Wide-bandgap two-dimensional (2D) β-TeO_(2) has been reported as a high-mobility p-type transparent semiconductor [Nat. Electron. 4 277 (2021)], attracting significant attention. This "breakthrough" not onl...Wide-bandgap two-dimensional (2D) β-TeO_(2) has been reported as a high-mobility p-type transparent semiconductor [Nat. Electron. 4 277 (2021)], attracting significant attention. This "breakthrough" not only challenges the conventional characterization of TeO_(2) as an insulator but also conflicts with the anticipated difficulty in hole doping of TeO_(2) by established chemical trends. Notably, the reported Fermi level of 0.9 eV above the valence band maximum actually suggests that the material is an insulator, contradicting the high hole density obtained by Hall effect measurement. Furthermore, the detected residual Se and the possible reduced elemental Te in the 2D β-TeO_(2) samples introduces complexity, considering that elemental Se, Te, and Te_(1−x)Se_(x) themselves are high-mobility p-type semiconductors. Therefore, doubts regarding the true cause of the p-type conductivity observed in the 2D β-TeO_(2) samples arise. In this Letter, we employ density functional theory calculations to illustrate that TeO_(2), whether in its bulk forms of α-, β-, or γ-TeO_(2), or in the 2D β-TeO_(2) nanosheets, inherently exhibits insulating properties and poses challenges in carrier doping due to its shallow conduction band minimum and deep valence band maximum. Our findings shed light on the insulating properties and doping difficulty of TeO_(2), contrasting with the claimed p-type conductivity in the 2D β-TeO_(2) samples, prompting inquiries into the true origin of the p-type conductivity.展开更多
p-type transparent oxide semiconductors(TOSs)are significant in the semiconductor industry,driving advancements in optoelectronic technologies for transparent electronic devices with unique properties.The recent disco...p-type transparent oxide semiconductors(TOSs)are significant in the semiconductor industry,driving advancements in optoelectronic technologies for transparent electronic devices with unique properties.The recent discovery of p-type behavior in SeO_(2) has stimulated interest and confusion in the scientific community.In this Letter,we employ density functional theory calculations to reveal the intrinsic intrinsic insulating characteristics of SeO_(2) and highlight the substantial challenges in carrier doping.Our electronic structure analyses indicate that the Se 5^(2) states are energetically positioned too low to effectively interact with the O 2p orbitals,resulting in a valence band maximum(VBM)primarily dominated by the O 2p orbitals.The deep and localized nature of the VBM of SeO_(2) limits its potential as a high-mobility p-type TOS.Defect calculations demonstrate that all intrinsic defects in SeO_(2) exhibit deep transition levels within the bandgap.Regardless of the synthesis conditions,the Fermi level consistently resides in the mid-gap region.Furthermore,deep intrinsic acceptors and donors exhibit negative formation energies in the n-type and p-type regions,respectively,facilitating spontaneous formation and impeding external doping efforts.Thus,the reported p-type conductivity in SeO_(2) samples is unlikely to be intrinsic and is more plausibly attributable to reduced elemental Se,a well-known p-type semiconductor.展开更多
The lattice-matched XBn structures of InAsSb,grown on GaSb substrates,exhibit high crystal quali⁃ty,and can achieve extremely low dark currents at high operating temperatures(HOT).Its superior performance is attribute...The lattice-matched XBn structures of InAsSb,grown on GaSb substrates,exhibit high crystal quali⁃ty,and can achieve extremely low dark currents at high operating temperatures(HOT).Its superior performance is attributed to the unipolar barrier,which blocks the majority carriers while allowing unhindered hole transport.To further explore the energy band and carrier transport mechanisms of the XBn unipolar barrier structure,this pa⁃per systematically investigates the influence of doping on the dark current,photocurrent,and tunneling character⁃istics of InAsSb photodetectors in the PBn structure.Three high-quality InAsSb samples with unintentionally doped absorption layers(AL)were prepared,with varying p-type doping concentrations in the GaSb contact layer(CL)and the AlAsSb barrier layer(BL).As the p-type doping concentration in the CL increased,the device’s turn-on bias voltage also increased,and p-type doping in the BL led to tunneling occurring at lower bias voltages.For the sample with UID BL,which exhibited an extremely low dark current of 5×10^(-6) A/cm^(2).The photocurrent characteristics were well-fitted using the back-to-back diode model,revealing the presence of two opposing space charge regions on either side of the BL.展开更多
Zinc oxide(ZnO) is a compound semiconductor with a direct band gap and high exciton binding energy.The unique property,i.e.,high efficient light emission at ultraviolet band,makes ZnO potentially applied to the shor...Zinc oxide(ZnO) is a compound semiconductor with a direct band gap and high exciton binding energy.The unique property,i.e.,high efficient light emission at ultraviolet band,makes ZnO potentially applied to the short-wavelength light emitting devices.However,efficient p-type doping is extremely hard for ZnO.Due to the wide band gap and low valence band energy,the self-compensation from donors and high ionization energy of acceptors are the two main problems hindering the enhancement of free hole concentration.Native defects in ZnO can be divided into donor-like and acceptorlike ones.The self-compensation has been found mainly to originate from zinc interstitial and oxygen vacancy related donors.While the acceptor-like defect,zinc vacancy,is thought to be linked to complex shallow acceptors in group-VA doped ZnO.Therefore,the understanding of the behaviors of the native defects is critical to the realization of high-efficient p-type conduction.Meanwhile,some novel ideas have been extensively proposed,like double-acceptor co-doping,acceptor doping in iso-valent element alloyed ZnO,etc.,and have opened new directions for p-type doping.Some of the approaches have been positively judged.In this article,we thus review the recent(2011-now) research progress of the native defects and p-type doping approaches globally.We hope to provide a comprehensive overview and describe a complete picture of the research status of the p-type doping in ZnO for the reference of the researchers in a similar area.展开更多
Zinc oxide (ZnO) is a wide band-gap material of the Ⅱ-Ⅵ group with excellent optical properties for optoelectronics applications, such as the flat panel displays and solar cells used in sports tournament. Despite ...Zinc oxide (ZnO) is a wide band-gap material of the Ⅱ-Ⅵ group with excellent optical properties for optoelectronics applications, such as the flat panel displays and solar cells used in sports tournament. Despite its advantages, the application of ZnO is hampered by the lack of stable p-type doping. In this paper, the recent progress in this field was briefly reviewed, and a comprehensive summary of the research was carded out on ZnO fabrication methods and its electrical, optical, and magnetic properties were presented.展开更多
The electronic structures and optical properties of B3 ZnO series of Zn4X4-yMy(X :O, S, Se or Te; M = N, Sb, C1 or I; y = 0 or 1) are studied by first-principles calculations using a pseudopotential plane-wave meth...The electronic structures and optical properties of B3 ZnO series of Zn4X4-yMy(X :O, S, Se or Te; M = N, Sb, C1 or I; y = 0 or 1) are studied by first-principles calculations using a pseudopotential plane-wave method. The results show that Zn d-X p orbital interactions play an important role in the p-type doping tendency in zinc-based Ⅱ-Ⅵ semiconductors. In ZnX, with increasing atomic number of X, Zn d-X p orbital interactions decrease and Zn s-X p orbital interactions increase. Additionally, substituting group-V elements for X will reduce the Zn d-X p orbital interactions while substituting group-VII elements for X will increase the Zn d-X p orbital interactions. The results also show that group-V-doped ZnX and group-Ⅷ-doped ZnX exhibit different optical behaviours due to their different orbital interaction effects.展开更多
We investigate the electronic structures and magnetic properties of ZnO doped with N,Cu,and(Cu+N)by using a first principles method and considering the strong correlation effect.It is interesting to compare these thre...We investigate the electronic structures and magnetic properties of ZnO doped with N,Cu,and(Cu+N)by using a first principles method and considering the strong correlation effect.It is interesting to compare these three systems.ZnO:N has weak p-type doping and unstable ferromagnetism,while ZnO:Cu becomes insulating due to the Jahn–Teller effect.Cu and N codoping can not only greatly improve the dopability of p-type doping accompanying the Jahn–Teller fading,but also enhance the ferromagnetism at the same time.The calculation results indicate that there is a win-win effect between N and Cu dopants in the ZnO:(Cu+N)system,which could possibly find applications in spintronics besides optoelectronics.展开更多
Cluster model with DV-Xαmethod is used to study the structural and electronic properties of the p-type doping of ZnSe.It is found that there is Jahn-Teller distortion for P doping and almost no Jahn-Teller distortion...Cluster model with DV-Xαmethod is used to study the structural and electronic properties of the p-type doping of ZnSe.It is found that there is Jahn-Teller distortion for P doping and almost no Jahn-Teller distortion for N doping,and that the impurity levels with respect to the maximum of valence band are 118 and 96meV for N and P doping,respectively.The reasons why N can serve as a better dopant than P for p-type ZnSe are discussed.展开更多
Al-rich nitride,as one of the most important ultra-wide band-gap(UWBG)semiconductors,currently plays the key role of deep ultraviolet(DUV)optoelectronics and potentially possesses the advantages of the huge global inv...Al-rich nitride,as one of the most important ultra-wide band-gap(UWBG)semiconductors,currently plays the key role of deep ultraviolet(DUV)optoelectronics and potentially possesses the advantages of the huge global investment in the manufacturing infrastructure associated with In Ga N material that has become the second most important semiconductor material after Si in the late 2010s[1,2].展开更多
The performance enhancement of MXene/semiconductor heterostructure-based light detectors is greatly restricted by the relatively small junction barrier due to the limited work function of MXenes.The work function of M...The performance enhancement of MXene/semiconductor heterostructure-based light detectors is greatly restricted by the relatively small junction barrier due to the limited work function of MXenes.The work function of MXenes can be largely adjusted to approach 600 meV through simple incorporation of V_(2)O_(5) via a charge transfer doping mechanism.Exploiting this strategy,the performance of MXene/GaN heterostructure-based deep ultraviolet(DUV)photodetectors has been greatly improved.Specifically,the photocurrent is enhanced by nearly 3 times,and the dark current is suppressed at the lowest order of magnitude,resulting in improved responsivity and specific detectivity of 121.6 mA/W and 2.23×10^(13) Jones,respectively,at 265 nm.The device also displays an ultralow dark current of 10^(-14) A,a fast response speed of 0.4 ms/15.1 ms,a large linear dynamic range exceeding 150 dB,and a high DUV/near ultraviolet rejection ratio of 2.41×10^(5).Owing to its good device performance,the detector is capable of sensing weak photon signals produced by a fire flame and functions as an optical receiver to transmit a text signal in a DUV light communication system.The proposed MXene doping method is expected to help develop MXene-based electronic/optoelectronic devices,and the present DUV photodetectors will find potential applications in DUV optoelectronic systems.展开更多
As a catalyst of the air cathode in zinc-air batteries,tungstic acid ferrous(FeWO_(4)),a nanoscale transition metal tungstate,shows a broad application prospect in the oxygen reduction reaction(ORR).While FeWO_(4)poss...As a catalyst of the air cathode in zinc-air batteries,tungstic acid ferrous(FeWO_(4)),a nanoscale transition metal tungstate,shows a broad application prospect in the oxygen reduction reaction(ORR).While FeWO_(4)possesses favorable electrochemical properties and thermodynamic stability,its intrinsic semiconductor characteristics result in a relatively slow electron transfer rate,limiting the ORR catalytic activity.In this work,the electronic structure of FeWO_(4)is significantly modulated by introducing phosphorus(P)atoms with abundant valence electrons.The P doping can adjust the electronic structure of FeWO_(4)and then optimize oxygen-containing intermediates'absorption/desorption efficiency to achieve improved ORR activity.Furthermore,the sodium chloride template is utilized to construct a porous carbon framework for anchoring phosphorus-doped iron tungstate(P-FeWO_(4)/PNC).The porous carbon skeleton provides numerous active sites for the absorption/desorption and redox reactions on the P-FeWO_(4)/PNC surface and serves as mass transport channels for reactants and intermediates.The P-FeWO_(4)/PNC demonstrates ORR performance(E1/2=0.86 V vs.RHE).Furthermore,the zinc-air batteries incorporating the P-FeWO_(4)/PNC composite demonstrate an increased peak power density(172.2 mW·cm^(-2)),high specific capacity(810.1 mAh·g^(-1)),and sustained long-term cycling stability lasting up to 240 h.This research not only contributes to the advancement of cost-effective tungsten-based non-precious metallic ORR catalysts,but also guides their utilization in zinc-air batteries.展开更多
Mn^(2+)-doped CsPbCl_(3)(Mn^(2+):CsPbCl_(3)) nanocrystals(NCs) have attracted considerable attention due to their unique strong and broad orange-red emission band,presenting promising applications in the field of phot...Mn^(2+)-doped CsPbCl_(3)(Mn^(2+):CsPbCl_(3)) nanocrystals(NCs) have attracted considerable attention due to their unique strong and broad orange-red emission band,presenting promising applications in the field of photoelectric devices.However,pristine Mn^(2+):CsPbCl_(3)NCs commonly suffer from low photoluminescence quantum yield(PL QY) and stability issues.Herein,we introduced europium ions(Eu^(3+))into Mn^(2+):CsPbCl_(3)NCs via the thermal injection synthesis method to obtain high performance Eu^(3+)and Mn^(2+)codoped CsPbCl_(3)(Eu^(3+)/Mn^(2+):CsPbCl_(3)) NCs.The maximum PL QY of the resulting Eu^(3+)/Mn^(2+):CsPbCl_(3)NCs reaches up to 90.92%.It is found that the doping of Eu^(3+)ions significantly reduces the non-radiative recombination caused by high defect states,and improves the energy transfer efficiency from exciton to Mn^(2+),thereby boosting the PL performance.Moreover,doping Eu^(3+)ions notably improves the UV-light and water stability of Mn^(2+):CsPbCl_(3)NCs.We further demonstrate the application versatility of Eu^(3+)/Mn^(2+):CsPbCl_(3)NCs in white light emitting diodes(WLEDs) and optical anticounterfeiting applications.This work provides a valuable perspective for the attainment of high performance Mn^(2+):CsPbCl_(3)NCs and lays a foundation for the codoping of other lanthanide ions to adjust the luminescence properties of Mn^(2+):CsPbCl_(3)NCs.展开更多
The van der Waals heterostructures have evolved as novel materials for complementing the Si-based semiconductor technologies.Group-10 noble metal dichalcogenides(e.g.,PtS_(2),PtSe_(2),PdS_(2),and PdSe_(2))have been li...The van der Waals heterostructures have evolved as novel materials for complementing the Si-based semiconductor technologies.Group-10 noble metal dichalcogenides(e.g.,PtS_(2),PtSe_(2),PdS_(2),and PdSe_(2))have been listed into two-dimensional(2D)materials toolkit to assemble van der Waals heterostructures.Among them,PdSe_(2) demonstrates advantages of high stability in air,high mobility,and wide tunable bandgap.However,the regulation of p-type doping of PdSe_(2) remains unsolved problem prior to fabricating p–n junction as a fundamental platform of semiconductor physics.Besides,a quantitative method for the controllable doping of PdSe_(2) is yet to be reported.In this study,the doping level of PdSe_(2) was correlated with the concentration of Lewis acids,for example,SnCl_(4),used for soaking.Considering the transfer characteristics,the threshold voltage(the gate voltage corresponding to the minimum drain current)increased after SnCl_(4) soaking treatment.PdSe_(2) transistors were soaked in SnCl_(4) solutions with five different concentrations.The threshold voltages from the as-obtained transfer curves were extracted for linear fitting to the threshold voltage versus doping concentration correlation equation.This study provides in-depth insights into the controllable p-type doping of PdSe_(2).It may also push forward the research of the regulation of conductivity behaviors of 2D materials.展开更多
Due to their superior fluorescence,phosphorescence,and catalytic capabilities,carbon dots(CDs),an emerging class of fluorescent carbon nanomaterials,have a wide range of potential applications.The properties of CDs ha...Due to their superior fluorescence,phosphorescence,and catalytic capabilities,carbon dots(CDs),an emerging class of fluorescent carbon nanomaterials,have a wide range of potential applications.The properties of CDs have recently been controlled extensively by heteroatom doping.Boron atoms have been effectively doped into the structure of CDs due to their similar size to carbon atoms and excellent electron-absorbing ability to further improve the performance of CDs.In this review,we summarize the research progress of boron-doped CDs in recent years from the aspects of doping strategies,effects of boron doping on different performances of CDs and applications.Starting from the two aspects of single boron doping and boron and other atom co-doping,from different precursor materials to different synthesis methods,the doping strategies of boron-doped CDs are reviewed in detail.Then,the effects of boron doping on the fluorescence,phosphorescence and catalytic performance of CDs and applications of boron-doped CDs in optical sensors,information encryption and anti-counterfeiting are discussed.Finally,we further provide a prospect towards the future development of boron-doped CDs.展开更多
While heteroatom doping serves as a powerful strategy for devising novel polycyclic aromatic hydrocarbons(PAHs), the further fine-tuning of optoelectronic properties via the precisely altering of doping patterns remai...While heteroatom doping serves as a powerful strategy for devising novel polycyclic aromatic hydrocarbons(PAHs), the further fine-tuning of optoelectronic properties via the precisely altering of doping patterns remains a challenge. Herein, by changing the doping positions of heteroatoms in a diindenopyrene skeleton, we report two isomeric boron, sulfur-embedded PAHs, named Anti-B_(2)S_(2) and Syn-B_(2)S_(2), as electron transporting semiconductors. Detailed structure-property relationship studies revealed that the varied heteroatom positions not only change their physicochemical properties, but also largely affect their solid-state packing modes and Lewis base-triggered photophysical responses. With their low-lying frontier molecular orbital levels, n-type characteristics with electron mobilities up to 1.5 × 10^(-3)cm^(2)V^(-1)s^(-1)were achieved in solution-processed organic field-effect transistors. Our work revealed the critical role of controlling heteroatom doping patterns for designing advanced PAHs.展开更多
Advancing high-voltage stability of layered sodium-ion oxides represents a pivotal avenue for their progress in energy storage applications.Despite this,a comprehensive understanding of the mechanisms underpinning the...Advancing high-voltage stability of layered sodium-ion oxides represents a pivotal avenue for their progress in energy storage applications.Despite this,a comprehensive understanding of the mechanisms underpinning their structural deterioration at elevated voltages remains insufficiently explored.In this study,we unveil a layer delamination phenomenon of Na_(0.67)Ni_(0.3)Mn_(0.7)O_(2)(NNM)within the 2.0-4.3 V voltage,attributed to considerable volumetric fluctuations along the c-axis and lattice oxygen reactions induced by the simultaneous Ni^(3+)/Ni^(4+)and anion redox reactions.By introducing Mg doping to diminished Ni-O antibonding,the anion oxidation-reduction reactions are effectively mitigated,and the structural integrity of the P2 phase remains firmly intact,safeguarding active sites and precluding the formation of novel interfaces.The Na_(0.67)Mg_(0.05)Ni_(0.25)Mn_(0.7)O_(2)(NMNM-5)exhibits a specific capacity of100.7 mA h g^(-1),signifying an 83%improvement compared to the NNM material within the voltage of2.0-4.3 V.This investigation underscores the intricate interplay between high-voltage stability and structural degradation mechanisms in layered sodium-ion oxides.展开更多
The construction of lateral p-n junctions is very important and challenging in two-dimensional(2D)semiconductor manufacturing process.Previous researches have demonstrated that vertical p-n junction can be prepared si...The construction of lateral p-n junctions is very important and challenging in two-dimensional(2D)semiconductor manufacturing process.Previous researches have demonstrated that vertical p-n junction can be prepared simply by vertical stacking of 2D materials.However,interface pollution and large area scalability are challenges that are difficult to overcome with vertical stacking technology.Constructing 2D lateral p-n homojunction is an effective strategy to address these issues.Spatially selective p-type doping of 2D semiconductors is expected to construct lateral p-n homojunction.In this work,we have developed a low-energy ion implantation system that reduces the implanted energy to 300 eV.Low-energy implantation can form a shallow implantation depth,which is more suitable for modulating the electrical and optical properties of 2D materials.Hence,we utilize low-energy ion implantation to directly dope nitrogen ions into few-layer WS_(2) and successfully realize a precise regulation for WS_(2) with its conductivity type transforming from n-type to bipolar or even p-type conduction.Furthermore,the universality of this method is demonstrated by extending it to other 2D semiconductors,including WSe_(2),SnS_(2) and MoS_(2).Based on this method,a lateral WS_(2) p-n homojunction is fabricated,which exhibits significant rectification characteristics.A photodetector based on p-n junction with photovoltaic effect is also prepared,and the open circuit voltage can reach to 0.39 V.This work provides an effective way for controllable doping of 2D semiconductors.展开更多
We investigated the effect of additional doping with Ce on the ionic conductivity of the Nb-doped Li_(7)La_(3)Zr_(2)O_(12)(LLZO)garnet ceramics using a combination of experimental and modeling approaches.Our results i...We investigated the effect of additional doping with Ce on the ionic conductivity of the Nb-doped Li_(7)La_(3)Zr_(2)O_(12)(LLZO)garnet ceramics using a combination of experimental and modeling approaches.Our results indicate that Ce doping can alter lattice parameters of the LLZNO,leading to the enhanced lithium ionic conductivity.The Ce,Nb co-doped LLZO(LLZNCO)structure with composition Li_(6.5)La_(3)Zr_(1.5-x)Nb_(0.5)Ce_(x)O_(12)(x=0.125)exhibits a lower activation energy(E_(a)=0.39 eV)than Li_(6.5)La_(3)Zr_(1.5)Nb_(0.5)O_(12)(LLZNO)(E_(a)=0.41 eV).Furthermore,Ce doping leads to an increase in Li~+conductivity from 6.4×10^(-4)to 7×10^(-4)S/cm at room temperature.In addition,we discuss the diffusivity and conductivity of our samples using ab initio molecular dynamics simulations and propose possible mechanisms to explain the enhanced Li-ion conductivity caused by co-doping with Ce and Nb.Our results demonstrate that the LLZNCO ceramics are promising candidates for potential solid-state electrolytes for Li-ion batteries.展开更多
The commercial viability of thermoelectric(TE)devices relies heavily on two factors:cost reduction and efficiency enhancement.In this study,we first produce p-type Cu_(12)Sb_(4)S_(16-x)(x=0,3,4)using a low-temperature...The commercial viability of thermoelectric(TE)devices relies heavily on two factors:cost reduction and efficiency enhancement.In this study,we first produce p-type Cu_(12)Sb_(4)S_(16-x)(x=0,3,4)using a low-temperature bottom-up approach and demonstrate Cu_(12)Sb_(4)S_(13)to show the best TE performance among the three tested compositions.Subsequently,the TE energy conversion efficiency of Cu_(12)Sb_(4)S_(13)is further enhanced by optimizing its electronic band structure through the incorporation of small amounts of tel-lurium.At an optimal Te content of 5 mol%,more than a twofold increase in the TE figure of merit(zT)is obtained.To gain insight into the mechanism of improvement on the transport properties of the mate-rial,we compare the interphase transport mechanism by incorporating nanodomains of different metals(Ag and Cu)into the Cu_(12)Sb_(4)S_(13)matrix.The improved electrical conductivity obtained with Cu_(12)Sb_(4)S_(13)-Te nanocomposites is attributed to a charge flooding of the Cu_(12)Sb_(4)S_(13)surface.In contrast,excessive down-ward band-bending at the interphases of Ag/Cu metal-semiconductor drastically reduces the electrical conductivity.Besides,a weighted mobility(μw)analysis shows a dominant thermal activation of carri-ers in Cu_(12)Sb_(4)S_(13)-Te nanocomposites.In this material,a strong decrease in lattice thermal conductivity is also found,which is associated with a phonon-carrier scattering mechanism.Our work shows the impor-tance of proper band-engineering in TE nanocomposites to decouple electrical and thermal transport to enhance TE performance,and the efficacy ofμw for electrical and thermal transport analysis.展开更多
The design of cost-effective and efficient metal-free carbon-based catalysts for the hydrogen evolution reaction(HER)is of great significance for increasing the production of clean hydrogen by the electrolysis of alka...The design of cost-effective and efficient metal-free carbon-based catalysts for the hydrogen evolution reaction(HER)is of great significance for increasing the production of clean hydrogen by the electrolysis of alkaline water.Precise control of the electronic structure by heteroatom doping has proven to be efficient for increasing catalytic activity.Nevertheless,both the structural characteristics and the underlying mechanism are not well understood,especially for doping with two different atoms,thus limiting the use of these catalysts.We report the production of phosphorus and nitrogen co-doped hollow carbon nanospheres(HCNs)by the copolymerization of pyrrole and aniline at a Triton X-100 micelle-interface,followed by doping with phytic acid and carbonization.The unique pore structure and defect-rich framework of the HCNs expose numerous active sites.Crucially,the combined effect of graphitic nitrogen and phosphorus-carbon bonds modulate the local electronic structure of adjacent C atoms and facilitates electron transfer.As a res-ult,the HCN carbonized at 1100°C exhibited superior HER activity and an outstanding stability(70 h at a current density of 10 mA cm^(−2))in alkaline water,because of the large number of graphitic nitrogen and phosphorus-carbon bonds.展开更多
基金supported by the National Natural Science Foundation of China(Grant Nos.52372150,12088101,and 11991060)the National Key R&D Program of China(Grant No.2022YFB4200305)。
文摘Wide-bandgap two-dimensional (2D) β-TeO_(2) has been reported as a high-mobility p-type transparent semiconductor [Nat. Electron. 4 277 (2021)], attracting significant attention. This "breakthrough" not only challenges the conventional characterization of TeO_(2) as an insulator but also conflicts with the anticipated difficulty in hole doping of TeO_(2) by established chemical trends. Notably, the reported Fermi level of 0.9 eV above the valence band maximum actually suggests that the material is an insulator, contradicting the high hole density obtained by Hall effect measurement. Furthermore, the detected residual Se and the possible reduced elemental Te in the 2D β-TeO_(2) samples introduces complexity, considering that elemental Se, Te, and Te_(1−x)Se_(x) themselves are high-mobility p-type semiconductors. Therefore, doubts regarding the true cause of the p-type conductivity observed in the 2D β-TeO_(2) samples arise. In this Letter, we employ density functional theory calculations to illustrate that TeO_(2), whether in its bulk forms of α-, β-, or γ-TeO_(2), or in the 2D β-TeO_(2) nanosheets, inherently exhibits insulating properties and poses challenges in carrier doping due to its shallow conduction band minimum and deep valence band maximum. Our findings shed light on the insulating properties and doping difficulty of TeO_(2), contrasting with the claimed p-type conductivity in the 2D β-TeO_(2) samples, prompting inquiries into the true origin of the p-type conductivity.
基金financially supported by the National Natural Science Foundation of China(Grant No.52372150)。
文摘p-type transparent oxide semiconductors(TOSs)are significant in the semiconductor industry,driving advancements in optoelectronic technologies for transparent electronic devices with unique properties.The recent discovery of p-type behavior in SeO_(2) has stimulated interest and confusion in the scientific community.In this Letter,we employ density functional theory calculations to reveal the intrinsic intrinsic insulating characteristics of SeO_(2) and highlight the substantial challenges in carrier doping.Our electronic structure analyses indicate that the Se 5^(2) states are energetically positioned too low to effectively interact with the O 2p orbitals,resulting in a valence band maximum(VBM)primarily dominated by the O 2p orbitals.The deep and localized nature of the VBM of SeO_(2) limits its potential as a high-mobility p-type TOS.Defect calculations demonstrate that all intrinsic defects in SeO_(2) exhibit deep transition levels within the bandgap.Regardless of the synthesis conditions,the Fermi level consistently resides in the mid-gap region.Furthermore,deep intrinsic acceptors and donors exhibit negative formation energies in the n-type and p-type regions,respectively,facilitating spontaneous formation and impeding external doping efforts.Thus,the reported p-type conductivity in SeO_(2) samples is unlikely to be intrinsic and is more plausibly attributable to reduced elemental Se,a well-known p-type semiconductor.
基金Supported by the Candidate Talents Training Fund of Yunnan Province(202205AC160054)the National Natural Science Foundation of China(62174156)。
文摘The lattice-matched XBn structures of InAsSb,grown on GaSb substrates,exhibit high crystal quali⁃ty,and can achieve extremely low dark currents at high operating temperatures(HOT).Its superior performance is attributed to the unipolar barrier,which blocks the majority carriers while allowing unhindered hole transport.To further explore the energy band and carrier transport mechanisms of the XBn unipolar barrier structure,this pa⁃per systematically investigates the influence of doping on the dark current,photocurrent,and tunneling character⁃istics of InAsSb photodetectors in the PBn structure.Three high-quality InAsSb samples with unintentionally doped absorption layers(AL)were prepared,with varying p-type doping concentrations in the GaSb contact layer(CL)and the AlAsSb barrier layer(BL).As the p-type doping concentration in the CL increased,the device’s turn-on bias voltage also increased,and p-type doping in the BL led to tunneling occurring at lower bias voltages.For the sample with UID BL,which exhibited an extremely low dark current of 5×10^(-6) A/cm^(2).The photocurrent characteristics were well-fitted using the back-to-back diode model,revealing the presence of two opposing space charge regions on either side of the BL.
基金Project supported by the State Key Program for Basic Research of China(Grant No.2011CB302003)the National Natural Science Foundation of China(Grant Nos.61274058,61322403,61504057,and 61574075)+1 种基金the Natural Science Foundation of Jiangsu Province,China(Grant Nos.BK20130013 and BK20150585)the Six Talent Peaks Project in Jiangsu Province,China(Grant No.2014XXRJ001)
文摘Zinc oxide(ZnO) is a compound semiconductor with a direct band gap and high exciton binding energy.The unique property,i.e.,high efficient light emission at ultraviolet band,makes ZnO potentially applied to the short-wavelength light emitting devices.However,efficient p-type doping is extremely hard for ZnO.Due to the wide band gap and low valence band energy,the self-compensation from donors and high ionization energy of acceptors are the two main problems hindering the enhancement of free hole concentration.Native defects in ZnO can be divided into donor-like and acceptorlike ones.The self-compensation has been found mainly to originate from zinc interstitial and oxygen vacancy related donors.While the acceptor-like defect,zinc vacancy,is thought to be linked to complex shallow acceptors in group-VA doped ZnO.Therefore,the understanding of the behaviors of the native defects is critical to the realization of high-efficient p-type conduction.Meanwhile,some novel ideas have been extensively proposed,like double-acceptor co-doping,acceptor doping in iso-valent element alloyed ZnO,etc.,and have opened new directions for p-type doping.Some of the approaches have been positively judged.In this article,we thus review the recent(2011-now) research progress of the native defects and p-type doping approaches globally.We hope to provide a comprehensive overview and describe a complete picture of the research status of the p-type doping in ZnO for the reference of the researchers in a similar area.
基金Funded by the National Social Science Fund Project(No.2012BTY014)
文摘Zinc oxide (ZnO) is a wide band-gap material of the Ⅱ-Ⅵ group with excellent optical properties for optoelectronics applications, such as the flat panel displays and solar cells used in sports tournament. Despite its advantages, the application of ZnO is hampered by the lack of stable p-type doping. In this paper, the recent progress in this field was briefly reviewed, and a comprehensive summary of the research was carded out on ZnO fabrication methods and its electrical, optical, and magnetic properties were presented.
基金Project supported by the National Natural Science Foundation of China (Grant No 10625416).
文摘The electronic structures and optical properties of B3 ZnO series of Zn4X4-yMy(X :O, S, Se or Te; M = N, Sb, C1 or I; y = 0 or 1) are studied by first-principles calculations using a pseudopotential plane-wave method. The results show that Zn d-X p orbital interactions play an important role in the p-type doping tendency in zinc-based Ⅱ-Ⅵ semiconductors. In ZnX, with increasing atomic number of X, Zn d-X p orbital interactions decrease and Zn s-X p orbital interactions increase. Additionally, substituting group-V elements for X will reduce the Zn d-X p orbital interactions while substituting group-VII elements for X will increase the Zn d-X p orbital interactions. The results also show that group-V-doped ZnX and group-Ⅷ-doped ZnX exhibit different optical behaviours due to their different orbital interaction effects.
基金Supported by the Project of Cultivating Innovative Talents for Colleges&Universities of Henan Province under Grant No 2002006the Natural Science Foundation of Department of Education of Henan Province under Grant No 2009B48003the Key Technologies R&D Program of Henan Province under Grant No 092102210005.
文摘We investigate the electronic structures and magnetic properties of ZnO doped with N,Cu,and(Cu+N)by using a first principles method and considering the strong correlation effect.It is interesting to compare these three systems.ZnO:N has weak p-type doping and unstable ferromagnetism,while ZnO:Cu becomes insulating due to the Jahn–Teller effect.Cu and N codoping can not only greatly improve the dopability of p-type doping accompanying the Jahn–Teller fading,but also enhance the ferromagnetism at the same time.The calculation results indicate that there is a win-win effect between N and Cu dopants in the ZnO:(Cu+N)system,which could possibly find applications in spintronics besides optoelectronics.
基金Supported by the'863'High Technology Program of China.
文摘Cluster model with DV-Xαmethod is used to study the structural and electronic properties of the p-type doping of ZnSe.It is found that there is Jahn-Teller distortion for P doping and almost no Jahn-Teller distortion for N doping,and that the impurity levels with respect to the maximum of valence band are 118 and 96meV for N and P doping,respectively.The reasons why N can serve as a better dopant than P for p-type ZnSe are discussed.
文摘Al-rich nitride,as one of the most important ultra-wide band-gap(UWBG)semiconductors,currently plays the key role of deep ultraviolet(DUV)optoelectronics and potentially possesses the advantages of the huge global investment in the manufacturing infrastructure associated with In Ga N material that has become the second most important semiconductor material after Si in the late 2010s[1,2].
基金financially supported by the National Natural Science Foundation of China(NSFC,62275002,51902078)the Anhui Provincial Natural Science Foundation(2008085MF205)the Fundamental Research Funds for the Central Universities(JZ2020HGTB0051)。
文摘The performance enhancement of MXene/semiconductor heterostructure-based light detectors is greatly restricted by the relatively small junction barrier due to the limited work function of MXenes.The work function of MXenes can be largely adjusted to approach 600 meV through simple incorporation of V_(2)O_(5) via a charge transfer doping mechanism.Exploiting this strategy,the performance of MXene/GaN heterostructure-based deep ultraviolet(DUV)photodetectors has been greatly improved.Specifically,the photocurrent is enhanced by nearly 3 times,and the dark current is suppressed at the lowest order of magnitude,resulting in improved responsivity and specific detectivity of 121.6 mA/W and 2.23×10^(13) Jones,respectively,at 265 nm.The device also displays an ultralow dark current of 10^(-14) A,a fast response speed of 0.4 ms/15.1 ms,a large linear dynamic range exceeding 150 dB,and a high DUV/near ultraviolet rejection ratio of 2.41×10^(5).Owing to its good device performance,the detector is capable of sensing weak photon signals produced by a fire flame and functions as an optical receiver to transmit a text signal in a DUV light communication system.The proposed MXene doping method is expected to help develop MXene-based electronic/optoelectronic devices,and the present DUV photodetectors will find potential applications in DUV optoelectronic systems.
基金supported by the National Natural Science Foundation of China(NSFC)(Nos.22178148 and 22278193)a Project Funded by the Priority Academic Program Development of Jiangsu Higher Education Institutions.
文摘As a catalyst of the air cathode in zinc-air batteries,tungstic acid ferrous(FeWO_(4)),a nanoscale transition metal tungstate,shows a broad application prospect in the oxygen reduction reaction(ORR).While FeWO_(4)possesses favorable electrochemical properties and thermodynamic stability,its intrinsic semiconductor characteristics result in a relatively slow electron transfer rate,limiting the ORR catalytic activity.In this work,the electronic structure of FeWO_(4)is significantly modulated by introducing phosphorus(P)atoms with abundant valence electrons.The P doping can adjust the electronic structure of FeWO_(4)and then optimize oxygen-containing intermediates'absorption/desorption efficiency to achieve improved ORR activity.Furthermore,the sodium chloride template is utilized to construct a porous carbon framework for anchoring phosphorus-doped iron tungstate(P-FeWO_(4)/PNC).The porous carbon skeleton provides numerous active sites for the absorption/desorption and redox reactions on the P-FeWO_(4)/PNC surface and serves as mass transport channels for reactants and intermediates.The P-FeWO_(4)/PNC demonstrates ORR performance(E1/2=0.86 V vs.RHE).Furthermore,the zinc-air batteries incorporating the P-FeWO_(4)/PNC composite demonstrate an increased peak power density(172.2 mW·cm^(-2)),high specific capacity(810.1 mAh·g^(-1)),and sustained long-term cycling stability lasting up to 240 h.This research not only contributes to the advancement of cost-effective tungsten-based non-precious metallic ORR catalysts,but also guides their utilization in zinc-air batteries.
基金Project supported by the National Natural Science Foundation of China (12174075)the Scientific and Technological Bases and Talents of Guangxi (Guike AD21220016)+1 种基金Guangxi Science and Technology Major Project(AA23073018)the special fund for Guangxi Bagui Scholars。
文摘Mn^(2+)-doped CsPbCl_(3)(Mn^(2+):CsPbCl_(3)) nanocrystals(NCs) have attracted considerable attention due to their unique strong and broad orange-red emission band,presenting promising applications in the field of photoelectric devices.However,pristine Mn^(2+):CsPbCl_(3)NCs commonly suffer from low photoluminescence quantum yield(PL QY) and stability issues.Herein,we introduced europium ions(Eu^(3+))into Mn^(2+):CsPbCl_(3)NCs via the thermal injection synthesis method to obtain high performance Eu^(3+)and Mn^(2+)codoped CsPbCl_(3)(Eu^(3+)/Mn^(2+):CsPbCl_(3)) NCs.The maximum PL QY of the resulting Eu^(3+)/Mn^(2+):CsPbCl_(3)NCs reaches up to 90.92%.It is found that the doping of Eu^(3+)ions significantly reduces the non-radiative recombination caused by high defect states,and improves the energy transfer efficiency from exciton to Mn^(2+),thereby boosting the PL performance.Moreover,doping Eu^(3+)ions notably improves the UV-light and water stability of Mn^(2+):CsPbCl_(3)NCs.We further demonstrate the application versatility of Eu^(3+)/Mn^(2+):CsPbCl_(3)NCs in white light emitting diodes(WLEDs) and optical anticounterfeiting applications.This work provides a valuable perspective for the attainment of high performance Mn^(2+):CsPbCl_(3)NCs and lays a foundation for the codoping of other lanthanide ions to adjust the luminescence properties of Mn^(2+):CsPbCl_(3)NCs.
基金the Natural Science Foundation of Shandong Province for Excellent Young Scholars(No.ZR2022YQ41)the fund(No.SKT2203)from the State Key Laboratories of Transducer Technology,Shanghai Institute of Microsystem and Information Technology+9 种基金Chinese Academy of Sciences for support.This work was partially supported by the National Key Research and Development Program of China(No.2022YFE0124200)the National Natural Science Foundation of China(No.U2241221)W.J.Z.thanks the Major innovation project of Shandong Province(No.2021CXGC010603)the National Natural Science Foundation of China(No.52022037)the Taishan Scholars Project Special Funds(No.TSQN201812083)The project was supported by the Foundation(No.GZKF202107)of State Key Laboratory of Biobased Material and Green PapermakingQilu University of Technology,Shandong Academy of Sciences.M.H.R.thanks the National Natural Science Foundation of China(No.52071225)the National Science Center and the Czech Republic under the ERDF program“Institute of Environmental Technology-Excellent Research”(No.CZ.02.1.01/0.0/0.0/16_019/0000853)the Sino-German Research Institute(No.GZ 1400)for supportS.X.H.thanks the National Natural Science Foundation of China(Nos.21976014 and 22276013)for funding,and thanks the Tianhe2-JK HPC for generous computer time.
文摘The van der Waals heterostructures have evolved as novel materials for complementing the Si-based semiconductor technologies.Group-10 noble metal dichalcogenides(e.g.,PtS_(2),PtSe_(2),PdS_(2),and PdSe_(2))have been listed into two-dimensional(2D)materials toolkit to assemble van der Waals heterostructures.Among them,PdSe_(2) demonstrates advantages of high stability in air,high mobility,and wide tunable bandgap.However,the regulation of p-type doping of PdSe_(2) remains unsolved problem prior to fabricating p–n junction as a fundamental platform of semiconductor physics.Besides,a quantitative method for the controllable doping of PdSe_(2) is yet to be reported.In this study,the doping level of PdSe_(2) was correlated with the concentration of Lewis acids,for example,SnCl_(4),used for soaking.Considering the transfer characteristics,the threshold voltage(the gate voltage corresponding to the minimum drain current)increased after SnCl_(4) soaking treatment.PdSe_(2) transistors were soaked in SnCl_(4) solutions with five different concentrations.The threshold voltages from the as-obtained transfer curves were extracted for linear fitting to the threshold voltage versus doping concentration correlation equation.This study provides in-depth insights into the controllable p-type doping of PdSe_(2).It may also push forward the research of the regulation of conductivity behaviors of 2D materials.
基金the Youth Talent Program Startup Foundation of Qufu Normal University(No.602601)the Natural Science Foundation of Rizhao(No.RZ2021ZR37)。
文摘Due to their superior fluorescence,phosphorescence,and catalytic capabilities,carbon dots(CDs),an emerging class of fluorescent carbon nanomaterials,have a wide range of potential applications.The properties of CDs have recently been controlled extensively by heteroatom doping.Boron atoms have been effectively doped into the structure of CDs due to their similar size to carbon atoms and excellent electron-absorbing ability to further improve the performance of CDs.In this review,we summarize the research progress of boron-doped CDs in recent years from the aspects of doping strategies,effects of boron doping on different performances of CDs and applications.Starting from the two aspects of single boron doping and boron and other atom co-doping,from different precursor materials to different synthesis methods,the doping strategies of boron-doped CDs are reviewed in detail.Then,the effects of boron doping on the fluorescence,phosphorescence and catalytic performance of CDs and applications of boron-doped CDs in optical sensors,information encryption and anti-counterfeiting are discussed.Finally,we further provide a prospect towards the future development of boron-doped CDs.
基金the National Natural Science Foundation of China (Nos.22375059, 22005133, 51922039 and52273174)Shenzhen Science and Technology Program (No.RCJC20200714114434015)+1 种基金Science and Technology Innovation Program of Hunan Province (No.2020RC5033)National Key Research and Development Program of China (No.2020YFC1807302) for financial support。
文摘While heteroatom doping serves as a powerful strategy for devising novel polycyclic aromatic hydrocarbons(PAHs), the further fine-tuning of optoelectronic properties via the precisely altering of doping patterns remains a challenge. Herein, by changing the doping positions of heteroatoms in a diindenopyrene skeleton, we report two isomeric boron, sulfur-embedded PAHs, named Anti-B_(2)S_(2) and Syn-B_(2)S_(2), as electron transporting semiconductors. Detailed structure-property relationship studies revealed that the varied heteroatom positions not only change their physicochemical properties, but also largely affect their solid-state packing modes and Lewis base-triggered photophysical responses. With their low-lying frontier molecular orbital levels, n-type characteristics with electron mobilities up to 1.5 × 10^(-3)cm^(2)V^(-1)s^(-1)were achieved in solution-processed organic field-effect transistors. Our work revealed the critical role of controlling heteroatom doping patterns for designing advanced PAHs.
基金the financial support from the National Natural Science Foundation of China(52202338)。
文摘Advancing high-voltage stability of layered sodium-ion oxides represents a pivotal avenue for their progress in energy storage applications.Despite this,a comprehensive understanding of the mechanisms underpinning their structural deterioration at elevated voltages remains insufficiently explored.In this study,we unveil a layer delamination phenomenon of Na_(0.67)Ni_(0.3)Mn_(0.7)O_(2)(NNM)within the 2.0-4.3 V voltage,attributed to considerable volumetric fluctuations along the c-axis and lattice oxygen reactions induced by the simultaneous Ni^(3+)/Ni^(4+)and anion redox reactions.By introducing Mg doping to diminished Ni-O antibonding,the anion oxidation-reduction reactions are effectively mitigated,and the structural integrity of the P2 phase remains firmly intact,safeguarding active sites and precluding the formation of novel interfaces.The Na_(0.67)Mg_(0.05)Ni_(0.25)Mn_(0.7)O_(2)(NMNM-5)exhibits a specific capacity of100.7 mA h g^(-1),signifying an 83%improvement compared to the NNM material within the voltage of2.0-4.3 V.This investigation underscores the intricate interplay between high-voltage stability and structural degradation mechanisms in layered sodium-ion oxides.
基金financially supported by the National Natural Science Foundation of China (12025503,U23B2072,12074293,and 12275198)the Fundamental Research Funds for the Center Universities (2042024kf0001 and 2042023kf0196).
文摘The construction of lateral p-n junctions is very important and challenging in two-dimensional(2D)semiconductor manufacturing process.Previous researches have demonstrated that vertical p-n junction can be prepared simply by vertical stacking of 2D materials.However,interface pollution and large area scalability are challenges that are difficult to overcome with vertical stacking technology.Constructing 2D lateral p-n homojunction is an effective strategy to address these issues.Spatially selective p-type doping of 2D semiconductors is expected to construct lateral p-n homojunction.In this work,we have developed a low-energy ion implantation system that reduces the implanted energy to 300 eV.Low-energy implantation can form a shallow implantation depth,which is more suitable for modulating the electrical and optical properties of 2D materials.Hence,we utilize low-energy ion implantation to directly dope nitrogen ions into few-layer WS_(2) and successfully realize a precise regulation for WS_(2) with its conductivity type transforming from n-type to bipolar or even p-type conduction.Furthermore,the universality of this method is demonstrated by extending it to other 2D semiconductors,including WSe_(2),SnS_(2) and MoS_(2).Based on this method,a lateral WS_(2) p-n homojunction is fabricated,which exhibits significant rectification characteristics.A photodetector based on p-n junction with photovoltaic effect is also prepared,and the open circuit voltage can reach to 0.39 V.This work provides an effective way for controllable doping of 2D semiconductors.
基金Project supported by the Scientific Research Startup Fund of Inner Mongolia University of Science and Technology(0303052202)Natural Science Foundation of Inner Mongolia Autonomous Region(2020ZD17,2022FX08)。
文摘We investigated the effect of additional doping with Ce on the ionic conductivity of the Nb-doped Li_(7)La_(3)Zr_(2)O_(12)(LLZO)garnet ceramics using a combination of experimental and modeling approaches.Our results indicate that Ce doping can alter lattice parameters of the LLZNO,leading to the enhanced lithium ionic conductivity.The Ce,Nb co-doped LLZO(LLZNCO)structure with composition Li_(6.5)La_(3)Zr_(1.5-x)Nb_(0.5)Ce_(x)O_(12)(x=0.125)exhibits a lower activation energy(E_(a)=0.39 eV)than Li_(6.5)La_(3)Zr_(1.5)Nb_(0.5)O_(12)(LLZNO)(E_(a)=0.41 eV).Furthermore,Ce doping leads to an increase in Li~+conductivity from 6.4×10^(-4)to 7×10^(-4)S/cm at room temperature.In addition,we discuss the diffusivity and conductivity of our samples using ab initio molecular dynamics simulations and propose possible mechanisms to explain the enhanced Li-ion conductivity caused by co-doping with Ce and Nb.Our results demonstrate that the LLZNCO ceramics are promising candidates for potential solid-state electrolytes for Li-ion batteries.
基金Dr.K.H.Lim acknowledges the financial support of the National Natural Science Foundation of China(Grant No.22208293)Research Funds of the Institute of Zhejiang University-Quzhou(Nos.IZQ2021RCZX003,IZQ2021RCZX002,IZQ2021KJ2024,IZQ2022KYZX09)+3 种基金supported by the State Key Laboratory of Fluorinated Greenhouse gases Replacement and Treatment(No.SKLFGGRT2022001)the State Key Laboratory of Electrical Insulation and Power Equipment(No.EIPE23201)Dr.Y.Liu acknowledges funding from the National Natural Science Foundation of China(NSFC)(Grants No.22209034)the Innovation and Entrepreneurship Project of Overseas Returnees in Anhui Province(Grants No.2022LCX002)。
文摘The commercial viability of thermoelectric(TE)devices relies heavily on two factors:cost reduction and efficiency enhancement.In this study,we first produce p-type Cu_(12)Sb_(4)S_(16-x)(x=0,3,4)using a low-temperature bottom-up approach and demonstrate Cu_(12)Sb_(4)S_(13)to show the best TE performance among the three tested compositions.Subsequently,the TE energy conversion efficiency of Cu_(12)Sb_(4)S_(13)is further enhanced by optimizing its electronic band structure through the incorporation of small amounts of tel-lurium.At an optimal Te content of 5 mol%,more than a twofold increase in the TE figure of merit(zT)is obtained.To gain insight into the mechanism of improvement on the transport properties of the mate-rial,we compare the interphase transport mechanism by incorporating nanodomains of different metals(Ag and Cu)into the Cu_(12)Sb_(4)S_(13)matrix.The improved electrical conductivity obtained with Cu_(12)Sb_(4)S_(13)-Te nanocomposites is attributed to a charge flooding of the Cu_(12)Sb_(4)S_(13)surface.In contrast,excessive down-ward band-bending at the interphases of Ag/Cu metal-semiconductor drastically reduces the electrical conductivity.Besides,a weighted mobility(μw)analysis shows a dominant thermal activation of carri-ers in Cu_(12)Sb_(4)S_(13)-Te nanocomposites.In this material,a strong decrease in lattice thermal conductivity is also found,which is associated with a phonon-carrier scattering mechanism.Our work shows the impor-tance of proper band-engineering in TE nanocomposites to decouple electrical and thermal transport to enhance TE performance,and the efficacy ofμw for electrical and thermal transport analysis.
基金financially supported by the project of the National Natural Science Foundation of China(52322203)the Key Research and Development Program of Shaanxi Province(2024GHZDXM-21)。
文摘The design of cost-effective and efficient metal-free carbon-based catalysts for the hydrogen evolution reaction(HER)is of great significance for increasing the production of clean hydrogen by the electrolysis of alkaline water.Precise control of the electronic structure by heteroatom doping has proven to be efficient for increasing catalytic activity.Nevertheless,both the structural characteristics and the underlying mechanism are not well understood,especially for doping with two different atoms,thus limiting the use of these catalysts.We report the production of phosphorus and nitrogen co-doped hollow carbon nanospheres(HCNs)by the copolymerization of pyrrole and aniline at a Triton X-100 micelle-interface,followed by doping with phytic acid and carbonization.The unique pore structure and defect-rich framework of the HCNs expose numerous active sites.Crucially,the combined effect of graphitic nitrogen and phosphorus-carbon bonds modulate the local electronic structure of adjacent C atoms and facilitates electron transfer.As a res-ult,the HCN carbonized at 1100°C exhibited superior HER activity and an outstanding stability(70 h at a current density of 10 mA cm^(−2))in alkaline water,because of the large number of graphitic nitrogen and phosphorus-carbon bonds.