Vacancy defect MoSeTe embedded in N and F co-doped carbon skeleton for high performance sodium ion batteries and hybrid capacitors

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.

Nitrogen and phosphorus co-doped activated carbon induces high density Cu^(+)active center for acetylene hydrochlorination

This work aims to solve the problems of low reaction activity of Cu-based catalysts and agglomeration of active centers in acetylene hydrochlorination.Cu-based catalysts supported by NAP co-doped activated carbon(AC)with different content(mCu-xNP/AC)were manufactured and applied in the acetylene hydrochlorination reaction.It was found that the doping of carriers N and P induced the transformation of Cu^(2+)to Cu^(+),and the catalytic activity was markedly improved.Under the optimal reaction temperature of 220℃,the gas hourly space velocity(GHSV)of C_(2)H_(2)was 90 h^(-1)and V_(HCl):V_(C_(2)H_(2))was 1.15.The initial activity of the 5%Cu-30 NP/AC catalyst reached 95.59%.Through some characterization methods showed the addition of N and P improved the dispersion of Cu in carbon,which increased the ratio of Cu^+/Cu^(2+).The measurement results confirmed that the chemisorption capacity of mCu-xNP/AC for C_(2)H_(2)decreased slightly,and the chemisorption capacity for HCl increased significantly,which was the reason for the increased activity of the catalyst.The conclusion provides a reference for the development of acetylene hydrochlorination Cu catalyst.

Microbial synthesis of N, P co-doped carbon supported PtCu catalysts for oxygen reduction reaction

Developing highly efficient and stable platinum-based electrocatalyst for oxygen reduction reaction(ORR) is critical to expediting commercialization of fuel cells.Herein,several PtCu alloy nanocatalysts supported on N,P co-doped carbon(PtCu/NPC) were prepared by microbial-sorption and carbonization-reduction.Among them,PtCu/NPC-700 ℃ exhibits excellent catalytic performance for ORR with a mass activity of 0.895 A mg_(pt)^(-1)(@0.9 V) which is 8.29 folds of commercial Pt/C.Additionally,the ECSA and MA of PtCu/NPC-700℃ only decrease by 14.2% and 18.7% respectively,while Pt/C decreases by 35.2% and 52.8% after 10,000 cycles of ADT test.Moreover,the PtCu/NPC-700℃ catalyst emanates a maximum power density of 715 mW cm^(-2) and only 11.1% loss of maximum power density after 10,000 ADTs in single-cell test,indicating PtCu/NPC-700℃ also manifests higher activity and durability in actual single-cell operation than Pt/C.This research provides an easy and novel strategy for developing highly active and durable Pt-based alloy catalyst.

Ultralong nitrogen/sulfur Co-doped carbon nano-hollowsphere chains with encapsulated cobalt nanoparticles for highly efficient oxygen electrocatalysis

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.

Construction of N,O co-doped carbon anchored with Co nanoparticles as efficient catalyst for furfural hydrodeoxygenation in ethanol

Hydrodeoxygenation of furfural(FF)into 2-methylfuran(MF)is a significant biomass utilization route.However,designing efficient and stable non-noble metal catalyst is still a huge challenge.Herein,we reported the N,O co-doped carbon anchored with Co nanoparticles(Co-SFB)synthesized by employing the organic ligands with the target heteroatoms.Raman,electron paramagnetic resonance(EPR),electrochemical impedance spectroscopy(EIS),and X-ray photoelectron spectroscopy(XPS)characterizations showed that the co-doping of N and O heteroatoms in the carbon support endows Co-SFB with enriched lone pair electrons,fast electron transfer ability,and strong metal-support interaction.These electronic properties resulted in strong FF adsorption as well as lower apparent reaction activation energy.At last,the obtained N,O co-doped Co/C catalyst showed excellent catalytic activity(nearly 100 mol%FF conversion and 94.6 mol%MF yield)and stability for in-situ dehydrogenation of FF into MF.This N,O co-doping strategy for the synthesis of highly efficient catalytic materials with controllable electronic state will provide an excellent opportunity to better understand the structure-function relationship.

Structural and Optical Properties of Cu2+ + Ce3+ Co-Doped ZnO by Solution Combustion Method

In this work, ZnO, Ce3+ doped ZnO (ZnO/Ce3+) and Cu2+ + Ce3+ co-doped ZnO (ZnO/Cu2+ + Ce3+ ) solid solutions powders were synthesized by a solution combustion method maintaining the Ce3+ ion concentration constant in 3%Wt while the Cu2+ ion concentration was varied in 1, 2, 3, 10 and 20%Wt. After its synthesis, all the samples were annealed at 900?C by 24 h. The ZnO, ZnO/Ce3+ and ZnO/Cu2+ + Ce3+ powders were structurally characterized using X-ray diffraction (XRD) technique, and the XRD patterns showed that for pure ZnO, Cu2+ undoped ZnO/Ce3+ and ZnO/Ce3+ doped with the Cu2+ ion, the three samples exhibited the hexagonal wurtzite ZnO crystalline structure. However, the morphology and particle size of both samples were observed by means of a scanning electron microscopy (SEM);from SEM image, it is observed that the crystallites of both samples are agglomerated forming bigger amorphous particles with an approximate average size of 1 μm. In addition, the photoluminescence of the ZnO, Ce3+ doped ZnO and Cu2+ + Ce3+ doped ZnO samples was measurement under an illumination of 209 nm wavelength (UV region): for the ZnO/Ce3+ sample, your emission spectrum is in the visible region from blue color until red color;the UV band of the ZnO is suppressed. The multicolor emission visible is attributed to the Ce3+ ion photoluminescence, while for the ZnO/Cu2+ + Ce3+, its emission PL spectrum is quenching by the Cu2+ ion, present in the ZnO crystalline.

Cu、N共掺杂TiO_(2)纳米管光催化重整甘油制备合成气

通过碱性水热-离子交换法制备了Cu、N共掺杂TiO_(2)纳米管(Cu/N-TNT),对其光催化重整甘油制备合成气性能进行了研究。结果表明,Cu/N-TNT具有富含氧空位(O_(v))的管状结构,N以Ti-N形式取代部分O形成杂质能级,Cu以Cu^(2+)形式掺杂在催化剂晶格间隙和表面,Cu、N共掺杂促进TiO_(2)表面电荷有效分离,有利于其光催化重整甘油制备合成气活性和选择性的提高。紫外光照射8h时,掺Cu量为0.15%的Cu/N-TNT催化剂上CO和H_(2)产量分别为7.3和8.5 mmol·g^(-1),是原始TiO_(2)的9.1和70.8倍,nH_(2)/nCO从0.52提高为1.18,nCO/nCO_(2)从0.21提高至0.42。Cu/N-TNT表面N和OV为醛类脱羰和甲酸脱水生成CO提供反应活性位点,Cu作为浅势阱提高光生电子-空穴分离效率。光生空穴(h+)是光催化重整甘油制备合成气过程中的主要活性物种,大量经基自由基(·OH)和超氧自由基(·O_(2)-)会导致甘油过度氧化,使CO选择性降低。

N-乙基咔唑-3-甲醛席夫碱荧光探针的合成及其检测Cu^(2+)性质

以咔唑为原料,经过两步反应制备得到N-乙基咔唑-3-甲醛,其结构经X射线单晶衍射测定属于单斜晶系,空间群为P2_(1)/n。再以N-乙基咔唑-3-甲醛与1,3-二氨-2-丙醇为原料,设计、合成了一种新型双席夫碱荧光探针分子CMP。借助荧光光谱在体积比为6∶4的DMSO/H_(2)O缓冲溶液(Tris-HCl,pH=7.0)中研究了探针CMP对Cu^(2+)的选择性识别。研究结果表明,探针CMP与Cu^(2+)以1∶2的比例配位,结合常数为1.52×10^(5) L·mol^(-1),检出限为0.205μmol·L^(-1)。回收实验表明,探针分子CMP可应用于环境水样中Cu^(2+)的检测。

Hierarchical sulfur and nitrogen co-doped carbon nanocages as efficient bifunctional oxygen electrocatalysts for rechargeable Zn-air battery

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.

Tuning interface mechanism of FeCo alloy embedded N,S-codoped carbon substrate for rechargeable Zn-air battery

The interface mechanism between catalyst and carbon substrate has been the focus of research.In this paper,the FeCo alloy embedded N,S co-doped carbon substrate bifunctional catalyst(FeCo/S-NC)is obtained by a simple one-step pyrolysis strategy.The experimental results and density functional theory(DFT)calculation show that the formation of FeCo alloy is conducive to promoting electron transfer,and the introduction of S atom can enhance the interaction between FeCo alloy and carbon substrate,thus inhibiting the migration and agglomeration of particles on the surface of carbon material.The FeCo/SNC catalysts show outstanding performance for oxygen reduction reaction(ORR)and oxygen evolution reaction(OER).FeCo/S-NC shows a high half-wave potential(E_(1/2)=0.8823 V)for ORR and a low overpotential at 10 mA cm^(-2)(E_(j=10)=299 mV)for OER.In addition,compared with Pt/C+RuO_(2) assembled Zn-air battery(ZAB),the FeCo/S-NC assembled ZAB exhibits a larger power density(198.8 mW cm^(-2)),a higher specific capacity(786.1 mA h g_(zn)~(-1)),and ultra-stable cycle performance.These results confirm that the optimized composition and the interfacial interaction between catalyst and carbon substrate synergistically enhance the electrochemical performance.

Construction of nitrogen and phosphorus co-doped graphene quantum dots/Bi5O7I composites for accelerated charge separation and enhanced photocatalytic degradation performance

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.

Integration of pore structure modulation and B,N co-doping for enhanced capacitance deionization of biomass-derived carbon

Biomass-derived carbon has demonstrated great potentials as advanced electrode for capacitive deionization(CDI),owing to good electroconductivity,easy availability,intrinsic pores/channels.However,conventional simple pyrolysis of biomass always generates inadequate porosity with limited surface area.Moreover,biomass-derived carbon also suffers from poor wettability and single physical adsorption of ions,resulting in limited desalination performance.Herein,pore structure optimization and element co-doping are integrated on banana peels(BP)-derived carbon to construct hierarchically porous and B,N co-doped carbon with large ions-accessible surface area.A unique expansionactivation(EA)strategy is proposed to modulate the porosity and specific surface area of carbon.Furthermore,B,N co-doping could increase the ions-accessible sites with improved hydrophilicity,and promote ions adsorption.Benefitting from the synergistic effect of hierarchical porosity and B,N co-doping,the resultant electrode manifest enhanced CDI performance for NaCl with large desalination capacity(29.5 mg g^(-1)),high salt adsorption rate(6.2 mg g^(-1)min^(-1)),and versatile adsorption ability for other salts.Density functional theory reveals the enhanced deionization mechanism by pore and B,N co-doping.This work proposes a facile EA strategy for pore structure modulation of biomass-derived carbon,and demonstrates great potentials of integrating pore and heteroatoms-doping on constructing high-performance CDI electrode.

Preparation by High-gravity Technology of a Cu/N-TiO_(2) Nanophotocatalyst for Photodegradation of Phenol Wastewater

TiO_(2) is a promising photocatalyst,but its practical use is restricted by its low catalytic efficiency caused by the large particle size and uneven size distribution,which arise from the limited contact area of the liquid-liquid interface during synthesis.Impinging stream-rotating packed bed(IS-RPB)reactors,which are used for process intensification,overcome the mixing limitation of traditional stirred-tank reactors and provide a micromixing environment at the molecular scale for the two liquid phases,which can reduce the particle size and distribution range.Cu/N-TiO_(2) nanoparticles were prepared in an IS-RPB reactor by the one-step precipitation method using urea as the nitrogen source,titanyl sulfate as the titanium source,copper chloride as the copper source,and ammonium hydroxide as the precipitant.The particle size of the photocatalyst was about 11.40 nm with a narrow size distribution measured by scanning electron microscopy and transmission electron microscopy.X-ray photoelectron spectroscopy showed that N replaced some O and was uniformly dispersed in the TiO_(2) lattice as interstitial and substitutional N.Cu replaced some Ti and was present as Cu^(2+).The synergistic effects of these two elements formed a new impurity energy level and reduced the band gap energy of the TiO_(2) nanoparticles.The specific surface area of the Cu/N-TiO_(2) nanoparticles was 152.97 m^(2)/g.The effects of the main factors on the degradation rate were studied,and the removal efficiency reached 100%under the optimal operating conditions after 2 h ultraviolet irradiation.The electron paramagnetic resonance measurements showed that the superoxide radical played a main role in the degradation process,whereas the photogenerated holes and hydroxyl radicals had weak effects.

Electronic Structure Magnetic Properties and Optical Properties of Co-doped AIN from First Principles

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.

Inherent mass transfer engineering of a Co,N co-doped carbon material towards oxygen reduction reaction

Oxygen reduction reaction (ORR) is an important process for the conversion and utilization of a wide range of renewable energy sources, and is critical for the shape of future energy scenario [1–10]. However, ORR is a complex four-electron transfer process and is kinetically sluggish. It is urgent to develop high-efficient electrocatalysts to solve this problem [11–15]. Up to now, precious metal-based catalysts such as Pt-based electrocatalysts have been widely studied and found to be one of the most efficient electrocatalysts for ORR. However, the high price and the small reserves limit their large-scale commercialization [10,16–23]. Therefore, in order to fulfill needs for the practical applications, it is necessary to develop low-cost electrocatalysts, also with high activity and great stability [19,24–28].

Multiple-dimensioned defect engineering for graphite felt electrode of vanadium redox flow battery

The scarcity of wettability,insufficient active sites,and low surface area of graphite felt(GF)have long been suppressing the performance of vanadium redox flow batteries(VRFBs).Herein,an ultra-homogeneous multipledimensioned defect,including nano-scale etching and atomic-scale N,O codoping,was used to modify GF by the molten salt system.NH_(4)Cl and KClO_(3) were added simultaneously to the system to obtain porous N/O co-doped electrode(GF/ON),where KClO_(3) was used to ultra-homogeneously etch,and O-functionalize electrode,and NH4Cl was used as N dopant,respectively.GF/ON presents better electrochemical catalysis for VO_(2)+/VO_(2)+ and V3+/V2+ reactions than only O-functionalized electrodes(GF/O)and GF.The enhanced electrochemical properties are attributed to an increase in active sites,surface area,and wettability,as well as the synergistic effect of N and O,which is also supported by the density functional theory calculations.Further,the cell using GF/ON shows higher discharge capacity,energy efficiency,and stability for cycling performance than the pristine cell at 140 mA cm^(−2) for 200 cycles.Moreover,the energy efficiency of the modified cell is increased by 9.7% from 55.2% for the pristine cell at 260 mA cm^(−2).Such an ultra-homogeneous etching with N and O co-doping through“boiling”molten salt medium provides an effective and practical application potential way to prepare superior electrodes for VRFB.

Cubic S/N co-doped TiO_(2) with rich oxygen vacancies from Ti-MOFs for efficient elimination of formaldehyde

The cubic S/N co-doped TiO_(2)(TNSx,x is the calcination temperature)photocatalysts with rich oxygen vacancies were obtained by high temperature calcination of sulfur powder and titanium-based MOFs NH_(2)-MIL-125 for the photocatalytic removal of gaseous formaldehyde(a volatile organic compound).Among the obtained catalysts,the presence of oxygen vacancies restricted photogenerated electron and holes recombination.98.00%removal of gaseous formaldehyde in 150 min could be achieved over TNS600 by xenon lamp.The removal efficiency for formaldehyde was well retained for five cycle experiment.The results from PL,TRPL and EIS revealed that TNS600 had the best separation efficiency of photogenerated electrons and holes,and the enhanced charge separation led to a significant increase in photocatalytic activity.The photocatalytic oxidation mechanism indicated that the ^(•)OH and ^(•)O_(2)−radicals were mainly involved in the efficient elimination of gaseous formaldehyde and were able to mineralize formaldehyde to H_(2)O and CO_(2).

Double-Doped Carbon-Based Electrodes with Nitrogen and Oxygen to Boost the Areal Capacity of Zinc-Bromine Flow Batteries

Ensuring a stable power output from renewable energy sources,such as wind and solar energy,depends on the development of large-scale and long-duration energy storage devices.Zinc–bromine fl ow batteries(ZBFBs)have emerged as cost-eff ective and high-energy-density solutions,replacing expensive all-vanadium fl ow batteries.However,uneven Zn deposition during charging results in the formation of problematic Zn dendrites,leading to mass transport polarization and self-discharge.Stable Zn plating and stripping are essential for the successful operation of high-areal-capacity ZBFBs.In this study,we successfully synthesized nitrogen and oxygen co-doped functional carbon felt(NOCF4)electrode through the oxidative polymerization of dopamine,followed by calcination under ambient conditions.The NOCF4 electrode eff ectively facilitates effi cient“shuttle deposition”of Zn during charging,signifi cantly enhancing the areal capacity of the electrode.Remarkably,ZBFBs utilizing NOCF4 as the anode material exhibited stable cycling performance for 40 cycles(approximately 240 h)at an areal capacity of 60 mA h/cm^(2).Even at a high areal capacity of 130 mA h/cm^(2),an impressive energy effi ciency of 76.98%was achieved.These fi ndings provide a promising pathway for the development of high-areal-capacity ZBFBs for advanced energy storage systems.

Construction of Cu-Zn Co-doped layered materials for sodium-ion batteries with high cycle stability

Due to its high operational voltage and energy density,P2-type Na_(0.67)Ni_(0.3)Mn_(0.7)O_(2) has become a leading cathode material for sodium-ion batteries(SIBs),which is an ideal option for large-scale energy storage.However,the practical application of P2-type Na_(0.67)Ni_(0.3)Mn_(0.7)O_(2) is limited by the capacity constraints and unwanted phase transitions,presenting significant challenges to the widespread application of SIBs.To address these challenges and optimize the electrochemical properties of the P2 phase cathode material,this study proposes a Cu and Zn co-doped strategy to improve the electrochemical performance.The incorporation of Cu/Zn can stabilize the P2-phase structure against P2-O2 phase transitions,thus enhancing its electrochemical properties.The as-obtained P2-type Na0.67[Ni_(0.3)Mn_(0.58)Cu_(0.09)Zn_(0.03)]O_(2) cathode material shows an impressive cycling stability,maintaining 80%capacity retention after 1000 cycles at 2 C.The cyclic voltammetry(CV)tests show that the Cu^(2+)/Cu^(3+)redox reaction is also involved in charge compensation during the charge/discharge process.

First-principles investigation on N/C co-doped CeO2

The N and C doping effects on the crystal structures, electronic and optical properties of fluorite structure CeO2 have been investigated using the first-principles calculation. Co-doping these two elements results in the local lattice distortion and volume expansion of CeO2. Compared with the energy hand structure of pure CeO2, some local energy levels appear in the forbidden band, which may facilitate the light absorption. Moreover, the enhanced photo-catalytic properties of CeO2 were explained through the absorption spectra and the selection rule of the band-to-band transitions.