Two-dimensional(2D)transition metal dichalcogenides(TMD)are atomically thin semiconductors with promising optoelectronic applications across the visible spectrum.However,their intrinsically weak light absorption and t...Two-dimensional(2D)transition metal dichalcogenides(TMD)are atomically thin semiconductors with promising optoelectronic applications across the visible spectrum.However,their intrinsically weak light absorption and the low photoluminescence quantum yield(PLQY)restrict their performance and potential use,especially in ultraviolet(UV)wavelength light ranges.Quantum dots(QD)derived from 2D materials(2D/QD)provide efficient light absorption and emission of which energy can be tuned for desirable light wavelength.In this study,we greatly enhanced the photon absorption and PLQY of monolayer(1L)tungsten disulfide(WS_(2))in the UV range via hybridization with 2D/QD,particularly titanium nitride MXene QD(Ti_(2)N MQD)and graphitic carbon nitride QD(GCNQD).With the hybridization of MQD or GCNQD,1LWS_(2)showed a maximum PL enhancement by 15 times with 300 nm wavelength excitation,while no noticeable enhancement was observed when the excitation photon energy was less than the bandgap of the QD,indicating that UV absorption by the QD played a crucial role in enhancing the light emission of 1L-WS_(2)in our 0D/2D hybrid system.Our findings present a convenient method for enhancing the photo-response of 1L-WS_(2)to UV light and offer exciting possibilities for harvesting UV energy using 1L-TMD.展开更多
Urea synthesis through the simultaneous electrocatalytic reduction of N_(2)and CO_(2)molecules under ambient conditions holds great promises as a sustainable alternative to its industrial production,in which the devel...Urea synthesis through the simultaneous electrocatalytic reduction of N_(2)and CO_(2)molecules under ambient conditions holds great promises as a sustainable alternative to its industrial production,in which the development of stable,highly efficient,and highly selective catalysts to boost the chemisorption,activation,and coupling of inert N_(2)and CO_(2)molecules remains rather challenging.Herein,by means of density functional theory computations,we proposed a new class of two-dimensional nanomaterials,namely,transition-metal phosphide monolayers(TM_(2)P,TM=Ti,Fe,Zr,Mo,and W),as the potential electrocatalysts for urea production.Our results showed that these TM_(2)P materials exhibit outstanding stability and excellent metallic properties.Interestingly,the Mo_(2)P monolayer was screened out as the best catalyst for urea synthesis due to its small kinetic energy barrier(0.35 eV)for C-N coupling,low limiting potential(-0.39 V),and significant suppressing effects on the competing side reactions.The outstanding catalytic activity of the Mo_(2)P monolayer can be ascribed to its optimal adsorption strength with the key^(*)NCON species due to its moderate positive charges on the Mo active sites.Our findings not only propose a novel catalyst with high-efficiency and high-selectivity for urea production but also further widen the potential applications of metal phosphides in electrocatalysis.展开更多
High theoretical capacity and unique layered structures make MoS_(2)a promising lithium-ion battery anode material.However,the anisotropic ion transport in layered structures and the poor intrinsic conductivity of MoS...High theoretical capacity and unique layered structures make MoS_(2)a promising lithium-ion battery anode material.However,the anisotropic ion transport in layered structures and the poor intrinsic conductivity of MoS_(2)lead to unacceptable ion transport capability.Here,we propose in-situ construction of interlayer electrostatic repulsion caused by Co^(2+)substituting Mo^(4+)between MoS_(2)layers,which can break the limitation of interlayer van der Waals forces to fabricate monolayer MoS_(2),thus establishing isotropic ion transport paths.Simultaneously,the doped Co atoms change the electronic structure of monolayer MoS_(2),thus improving its intrinsic conductivity.Importantly,the doped Co atoms can be converted into Co nanoparticles to create a space charge region to accelerate ion transport.Hence,the Co-doped monolayer MoS_(2)shows ultrafast lithium ion transport capability in half/full cells.This work presents a novel route for the preparation of monolayer MoS_(2)and demonstrates its potential for application in fast-charging lithium-ion batteries.展开更多
As a two-dimensional(2D)material,monolayer MoS2which limits its optical applications has a low absorption efficiency.In this paper,we propose a three-band perfect metamaterial absorber in the visible light range based...As a two-dimensional(2D)material,monolayer MoS2which limits its optical applications has a low absorption efficiency.In this paper,we propose a three-band perfect metamaterial absorber in the visible light range based on monolayer MoS_(2).The peak absorptivity of the structure at each resonance wavelength is nearly perfect,moreover,the light absorption of monolayer MoS2is obviously enhanced at the three resonant wavelengths.The dielectric–dielectric–metal structure we designed produces the coupling of Fabry–Perot resonance and high-order diffraction guided-mode resonance at different absorption peaks,which has been proved by the slab waveguide theory.In addition,the multi-modal absorption phenomenon is explained by extracting the equivalent impedance.The results show that we can adjust the absorption peak wavelength by regulating the parameters of the structure.This structure not only provides an idea for enhancing the interaction between light and two-dimensional materials but also has potential applications for optical detection devices.展开更多
The design and preparation of novel quantum materials with atomic precision are crucial for exploring new physics and for device applications.Electron irradiation has been demonstrated as an effective method for prepa...The design and preparation of novel quantum materials with atomic precision are crucial for exploring new physics and for device applications.Electron irradiation has been demonstrated as an effective method for preparing novel quantum materials and quantum structures that could be challenging to obtain otherwise.It features the advantages of precise control over the patterning of such new materials and their integration with other materials with different functionalities.Here,we present a new strategy for fabricating freestanding monolayer SiC within nanopores of a graphene membrane.By regulating the energy of the incident electron beam and the in-situ heating temperature in a scanning transmission electron microscope(STEM),we can effectively control the patterning of nanopores and subsequent growth of monolayer SiC within the graphene lattice.The resultant SiC monolayers seamlessly connect with the graphene lattice,forming a planar structure distinct by a wide direct bandgap.Our in-situ STEM observations further uncover that the growth of monolayer SiC within the graphene nanopore is driven by a combination of bond rotation and atom extrusion,providing new insights into the atom-by-atom self-assembly of freestanding two-dimensional(2D)monolayers.展开更多
The polarization switching plays a crucial role in controlling the final products in the catalytic pro-cess.The effect of polarization orientation on nitrogen reduction was investigated by anchoring transition metal a...The polarization switching plays a crucial role in controlling the final products in the catalytic pro-cess.The effect of polarization orientation on nitrogen reduction was investigated by anchoring transition metal atoms to form active centers on ferroelectric material In_(2)Se_(3).During the polariza-tion switching process,the difference in surface electrostatic potential leads to a redistribution of electronic states.This affects the interaction strength between the adsorbed small molecules and the catalyst substrate,thereby altering the reaction barrier.In addition,the surface states must be considered to prevent the adsorption of other small molecules(such as*O,*OH,and*H).Further-more,the V@↓-In_(2)Se_(3)possesses excellent catalytic properties,high electrochemical and thermody-namic stability,which facilitates the catalytic process.Machine learning also helps us further ex-plore the underlying mechanisms.The systematic investigation provides novel insights into the design and application of two-dimensional switchable ferroelectric catalysts for various chemical processes.展开更多
This work details a study based on HfS_(2 )transistors utilizing an n-octadecylphosphonic acid-based self-assembled monolayer(SAM)as the gate dielectric.The fabrication of the SAM-based two-dimensional(2D)material tra...This work details a study based on HfS_(2 )transistors utilizing an n-octadecylphosphonic acid-based self-assembled monolayer(SAM)as the gate dielectric.The fabrication of the SAM-based two-dimensional(2D)material transistor is simple and can be used to improve the quality of the interface of air-sensitive 2D materials.In comparison to HfS_(2) transistors utilizing a conventional Al_2O_(3) gate insulator by atomic layer deposition,HfS_(2) transistors utilizing an SAM as the gate dielectric can reduce the operation region from 4 V to 2 V,enhance the field-effect mobility from 0.03 cm^2/Vs to 0.75 cm^2/Vs,improve the sub-threshold swing from 404 m V/dec to 156 m V/dec,and optimize the hysteresis to 0.03 V,thus demonstrating improved quality of the semiconductor/insulator interface.展开更多
Transition-metal dichalcogenide(TMD) semiconductors have attracted interest as photoelectrochemical(PEC) electrodes due to their novel band-gap structures,optoelectronic properties, and photocatalytic activities.Howev...Transition-metal dichalcogenide(TMD) semiconductors have attracted interest as photoelectrochemical(PEC) electrodes due to their novel band-gap structures,optoelectronic properties, and photocatalytic activities.However, the photo-harvesting efficiency still requires improvement. In this study, A TMD stacked heterojunction structure was adopted to further enhance the performance of the PEC cathode. A P-type WSe_2 and an N-type Mo S_2 monolayer were stacked layer-by-layer to build a ultrathin vertical heterojunction using a micro-fabrication method.In situ measurement was employed to characterize the intrinsic PEC performance on a single-sheet heterostructure.Benefitting from its built-in electric field and type II band alignment, the MoS_2/WSe_2 bilayer heterojunction exhibited exceptional photocatalytic activity and a high incident photo-to-current conversion efficiency(IPCE). Comparing with the monolayer WSe_2 cathode, the PEC current and the IPCE of the bilayer heterojunction increased by a factor of 5.6 and enhanced 50%, respectively. The intriguing performance renders the MoS_2/WSe_2 heterojunction attractive for application in high-performance PEC water splitting.展开更多
Searching for two-dimensional（2 D） stable materials with direct band gap and high carrier mobility has attracted great attention for their electronic device applications.Using the first principles calculations and p...Searching for two-dimensional（2 D） stable materials with direct band gap and high carrier mobility has attracted great attention for their electronic device applications.Using the first principles calculations and particle swarm optimization（PSO） method,we predict a new 2 D stable material（HfNZ monolayer） with the global minimum of 2 D space.The HfNZ monolayer possesses direct band gap（～1.46 eV） and it is predicted to have high carrier mobilities(～103 cm2·V-1·s-1)from deformation potential theory.The direct band gap can be well maintained and flexibly modulated by applying an easily external strain under the strain conditions.In addition,the newly predicted HfN2 monolayer possesses good thermal,dynamical,and mechanical stabilities,which are verified by ab initio molecular dynamics simulations,phonon dispersion and elastic constants.These results demonstrate that HfN2 monolayer is a promising candidate in future microelectronic devices.展开更多
To maximize the catalytic performance of MoS_(2) in the hydrogen evolution reaction,we investigate the electrocatalytic and photocatalytic performance of monolayer MoS_(2) doped with noble metal(Ag,Au,Cu,Pd,and Pt)usi...To maximize the catalytic performance of MoS_(2) in the hydrogen evolution reaction,we investigate the electrocatalytic and photocatalytic performance of monolayer MoS_(2) doped with noble metal(Ag,Au,Cu,Pd,and Pt)using first principles calculation combined with the climbing image nudged elastic band method.We find the band gap of the monolayer MoS_(2) is reduced significantly by the noble metal doping,which is unfavorable to improving its photocatalytic performance.The optical absorption coefficient shows that the doping does not increase the ability of the monolayer MoS_(2) to absorb visible light.The monolayer MoS_(2) doped with the noble metal is not a potential photocatalyst for the hydrogen evolution reaction because the band edge position of the conduction band minimum is lower than-4.44 eV,the reduction potential of H^(+)/H_(2).Fortunately,the band gap reduction increases the electron transport performance of the monolayer MoS_(2),and the activation energy of water splitting is greatly reduced by the noble metal doping,especially the Pt doping.On the whole,noble metal doping can enhance the electrocatalytic performance of the monolayer MoS_(2).展开更多
Formaldehyde(HCHO) is a common indoor pollutant, long-term exposure to HCHO may harm human health. Its efficient removal at mild conditions is still challenging. The catalytic oxidation of HCHO molecules on a single a...Formaldehyde(HCHO) is a common indoor pollutant, long-term exposure to HCHO may harm human health. Its efficient removal at mild conditions is still challenging. The catalytic oxidation of HCHO molecules on a single atomic catalyst, Ti-decorated Ti3C2O2(Ti/Ti3C2O2) monolayer, is investigated by performing the first principles calculations in this work. It demonstrates that Ti atoms can be easily well dispersed at the form of single atom on Ti3C2O2 monolayer without aggregation. For HCHO catalytic oxidation, both Langmuir-Hinshelwood(LH) and Eley-Rideal(ER) mechanisms are considered. The results show that the step of HCHO dissociative adsorption on Ti/Ti3C2O2 with activated O2 can release high energy of 4.05 e V based on the ER mechanism, which can help to overcome the energy barrier(1.04 e V) of the subsequent reaction steps. The charge transfer from *OH group to CO molecule(dissociated from HCHO) not only promotes *OH group activation but also plays an important role in the H2 O generation along the ER mechanism. Therefore, HCHO can be oxidized easily on Ti/Ti3C2O2 monolayer, this work could provide significant guidance to develop effective non-noble metal catalysts for HCHO oxidation and broaden the applications of MXene-based materials.展开更多
基金supported by National Research Foundation of Korea (NRF)funded by the Ministry of Education (2021R1A6A1A03039696,2022R1A2C2009412)
文摘Two-dimensional(2D)transition metal dichalcogenides(TMD)are atomically thin semiconductors with promising optoelectronic applications across the visible spectrum.However,their intrinsically weak light absorption and the low photoluminescence quantum yield(PLQY)restrict their performance and potential use,especially in ultraviolet(UV)wavelength light ranges.Quantum dots(QD)derived from 2D materials(2D/QD)provide efficient light absorption and emission of which energy can be tuned for desirable light wavelength.In this study,we greatly enhanced the photon absorption and PLQY of monolayer(1L)tungsten disulfide(WS_(2))in the UV range via hybridization with 2D/QD,particularly titanium nitride MXene QD(Ti_(2)N MQD)and graphitic carbon nitride QD(GCNQD).With the hybridization of MQD or GCNQD,1LWS_(2)showed a maximum PL enhancement by 15 times with 300 nm wavelength excitation,while no noticeable enhancement was observed when the excitation photon energy was less than the bandgap of the QD,indicating that UV absorption by the QD played a crucial role in enhancing the light emission of 1L-WS_(2)in our 0D/2D hybrid system.Our findings present a convenient method for enhancing the photo-response of 1L-WS_(2)to UV light and offer exciting possibilities for harvesting UV energy using 1L-TMD.
基金financially supported in China by Natural Science Funds for Distinguished Young Scholars of Heilongjiang Province(No.JC2018004)Natural Science Foundation of Heilongjiang Province of China(No.TD2020B001)in the USA by NSF-CREST Center for Innovation,Research,and Education in Environmental Nanotechnology(CIRE2N)(No.HRD-1736093)
文摘Urea synthesis through the simultaneous electrocatalytic reduction of N_(2)and CO_(2)molecules under ambient conditions holds great promises as a sustainable alternative to its industrial production,in which the development of stable,highly efficient,and highly selective catalysts to boost the chemisorption,activation,and coupling of inert N_(2)and CO_(2)molecules remains rather challenging.Herein,by means of density functional theory computations,we proposed a new class of two-dimensional nanomaterials,namely,transition-metal phosphide monolayers(TM_(2)P,TM=Ti,Fe,Zr,Mo,and W),as the potential electrocatalysts for urea production.Our results showed that these TM_(2)P materials exhibit outstanding stability and excellent metallic properties.Interestingly,the Mo_(2)P monolayer was screened out as the best catalyst for urea synthesis due to its small kinetic energy barrier(0.35 eV)for C-N coupling,low limiting potential(-0.39 V),and significant suppressing effects on the competing side reactions.The outstanding catalytic activity of the Mo_(2)P monolayer can be ascribed to its optimal adsorption strength with the key^(*)NCON species due to its moderate positive charges on the Mo active sites.Our findings not only propose a novel catalyst with high-efficiency and high-selectivity for urea production but also further widen the potential applications of metal phosphides in electrocatalysis.
基金financially supported by Shenzhen Key Laboratory of Advanced Energy Storage(No.ZDSYS20220401141000001)the Research Grants Council of the Hong Kong Special Administrative Region,China(Project No.R6005-20)。
文摘High theoretical capacity and unique layered structures make MoS_(2)a promising lithium-ion battery anode material.However,the anisotropic ion transport in layered structures and the poor intrinsic conductivity of MoS_(2)lead to unacceptable ion transport capability.Here,we propose in-situ construction of interlayer electrostatic repulsion caused by Co^(2+)substituting Mo^(4+)between MoS_(2)layers,which can break the limitation of interlayer van der Waals forces to fabricate monolayer MoS_(2),thus establishing isotropic ion transport paths.Simultaneously,the doped Co atoms change the electronic structure of monolayer MoS_(2),thus improving its intrinsic conductivity.Importantly,the doped Co atoms can be converted into Co nanoparticles to create a space charge region to accelerate ion transport.Hence,the Co-doped monolayer MoS_(2)shows ultrafast lithium ion transport capability in half/full cells.This work presents a novel route for the preparation of monolayer MoS_(2)and demonstrates its potential for application in fast-charging lithium-ion batteries.
基金the Strategic Priority Research Program of Chinese Academy of Sciences(Grant No.XDB43010000)the National Natural Science Foundation of China(Grant Nos.61835011 and 12075244)+1 种基金Key Research Projects of the Frontier Science of the Chinese Academy of Sciences(Grant No.QYZDY-SSW-JSC004)the National Key Research and Development Program of China(Grant No.2020YFB2206103).
文摘As a two-dimensional(2D)material,monolayer MoS2which limits its optical applications has a low absorption efficiency.In this paper,we propose a three-band perfect metamaterial absorber in the visible light range based on monolayer MoS_(2).The peak absorptivity of the structure at each resonance wavelength is nearly perfect,moreover,the light absorption of monolayer MoS2is obviously enhanced at the three resonant wavelengths.The dielectric–dielectric–metal structure we designed produces the coupling of Fabry–Perot resonance and high-order diffraction guided-mode resonance at different absorption peaks,which has been proved by the slab waveguide theory.In addition,the multi-modal absorption phenomenon is explained by extracting the equivalent impedance.The results show that we can adjust the absorption peak wavelength by regulating the parameters of the structure.This structure not only provides an idea for enhancing the interaction between light and two-dimensional materials but also has potential applications for optical detection devices.
基金supports from the Electron Microscopy Center at the University of Chinese Academy of Sciencesfinancially supported by the Ministry of Science and Technology (MOST)of China (Grant No.2018YFE0202700)+3 种基金the Beijing Outstanding Young Scientist Program (Grant No.BJJWZYJH01201914430039)the China National Postdoctoral Program for Innovative Talents (Grant No.BX2021301)the Fundamental Research Funds for the Central Universitiesthe Research Funds of Renmin University of China (Grants No.22XNKJ30)。
文摘The design and preparation of novel quantum materials with atomic precision are crucial for exploring new physics and for device applications.Electron irradiation has been demonstrated as an effective method for preparing novel quantum materials and quantum structures that could be challenging to obtain otherwise.It features the advantages of precise control over the patterning of such new materials and their integration with other materials with different functionalities.Here,we present a new strategy for fabricating freestanding monolayer SiC within nanopores of a graphene membrane.By regulating the energy of the incident electron beam and the in-situ heating temperature in a scanning transmission electron microscope(STEM),we can effectively control the patterning of nanopores and subsequent growth of monolayer SiC within the graphene lattice.The resultant SiC monolayers seamlessly connect with the graphene lattice,forming a planar structure distinct by a wide direct bandgap.Our in-situ STEM observations further uncover that the growth of monolayer SiC within the graphene nanopore is driven by a combination of bond rotation and atom extrusion,providing new insights into the atom-by-atom self-assembly of freestanding two-dimensional(2D)monolayers.
文摘The polarization switching plays a crucial role in controlling the final products in the catalytic pro-cess.The effect of polarization orientation on nitrogen reduction was investigated by anchoring transition metal atoms to form active centers on ferroelectric material In_(2)Se_(3).During the polariza-tion switching process,the difference in surface electrostatic potential leads to a redistribution of electronic states.This affects the interaction strength between the adsorbed small molecules and the catalyst substrate,thereby altering the reaction barrier.In addition,the surface states must be considered to prevent the adsorption of other small molecules(such as*O,*OH,and*H).Further-more,the V@↓-In_(2)Se_(3)possesses excellent catalytic properties,high electrochemical and thermody-namic stability,which facilitates the catalytic process.Machine learning also helps us further ex-plore the underlying mechanisms.The systematic investigation provides novel insights into the design and application of two-dimensional switchable ferroelectric catalysts for various chemical processes.
基金Supported by the Japan Society for the Promotion of Science under Grant No JP25107004
文摘This work details a study based on HfS_(2 )transistors utilizing an n-octadecylphosphonic acid-based self-assembled monolayer(SAM)as the gate dielectric.The fabrication of the SAM-based two-dimensional(2D)material transistor is simple and can be used to improve the quality of the interface of air-sensitive 2D materials.In comparison to HfS_(2) transistors utilizing a conventional Al_2O_(3) gate insulator by atomic layer deposition,HfS_(2) transistors utilizing an SAM as the gate dielectric can reduce the operation region from 4 V to 2 V,enhance the field-effect mobility from 0.03 cm^2/Vs to 0.75 cm^2/Vs,improve the sub-threshold swing from 404 m V/dec to 156 m V/dec,and optimize the hysteresis to 0.03 V,thus demonstrating improved quality of the semiconductor/insulator interface.
基金supported by the National Natural Science Foundation of China (Grant Nos.51290271,51672314)the Guangdong Natural Science Foundation (Grant No.2016A030313359)+2 种基金the Science and Technology Program of Guangzhou (Grant No.201707010224)the Science and Technology Department of Guangdong Provincethe Fundamental Research Funds for the Central Universities
文摘Transition-metal dichalcogenide(TMD) semiconductors have attracted interest as photoelectrochemical(PEC) electrodes due to their novel band-gap structures,optoelectronic properties, and photocatalytic activities.However, the photo-harvesting efficiency still requires improvement. In this study, A TMD stacked heterojunction structure was adopted to further enhance the performance of the PEC cathode. A P-type WSe_2 and an N-type Mo S_2 monolayer were stacked layer-by-layer to build a ultrathin vertical heterojunction using a micro-fabrication method.In situ measurement was employed to characterize the intrinsic PEC performance on a single-sheet heterostructure.Benefitting from its built-in electric field and type II band alignment, the MoS_2/WSe_2 bilayer heterojunction exhibited exceptional photocatalytic activity and a high incident photo-to-current conversion efficiency(IPCE). Comparing with the monolayer WSe_2 cathode, the PEC current and the IPCE of the bilayer heterojunction increased by a factor of 5.6 and enhanced 50%, respectively. The intriguing performance renders the MoS_2/WSe_2 heterojunction attractive for application in high-performance PEC water splitting.
基金Project supported by the National Natural Science Foundation(Grant No.U1404108)the Innovative Talents of Universities in Henan Province of China(Grant No.17HASTIT013)+1 种基金the Basic and Frontier Technology Research Program of Henan Province of China(Grant No.162300410056)the Key Scientific Research Projects of Higher Institutions in Henan Province of China(Grant No.19A140018).
文摘Searching for two-dimensional（2 D） stable materials with direct band gap and high carrier mobility has attracted great attention for their electronic device applications.Using the first principles calculations and particle swarm optimization（PSO） method,we predict a new 2 D stable material（HfNZ monolayer） with the global minimum of 2 D space.The HfNZ monolayer possesses direct band gap（～1.46 eV） and it is predicted to have high carrier mobilities(～103 cm2·V-1·s-1)from deformation potential theory.The direct band gap can be well maintained and flexibly modulated by applying an easily external strain under the strain conditions.In addition,the newly predicted HfN2 monolayer possesses good thermal,dynamical,and mechanical stabilities,which are verified by ab initio molecular dynamics simulations,phonon dispersion and elastic constants.These results demonstrate that HfN2 monolayer is a promising candidate in future microelectronic devices.
基金the Joint Funds of the National Natural Science Foundation of China(Grant No.U1967212)the National Science and Technology Major Project of China(Grant No.2019XS06004009)the Fundamental Research Funds for the Central Universities(Grant No.2018ZD10).
文摘To maximize the catalytic performance of MoS_(2) in the hydrogen evolution reaction,we investigate the electrocatalytic and photocatalytic performance of monolayer MoS_(2) doped with noble metal(Ag,Au,Cu,Pd,and Pt)using first principles calculation combined with the climbing image nudged elastic band method.We find the band gap of the monolayer MoS_(2) is reduced significantly by the noble metal doping,which is unfavorable to improving its photocatalytic performance.The optical absorption coefficient shows that the doping does not increase the ability of the monolayer MoS_(2) to absorb visible light.The monolayer MoS_(2) doped with the noble metal is not a potential photocatalyst for the hydrogen evolution reaction because the band edge position of the conduction band minimum is lower than-4.44 eV,the reduction potential of H^(+)/H_(2).Fortunately,the band gap reduction increases the electron transport performance of the monolayer MoS_(2),and the activation energy of water splitting is greatly reduced by the noble metal doping,especially the Pt doping.On the whole,noble metal doping can enhance the electrocatalytic performance of the monolayer MoS_(2).
文摘Formaldehyde(HCHO) is a common indoor pollutant, long-term exposure to HCHO may harm human health. Its efficient removal at mild conditions is still challenging. The catalytic oxidation of HCHO molecules on a single atomic catalyst, Ti-decorated Ti3C2O2(Ti/Ti3C2O2) monolayer, is investigated by performing the first principles calculations in this work. It demonstrates that Ti atoms can be easily well dispersed at the form of single atom on Ti3C2O2 monolayer without aggregation. For HCHO catalytic oxidation, both Langmuir-Hinshelwood(LH) and Eley-Rideal(ER) mechanisms are considered. The results show that the step of HCHO dissociative adsorption on Ti/Ti3C2O2 with activated O2 can release high energy of 4.05 e V based on the ER mechanism, which can help to overcome the energy barrier(1.04 e V) of the subsequent reaction steps. The charge transfer from *OH group to CO molecule(dissociated from HCHO) not only promotes *OH group activation but also plays an important role in the H2 O generation along the ER mechanism. Therefore, HCHO can be oxidized easily on Ti/Ti3C2O2 monolayer, this work could provide significant guidance to develop effective non-noble metal catalysts for HCHO oxidation and broaden the applications of MXene-based materials.
