S and Co co-doped carbon catalysts were prepared via pyrolysis of MOF-71 and thiourea mixtures at 800℃at a mass ratio of MOF-71 to thiourea of 1:0.1 to effectively activate peroxymonosulfate(PMS)for methylene blue(MB...S and Co co-doped carbon catalysts were prepared via pyrolysis of MOF-71 and thiourea mixtures at 800℃at a mass ratio of MOF-71 to thiourea of 1:0.1 to effectively activate peroxymonosulfate(PMS)for methylene blue(MB)degradation.The effects of two different mixing routes were identified on the MB degradation performance.Particularly,the catalyst obtained by the alcohol solvent evaporation(MOF-AEP)mixing route could degrade 95.60%MB(50 mg/L)within 4 min(degradation rate:K=0.78 min^(-1)),which was faster than that derived from the direct grinding method(MOF-DGP,80.97%,K=0.39 min^(-1)).X-ray photoelectron spectroscopy revealed that the Co-S content of MOF-AEP(43.39at%)was less than that of MOF-DGP(54.73at%),and the proportion of C-S-C in MOF-AEP(13.56at%)was higher than that of MOF-DGP(10.67at%).Density functional theory calculations revealed that the adsorption energy of Co for PMS was -2.94 eV when sulfur was doped as C-S-C on the carbon skeleton,which was higher than that when sulfur was doped next to cobalt in the form of Co-S bond(-2.86 eV).Thus,the C-S-C sites might provide more contributions to activate PMS compared with Co-S.Furthermore,the degradation parameters,including pH and MOF-AEP dosage,were investigated.Finally,radical quenching experiments and electron paramagnetic resonance(EPR)measurements revealed that ^(1)O_(2)might be the primary catalytic species,whereas·O~(2-)might be the secondary one in degrading MB.展开更多
Sodium-ion batteries(SIBs) and hybrid capacitors(SIHCs) have garnered significant attention in energy storage due to their inherent advantages,including high energy density,cost-effectiveness,and enhanced safety.Howev...Sodium-ion batteries(SIBs) and hybrid capacitors(SIHCs) have garnered significant attention in energy storage due to their inherent advantages,including high energy density,cost-effectiveness,and enhanced safety.However,developing high-performance anode materials to improve sodium storage performa nce still remains a major challenge.Here,a facile one-pot method has been developed to fabricate a hybrid of MoSeTe nanosheets implanted within the N,F co-doped honeycomb carbon skeleton(MoSeTe/N,F@C).Experimental results demonstrate that the incorporation of large-sized Te atoms into MoSeTe nanosheets enlarges the layer spacing and creates abundant anion vacancies,which effectively facilitate the insertion/extraction of Na^(+) and provide numerous ion adsorption sites for rapid surface capacitive behavior.Additionally,the heteroatoms N,F co-doped honeycomb carbon skeleton with a highly conductive network can restrain the volume expansion and boost reaction kinetics within the electrode.As anticipated,the MoSeTe/N,F@C anode exhibits high reversible capacities along with exceptional cycle stability.When coupled with Na_(3)V_(2)(PO_(4))_(3)@C(NVPF@C) to form SIB full cells,the anode delivers a reversible specific capacity of 126 mA h g^(-1) after 100 cycles at 0.1 A g^(-1).Furthermore,when combined with AC to form SIHC full cells,the anode demonstrates excellent cycling stability with a reversible specific capacity of50 mA h g^(-1) keeping over 3700 cycles at 1.0 A g^(-1).In situ XRD,ex situ TEM characterization,and theoretical calculations(DFT) further confirm the reversibility of sodium storage in MoSeTe/N,F@C anode materials during electrochemical reactions,highlighting their potential for widespread practical application.This work provides new insights into the promising utilization of advanced transition metal dichalcogenides as anode materials for Na^(+)-based energy storage devices.展开更多
A series of photocatalysts of un-doped, single-doped and co-doped nanometer titanium diox- ide (TiO2) have been successfully prepared by template method using Fe(NO3)3.9H2O, La(NO3)3.6H2O, and tetrabutyl titanat...A series of photocatalysts of un-doped, single-doped and co-doped nanometer titanium diox- ide (TiO2) have been successfully prepared by template method using Fe(NO3)3.9H2O, La(NO3)3.6H2O, and tetrabutyl titanate as precursors and glucan as template. Scanning electron microscopy, X-ray diffraction, and N2 adsorption-desorption measurement were employed to characterize the morphology, crystal structure and surface structure of the samples. The photo-absorbance of the obtained catalysts was measured by UV-Vis absorption spectroscopy, and the photocatalytic activities of the prepared samples under UV and visible light were estimated by measuring the degradation rate of methyl orange in an aqueous solution. The characterizations indicated that the prepared photocatalysts consisted of anatase phase and possessed high surface area of ca. 163-176 m2/g. It was shown that the Fe and La co-doped nano-TiO2 could be activated by visible light and could thus be used as an effective catalyst in photo-oxidation reactions. The synergistic effect of Fe and La co-doping played an important role in improving the photocatalytic activity. In addition, the possibility of cyclic usage of co-doped nano-TiO2 was also confirmed, the photocatalytic activity of codoped nano-TiO2 remained above 89.6% of the fresh sample after being used four times.展开更多
In order to improve the photocatalytic performance of mesoporous titania under visible light, a series of photocatalysts of S and Ag co-doped mesoporous titania have been successfully prepared by template method using...In order to improve the photocatalytic performance of mesoporous titania under visible light, a series of photocatalysts of S and Ag co-doped mesoporous titania have been successfully prepared by template method using thiourea, AgNO3 and tetrabutyl titanate as precursors and Pluronic P123 (EO20PO70EO20) as template. Scanning electron microscopy (SEM), X-ray diffraction (XRD), nitrogen adsorption-desorption measurements, and UV-visible spectroscopy (UV-Vis) were employed to characterize the morphology, crystal structure, surface structure, and optical absorption properties of the samples. The microcrystal of the photocatalysts consisted of anatase phase and was approximately present in the form of spherical particle. The photocatalytic performance was studied by photodegradation methyl orange (MO) in water under UV and visible light irradiation. The calcination temperature and the doping content influenced the photoactivity. In addition, the possibility of cyclic usage of co-doped mesoporous titania was also confirmed, the photocatalytic activity of mesoporous titania remained above 89% of that of the fresh sample after being used four times. It was shown that the co-doped mesoporous titania could be activated by visible light and could thus be potentially applied for the treatment of water contaminated by organic pollutants. The synergistic effect of sulfur and silver co-doping played an important role in improving the photocatalytic activity.展开更多
The nitrogen and fluorine co doped TiO 2 polycrystalline powder was synthesized by calcinations of the hydrolysis product of tetra butyl titanate with ammonium fluoride. Nitrogen and fluorine co doping causes the abso...The nitrogen and fluorine co doped TiO 2 polycrystalline powder was synthesized by calcinations of the hydrolysis product of tetra butyl titanate with ammonium fluoride. Nitrogen and fluorine co doping causes the absorption edge of TiO 2 to shift to a lower energy region. The photocatalytic activity of co doped TiO 2 with anatase phases was found to be 2 4 times higher than that of the commercial TiO 2 photocatalyst Degussa P25 for phenol decomposition under visible light irradiation. The co doped TiO 2 powders only contain anatase phases even at 1000℃. Apparently, ammonium fluoride added retarded phase transformation of the TiO 2 powders from anatase to rutile. The substitutional fluorine and interstitial nitrogen atoms in co doped TiO 2 polycrystalline powder were responsible for the vis light response and caused the absorption edge of TiO 2 to shift to a lower energy region.展开更多
This paper reports that the Zn0.95Co0.05O polycrystalline powder and thin film were prepared by sol-gel technique under the similar preparation conditions. The former does not show typical ferromagnetic behaviour, whi...This paper reports that the Zn0.95Co0.05O polycrystalline powder and thin film were prepared by sol-gel technique under the similar preparation conditions. The former does not show typical ferromagnetic behaviour, while the latter exhibits obvious ferromagnetic properties at 5 K and room temperature. The UV-vis spectra and x-ray absorption spectra show that Co2+ ions are homogeneously incorporated into ZnO lattice without forming secondary phases.The distinct difference between film and powder sample is the c-axis (002) preferential orientation indicated by the x-ray diffraction pattern and field emission scanning electron microscopy measurement, which may be the reason why Zn0.95Co0.05O film shows ferromagnetic behaviour.展开更多
Transition metal-doping could effectively extend the light response range of TiO _2 photocatalysts from the ultraviolet(UV)to the visible region.Co-doped brookite titanium dioxide(Co–TiO_2)photocatalysts were synthes...Transition metal-doping could effectively extend the light response range of TiO _2 photocatalysts from the ultraviolet(UV)to the visible region.Co-doped brookite titanium dioxide(Co–TiO_2)photocatalysts were synthesized via the hydrothermal method with titanium tetrachloride as the raw material and cobalt chloride hexahydrate as the dopant.The prepared Co–TiO_2 photocatalysts were characterized by X-ray diffraction(XRD),scanning electron microscopy(SEM),transmission electron microscopy(TEM),Raman spectroscopy,X-ray photoelectron spectroscopy(XPS)and UV–Vis diffuse reflectance spectroscopy(UV–Vis DRS).The photocatalytic activities of Co–TiO _2 photocatalysts were evaluated by photocatalytic degradation of isopropanol alcohol(IPA),a typical volatile organic compound(VOC),under visible light.The influences ofdifferent Co doping rates,initial concentrations of IPA gas and the amounts of photocatalyst addition were also studied.At the same time,the enhancement mechanism ofcobalt ions as a trap for photogenerated holes was discussed.Thus,we found the optimum doping rate,initial concentration of IPA gas and amount of photocatalyst to add.The results show that the mesoporous Co–TiO _2 photocatalysts possess smaller size particles,larger specific surface area,lower forbidden bandgap energy(Eg)and better photocatalytic activity than pure brookite TiO _2.When the doping of Co was 7% by mass,the initial concentration ofIPA gas was 1.0×10^(-6 )mol/L and the addition of Co–TiO_2 photocatalysts was 50 mg,the best photocatalytic activity was achieved.Furthermore,the degradation rate ofIPA was up to 91%,which shows great potential for waste water treatment.展开更多
Renewable lignin used for synthesizing materials has been proven to be highly potential in specific electrochemistry.Here,we report a simple method to synthesize nitrogen and sulfur co-doped carbon nanosheets by using...Renewable lignin used for synthesizing materials has been proven to be highly potential in specific electrochemistry.Here,we report a simple method to synthesize nitrogen and sulfur co-doped carbon nanosheets by using bagasse lignin,denoted as lignin-derived carbon(LC).By adjusting the ratio of nitrogen source and annealing temperature,we obtained the ultrathin graphitic lignin carbon(LC-4-1000)with abundant wrinkles with high surface area of 1208 m2g_1 and large pore volume of 1.40 cm3g_1.In alkaline medium,LC-4-1000 has more positive half-wave potential and nearly current density compared to commercial Pt/C for oxygen reduction reaction(ORR).More importantly,LC-4-1000 also exhibits comparable activity and superior stability for ORR in acid medium due to its high graphitic N ratio and a direct four electron pathway for ORR.This study develops a cost-effective and highly efficient method to prepare biocarbon catalyst for ORR in fuel cells.展开更多
(La, N) co-doped TiO2 photocatalysts were synthesized using TiC14 sol-gel autoignidng synthesis (SAS) starting from a complex compound system of TiCl4-La(NO3)3-citric acid-NH4NO3-NHyH2O, in which the (La, N) c...(La, N) co-doped TiO2 photocatalysts were synthesized using TiC14 sol-gel autoignidng synthesis (SAS) starting from a complex compound system of TiCl4-La(NO3)3-citric acid-NH4NO3-NHyH2O, in which the (La, N) co-doped process was accompushed in the formation of TiO2 nanocrystals. The prepared samples were characterized by using X-ray diffraction (XRD), X-ray photoemission spectroscopy (XPS) and UV-vis diffuse reflectance spectra. The results indicated that nitrogen and lanthanum were incorporated into the lattice and interstices of titania nanocrystals, which resulted in narrowing the band gap and promoting the separation of photoexcited hole-electron pairs, respectively, and showing expected red-shifts and enhanced photocatalytic activity under visible light. The mechanism on nitrogen doping and enhancement in photocatalyfic activity of (La, N) co-doped titania by SAS was discussed in detail.展开更多
Oxidized asphaltene (OA), a thermosetting material with plenty of functional groups, is synthesized from asphaltene (A) using HNO3]HzSO4 as the oxidizing agent. Boron, nitrogen co-doped porous carbon (BNC-OA) is...Oxidized asphaltene (OA), a thermosetting material with plenty of functional groups, is synthesized from asphaltene (A) using HNO3]HzSO4 as the oxidizing agent. Boron, nitrogen co-doped porous carbon (BNC-OA) is prepared by carbonization of the mixture of boric acid and OA at 1173 K in an argon atmosphere. X-ray photoelectron spectroscopy (XPS) characterization reveals that the BNC-OA has a nitrogen content of 3.26 at.% and a boron content of 1.31 at.%, while its oxidation-free counterpart (BNC-SA) has a nitrogen content of 1.61 at.% and a boron content of 3.02 at.%. The specific surface area and total pore volume of BNC-OA are 1103 m2·g^-1 and 0.921 cm3·g^-1, respectively. At a current density of 0.1 A·g^-1, the specific capacitance of BNC-OA is 335 F·g^-1 and the capacitance retention can still reach 83% at 1 A·g^-1. The analysis shows that the superior electrochemical performance of the BNC-OA is attributed to the pseudocapacitance behavior of surface heteroatom functional groups and an abundant pore-structure. Boron, nitrogen co-doped porous carbon is a promising electrode material for supercapacitors.展开更多
A novel lanthanum and sulfur co-doped TiO2 photocatalyst was synthesized by precipitation- dipping method, and characterized by X-ray diffraction(XRD), transmission electron microscopy(TEM) and UV-Vis diffuse refl...A novel lanthanum and sulfur co-doped TiO2 photocatalyst was synthesized by precipitation- dipping method, and characterized by X-ray diffraction(XRD), transmission electron microscopy(TEM) and UV-Vis diffuse reflectance spectroscopy. Compared with the S-doped TiO, La-doped TiO2 and the standard Degussa P25 photocatalysts, the lanthanum and sulfur co-doped TiO2 photocatalyst (the molar percentage of La is 3.0%) calcined at 450 ℃ for 2 h showed the strongest absorption for visible light and highest activities for degradation of reactive blue 19 dye in aqueous solution under visible light(λ〉400 nm) irradiation. It was also discovered that the co-doping of lanthanum and sulfur hindered the aggregation and growth of TiO2 particles, and the doping of lanthanum reduced slightly the phase transition temperature ofTiO2 from anatase to rutile.展开更多
Exploring inexpensive and efficient bifunctional electrocatalysts for oxygen reduction reaction(ORR) and oxygen evolution reaction(OER) is critical for rechargeable metal-air batteries. Herein, we report a new 3D hier...Exploring inexpensive and efficient bifunctional electrocatalysts for oxygen reduction reaction(ORR) and oxygen evolution reaction(OER) is critical for rechargeable metal-air batteries. Herein, we report a new 3D hierarchical sulfur and nitrogen co-doped carbon nanocages(hSNCNC) as a promising bifunctional oxygen electrocatalyst by an in-situ MgO template method with pyridine and thiophene as the mixed precursor. The as-prepared h SNCNC exhibits a positive half-wave potential of 0.792 V(vs. reversible hydrogen electrode, RHE) for ORR, and a low operating potential of 1.640 V at a 10 mA cm-2 current density for OER. The reversible oxygen electrode index is 0.847 V, far superior to commercial Pt/C and IrO2,which reaches the top level of the reported bifunctional catalysts. Consequently, the hSNCNC as air cathodes in an assembled Zn-air battery features low charge/discharge overpotential and long lifetime. The remarkable properties arises from the introduced multiple heteroatom dopants and stable 3D hierarchical structure with multi-scale pores, which provides the abundant uniform high-active S and N species and efficient charge transfer as well as mass transportation. These results demonstrate the potential strategy in developing suitable carbon-based bi-/multi-functional catalysts to enable the next generation of the rechargeable metal-air batteries.展开更多
Silicon-based(Si)materials are promising anodes for lithium-ion batteries(LIBs)because of their ultrahigh theoretical capacity of 4200 mA h g^(−1).However,commercial applications of Si anodes have been hindered by the...Silicon-based(Si)materials are promising anodes for lithium-ion batteries(LIBs)because of their ultrahigh theoretical capacity of 4200 mA h g^(−1).However,commercial applications of Si anodes have been hindered by their drastic volume variation(∼300%)and low electrical conductivity.Here,to tackle the drawbacks,a hierarchical Si anode with double-layer coatings of a SiOx inner layer and a nitrogen(N),boron(B)co-doped carbon(C-NB)outer layer is elaborately designed by copyrolysis of Si-OH structures and a H3BO_(3)-doped polyaniline polymer on the Si surface.Compared with the pristine Si anodes(7mA h g^(−1) at 0.5 A g^(−1) after 340 cycles and 340 mA h g^(−1) at 5 A g^(−1)),the modified Si-based materials(Si@SiOx@C-NB nanospheres)present su perior cycling stability(reversible 1301 mA h g^(−1) at 0.5 A g^(−1) after 340 cycles)as well as excellent rate capability(690mA h g^(−1) at 5 A g^(−1))when used as anodes in LIBs.The unique double-layer coating structure,in which the inner amorphous SiOx layer acts as a buffer matrix and the outer defect-rich carbon enhances the electron diffusion of the whole anode,makes it possible to de liver excellent electrochemical properties.These results indicate that our double-layer coating strategy is a promising approach not only for the devel opment of sustainable Si anodes but also for the design of multielement-doped carbon nanomaterials.展开更多
The development of simple and effective strategies to prepare electrocatalysts,which possess unique and stable structures comprised of metal/nonmetallic atoms for oxygen reduction reaction(ORR)and oxygen evolution rea...The development of simple and effective strategies to prepare electrocatalysts,which possess unique and stable structures comprised of metal/nonmetallic atoms for oxygen reduction reaction(ORR)and oxygen evolution reaction(OER),is currently an urgent issue.Herein,an efficient bifunctional electrocatalyst featured by ultralong N,S-doped carbon nano-hollow-sphere chains about 1300 nm with encapsulated Co nanoparticles(Co-CNHSCs)is developed.The multifunctional catalytic properties of Co together with the heteroatom-induced charge redistribution(i.e.,modulating the electronic structure of the active site)result in superior catalytic activities toward OER and ORR in alkaline media.The optimized catalyst Co-CNHSC-3 displays an outstanding electrocatalytic ability for ORR and OER,a high specific capacity of 1023.6 mAh gZn^(-1),and excellent reversibility after 80 h at 10mA cm^(-2)in a Zn-air battery system.This work presents a new strategy for the design and synthesis of efficient multifunctional carbon-based catalysts for energy storage and conversion devices.展开更多
Nitrogen and sulfur co-doped porous nanocarbon (ZIF-C-N-S) catalyst was successfully synthesized derived from ZIF-8 and thiourea precursors.The electrochemical measurements indicate that the as-obtained ZIF-C-N-S cata...Nitrogen and sulfur co-doped porous nanocarbon (ZIF-C-N-S) catalyst was successfully synthesized derived from ZIF-8 and thiourea precursors.The electrochemical measurements indicate that the as-obtained ZIF-C-N-S catalyst exhibits higher electrocatalytic activity for oxygen reduction reaction (ORR) in alkaline electrolyte and superior durability-longer than commercial Pt/C catalyst.The enhancment of electrocatalytic activity mainly be come from the open pore structure,large specific surface area as well as the synergistic effect resulted from the co-doping of N and S atoms.In addition,the ZIF-C-N-S catalyst is also used as the air cathode catalyst in the microbial fuel cell (MFC) device.The maximum power density and stable output voltage of ZIF-C-N-S based MFC are 1315 mW/m2 and 0.48 V,respectively,which is better than that of Pt/C based MFC.展开更多
Nitrogen and phosphorus co-doped graphene quantum dot-modified Bi5O7 I(NPG/Bi5O7 I)nanorods were fabricated via a simple solvothermal method.The morphology,structure,and optical properties of the as-prepared samples w...Nitrogen and phosphorus co-doped graphene quantum dot-modified Bi5O7 I(NPG/Bi5O7 I)nanorods were fabricated via a simple solvothermal method.The morphology,structure,and optical properties of the as-prepared samples were investigated by X-ray diffraction,scanning electron microscopy,high-resolution transmission electron microscopy,X-ray photoelectron spectroscopy(XPS),and diffused reflectance spectroscopy.The photocatalytic performance was estimated by degrading the broad-spectrum antibiotics tetracycline and enrofloxacin under visible light irradiation.The photodegradation activity of Bi5O7 I improved after its surface was modified with NPGs,which was attributed to an increase in the photogenerated charge transport rate and a decrease in the electron-hole pair recombination efficiency.From the electron spin resonance spectra,XPS valence band data,and free radical trapping experiment results,the main active substances involved in the photocatalytic degradation process were determined to be photogenerated holes and superoxide radicals.A possible photocatalytic degradation mechanism for NPG/Bi5O7 I nanorods was proposed.展开更多
yb^3+:Er^3+ co-doped oxy-fluoride ceramics glass has been prepared. The mechanism of up-conversion emissions about Er^3+ was discussed, and the temperature properties of green up-conversion fluorescence between 30...yb^3+:Er^3+ co-doped oxy-fluoride ceramics glass has been prepared. The mechanism of up-conversion emissions about Er^3+ was discussed, and the temperature properties of green up-conversion fluorescence between 303 and 823 K were investigated. The results show that the sensitivity of this sample reaches its maximum value, about 0.0047 K^-1, when the temperature is 383 K, indicating that this kind of sample can be used as high temperature and high sensitivity optical temperature sensor.展开更多
Developing high power and energy supercapacitors(SCs)is a long-pursued goal for the application in transportation and energy storage station.Herein,a rationally-designed Co-doped nickel oxide nanosheets@carbon-welded ...Developing high power and energy supercapacitors(SCs)is a long-pursued goal for the application in transportation and energy storage station.Herein,a rationally-designed Co-doped nickel oxide nanosheets@carbon-welded carbon nanotube foam(Co-doped NiO@WCNTF)as freestanding electrode is successfully prepared for high power and energy SCs.The WCNTF framework with high specific surface area provides three dimensional highly conductive network for fast charge transport and ensures high loading of active materials(9.2 mg/cm2).Moreover,porous Co-doped NiO nanosheets uniformly anchored on the WCNTF framework enable rapid charge kinetics due to the high intrinsic conductivity of Co-doped Ni O nanosheets and their good contact with conductive WCNTF substrate.As a result,the unique integrated electrode with 3D architecture exhibits an ultrahigh specific capacitance of 11.45 F/cm2 at 5 mA/cm2,outstanding rate capability(11.45 F/cm2 at 5 mA/cm2 and a capacitance retention of 86.2%at 30 mA/cm2)and good cycling stability,suggesting great potential for high performance supercapacitor.展开更多
The electronic structure, magnetic properties, and optical properties of Co-doped AIN are investigated based upon the Perdew-Burke-Ernzerhof form of generalized gradient approximation within the density functional the...The electronic structure, magnetic properties, and optical properties of Co-doped AIN are investigated based upon the Perdew-Burke-Ernzerhof form of generalized gradient approximation within the density functional theory. The band gaps narrowing of AI1-x Cox N are found with the increase of Co concentrations. The analyses of the band structures and density of states show that AI1-xCoxN alloys exhibit a halfometallie character. Moreover, we have succeeded in demonstrating that Co doped AIN system in x = 0.125 is always antiferromagnetie, which is in good agreement with the experimental results. Besides, it is shown that the insertion of Co atom leads to redshift of the optical absorption edge. Finally, the optical constants of pure A1N and AI1-xCoxN alloy, such as loss function, refractive index and reflectivity, are discussed.展开更多
Although there have been many reports of metal doping to ameliorate the drawbacks of hematite as the photoanode for water oxidation, most of them focused on monometallic doping, and only a few of them payed attention ...Although there have been many reports of metal doping to ameliorate the drawbacks of hematite as the photoanode for water oxidation, most of them focused on monometallic doping, and only a few of them payed attention to bimetallic doping. What is worse, the synergetic mechanism between two metal dopants was not sufficiently studied, especially the density functional theory(DFT) calculation. In this work, the n-type hematite was synthesized by introducing Ti dopant into hematite through the hydrothermal method, and dipping-sintering treatment was employed to further introduce homogeneously dispersed Zn dopant into that, forming the Ti, Zn co-doped hematite. Under the optimal condition, Tidoped hematite photoanode reached approximately 2-times enhancement of the photocurrent density compared with the pristine one at 1.23 V vs. RHE, while Ti, Zn co-doped hematite anode obtained another25% elevation. UV–Vis spectroscopy, Mott–Schottky plots, EIS analysis, photo-oxidation of hole scavenger(H2O2), and DFT calculation were employed to understand the role of Ti, Zn dopant. Based on the obtained results, the synergetic mechanism of two dopants was discussed, i.e., the improvement of PEC performance of Ti, Zn co-doped hematite photoanode was possibly attributed to greater carrier density and improved charge separation efficiency at the surface of hematite. This work provides new strategy and understanding of the improvement of PEC performance of hematite by doping engineering.展开更多
基金financially supported by the National Natural Science Foundation of China(Nos.51602018 and 51902018)the Natural Science Foundation of Beijing Municipality(No.2154052)+3 种基金the China Postdoctoral Science Foundation(No.2014M560044)the Fundamental Research Funds for the Central Universities(No.FRF-MP-20-22)USTB Research Center for International People-to-people Exchange in Science,Technology and Civilization(No.2022KFYB007)Education and Teaching Reform Foundation at University of Science and Technology Beijing(Nos.2023JGC027,KC2022QYW06,and KC2022TS09)。
文摘S and Co co-doped carbon catalysts were prepared via pyrolysis of MOF-71 and thiourea mixtures at 800℃at a mass ratio of MOF-71 to thiourea of 1:0.1 to effectively activate peroxymonosulfate(PMS)for methylene blue(MB)degradation.The effects of two different mixing routes were identified on the MB degradation performance.Particularly,the catalyst obtained by the alcohol solvent evaporation(MOF-AEP)mixing route could degrade 95.60%MB(50 mg/L)within 4 min(degradation rate:K=0.78 min^(-1)),which was faster than that derived from the direct grinding method(MOF-DGP,80.97%,K=0.39 min^(-1)).X-ray photoelectron spectroscopy revealed that the Co-S content of MOF-AEP(43.39at%)was less than that of MOF-DGP(54.73at%),and the proportion of C-S-C in MOF-AEP(13.56at%)was higher than that of MOF-DGP(10.67at%).Density functional theory calculations revealed that the adsorption energy of Co for PMS was -2.94 eV when sulfur was doped as C-S-C on the carbon skeleton,which was higher than that when sulfur was doped next to cobalt in the form of Co-S bond(-2.86 eV).Thus,the C-S-C sites might provide more contributions to activate PMS compared with Co-S.Furthermore,the degradation parameters,including pH and MOF-AEP dosage,were investigated.Finally,radical quenching experiments and electron paramagnetic resonance(EPR)measurements revealed that ^(1)O_(2)might be the primary catalytic species,whereas·O~(2-)might be the secondary one in degrading MB.
基金supported by the National Natural Science Foundation of China(No.52002320,and 51972267)the China Postdoctoral Science Foundation(No.2022M712574)+3 种基金the Science Foundation of Shaanxi Province(2022GD-TSLD-18,No.2023-JCZD-03)Natural Science Foundation of Shaanxi Province(No.2022GY-372,2021GY-153)Industrial Projects Foundation of Ankang Science and Technology Bureau(No.AK2020-GY02-2)the Platform Construction Projects and Technology Service Teams of Ankang University(No.2021AYPT12 and 2022TD07)。
文摘Sodium-ion batteries(SIBs) and hybrid capacitors(SIHCs) have garnered significant attention in energy storage due to their inherent advantages,including high energy density,cost-effectiveness,and enhanced safety.However,developing high-performance anode materials to improve sodium storage performa nce still remains a major challenge.Here,a facile one-pot method has been developed to fabricate a hybrid of MoSeTe nanosheets implanted within the N,F co-doped honeycomb carbon skeleton(MoSeTe/N,F@C).Experimental results demonstrate that the incorporation of large-sized Te atoms into MoSeTe nanosheets enlarges the layer spacing and creates abundant anion vacancies,which effectively facilitate the insertion/extraction of Na^(+) and provide numerous ion adsorption sites for rapid surface capacitive behavior.Additionally,the heteroatoms N,F co-doped honeycomb carbon skeleton with a highly conductive network can restrain the volume expansion and boost reaction kinetics within the electrode.As anticipated,the MoSeTe/N,F@C anode exhibits high reversible capacities along with exceptional cycle stability.When coupled with Na_(3)V_(2)(PO_(4))_(3)@C(NVPF@C) to form SIB full cells,the anode delivers a reversible specific capacity of 126 mA h g^(-1) after 100 cycles at 0.1 A g^(-1).Furthermore,when combined with AC to form SIHC full cells,the anode demonstrates excellent cycling stability with a reversible specific capacity of50 mA h g^(-1) keeping over 3700 cycles at 1.0 A g^(-1).In situ XRD,ex situ TEM characterization,and theoretical calculations(DFT) further confirm the reversibility of sodium storage in MoSeTe/N,F@C anode materials during electrochemical reactions,highlighting their potential for widespread practical application.This work provides new insights into the promising utilization of advanced transition metal dichalcogenides as anode materials for Na^(+)-based energy storage devices.
文摘A series of photocatalysts of un-doped, single-doped and co-doped nanometer titanium diox- ide (TiO2) have been successfully prepared by template method using Fe(NO3)3.9H2O, La(NO3)3.6H2O, and tetrabutyl titanate as precursors and glucan as template. Scanning electron microscopy, X-ray diffraction, and N2 adsorption-desorption measurement were employed to characterize the morphology, crystal structure and surface structure of the samples. The photo-absorbance of the obtained catalysts was measured by UV-Vis absorption spectroscopy, and the photocatalytic activities of the prepared samples under UV and visible light were estimated by measuring the degradation rate of methyl orange in an aqueous solution. The characterizations indicated that the prepared photocatalysts consisted of anatase phase and possessed high surface area of ca. 163-176 m2/g. It was shown that the Fe and La co-doped nano-TiO2 could be activated by visible light and could thus be used as an effective catalyst in photo-oxidation reactions. The synergistic effect of Fe and La co-doping played an important role in improving the photocatalytic activity. In addition, the possibility of cyclic usage of co-doped nano-TiO2 was also confirmed, the photocatalytic activity of codoped nano-TiO2 remained above 89.6% of the fresh sample after being used four times.
基金This work was supported by the National Natural Sci- ence Foundation of China (No.41373127) and the Liaoning Provincial Natural Science Foundation of China (No.2013020121).
文摘In order to improve the photocatalytic performance of mesoporous titania under visible light, a series of photocatalysts of S and Ag co-doped mesoporous titania have been successfully prepared by template method using thiourea, AgNO3 and tetrabutyl titanate as precursors and Pluronic P123 (EO20PO70EO20) as template. Scanning electron microscopy (SEM), X-ray diffraction (XRD), nitrogen adsorption-desorption measurements, and UV-visible spectroscopy (UV-Vis) were employed to characterize the morphology, crystal structure, surface structure, and optical absorption properties of the samples. The microcrystal of the photocatalysts consisted of anatase phase and was approximately present in the form of spherical particle. The photocatalytic performance was studied by photodegradation methyl orange (MO) in water under UV and visible light irradiation. The calcination temperature and the doping content influenced the photoactivity. In addition, the possibility of cyclic usage of co-doped mesoporous titania was also confirmed, the photocatalytic activity of mesoporous titania remained above 89% of that of the fresh sample after being used four times. It was shown that the co-doped mesoporous titania could be activated by visible light and could thus be potentially applied for the treatment of water contaminated by organic pollutants. The synergistic effect of sulfur and silver co-doping played an important role in improving the photocatalytic activity.
文摘The nitrogen and fluorine co doped TiO 2 polycrystalline powder was synthesized by calcinations of the hydrolysis product of tetra butyl titanate with ammonium fluoride. Nitrogen and fluorine co doping causes the absorption edge of TiO 2 to shift to a lower energy region. The photocatalytic activity of co doped TiO 2 with anatase phases was found to be 2 4 times higher than that of the commercial TiO 2 photocatalyst Degussa P25 for phenol decomposition under visible light irradiation. The co doped TiO 2 powders only contain anatase phases even at 1000℃. Apparently, ammonium fluoride added retarded phase transformation of the TiO 2 powders from anatase to rutile. The substitutional fluorine and interstitial nitrogen atoms in co doped TiO 2 polycrystalline powder were responsible for the vis light response and caused the absorption edge of TiO 2 to shift to a lower energy region.
文摘This paper reports that the Zn0.95Co0.05O polycrystalline powder and thin film were prepared by sol-gel technique under the similar preparation conditions. The former does not show typical ferromagnetic behaviour, while the latter exhibits obvious ferromagnetic properties at 5 K and room temperature. The UV-vis spectra and x-ray absorption spectra show that Co2+ ions are homogeneously incorporated into ZnO lattice without forming secondary phases.The distinct difference between film and powder sample is the c-axis (002) preferential orientation indicated by the x-ray diffraction pattern and field emission scanning electron microscopy measurement, which may be the reason why Zn0.95Co0.05O film shows ferromagnetic behaviour.
基金supported by the National Key Basic Research and Development Program of China ("973" program,nos. 2012CB720100 and 2014CB239300)the National Natural Science Foundation of China (nos.21406164 and 21466035)+1 种基金the Science and Technology Innovation Guide Funds of Civil Aviation Administration of China (MHRD20140209)the Fundamental Research Funds for the Central Universities (no.3122016L016)
文摘Transition metal-doping could effectively extend the light response range of TiO _2 photocatalysts from the ultraviolet(UV)to the visible region.Co-doped brookite titanium dioxide(Co–TiO_2)photocatalysts were synthesized via the hydrothermal method with titanium tetrachloride as the raw material and cobalt chloride hexahydrate as the dopant.The prepared Co–TiO_2 photocatalysts were characterized by X-ray diffraction(XRD),scanning electron microscopy(SEM),transmission electron microscopy(TEM),Raman spectroscopy,X-ray photoelectron spectroscopy(XPS)and UV–Vis diffuse reflectance spectroscopy(UV–Vis DRS).The photocatalytic activities of Co–TiO _2 photocatalysts were evaluated by photocatalytic degradation of isopropanol alcohol(IPA),a typical volatile organic compound(VOC),under visible light.The influences ofdifferent Co doping rates,initial concentrations of IPA gas and the amounts of photocatalyst addition were also studied.At the same time,the enhancement mechanism ofcobalt ions as a trap for photogenerated holes was discussed.Thus,we found the optimum doping rate,initial concentration of IPA gas and amount of photocatalyst to add.The results show that the mesoporous Co–TiO _2 photocatalysts possess smaller size particles,larger specific surface area,lower forbidden bandgap energy(Eg)and better photocatalytic activity than pure brookite TiO _2.When the doping of Co was 7% by mass,the initial concentration ofIPA gas was 1.0×10^(-6 )mol/L and the addition of Co–TiO_2 photocatalysts was 50 mg,the best photocatalytic activity was achieved.Furthermore,the degradation rate ofIPA was up to 91%,which shows great potential for waste water treatment.
基金financial support from the National Natural Science Foundation of China (Nos. 21476089, 21373091)the Provincial Science and Technology Project of Guangdong (No. 2014A030312007)
文摘Renewable lignin used for synthesizing materials has been proven to be highly potential in specific electrochemistry.Here,we report a simple method to synthesize nitrogen and sulfur co-doped carbon nanosheets by using bagasse lignin,denoted as lignin-derived carbon(LC).By adjusting the ratio of nitrogen source and annealing temperature,we obtained the ultrathin graphitic lignin carbon(LC-4-1000)with abundant wrinkles with high surface area of 1208 m2g_1 and large pore volume of 1.40 cm3g_1.In alkaline medium,LC-4-1000 has more positive half-wave potential and nearly current density compared to commercial Pt/C for oxygen reduction reaction(ORR).More importantly,LC-4-1000 also exhibits comparable activity and superior stability for ORR in acid medium due to its high graphitic N ratio and a direct four electron pathway for ORR.This study develops a cost-effective and highly efficient method to prepare biocarbon catalyst for ORR in fuel cells.
文摘(La, N) co-doped TiO2 photocatalysts were synthesized using TiC14 sol-gel autoignidng synthesis (SAS) starting from a complex compound system of TiCl4-La(NO3)3-citric acid-NH4NO3-NHyH2O, in which the (La, N) co-doped process was accompushed in the formation of TiO2 nanocrystals. The prepared samples were characterized by using X-ray diffraction (XRD), X-ray photoemission spectroscopy (XPS) and UV-vis diffuse reflectance spectra. The results indicated that nitrogen and lanthanum were incorporated into the lattice and interstices of titania nanocrystals, which resulted in narrowing the band gap and promoting the separation of photoexcited hole-electron pairs, respectively, and showing expected red-shifts and enhanced photocatalytic activity under visible light. The mechanism on nitrogen doping and enhancement in photocatalyfic activity of (La, N) co-doped titania by SAS was discussed in detail.
基金Project supported by the National Natural Science Foundation of China(Grant No.21276045)
文摘Oxidized asphaltene (OA), a thermosetting material with plenty of functional groups, is synthesized from asphaltene (A) using HNO3]HzSO4 as the oxidizing agent. Boron, nitrogen co-doped porous carbon (BNC-OA) is prepared by carbonization of the mixture of boric acid and OA at 1173 K in an argon atmosphere. X-ray photoelectron spectroscopy (XPS) characterization reveals that the BNC-OA has a nitrogen content of 3.26 at.% and a boron content of 1.31 at.%, while its oxidation-free counterpart (BNC-SA) has a nitrogen content of 1.61 at.% and a boron content of 3.02 at.%. The specific surface area and total pore volume of BNC-OA are 1103 m2·g^-1 and 0.921 cm3·g^-1, respectively. At a current density of 0.1 A·g^-1, the specific capacitance of BNC-OA is 335 F·g^-1 and the capacitance retention can still reach 83% at 1 A·g^-1. The analysis shows that the superior electrochemical performance of the BNC-OA is attributed to the pseudocapacitance behavior of surface heteroatom functional groups and an abundant pore-structure. Boron, nitrogen co-doped porous carbon is a promising electrode material for supercapacitors.
基金the National Natural Science Foundation of China(No.20677008)the Innovation Foundation of Donghua University for Doctors
文摘A novel lanthanum and sulfur co-doped TiO2 photocatalyst was synthesized by precipitation- dipping method, and characterized by X-ray diffraction(XRD), transmission electron microscopy(TEM) and UV-Vis diffuse reflectance spectroscopy. Compared with the S-doped TiO, La-doped TiO2 and the standard Degussa P25 photocatalysts, the lanthanum and sulfur co-doped TiO2 photocatalyst (the molar percentage of La is 3.0%) calcined at 450 ℃ for 2 h showed the strongest absorption for visible light and highest activities for degradation of reactive blue 19 dye in aqueous solution under visible light(λ〉400 nm) irradiation. It was also discovered that the co-doping of lanthanum and sulfur hindered the aggregation and growth of TiO2 particles, and the doping of lanthanum reduced slightly the phase transition temperature ofTiO2 from anatase to rutile.
基金financial support from the National Natural Science Foundation of China (21773111, 21473089, 21573107 and 51571110)the National Key Research and Development Program of China (2017YFA0206503, 2018YFA0209103)+1 种基金Priority Academic Program Development of Jiangsu Higher Education Institutions, Fundamental Research Funds for the Central Universitiesthe program B for outstanding PhD candidate of Nanjing University (201702B049)
文摘Exploring inexpensive and efficient bifunctional electrocatalysts for oxygen reduction reaction(ORR) and oxygen evolution reaction(OER) is critical for rechargeable metal-air batteries. Herein, we report a new 3D hierarchical sulfur and nitrogen co-doped carbon nanocages(hSNCNC) as a promising bifunctional oxygen electrocatalyst by an in-situ MgO template method with pyridine and thiophene as the mixed precursor. The as-prepared h SNCNC exhibits a positive half-wave potential of 0.792 V(vs. reversible hydrogen electrode, RHE) for ORR, and a low operating potential of 1.640 V at a 10 mA cm-2 current density for OER. The reversible oxygen electrode index is 0.847 V, far superior to commercial Pt/C and IrO2,which reaches the top level of the reported bifunctional catalysts. Consequently, the hSNCNC as air cathodes in an assembled Zn-air battery features low charge/discharge overpotential and long lifetime. The remarkable properties arises from the introduced multiple heteroatom dopants and stable 3D hierarchical structure with multi-scale pores, which provides the abundant uniform high-active S and N species and efficient charge transfer as well as mass transportation. These results demonstrate the potential strategy in developing suitable carbon-based bi-/multi-functional catalysts to enable the next generation of the rechargeable metal-air batteries.
基金supported by Joint Funds of the National Natural Science Foundation of China(U20A20280)the National Natural Science Foundation of China(21805083,52074119)+3 种基金the Academy of Sciences large apparatus United Fund of China(U1832187)the Scientific Research Fund of Hunan Provincial Education Department(19K058)the Science and Technology Planning Project of Hunan Province(2018TP1017)the High-Tech Leading Plan of Hunan Province(2020GK2072).
文摘Silicon-based(Si)materials are promising anodes for lithium-ion batteries(LIBs)because of their ultrahigh theoretical capacity of 4200 mA h g^(−1).However,commercial applications of Si anodes have been hindered by their drastic volume variation(∼300%)and low electrical conductivity.Here,to tackle the drawbacks,a hierarchical Si anode with double-layer coatings of a SiOx inner layer and a nitrogen(N),boron(B)co-doped carbon(C-NB)outer layer is elaborately designed by copyrolysis of Si-OH structures and a H3BO_(3)-doped polyaniline polymer on the Si surface.Compared with the pristine Si anodes(7mA h g^(−1) at 0.5 A g^(−1) after 340 cycles and 340 mA h g^(−1) at 5 A g^(−1)),the modified Si-based materials(Si@SiOx@C-NB nanospheres)present su perior cycling stability(reversible 1301 mA h g^(−1) at 0.5 A g^(−1) after 340 cycles)as well as excellent rate capability(690mA h g^(−1) at 5 A g^(−1))when used as anodes in LIBs.The unique double-layer coating structure,in which the inner amorphous SiOx layer acts as a buffer matrix and the outer defect-rich carbon enhances the electron diffusion of the whole anode,makes it possible to de liver excellent electrochemical properties.These results indicate that our double-layer coating strategy is a promising approach not only for the devel opment of sustainable Si anodes but also for the design of multielement-doped carbon nanomaterials.
基金Collaborative Innovation Center of Suzhou Nano Science and TechnologyNational Natural Science Foundation of China,Grant/Award Numbers:21773163,22271203+3 种基金EPSRC for an Overseas Travel Grant,Grant/Award Number:EP/R023816/1State Key Laboratory of Organometallic Chemistry of Shanghai Institute of Organic Chemistry,Grant/Award Number:KF2021005Priority Academic Program Development of Jiangsu Higher Education InstitutionsProject of Scientific and Technologic Infrastructure of Suzhou,Grant/Award Number:SZS201905。
文摘The development of simple and effective strategies to prepare electrocatalysts,which possess unique and stable structures comprised of metal/nonmetallic atoms for oxygen reduction reaction(ORR)and oxygen evolution reaction(OER),is currently an urgent issue.Herein,an efficient bifunctional electrocatalyst featured by ultralong N,S-doped carbon nano-hollow-sphere chains about 1300 nm with encapsulated Co nanoparticles(Co-CNHSCs)is developed.The multifunctional catalytic properties of Co together with the heteroatom-induced charge redistribution(i.e.,modulating the electronic structure of the active site)result in superior catalytic activities toward OER and ORR in alkaline media.The optimized catalyst Co-CNHSC-3 displays an outstanding electrocatalytic ability for ORR and OER,a high specific capacity of 1023.6 mAh gZn^(-1),and excellent reversibility after 80 h at 10mA cm^(-2)in a Zn-air battery system.This work presents a new strategy for the design and synthesis of efficient multifunctional carbon-based catalysts for energy storage and conversion devices.
基金the National Natural Science Foundation of China(No.51472034)the Opening Project of Key Laboratory of Optoelectronic Chemical Materials and Devices,Ministry of Education,Jianghan University(No.JDGD-201806)。
文摘Nitrogen and sulfur co-doped porous nanocarbon (ZIF-C-N-S) catalyst was successfully synthesized derived from ZIF-8 and thiourea precursors.The electrochemical measurements indicate that the as-obtained ZIF-C-N-S catalyst exhibits higher electrocatalytic activity for oxygen reduction reaction (ORR) in alkaline electrolyte and superior durability-longer than commercial Pt/C catalyst.The enhancment of electrocatalytic activity mainly be come from the open pore structure,large specific surface area as well as the synergistic effect resulted from the co-doping of N and S atoms.In addition,the ZIF-C-N-S catalyst is also used as the air cathode catalyst in the microbial fuel cell (MFC) device.The maximum power density and stable output voltage of ZIF-C-N-S based MFC are 1315 mW/m2 and 0.48 V,respectively,which is better than that of Pt/C based MFC.
文摘Nitrogen and phosphorus co-doped graphene quantum dot-modified Bi5O7 I(NPG/Bi5O7 I)nanorods were fabricated via a simple solvothermal method.The morphology,structure,and optical properties of the as-prepared samples were investigated by X-ray diffraction,scanning electron microscopy,high-resolution transmission electron microscopy,X-ray photoelectron spectroscopy(XPS),and diffused reflectance spectroscopy.The photocatalytic performance was estimated by degrading the broad-spectrum antibiotics tetracycline and enrofloxacin under visible light irradiation.The photodegradation activity of Bi5O7 I improved after its surface was modified with NPGs,which was attributed to an increase in the photogenerated charge transport rate and a decrease in the electron-hole pair recombination efficiency.From the electron spin resonance spectra,XPS valence band data,and free radical trapping experiment results,the main active substances involved in the photocatalytic degradation process were determined to be photogenerated holes and superoxide radicals.A possible photocatalytic degradation mechanism for NPG/Bi5O7 I nanorods was proposed.
基金Project supported by the National Natural Science Foundation of China (Grant No. 10804015 )the Science Foundation of the Education Department of Liaoning Province of China (Grant No. 2009A417)
文摘yb^3+:Er^3+ co-doped oxy-fluoride ceramics glass has been prepared. The mechanism of up-conversion emissions about Er^3+ was discussed, and the temperature properties of green up-conversion fluorescence between 303 and 823 K were investigated. The results show that the sensitivity of this sample reaches its maximum value, about 0.0047 K^-1, when the temperature is 383 K, indicating that this kind of sample can be used as high temperature and high sensitivity optical temperature sensor.
基金the National Natural Science Foundation of China(U1710122,51862035 and 21773293)the Science and Technology Project of Jiangxi Province(20181ACH80008,20181ACE50012,20192BCD40017 and 20192ACB80002)+1 种基金Jiangxi Double Thousand Talent Program(S2018LQCQ0016)Suzhou Science and Technology Plan Projects(SYG201831)。
文摘Developing high power and energy supercapacitors(SCs)is a long-pursued goal for the application in transportation and energy storage station.Herein,a rationally-designed Co-doped nickel oxide nanosheets@carbon-welded carbon nanotube foam(Co-doped NiO@WCNTF)as freestanding electrode is successfully prepared for high power and energy SCs.The WCNTF framework with high specific surface area provides three dimensional highly conductive network for fast charge transport and ensures high loading of active materials(9.2 mg/cm2).Moreover,porous Co-doped NiO nanosheets uniformly anchored on the WCNTF framework enable rapid charge kinetics due to the high intrinsic conductivity of Co-doped Ni O nanosheets and their good contact with conductive WCNTF substrate.As a result,the unique integrated electrode with 3D architecture exhibits an ultrahigh specific capacitance of 11.45 F/cm2 at 5 mA/cm2,outstanding rate capability(11.45 F/cm2 at 5 mA/cm2 and a capacitance retention of 86.2%at 30 mA/cm2)and good cycling stability,suggesting great potential for high performance supercapacitor.
基金Supported by the Fundamental Research Funds for the Central Universities under Grant Nos.BUPT2009RC0412 and 10979065the National High Technology Research and Development Program of China under Grant No.2009AA03Z405the National Natural Science Foundation of China under Grant Nos.60644004 and 10979065
文摘The electronic structure, magnetic properties, and optical properties of Co-doped AIN are investigated based upon the Perdew-Burke-Ernzerhof form of generalized gradient approximation within the density functional theory. The band gaps narrowing of AI1-x Cox N are found with the increase of Co concentrations. The analyses of the band structures and density of states show that AI1-xCoxN alloys exhibit a halfometallie character. Moreover, we have succeeded in demonstrating that Co doped AIN system in x = 0.125 is always antiferromagnetie, which is in good agreement with the experimental results. Besides, it is shown that the insertion of Co atom leads to redshift of the optical absorption edge. Finally, the optical constants of pure A1N and AI1-xCoxN alloy, such as loss function, refractive index and reflectivity, are discussed.
基金supported by Major Science and Technology Project of Water Pollution Control and Management(No.2017ZX07101003)Zhejiang Provincial Natural Science Foundation of China under Grant no.LR17B060003financially supported by the Natural Science Foundation of China(Project Nos.21436007,21522606,21476201,21676246,U1462201,and 21776248)
文摘Although there have been many reports of metal doping to ameliorate the drawbacks of hematite as the photoanode for water oxidation, most of them focused on monometallic doping, and only a few of them payed attention to bimetallic doping. What is worse, the synergetic mechanism between two metal dopants was not sufficiently studied, especially the density functional theory(DFT) calculation. In this work, the n-type hematite was synthesized by introducing Ti dopant into hematite through the hydrothermal method, and dipping-sintering treatment was employed to further introduce homogeneously dispersed Zn dopant into that, forming the Ti, Zn co-doped hematite. Under the optimal condition, Tidoped hematite photoanode reached approximately 2-times enhancement of the photocurrent density compared with the pristine one at 1.23 V vs. RHE, while Ti, Zn co-doped hematite anode obtained another25% elevation. UV–Vis spectroscopy, Mott–Schottky plots, EIS analysis, photo-oxidation of hole scavenger(H2O2), and DFT calculation were employed to understand the role of Ti, Zn dopant. Based on the obtained results, the synergetic mechanism of two dopants was discussed, i.e., the improvement of PEC performance of Ti, Zn co-doped hematite photoanode was possibly attributed to greater carrier density and improved charge separation efficiency at the surface of hematite. This work provides new strategy and understanding of the improvement of PEC performance of hematite by doping engineering.