during charge/discharge process.When applied this interesting anode electrode for PIBs,the rGO@Fe_(7)S_(8) exhibits excellent electrochemical performance.It delivers a high reversible specific capacity of 445 mAh g^(-1) at 50 mA g^(-1),excellent rate performance(284 mAhg^(-1)at 500 mA g^(-1) and 237 mAh g^(-1) at 1000 mA g^(-1)),and a high cycling stability at 100 mA g^(-1)(maintained 355 mAh g^(-1) after 300 cycles).展开更多
Due to the high specific capacity and energy density, lithium–sulfur battery is regarded as a potential energy storage conversion system. However, the serious shuttle effect and the sluggish electrochemical reaction ...Due to the high specific capacity and energy density, lithium–sulfur battery is regarded as a potential energy storage conversion system. However, the serious shuttle effect and the sluggish electrochemical reaction kinetics impede the practical use of lithium–sulfur battery. In the interests of breaking through the above knotty problems, herein we propose to use the polar flower-like Zn O modified by Bi OI nanoparticles as bifunctional host with catalytic and adsorption ability for polysulfides in lithium–sulfur battery.It can be found that this adsorption/catalytic host integrates the functions of adsorption and mutual catalytic conversion of polysulfides, in which the polar flower-like Zn O can effectively capture the polysulfides through strong polar-polar interaction, simultaneously the BiOI nanoparticles can accelerate the mutual conversion of polysulfides to Li2 S through reducing the activation energy and conversion energy barrier required for the electrochemical reaction. As a result, under a sulfur loading of 2.5 mg cm^(-2), the lithium–sulfur battery with Zn O/Bi OI/CNT/S as cathode reveals a considerable initial specific capacity of1267 mAh g^(-1) at a current density of 0.1 C. Even the current density increased to 1 C, the capacity can reach as 873.4 mAh g^(-1), together with a good capacity retention of 67.1% after 400 cycles. Therefore,after systematically study the positive effects of the flower-like ZnO modified by catalytic BiOI nanoparticles on the adsorption and catalytic conversion of polysulfides, this work provides a new idea for the development and application of high-performance lithium–sulfur batteries.展开更多
A novel flower-like hydrated magnesium carbonate hydroxide, Mg5 (CO3 )4 (OH)2·4H2O, with micro-structure composed of individual thin nano-sheets was synthesized using a facile solution route without the use o...A novel flower-like hydrated magnesium carbonate hydroxide, Mg5 (CO3 )4 (OH)2·4H2O, with micro-structure composed of individual thin nano-sheets was synthesized using a facile solution route without the use of template or organic surfactant. Reaction time has an important effect on the final morphology of the product. The micro-structure and morphology of Mg5 (CO3)4 (OH)2·4H2O were characterized by means of X-ray diffractometry (XRD), fieldemission scanning electron microscopy(FE-SEM). Brunauer-Emmett-Teller(BET) surface areas of the samples were also measured. The probable formation mechanism of flower-like micro-structure was discussed. It was found that Mg5 (CO3)4( OH)2·4H2O with flower-like micro-structure was a novel and efficient catalyst for the synthesis of diphenyl carbonate (DPC) by transesterification of dimethyl carbonate (DMC) with phenol.展开更多
Developing cost-effective electrocatalysts for oxygen evolution reaction (OER) in basic media is critical to hydrogen production from renewable energy. Herein, in-situ electrodeposited flower-like NiFeO x H y and NiFe...Developing cost-effective electrocatalysts for oxygen evolution reaction (OER) in basic media is critical to hydrogen production from renewable energy. Herein, in-situ electrodeposited flower-like NiFeO x H y and NiFeO x H y /rGO composite electrocatalysts on Ni foam for OER are reported. The active sites of the flower-like electrocatalysts are increased significantly due to the enhanced NiFeO x H y surface areas and numerous exposed layered edges and edge defects. Reduced graphene oxide (rGO) has been introduced to fabricate NiFeO x H y /rGO composite film, further improving the conductivity and OER performance of the flower-like NiFeO x H y . The optimized NiFeO x H y /rGO exhibits superior OER performance with a Tafel slope of 29.11 mV/decade, an overpotential of 200 mV at 10 mA/cm 2 in 1 mol/L KOH and favorable long-term stability.展开更多
In this work,a facile and effective strategy to prepare three-dimensional(3D)hierarchical flower-like Mg–Al layered double hydroxides(3D-LDH)was developed via a one-step double-drop coprecipitation method usingγ-Al ...In this work,a facile and effective strategy to prepare three-dimensional(3D)hierarchical flower-like Mg–Al layered double hydroxides(3D-LDH)was developed via a one-step double-drop coprecipitation method usingγ-Al 2O 3particles as a template.The characterization and experimental results showed that the calcined product,3D-LDO,features a large specific surface area of 204.2 m^(2)/g,abundant active sites,and excellent adsorption performance for Congo red(CR),methyl orange(MO),and methyl blue(MB).The maximum adsorption capacities of 3D-LDO for CR,MO,and MB were 1428.6,476.2,and 1666.7 mg/g,respectively;such performance is superior to that of most reported adsorbents.The adsorption mechanism of organic anionic dyes by 3D-LDO was extensively investigated and attributed to surface adsorption,the memory effect of 3D-LDO,and the unique 3D hierarchical flower-like structure of the adsorbent.Recycling performance tests revealed that3D-LDO has satisfactory reusability for the three organic anionic dyes.展开更多
Cement,phosphorous slag(PS),and steel slag(SS)were used to prepare low-carbon cementitious materials,and triisopropanolamine(TIPA)was used to improve the mechanical properties by controlling the hydration process.The ...Cement,phosphorous slag(PS),and steel slag(SS)were used to prepare low-carbon cementitious materials,and triisopropanolamine(TIPA)was used to improve the mechanical properties by controlling the hydration process.The experimental results show that,by using 0.06%TIPA,the compressive strength of cement containing 60%PS or 60%SS could be enhanced by 12%or 18%at 28 d.The presence of TIPA significantly affected the hydration process of PS and SS in cement.In the early stage,TIPA accelerated the dissolution of Al in PS,and the formation of carboaluminate hydrate was facilitated,which could induce the hydration;TIPA promoted the dissolution of Fe in SS,and the formation of Fe-monocarbonate,which was precipitated on the surface of SS,resulting in the postponement of hydration,especially for the high SS content.In the later stage,under the continuous solubilization effect of TIPA,the hydration of PS and SS could refine the pore structure.It was noted that compared with portland cement,the carbon emissions of cement-PS-TIPA and cement-SS-TIPA was reduced by 52%and 49%,respectively.展开更多
Flower-like tungsten disulfide(WS_(2))with a diameter of 5-10μm is prepared by chemical vapor deposition(CVD).Scanning electron microscopy(SEM),energy dispersive spectrometer(EDS),Raman spectroscopy,and ultraviolet-v...Flower-like tungsten disulfide(WS_(2))with a diameter of 5-10μm is prepared by chemical vapor deposition(CVD).Scanning electron microscopy(SEM),energy dispersive spectrometer(EDS),Raman spectroscopy,and ultraviolet-visible(UV-vis)spectroscopy are used to characterize its morphological and optical properties,and its growth mechanism is discussed.The key factors for the formation of flower-like WS_(2)are determined.Firstly,the cooling process causes the generation of nucleation dislocations,and then the"leaf"growth of flower-like WS_(2)is achieved by increasing the temperature.展开更多
This paper proposes a method of utilizing a flower-like MnOx nanozyme to conduct a colorimetric detection of ascorbic acid.The nanozyme is obtained by a chain of reaction of K3[Fe(CN)6],MnSO4·H2O,polyvinyl pyrrol...This paper proposes a method of utilizing a flower-like MnOx nanozyme to conduct a colorimetric detection of ascorbic acid.The nanozyme is obtained by a chain of reaction of K3[Fe(CN)6],MnSO4·H2O,polyvinyl pyrrolidone(PVP),NH4F,ethanol,and water.During the experimental process,the flower-like nanozyme is added to the mixed solution,including phosphate buffer,H2O2,and 3,3’,5,5’-tetramethylbe nzidine(TMB).The optimum reaction condition as following:pH 3.0,30μL 500mM H2O2,25μL 92 mM TMB,and 30μL 0.1mM nanozyme.Under the optimum condition,the detection range is 2-26mM,and the linear detection range is 2-20mM.展开更多
Doping in Si nanocrystals is an interesting topic and directly studying the distribution of dopants in phosphorous/boron co-doping is an important issue facing the scientific community.In this study,atom probe tomogra...Doping in Si nanocrystals is an interesting topic and directly studying the distribution of dopants in phosphorous/boron co-doping is an important issue facing the scientific community.In this study,atom probe tomography is performed to study the structures and distribution of impurity in phosphorous/boron co-doped Si nanocrystals/SiO_(2) multilayers.Compared with phosphorous singly doped Si nanocrystals,it is interesting to find that the concentration of phosphorous in co-doped samples can be significantly improved.Theoretical simulation suggests that phosphorous-boron pairs are formed in co-doped Si nanocrystals with the lowest formation energy,which also reduces the formation energy of phosphorous in Si nanocrystals.The results indicate that co-doping can promote the entry of phosphorous impurities into the near-surface and inner sites of Si nanocrystals,which provides an interesting way to regulate the electronic and optical properties of Si nanocrystals such as the observed enhancement of conductivity and sub-band light emission.展开更多
The phosphors of KY_(1-x)(MoO_(4))_(2-y)(WO_(4))y:xLn^(3+)(Ln^(3+)=Tm^(3+),Dy^(3+),Eu^(3+))were synthesized by using a sol-gel method.Then,the crystal structure,luminescence properties,energy transfer,and white emissi...The phosphors of KY_(1-x)(MoO_(4))_(2-y)(WO_(4))y:xLn^(3+)(Ln^(3+)=Tm^(3+),Dy^(3+),Eu^(3+))were synthesized by using a sol-gel method.Then,the crystal structure,luminescence properties,energy transfer,and white emission of the prepared materials were researched.The molar ratio of the anion group on the photoluminescence(PL)emission and excitation intensity were investigated,revealing that the optimum intensity could be obtained by using=3:1.The optimal Dy^(3+) doping concentration of KY(MoO_(4))1.5(WO4)0.5was obtained.In addition,the color-tunable emissions of Dy^(3+)/Eu^(3+)-codoped KY(MoO_(4))1.5(WO4)0.5phosphors were observed because of the effective energy transfer(ET)from Dy^(3+)to Eu^(3+)ions.Finally,by doping appropriate concentrations of Tm^(3+),Dy^(3+),and Eu^(3+)and different concentrations of(WO_(4))^(2-),white light emitting phosphors KY_(0.92)(WO_(4))2:0.01Tm^(3+),0.06Dy^(3+),0.01Eu^(3+)with excellent color-rending properties were obtained.The chromaticity coordinate was calculated as(x=0.3238,y=0.3173),closing to the artificial daylight(D65,x=0.313,y=0.329)illuminant,and which indicates the potential application of near ultraviolet White light-emitting diodes(WLEDs).展开更多
Owing to their high luminous efficiency and tunable emission in both red light and far-red light regions,Mn^(4+)ion-activated phosphors have appealed significant interest in photoelectric and energy conversion devices...Owing to their high luminous efficiency and tunable emission in both red light and far-red light regions,Mn^(4+)ion-activated phosphors have appealed significant interest in photoelectric and energy conversion devices such as white light emitting diode(W-LED),plant cultivation LED,and temperature thermometer.Up to now,Mn^(4+)has been widely introduced into the lattices of various inorganic hosts for brightly redemitting phosphors.However,how to correlate the structure-activity relationship between host framework,luminescence property,and photoelectric device is urgently demanded.In this review,we thoroughly summarize the recent advances of Mn^(4+)doped phosphors.Meanwhile,several strategies like co-doping and defect passivation for improving Mn^(4+)emission are also discussed.Most importantly,the relationship between the protocols for tailoring the structures of Mn^(4+)doped phosphors,increased luminescence performance,and the targeted devices with efficient photoelectric and energy conversion efficiency is deeply correlated.Finally,the challenges and perspectives of Mn^(4+)doped phosphors for practical applications are anticipated.We cordially anticipate that this review can deliver a deep comprehension of not only Mn^(4+)luminescence mechanism but also the crystal structure tailoring strategy of phosphors,so as to spur innovative thoughts in designing advanced phosphors and deepening the applications.展开更多
The efficient separation of amphoteric organic compounds from dilute solutions is of great importance in the industrial field. In the present work, the reactive extractions of 4-hydroxypyridine(4-HP) with tributyl pho...The efficient separation of amphoteric organic compounds from dilute solutions is of great importance in the industrial field. In the present work, the reactive extractions of 4-hydroxypyridine(4-HP) with tributyl phosphate(TBP), di(2-ethylhexyl) phosphoric acid(D2EHPA) and TBP + D2EHPA dissolved in 1-octanol were investigated, respectively. The influences of the initial concentrations of TBP, D2EHPA and TBP + D2EHPA on distribution ratio(D) were discussed, as well as the reactive extraction mechanism were proposed. The obvious intensification effect was observed when the mixture of TBP and D2EHPA was used as extractant. The best extraction conditions were found to be of the molar ratio of D2EHPA and TBP at 2:1 and the equilibrium aqueous pH at 3.50-4.50. D values increased with the increase of the total concentration of TBP and D2EHPA in 1-octanol. Especially, the analysis on the extraction mechanisms clearly indicate(i) TBP in 1-octanol shows negligible reactive extraction toward 4-HP,(ii) D2EHPA in 1-octanol exhibits moderate extraction effect by forming 4-HP:D2EHPA(1:1) and 4-HP:2D2EHPA(1:2) type complexes, while(iii) D2EHPA in TBP/1-octanol demonstrates the maximum distribution ratio with the 4-HP:D2EHPA(1:1) type complex domination. The discussion provides new insights on the mechanism and opens a new way for the intensified extraction of amphoteric organic compounds by using the mixture of multiple extractants in the diluent.展开更多
Electrochemical N_(2) reduction reaction(eNRR) over Cu-based catalysts suffers from an intrinsically low activity of Cu for activation of stable N_(2) molecules and the limited supply of N_(2) to the catalyst due to i...Electrochemical N_(2) reduction reaction(eNRR) over Cu-based catalysts suffers from an intrinsically low activity of Cu for activation of stable N_(2) molecules and the limited supply of N_(2) to the catalyst due to its low solubility in aqueous electrolytes.Herein,we propose phosphorus-activated Cu electrocatalysts to generate electron-deficient Cu sites on the catalyst surface to promote the adsorption of N_(2) molecules.The eNRR system is further modified using a gas diffusion electrode(GDE) coated with polytetrafluoroethylene(PTFE) to form an effective three-phase boundary of liquid water-gas N_(2)-solid catalyst to facilitate easy access of N_(2) to the catalytic sites.As a result,the new catalyst in the flow-type cell records a Faradaic efficiency of 13.15% and an NH_(3) production rate of 7.69 μg h^(-1) cm^(-2) at-0.2 V_(RHE),which represent 3.56 and 59.2 times increases from those obtained with a pristine Cu electrode in a typical electrolytic cell.This work represents a successful demonstration of dual modification strategies;catalyst modification and N_(2) supplying system engineering,and the results would provide a useful platform for further developments of electrocatalysts and reaction systems.展开更多
基金Funded by the National Natural Science Foundation of China(No.52272072)the Independent Innovation Projects of the Hubei Longzhong Laboratory(No.2022ZZ-13)。
文摘A series of spinel-type Mg_(0.25-x)Al_(2.57)O_(3.79)N_(0.21):xMn^(2+)(MgAlON:xMn^(2+))phosphors were synthesized by the solid-state reaction route.The transparent ceramic phosphors were fabricated by pressureless sintering followed by hot-isostatic pressing(HIP).The crystal structure,luminescence and mechanical properties of the samples were systematically investigated.The transparent ceramic phosphors with tetrahedrally coordinated Mn^(2+)show strong green emission centered around 515 nm under blue light excitation.As the Mn^(2+)concentration increases,the crystal lattice expands slightly,resulting in a variation of crystal field and a slight red-shift of green emission peak.Six weak absorption peaks in the transmittance spectra originate from the spin-forbidden ^(4)T_(1)(^(4)G)→^(6)A_(1) transition of Mn^(2+).The decay time was found to decrease from 5.66 to 5.16 ms with the Mn^(2+)concentration.The present study contributes to the systematic understanding of crystal structure and properties of MgAlON:xMn^(2+)green-emitting transparent ceramic phosphor which has a potential application in high-power light-emitting diodes.
基金financially supported by the National Natural Science Foundation of China (52172192)the Young Top-Notch Talent of National Ten Thousand Talent Program (W03070054)。
文摘Graphene's large theoretical surface area and high conductivity make it an attractive anode material for potassium-ion batteries(PIBs).However,its practical application is hindered by small interlayer distance and long ion transfer distance.Herein,this paper aims to address the issue by introducing MXene through a simple and scalable method for assembling graphene and realizing ultrahigh P doping content.The findings reveal that MXene and P-C bonds have a "pillar effect" on the structure of graphene,and the P-C bond plays a primary role.In addition,N/P co-doping introduces abundant defects,providing more active sites for K^(+) storage and facilitating K^(+) adsorption.As expected,the developed ultrahigh phosphorous/nitrogen co-doped flexible reduced graphene oxide/MXene(NPrGM) electrode exhibits remarkable reversible discharge capacity(554 mA hg^(-1) at 0.05 A g^(-1)),impressive rate capability(178 mA h g^(-1) at 2 A g^(-1)),and robust cyclic stability(0.0005% decay per cycle after 10,000 cycles at 2 A g^(-1)).Furthermore,the assembled activated carbon‖NPrGM potassium-ion hybrid capacitor(PIHC) can deliver an impressive energy density of 131 W h kg^(-1) and stable cycling performance with 98.1% capacitance retention after5000 cycles at 1 A g^(-1).Such a new strategy will effectively promote the practical application of graphene materials in PIBs/PIHCs and open new avenues for the scalable development of flexible films based on two-dimensional materials for potential applications in energy storage,thermal interface,and electromagnetic shielding.
基金Funded by the Primary Research and Development Plan of Jiangsu Province(No.BE2016175)。
文摘In this study,a single-doped phosphors yttrium aluminum garnet(Y_(3)Al_(5)O_(12),YAG):Ce^(3+),single-doped YAG:Sc^(3+),and double-doped phosphors YAG:Ce^(3+),Sc^(3+) were prepared by spark plasma sintering(SPS)(lower than 1 200℃).The characteristics of synthesized phosphors were determined using scanning electron microscopy(SEM),X-ray diffraction(XRD),and fluorescence spectroscopy.During SPS,the lattice structure of YAG was maintained by the added Ce^(3+) and Sc^(3+).The emission wavelength of YAG:Ce^(3+) prepared from SPS(425-700 nm) was wider compared to that of YAG:Ce^(3+) prepared from high-temperature solid-state reaction(HSSR)(500-700 nm).The incorporation of low-dose Sc^(3+) in YAG:Ce^(3+) moved the emission peak towards the short wavelength.
基金National Natural Science Foundation of China,Grant/Award Number:NSFC‐U1904215National Research Foundation of Korea,Grant/Award Number:2021R1A2C2012127。
文摘Phase engineering is an efficient strategy for enhancing the kinetics of electrocatalytic reactions.Herein,phase engineering was employed to prepare high‐performance phosphorous‐doped biphase(1T/2H)MoS_(2)(P‐BMS)nanoflakes for hydrogen evolution reaction(HER).The doping of MoS_(2)with P atoms modifies its electronic structure and optimizes its electrocatalytic reaction kinetics,which significantly enhances its electrical conductivity and structural stability,which are verified by various characterization tools,including X‐ray photoelectron spectroscopy,high‐resolution transmission electron microscopy,X‐ray absorption near‐edge spectroscopy,and extended X‐ray absorption fine structure.Moreover,the hierarchically formed flakes of P‐BMS provide numerous catalytic surface‐active sites,which remarkably enhance its HER activity.The optimized P‐BMS electrocatalysts exhibit low overpotentials(60 and 72 mV at 10 mA cm^(−2))in H_(2)SO_(4)(0.5 M)and KOH(1.0 M),respectively.The mechanism of improving the HER activity of the material was systematically studied using density functional theory calculations and various electrochemical characterization techniques.This study has shown that phase engineering is a promising strategy for enhancing the H*adsorption of metal sulfides.
基金financial supports for this research from the National Basic Research Program of China(2018YFB1502104)the National Natural Science Foundation of China(51571179 and 51671173)the Open Fund of the Guangdong Provincial Key Laboratory of Advance Energy Storage Materials。
文摘Magnesium hydride has been seen as a potential material for solid state hydrogen storage,but the kinetics and thermodynamics obstacles have hindered its development and application.Three-dimensional flower-like TiO2@C and TiO2 were synthesized as the catalyst for MgH2 system and great catalytic activities are acquired in the hydrogen sorption properties.Experiments also show that the flower-like TiO2@C is superior to flower-like TiO2 in improving the hydrogen storage properties of MgH2.The hydrogen desorption onset and peak temperatures of flower-like TiO2 doped MgH2 is reduced to 199.2℃and 245.4℃,while the primitive MgH2 starts to release hydrogen at 294.6℃and the rapid dehydrogenation temperature is even as high as 362.6℃.The onset and peak temperatures of flower-like TiO2@C doped MgH2 are further reduced to 180.3℃and 233.0℃.The flower-like TiO2@C doped MgH2 composite can release6.0 wt%hydrogen at 250℃within 7 min,and 4.86 wt%hydrogen at 225℃within 60 min,while flowerlike TiO2 doped MgH2 can release 6.0 wt%hydrogen at 250℃within 8 min,and 3.89 wt%hydrogen at225℃within 60 min.Hydrogen absorption kinetics is also improved dramatically.Moreover,compared with primitive MgH2 and the flower-like TiO2 doped MgH2,the activation energy of flower-like TiO2@C doped MgH2 is significantly decreased to 67.10 kJ/mol.All the improvement of hydrogen sorption properties can be ascribed to the flower-like structure and the two-phase coexistence of TiO2 and amorphous carbon.Such phase composition and unique structure are proved to be the critical factor to improve the hydrogen sorption properties of MgH2,which can be considered as the new prospect for improving the kinetics of light-metal hydrogen storage materials.
基金financially supported by the Funding of Shenyang Ligong University’s Research Support Program for High-level Talents (No.1010147000802)the National Natural Science Foundation of China (Nos.52004165 and 51774070)。
文摘Flower-like ZnO microstructures were successfully produced using a hydrothermal method employing ZnSO_(4)/(NH_(4))_(2)SO_(4) as a raw material.The effect of the operating parameters of the hydrothermal temperature, OH^(-)/Zn^(2+) molar ratio, time, and amount of dispersant on the phase structure and micromorphology of the ZnO particles were investigated.The synthesis conditions of the flower-like ZnO microstructures were: hydrothermal temperature of 160℃, OH^(-)/Zn^(2+) molar ratio of 5:1, reaction time of 4 h, and 4 mL of dispersant.The flower-like ZnO microstructures were comprised of hexagon-shaped ZnO rods arranged in a radiatively.Degradation experiments of Rhodamine B with the flower-like ZnO microstructures demonstrated a degradation efficiency of 97.6% after 4 h of exposure to sunshine, indicating excellent photocatalytic capacity.The growth mechanism of the flower-like ZnO microstructures was presented.
基金Funded by the National Natural Science Foundation of China (No.21076131)the Foundation of Educational Commission of Hubei Province,China(No.D20122904)
文摘Calcium carbonate with three-dimensional chrysanthemun flower-like structure was successfully prepared from calcium chloride and sodium carbonate ethanol/water mixed solution by a simple precipitation method,using trisodium citrate as crystal modifier.The experimental results show that the three-dimensional structure of chrysanthemun flower-like calcium carbonate is built up with several symmetrical micrometer multi-layer petals arranged around the multi-layer pancake-liked center,and the micrometer center and petals are assemblied by a large number of nanometer spherical particles with size 10-20 nm.It is found that the amount of trisodium citrate,the ethanol volume content has an important influence on the formation of this morphology.A possible mechanism is proposed to explain the formation of three-dimensional chrysanthemun flower-like calcium carbonate according the results.Scanning electron microscopy(SEM),X-ray powder diffraction(XRD),flourier transform infrared spectroscopy(FT-IR),thermogravimety analysis(TG),transmission electron microscopy(TEM) equipped with energy-dispersive X-ray(EDX),and selected area electron diffraction(SAED) were used to characterize the crystals.
基金financially supported by the National Natural Science Foundation of China(No.21872045)。
文摘Finding easy-to-operate strategy to obtain anode material with well-designed structure and excellent electrochemical performance is necessary to promote the development of the future potassium-ion batteries(PIBs).In this work,we synthesized reduced graphene oxide doping flower-like Fe_(7)S_(8) nanosheets electrode materials using one-step hydrothermal strategy.The rGO@Fe_(7)S_(8) composite is composed of homogeneous Fe_(7)S_(8) and reduced graphene oxide thin nanosheets.This unique structure not only promotes the penetration of electrolyte and increases the conductive of the pure Fe_(7)S_(8) electrode materials,but also relieves the volume expansion of K^(+) during charge/discharge process.When applied this interesting anode electrode for PIBs,the rGO@Fe_(7)S_(8) exhibits excellent electrochemical performance.It delivers a high reversible specific capacity of 445 mAh g^(-1) at 50 mA g^(-1),excellent rate performance(284 mAhg^(-1)at 500 mA g^(-1) and 237 mAh g^(-1) at 1000 mA g^(-1)),and a high cycling stability at 100 mA g^(-1)(maintained 355 mAh g^(-1) after 300 cycles).
基金supported financially by the National Key Research and Development Program of China (2018YFB0104200)the Key Project of Strategic New Industry of Hunan Province (No. 2019GK2032)。
文摘Due to the high specific capacity and energy density, lithium–sulfur battery is regarded as a potential energy storage conversion system. However, the serious shuttle effect and the sluggish electrochemical reaction kinetics impede the practical use of lithium–sulfur battery. In the interests of breaking through the above knotty problems, herein we propose to use the polar flower-like Zn O modified by Bi OI nanoparticles as bifunctional host with catalytic and adsorption ability for polysulfides in lithium–sulfur battery.It can be found that this adsorption/catalytic host integrates the functions of adsorption and mutual catalytic conversion of polysulfides, in which the polar flower-like Zn O can effectively capture the polysulfides through strong polar-polar interaction, simultaneously the BiOI nanoparticles can accelerate the mutual conversion of polysulfides to Li2 S through reducing the activation energy and conversion energy barrier required for the electrochemical reaction. As a result, under a sulfur loading of 2.5 mg cm^(-2), the lithium–sulfur battery with Zn O/Bi OI/CNT/S as cathode reveals a considerable initial specific capacity of1267 mAh g^(-1) at a current density of 0.1 C. Even the current density increased to 1 C, the capacity can reach as 873.4 mAh g^(-1), together with a good capacity retention of 67.1% after 400 cycles. Therefore,after systematically study the positive effects of the flower-like ZnO modified by catalytic BiOI nanoparticles on the adsorption and catalytic conversion of polysulfides, this work provides a new idea for the development and application of high-performance lithium–sulfur batteries.
基金Supported by the National Natural Science Foundation of China(Nos.20671011,20331010,90406002and90406024)the 111 Project(No.B07012)the Key Laboratory of Structural Chemistry Foundation(No.060017).
文摘A novel flower-like hydrated magnesium carbonate hydroxide, Mg5 (CO3 )4 (OH)2·4H2O, with micro-structure composed of individual thin nano-sheets was synthesized using a facile solution route without the use of template or organic surfactant. Reaction time has an important effect on the final morphology of the product. The micro-structure and morphology of Mg5 (CO3)4 (OH)2·4H2O were characterized by means of X-ray diffractometry (XRD), fieldemission scanning electron microscopy(FE-SEM). Brunauer-Emmett-Teller(BET) surface areas of the samples were also measured. The probable formation mechanism of flower-like micro-structure was discussed. It was found that Mg5 (CO3)4( OH)2·4H2O with flower-like micro-structure was a novel and efficient catalyst for the synthesis of diphenyl carbonate (DPC) by transesterification of dimethyl carbonate (DMC) with phenol.
文摘Developing cost-effective electrocatalysts for oxygen evolution reaction (OER) in basic media is critical to hydrogen production from renewable energy. Herein, in-situ electrodeposited flower-like NiFeO x H y and NiFeO x H y /rGO composite electrocatalysts on Ni foam for OER are reported. The active sites of the flower-like electrocatalysts are increased significantly due to the enhanced NiFeO x H y surface areas and numerous exposed layered edges and edge defects. Reduced graphene oxide (rGO) has been introduced to fabricate NiFeO x H y /rGO composite film, further improving the conductivity and OER performance of the flower-like NiFeO x H y . The optimized NiFeO x H y /rGO exhibits superior OER performance with a Tafel slope of 29.11 mV/decade, an overpotential of 200 mV at 10 mA/cm 2 in 1 mol/L KOH and favorable long-term stability.
基金supported by the National Key R&D Program of China(No.2017YFB0602702-02)。
文摘In this work,a facile and effective strategy to prepare three-dimensional(3D)hierarchical flower-like Mg–Al layered double hydroxides(3D-LDH)was developed via a one-step double-drop coprecipitation method usingγ-Al 2O 3particles as a template.The characterization and experimental results showed that the calcined product,3D-LDO,features a large specific surface area of 204.2 m^(2)/g,abundant active sites,and excellent adsorption performance for Congo red(CR),methyl orange(MO),and methyl blue(MB).The maximum adsorption capacities of 3D-LDO for CR,MO,and MB were 1428.6,476.2,and 1666.7 mg/g,respectively;such performance is superior to that of most reported adsorbents.The adsorption mechanism of organic anionic dyes by 3D-LDO was extensively investigated and attributed to surface adsorption,the memory effect of 3D-LDO,and the unique 3D hierarchical flower-like structure of the adsorbent.Recycling performance tests revealed that3D-LDO has satisfactory reusability for the three organic anionic dyes.
基金Funded by the Key Public Welfare Special Project of Henan Province(No.201300311000)the Major Technical Innovation Project in Hubei Province of China(No.2020BED025)。
文摘Cement,phosphorous slag(PS),and steel slag(SS)were used to prepare low-carbon cementitious materials,and triisopropanolamine(TIPA)was used to improve the mechanical properties by controlling the hydration process.The experimental results show that,by using 0.06%TIPA,the compressive strength of cement containing 60%PS or 60%SS could be enhanced by 12%or 18%at 28 d.The presence of TIPA significantly affected the hydration process of PS and SS in cement.In the early stage,TIPA accelerated the dissolution of Al in PS,and the formation of carboaluminate hydrate was facilitated,which could induce the hydration;TIPA promoted the dissolution of Fe in SS,and the formation of Fe-monocarbonate,which was precipitated on the surface of SS,resulting in the postponement of hydration,especially for the high SS content.In the later stage,under the continuous solubilization effect of TIPA,the hydration of PS and SS could refine the pore structure.It was noted that compared with portland cement,the carbon emissions of cement-PS-TIPA and cement-SS-TIPA was reduced by 52%and 49%,respectively.
基金Project supported by the Joint Research Funds of Department of Science&Technology of Shaanxi Province and Northwestern Polytechnical University(Grant No.2020GXLH-Z-029)。
文摘Flower-like tungsten disulfide(WS_(2))with a diameter of 5-10μm is prepared by chemical vapor deposition(CVD).Scanning electron microscopy(SEM),energy dispersive spectrometer(EDS),Raman spectroscopy,and ultraviolet-visible(UV-vis)spectroscopy are used to characterize its morphological and optical properties,and its growth mechanism is discussed.The key factors for the formation of flower-like WS_(2)are determined.Firstly,the cooling process causes the generation of nucleation dislocations,and then the"leaf"growth of flower-like WS_(2)is achieved by increasing the temperature.
文摘This paper proposes a method of utilizing a flower-like MnOx nanozyme to conduct a colorimetric detection of ascorbic acid.The nanozyme is obtained by a chain of reaction of K3[Fe(CN)6],MnSO4·H2O,polyvinyl pyrrolidone(PVP),NH4F,ethanol,and water.During the experimental process,the flower-like nanozyme is added to the mixed solution,including phosphate buffer,H2O2,and 3,3’,5,5’-tetramethylbe nzidine(TMB).The optimum reaction condition as following:pH 3.0,30μL 500mM H2O2,25μL 92 mM TMB,and 30μL 0.1mM nanozyme.Under the optimum condition,the detection range is 2-26mM,and the linear detection range is 2-20mM.
基金Project supported by the National Key Research and Development Program of China (Grant No.2018YFB2200101)the National Natural Science Foundation of China (Grant Nos.62004078 and 61921005)+4 种基金Natural Science Foundation of Jiangsu Province (Grant No.BK20201073)Natural Science Foundation of Ningbo (Grant No.2021J068)ANR DONNA (Grant No.ANR-18-CE09-0034)Leading Innovative and Entrepreneur Team Introduction Program of Hangzhou (Grant No.TD2022012)partially supported by the CNRS Federation IRMA-FR 3095。
文摘Doping in Si nanocrystals is an interesting topic and directly studying the distribution of dopants in phosphorous/boron co-doping is an important issue facing the scientific community.In this study,atom probe tomography is performed to study the structures and distribution of impurity in phosphorous/boron co-doped Si nanocrystals/SiO_(2) multilayers.Compared with phosphorous singly doped Si nanocrystals,it is interesting to find that the concentration of phosphorous in co-doped samples can be significantly improved.Theoretical simulation suggests that phosphorous-boron pairs are formed in co-doped Si nanocrystals with the lowest formation energy,which also reduces the formation energy of phosphorous in Si nanocrystals.The results indicate that co-doping can promote the entry of phosphorous impurities into the near-surface and inner sites of Si nanocrystals,which provides an interesting way to regulate the electronic and optical properties of Si nanocrystals such as the observed enhancement of conductivity and sub-band light emission.
文摘The phosphors of KY_(1-x)(MoO_(4))_(2-y)(WO_(4))y:xLn^(3+)(Ln^(3+)=Tm^(3+),Dy^(3+),Eu^(3+))were synthesized by using a sol-gel method.Then,the crystal structure,luminescence properties,energy transfer,and white emission of the prepared materials were researched.The molar ratio of the anion group on the photoluminescence(PL)emission and excitation intensity were investigated,revealing that the optimum intensity could be obtained by using=3:1.The optimal Dy^(3+) doping concentration of KY(MoO_(4))1.5(WO4)0.5was obtained.In addition,the color-tunable emissions of Dy^(3+)/Eu^(3+)-codoped KY(MoO_(4))1.5(WO4)0.5phosphors were observed because of the effective energy transfer(ET)from Dy^(3+)to Eu^(3+)ions.Finally,by doping appropriate concentrations of Tm^(3+),Dy^(3+),and Eu^(3+)and different concentrations of(WO_(4))^(2-),white light emitting phosphors KY_(0.92)(WO_(4))2:0.01Tm^(3+),0.06Dy^(3+),0.01Eu^(3+)with excellent color-rending properties were obtained.The chromaticity coordinate was calculated as(x=0.3238,y=0.3173),closing to the artificial daylight(D65,x=0.313,y=0.329)illuminant,and which indicates the potential application of near ultraviolet White light-emitting diodes(WLEDs).
基金financially supported by the National Natural Science Foundation of China(52072101,51972088,U20A20122 and U1663225)the Program for Changjiang Scholars and Innovative Research Team in University(IRT_15R52)of the Chinese Ministry of Education+2 种基金the Program of Introducing Talents of Discipline to Universities-Plan 111(Grant No.B20002)from the Ministry of Science and Technology and the Ministry of Education of ChinaHubei Provincial Department of Education for the“Chutian Scholar”programsupported by the European Commission Interreg V FranceWallonie-Vlaanderen project“Depollut Air”。
文摘Owing to their high luminous efficiency and tunable emission in both red light and far-red light regions,Mn^(4+)ion-activated phosphors have appealed significant interest in photoelectric and energy conversion devices such as white light emitting diode(W-LED),plant cultivation LED,and temperature thermometer.Up to now,Mn^(4+)has been widely introduced into the lattices of various inorganic hosts for brightly redemitting phosphors.However,how to correlate the structure-activity relationship between host framework,luminescence property,and photoelectric device is urgently demanded.In this review,we thoroughly summarize the recent advances of Mn^(4+)doped phosphors.Meanwhile,several strategies like co-doping and defect passivation for improving Mn^(4+)emission are also discussed.Most importantly,the relationship between the protocols for tailoring the structures of Mn^(4+)doped phosphors,increased luminescence performance,and the targeted devices with efficient photoelectric and energy conversion efficiency is deeply correlated.Finally,the challenges and perspectives of Mn^(4+)doped phosphors for practical applications are anticipated.We cordially anticipate that this review can deliver a deep comprehension of not only Mn^(4+)luminescence mechanism but also the crystal structure tailoring strategy of phosphors,so as to spur innovative thoughts in designing advanced phosphors and deepening the applications.
基金supported by the Science and Technology Research Project of Henan Province (192102310490 and 212102310505)。
文摘The efficient separation of amphoteric organic compounds from dilute solutions is of great importance in the industrial field. In the present work, the reactive extractions of 4-hydroxypyridine(4-HP) with tributyl phosphate(TBP), di(2-ethylhexyl) phosphoric acid(D2EHPA) and TBP + D2EHPA dissolved in 1-octanol were investigated, respectively. The influences of the initial concentrations of TBP, D2EHPA and TBP + D2EHPA on distribution ratio(D) were discussed, as well as the reactive extraction mechanism were proposed. The obvious intensification effect was observed when the mixture of TBP and D2EHPA was used as extractant. The best extraction conditions were found to be of the molar ratio of D2EHPA and TBP at 2:1 and the equilibrium aqueous pH at 3.50-4.50. D values increased with the increase of the total concentration of TBP and D2EHPA in 1-octanol. Especially, the analysis on the extraction mechanisms clearly indicate(i) TBP in 1-octanol shows negligible reactive extraction toward 4-HP,(ii) D2EHPA in 1-octanol exhibits moderate extraction effect by forming 4-HP:D2EHPA(1:1) and 4-HP:2D2EHPA(1:2) type complexes, while(iii) D2EHPA in TBP/1-octanol demonstrates the maximum distribution ratio with the 4-HP:D2EHPA(1:1) type complex domination. The discussion provides new insights on the mechanism and opens a new way for the intensified extraction of amphoteric organic compounds by using the mixture of multiple extractants in the diluent.
基金supported by the Climate Change Response Project (NRF-2019M1A2A2065612)the Brainlink Project (NRF2022H1D3A3A01081140)+3 种基金the NRF-2021R1A4A3027878 and the No. RS-2023-00212273 funded by the Ministry of Science and ICT of Korea via National Research Foundationresearch funds from Hanhwa Solutions Chemicals (1.220029.01)UNIST (1.190013.01)supported by the Institute for Basic Science (IBS-R019-D1)。
文摘Electrochemical N_(2) reduction reaction(eNRR) over Cu-based catalysts suffers from an intrinsically low activity of Cu for activation of stable N_(2) molecules and the limited supply of N_(2) to the catalyst due to its low solubility in aqueous electrolytes.Herein,we propose phosphorus-activated Cu electrocatalysts to generate electron-deficient Cu sites on the catalyst surface to promote the adsorption of N_(2) molecules.The eNRR system is further modified using a gas diffusion electrode(GDE) coated with polytetrafluoroethylene(PTFE) to form an effective three-phase boundary of liquid water-gas N_(2)-solid catalyst to facilitate easy access of N_(2) to the catalytic sites.As a result,the new catalyst in the flow-type cell records a Faradaic efficiency of 13.15% and an NH_(3) production rate of 7.69 μg h^(-1) cm^(-2) at-0.2 V_(RHE),which represent 3.56 and 59.2 times increases from those obtained with a pristine Cu electrode in a typical electrolytic cell.This work represents a successful demonstration of dual modification strategies;catalyst modification and N_(2) supplying system engineering,and the results would provide a useful platform for further developments of electrocatalysts and reaction systems.