Hypercrosslinked polymers(HCPs)with large surface areas,high intrinsic porosities and low production costs may be available platforms for iodine capture.However,the lack of iodine-philicity binding sites limits their ...Hypercrosslinked polymers(HCPs)with large surface areas,high intrinsic porosities and low production costs may be available platforms for iodine capture.However,the lack of iodine-philicity binding sites limits their adsorption capacity.Here we use vapor-phase postsynthetic amination strategy to introduce electron-donating amino groups into the prefabricated HCPs for enhancing their iodine capture performance.Through simple vapor-phase exposure,the halogen-containing HCPs can be grafted by amines through nucleophilic substitution toward chloro groups.Combining with the abundant amino groups and high porosities,the amino-functionalized porous polymers show substantially increased iodine adsorption capacity,about 221%as that of original one,accompanied by excellent recyclability.Mechanism investigations reveal the key roles of the electron-donor amino groups andπ-conjugated benzene rings along with structure characteristics of porous polymer frameworks in iodine capture.Moreover,this vapor-phase amination strategy shows good generality and can be extended to various amines,e.g.,ethylenediamine,1,3-diaminopropane and diethylenetriamine.Our work proves that this simple vapor-phase postsynthetic functionalization strategy may be applied in other porous polymers with wide application prospects in adsorption,separation and storage.展开更多
Urea,paracetamol and glutamine(based on the expired drugs)were selected as vapor-phase corrosion inhibitors(VCIs)to study their corrosion protection effect on red copper in simulated marine atmospheric environment by ...Urea,paracetamol and glutamine(based on the expired drugs)were selected as vapor-phase corrosion inhibitors(VCIs)to study their corrosion protection effect on red copper in simulated marine atmospheric environment by using weight loss,electrochemical measurement techniques(specially designed electrochemical testing device for simulating marine atmospheric environments)and surface morphology characterization analysis(SEM/EDS,XRD,RAMAN,XPS).Weight loss results show that the three corrosion inhibitors have good corrosion inhibition effect on red copper,and the corrosion inhibition efficiency in the order of glutamine(83.62%)>urea(68.46%)>paracetamol(61.47%).Surface morphology characterization analysis provides evidence of adsorption of corrosion inhibitors molecules on the red copper surface,thus forming a protective film that blocked the red copper surface from the aggressive chloride ion attack.展开更多
Design and preparation of highly efficient zeolite catalysts for gas-phase Beckmann rearrangement of cyclohexanone oxime to caprolactam are attractive but still challenging.Herein,we show a one-pot synthesis of silica...Design and preparation of highly efficient zeolite catalysts for gas-phase Beckmann rearrangement of cyclohexanone oxime to caprolactam are attractive but still challenging.Herein,we show a one-pot synthesis of silicalite-1 zeolite nanosheets with rich H-bonded silanols.The key to this success is the use of urea in the synthetic system.Catalytic tests of cyclohexanone oxime gas-phase Beckmann rearrangement show that the silicalite-1 zeolite nanosheets with H-bonded silanols exhibit higher selectivity for caprolactam and longer reaction lifetime than those of the conventional silicalite-1 zeolite.Theoretical simulations reveal that the ammonium decomposed by urea is a critical additive for the formation of H-bond silanols.Obviously,one-pot synthesis of silicalite-1 zeolite nanosheets with rich H-bonded silanols plus excellent catalytic performance in the Beckmann rearrangement offer a new opportunity for development of highly efficient zeolites for catalytic applications in the future.展开更多
Among the synthesis techniques for graphene,chemical vapor deposition(CVD)enables the direct growth of graphene films on insulating substrates.Its advantages include uniform coverage,high quality,scalability,and compa...Among the synthesis techniques for graphene,chemical vapor deposition(CVD)enables the direct growth of graphene films on insulating substrates.Its advantages include uniform coverage,high quality,scalability,and compatibility with industrial processes.Graphene is chemically inert and has a zero-bandgap which poses a problem for its use as a functional layer,and nitrogen doping has become an important way to overcome this.Post-plasma treatment has been explored for the synthesis of nitrogen-doped graphene,but the procedures are intricate and not suitable for large-scale production.We report the direct synthesis of nitrogen-doped graphene on a 4-inch sapphire wafer by ethanol-assisted CVD employing pyridine as the carbon feedstock,where the nitrogen comes from the pyridine and the hydroxyl group in ethanol improves the quality of the graphene produced.Additionally,the types of nitrogen dopant produced and their effects on III-nitride epitaxy were also investigated,resulting in the successful illumination of LED devices.This work presents an effective synthesis strategy for the preparation of nitrogen-doped graphene,and provides a foundation for designing graphene functional layers in optoelectronic devices.展开更多
High-quality antiferromagnetic(AFM)θ-phase manganese nitride(MnN)films were successfully grown on MgO(001)substrates by plasma-assisted molecular beam epitaxy.Structural analysis confirms the high-quality MnN film ha...High-quality antiferromagnetic(AFM)θ-phase manganese nitride(MnN)films were successfully grown on MgO(001)substrates by plasma-assisted molecular beam epitaxy.Structural analysis confirms the high-quality MnN film has a tetragonal distortion with a c/a ratio of~0.98.The film exhibits exceptional stability in both aqueous and ambient conditions,which is a crucial factor for practical applications.Electrical transport reveals its metallic behavior with an upturn at low temperatures,which could be attributed to the Kondo effect originated from nitrogen vacancy-induced magnetic impurities.Room temperature exchange bias has been demonstrated in a MnN/CoFeB heterostructure,verifying the AFM ordering of MnN.Considering its high Néel temperature~650 K,superior stability,and low-cost,this work highlights the epitaxial MnN films as a promising candidate for AFM spintronic applications.展开更多
We introduce our state-of-the art of“vacuum consistent electrochemistry”to an investigation of the interfaces between oxides and ionic liquid(IL).Pulsed laser deposition(PLD)has been one of the powerful and sophisti...We introduce our state-of-the art of“vacuum consistent electrochemistry”to an investigation of the interfaces between oxides and ionic liquid(IL).Pulsed laser deposition(PLD)has been one of the powerful and sophisticated techniques to realize nanoscale preparation of high-quality epitaxial oxide thin films.On the other hand,electrochemistry is a simple,very sensitive,and non-destructive analysis technique for solid-liquid interfaces.To ensure the reproducibility in experiment of the interfaces of such epitaxial oxide films,as well as bulk oxide single-crystals,with IL,we employ a home-built PLD-electrochemical(EC)system with IL as an electrolyte.The system allows one to perform all-in-vacuum experiments during the preparation of well-defined oxide electrode surfaces to their electrochemical analyses.The topics include electrochemical evaluations of the oxide’s own properties,such as carrier density and relative permittivity,and the interfacial properties of oxides in contact with IL,such as flat band potential and electric double layer(EDL)capacitance,ending with future perspectives in all-solid-state electrochemistry.展开更多
This paper discusses the influence of Sb/In ratio on the transport properties and crystal quality of the 200 nm InAs_(x)Sb_(1-x)thin film.The Sb content of InAs_(x)Sb_(1-x)thin film in all samples was verified by HRXR...This paper discusses the influence of Sb/In ratio on the transport properties and crystal quality of the 200 nm InAs_(x)Sb_(1-x)thin film.The Sb content of InAs_(x)Sb_(1-x)thin film in all samples was verified by HRXRD of the symmetrical 004 reflections and asymmetrical 115 reflections.The calculation results show that the Sb component was 0.6 in the InAs_(x)Sb_(1-x)thin film grown under the conditions of Sb/In ratio of 6 and As/In ratio of 3,which has the highest electron mobility(28560 cm^(2)/V·s)at 300 K.At the same time,the influence ofⅤ/Ⅲratio on the transport properties and crystal quality of Al_(0.2)In_(0.8)Sb/InAs_(x)Sb_(1-x)quantum well heterostructures also has been investigated.As a result,the Al_(0.2)In_(0.8)Sb/InAs_(0.4)Sb_(0.6)quantum well heterostructure with a channel thickness of 30 nm grown under the conditions of Sb/In ratio of 6 and As/In ratio of 3 has a maximum electron mobility of 28300 cm^(2)/V·s and a minimum RMS roughness of 0.68 nm.Through optimizing the growth conditions,our samples have higher electron mobility and smoother surface morphology.展开更多
We have investigated homoepitaxy of Al N films grown by molecular beam epitaxy(MBE)on Al N/sapphire templates.The MBE epitaxy of Al N at the low temperature range,which is suitable for Al Ga N,encounters significant c...We have investigated homoepitaxy of Al N films grown by molecular beam epitaxy(MBE)on Al N/sapphire templates.The MBE epitaxy of Al N at the low temperature range,which is suitable for Al Ga N,encounters significant challenge in preventing Al droplet and pits,since the migration and desorption rate of Al atom are very low.In contrast,by elevating the growth temperature,such a difficulty can be effectively overcome,and we were able to grow Al N films with much improved surface morphology and obtained step flow growth mode without any Al droplets and pits.The cathodoluminescence spectroscopy indicate that the impurity incorporation and defect generation in the Al N epilayers was suppressed by elevating the growth temperature.A systematic investigation on the influence of Al beam flux and growth temperature in a very wide range on the Al N films has been conducted,and a comprehensive growth diagram of MBE Al N has been obtained.展开更多
Nickel oxide(NiO)based gas sensors have at-tracted intense attention due to its high re-sponse to hydrogen sulfide(H_(2)S)gas.It has been demonstrated that the NiO sensors with exposed(111)facet exhibit excellent perf...Nickel oxide(NiO)based gas sensors have at-tracted intense attention due to its high re-sponse to hydrogen sulfide(H_(2)S)gas.It has been demonstrated that the NiO sensors with exposed(111)facet exhibit excellent perfor-mance,but the single-orientation NiO sensors with exposed(111)facet have rarely been studied.In this work,high quality(111)-ori-ented NiO epitaxial films were fabricated by pulsed laser deposition.Detailed crystalline structural information was revealed by using synchrotron based X-ray diffraction(XRD)technology.These NiO thin films show good se-lectivity for H_(2)S gas detection.Without further modification,the highest response to 100 ppm H_(2)S was measured to be 13.07 at 300℃,and limit of detection(LOD)could be as low as 186 ppb.Fitting of the electrical response curves during adsorption and desorption of H_(2)S gas indicates the two-site Langmuir kinetic processes.Combining with XPS and XAS measure-ments,the mechanism was discussed.Density functional theory(DFT)calculations show that NiO with exposed(111)facets has the most negative adsorption energy,indicating more sen-sitive to H_(2)S.These results could inspire more studies of metal oxide semiconductor-based gas sensors with specific surface.展开更多
Confining particles in one-dimensional(1D)systems profoundly modifies their electronic behaviors,which have been extensively demonstrated in carbon nanotubes and atomic chains.Structural instabilities and electron loc...Confining particles in one-dimensional(1D)systems profoundly modifies their electronic behaviors,which have been extensively demonstrated in carbon nanotubes and atomic chains.Structural instabilities and electron localizations often dominate the conductivity of 1D nanowires.Here,we successfully grew Bi single nanowires and nanowire arrays on Pb-√7×√3substrates via molecular beam epitaxy,both of which exhibit metallic behavior.Using scanning tunneling microscopy and first-principles density functional theory calculations,the interwire coupling and the correlation between nanowire bundles and electronic properties are investigated.A characteristic peak at 0.75 e V is observed on single wires and wire bundles of up to four nanowires,whereas interwire coupling weakens it and makes it disappear for wire bundles of five and above.These findings illustrate that the interwire coupling plays a critical role in the electronic structure of the1D system,which provides insights for the design of nano-electronics materials.展开更多
Anti-phase domain defects easily form in the in-plane GaAs nanowires(NWs)grown on CMOS-compatiblegroup IV substrates,which makes it difficult to obtain GaAs NWs with a designed length and also leads to asignificant li...Anti-phase domain defects easily form in the in-plane GaAs nanowires(NWs)grown on CMOS-compatiblegroup IV substrates,which makes it difficult to obtain GaAs NWs with a designed length and also leads to asignificant limitation in the growth of high-quality in-plane GaAs NW networks on such substrates.Here,wereport on the selective area growth of anti-phase domain-free in-plane GaAs NWs and NW networks on Ge(111)substrates.Detailed structural studies confirm that the GaAs NW grown using a large pattern period and GaAsNW networks grown by adding the Sb are both high-quality pure zinc-blende single crystals free of stackingfaults,twin defects,and anti-phase domain defects.Room-temperature photoluminescence measurements show asubstantial improvement in crystal quality and good consistency and uniformity of the GaAs NW networks.Ourwork provides useful insights into the controlled growth of high-quality anti-phase domain-defects-free in-planeIII-V NWs and NW networks.展开更多
Intermetallic Pt-based nanoparticles have displayed excellent activity for the oxygen reduction reaction(ORR)in fuel cells.However,it remains a great challenge to synthesize highly atomically ordered Pt-based nanopart...Intermetallic Pt-based nanoparticles have displayed excellent activity for the oxygen reduction reaction(ORR)in fuel cells.However,it remains a great challenge to synthesize highly atomically ordered Pt-based nanoparticle catalysts because the formation of an atomically ordered structure usually requires high-temperature annealing accompanied by grain sintering.Here we report the direct epitaxial growth of well-aligned,highly atomically ordered Pt3 Fe and PtFe nanoparticles(<5 nm)on single-walled carbon nanotube(SWCNT)bundles films.The long-range periodically symmetric van der Waals(vdW)interac-tions between SWCNT bundles and Pt-Fe nanoparticles play an important role in promoting not only the alignment ordering of inter-nanoparticles but also the atomic ordering of intra-nanoparticles.The ordered Pt_(3)Fe/SWCNT catalyst showed enhanced ORR catalytic performance of 2.3-fold higher mass activity and 3.1-fold higher specific activity than commercial Pt/C.Moreover,the formation of an interlocked inter-face and strong vdW interaction endow the Pt-Fe/SWCNT catalysts with extreme long-term stability in potential cycling and excellent anti-thermal sintering ability.展开更多
MnSAPO-34 molecular sieves were synthesized by vapor-phase transport （VPT） method using triethylamine （Et3N） as a structure directing agent （SDA）, and were characterized by XRD, BET, SEM, UV-Vis, FT-IR, and TG a...MnSAPO-34 molecular sieves were synthesized by vapor-phase transport （VPT） method using triethylamine （Et3N） as a structure directing agent （SDA）, and were characterized by XRD, BET, SEM, UV-Vis, FT-IR, and TG analy- ses. The influence of the zeolite crystallization conditions and the dry-gel composition were investigated. The results showed that the synthesis conditions had an effect on the crystalline phase. Pure MnSAPO-34 had been obtained when it was crystallized at 140 C for 18 hours. The ratio of MnO/A1203 in the starting gel ranging from 0.1 to 0.2 resulted in pure MnSAPO-34 with a CHA topology. Beyond this scope, MnSAPO-5 with an AFI topology structure was obtained as an impurity substance. UV-Vis spectroscopy and FT-IR spectroscopy study indicated that manganese was incorporated into the framework of the molecular sieve. The catalytic performance of MnSAPO-34 molecular sieve was tested by ketalization reaction of l, 2-propanediol with cyclohexanone. High yield of cyclohexanone-1, 2-propanediol ketal was obtained.展开更多
Kinetic regularities of 4-phenyl-o-tolunitrile ammoxidation on V-Sb-Bi-Zr/γ-Al2O3 oxide catalyst in the temperature interval 633 - 673 K have been studied. It has been established that rates of conversion of 4-phenyl...Kinetic regularities of 4-phenyl-o-tolunitrile ammoxidation on V-Sb-Bi-Zr/γ-Al2O3 oxide catalyst in the temperature interval 633 - 673 K have been studied. It has been established that rates of conversion of 4-phenyl-o-tolu- nitrile into the aimed 4-phenylphthalonitrile and CO2 are described by half-order equation on concentration of substratum and to be independent of the oxygen and ammonia partial pressures. It has been revealed that formation of 4-phenylphthalimide from byproducts is due to hydrolysis of 4-phenylphthalonitrile;carbon dioxide is produced by oxidation of 4-phenyl-o-tolunitrile and decarboxylation of 4-phenylphthalimide, and 4-phenylben- zonitrile is produced from 4-phenyl-o-tolunitrile and 4-phenylphthalimide.展开更多
High quality Co-doped ZnO thin films are grown on single crystalline Al2O3（0001） and ZnO（0001） substrates by oxygen plasma assisted molecular beam epitaxy at a relatively lower substrate temperature of 450℃. The ...High quality Co-doped ZnO thin films are grown on single crystalline Al2O3（0001） and ZnO（0001） substrates by oxygen plasma assisted molecular beam epitaxy at a relatively lower substrate temperature of 450℃. The epitaxial conditions are examined with in-situ reflection high energy electron diffraction （RHEED） and ex-situ high resolution x-ray diffraction （HRXRD）. The epitaxial thin films are single crystal at film thickness smaller than 500nm and nominal concentration of Co dopant up to 20%. It is indicated that the Co cation is incorporated into the ZnO matrix as Co^2＋ substituting Zn^2＋ ions. Atomic force microscopy shows smooth surfaces with rms roughness of 1.9 nm. Room-temperature magnetization measurements reveal that the Co-doped ZnO thin films are ferromagnetic with Curie temperatures Tc above room temperature.展开更多
Ex situ characterization techniques in molecular beam epitaxy(MBE)have inherent limitations,such as being prone to sample contamination and unstable surfaces during sample transfer from the MBE chamber.In recent years...Ex situ characterization techniques in molecular beam epitaxy(MBE)have inherent limitations,such as being prone to sample contamination and unstable surfaces during sample transfer from the MBE chamber.In recent years,the need for improved accuracy and reliability in measurement has driven the increasing adoption of in situ characterization techniques.These techniques,such as reflection high-energy electron diffraction,scanning tunneling microscopy,and X-ray photoelectron spectroscopy,allow direct observation of film growth processes in real time without exposing the sample to air,hence offering insights into the growth mechanisms of epitaxial films with controlled properties.By combining multiple in situ characterization techniques with MBE,researchers can better understand film growth processes,realizing novel materials with customized properties and extensive applications.This review aims to overview the benefits and achievements of in situ characterization techniques in MBE and their applications for material science research.In addition,through further analysis of these techniques regarding their challenges and potential solutions,particularly highlighting the assistance of machine learning to correlate in situ characterization with other material information,we hope to provide a guideline for future efforts in the development of novel monitoring and control schemes for MBE growth processes with improved material properties.展开更多
In order to obtain bi epitaxial 45° grain boundary YBa 2Cu 3O 7 (YBCO) junctions, the in plane epitaxy of CeO 2 films on both MgO films and SrTiO 3 substrates was studied. Using magnetron sputtering techni...In order to obtain bi epitaxial 45° grain boundary YBa 2Cu 3O 7 (YBCO) junctions, the in plane epitaxy of CeO 2 films on both MgO films and SrTiO 3 substrates was studied. Using magnetron sputtering technique and decreasing the substrate temperature, 100% CeO 2∥MgO in plane orientation for bi epitaxial grain boundary junction can be obtained.展开更多
Two-dimensional materials have been widely used to tune the growth and energy-level alignment of perovskites.However,their incomplete passivation and chaotic usage amounts are not conducive to the preparation of highq...Two-dimensional materials have been widely used to tune the growth and energy-level alignment of perovskites.However,their incomplete passivation and chaotic usage amounts are not conducive to the preparation of highquality perovskite films.Herein,we succeeded in obtaining higher-quality CsPbBr_(3)films by introducing large-area monolayer graphene as a stable physical overlay on top of TiO_(2)substrates.Benefiting from the inert and atomic smooth graphene surface,the CsPbBr_(3)film grown on top by the van der Waal epitaxy has higher crystallinity,improved(100)orientation,and an average domain size of up to 1.22μm.Meanwhile,a strong downward band bending is observed at the graphene/perovskite interface,improving the electron extraction to the electron transport layers(ETL).As a result,perovskite film grown on graphene has lower photoluminescence(PL)intensity,shorter carrier lifetime,and fewer defects.Finally,a photovoltaic device based on epitaxy CsPbBr_(3)film is fabricated,exhibiting power conversion efficiency(PCE)of up to 10.64%and stability over 2000 h in the air.展开更多
The Si overlayers are grown by molecular beam epitaxy on atomically smllth Er_(2)O_(3)(111)films prepared on Si(111)substrates.Single crystalline Si overlayers are achieved and are evident due to the spot-like reflect...The Si overlayers are grown by molecular beam epitaxy on atomically smllth Er_(2)O_(3)(111)films prepared on Si(111)substrates.Single crystalline Si overlayers are achieved and are evident due to the spot-like reflective high energy electron diffraction(RHEED)patterns and x-ray diffraction patterns.The epitaxial relationship of the Si overlayer along the surface with respect to the orientation of Er_(2)O_(3)and the Si substrate is as follows:overgrown Si(111)//Er_(2)O_(3)(111)//Si(111).The rough surface of Si overlayers,as identified by both RHEED patterns and atomic force microscopy images,indicates a three-dimensional growth mode.The reason for this is based on the interfacial energy argument.Further growth of Er_(2)O_(3)films on this rough Si overlayer leads to the polycrystalline nature of the topmost Er2O3 layer.展开更多
Vapor-phase nitration of benzene over solid acid catalyst is expected to be a clean process with no sulfuric acid waste. We investigated this process over solid acidic catalysts utilizing diluted nitric acid (60-70%)...Vapor-phase nitration of benzene over solid acid catalyst is expected to be a clean process with no sulfuric acid waste. We investigated this process over solid acidic catalysts utilizing diluted nitric acid (60-70%) as nitrating agent, and found that supported sulfuric acid catalyst exhibited a very high catalytic activity. Under the conditions of reaction temperature 160-170℃, space velocity (SV) 1200 h-1, the yield and the space-time yield (STY) of nitrobenzene (NB) based on HNO3 were more than 98% and 0.75 kg穔gcat-1穐-1 over 10% H2SO4/SiO2 (by weight) catalyst respectively.展开更多
基金financially supported by National Natural Science Foundation of China(No.22178143)Guangdong Basic and Applied Basic Research Foundation(Nos.2021A1515110365 and2020B1515120036)+3 种基金Natural Science Foundation of Anhui Higher Education Institutions(No.2023AH050168)Innovation and Entrepreneurship Training Program for China College Students(No.202310878049)Director Foundation of Anhui Province Engineering Laboratory of Advanced Building Materials(No.JZCL2305ZR)Ph.D.Startup Foundation of Anhui Jianzhu University(No.2023QDZ34)。
文摘Hypercrosslinked polymers(HCPs)with large surface areas,high intrinsic porosities and low production costs may be available platforms for iodine capture.However,the lack of iodine-philicity binding sites limits their adsorption capacity.Here we use vapor-phase postsynthetic amination strategy to introduce electron-donating amino groups into the prefabricated HCPs for enhancing their iodine capture performance.Through simple vapor-phase exposure,the halogen-containing HCPs can be grafted by amines through nucleophilic substitution toward chloro groups.Combining with the abundant amino groups and high porosities,the amino-functionalized porous polymers show substantially increased iodine adsorption capacity,about 221%as that of original one,accompanied by excellent recyclability.Mechanism investigations reveal the key roles of the electron-donor amino groups andπ-conjugated benzene rings along with structure characteristics of porous polymer frameworks in iodine capture.Moreover,this vapor-phase amination strategy shows good generality and can be extended to various amines,e.g.,ethylenediamine,1,3-diaminopropane and diethylenetriamine.Our work proves that this simple vapor-phase postsynthetic functionalization strategy may be applied in other porous polymers with wide application prospects in adsorption,separation and storage.
基金Project(ZR2023ME063)supported by the Shandong Provincial Natural Science Foundation,ChinaProject(121311KYSB20210005)supported by the Overseas Science and Education Cooperation Center Deployment Project,ChinaProject supported by the Qingdao Expert Workstation for Intelligent Anticorrosion for Water Diversion Project,China。
文摘Urea,paracetamol and glutamine(based on the expired drugs)were selected as vapor-phase corrosion inhibitors(VCIs)to study their corrosion protection effect on red copper in simulated marine atmospheric environment by using weight loss,electrochemical measurement techniques(specially designed electrochemical testing device for simulating marine atmospheric environments)and surface morphology characterization analysis(SEM/EDS,XRD,RAMAN,XPS).Weight loss results show that the three corrosion inhibitors have good corrosion inhibition effect on red copper,and the corrosion inhibition efficiency in the order of glutamine(83.62%)>urea(68.46%)>paracetamol(61.47%).Surface morphology characterization analysis provides evidence of adsorption of corrosion inhibitors molecules on the red copper surface,thus forming a protective film that blocked the red copper surface from the aggressive chloride ion attack.
文摘Design and preparation of highly efficient zeolite catalysts for gas-phase Beckmann rearrangement of cyclohexanone oxime to caprolactam are attractive but still challenging.Herein,we show a one-pot synthesis of silicalite-1 zeolite nanosheets with rich H-bonded silanols.The key to this success is the use of urea in the synthetic system.Catalytic tests of cyclohexanone oxime gas-phase Beckmann rearrangement show that the silicalite-1 zeolite nanosheets with H-bonded silanols exhibit higher selectivity for caprolactam and longer reaction lifetime than those of the conventional silicalite-1 zeolite.Theoretical simulations reveal that the ammonium decomposed by urea is a critical additive for the formation of H-bond silanols.Obviously,one-pot synthesis of silicalite-1 zeolite nanosheets with rich H-bonded silanols plus excellent catalytic performance in the Beckmann rearrangement offer a new opportunity for development of highly efficient zeolites for catalytic applications in the future.
基金National Natural Science Foundation of China(T2188101)。
文摘Among the synthesis techniques for graphene,chemical vapor deposition(CVD)enables the direct growth of graphene films on insulating substrates.Its advantages include uniform coverage,high quality,scalability,and compatibility with industrial processes.Graphene is chemically inert and has a zero-bandgap which poses a problem for its use as a functional layer,and nitrogen doping has become an important way to overcome this.Post-plasma treatment has been explored for the synthesis of nitrogen-doped graphene,but the procedures are intricate and not suitable for large-scale production.We report the direct synthesis of nitrogen-doped graphene on a 4-inch sapphire wafer by ethanol-assisted CVD employing pyridine as the carbon feedstock,where the nitrogen comes from the pyridine and the hydroxyl group in ethanol improves the quality of the graphene produced.Additionally,the types of nitrogen dopant produced and their effects on III-nitride epitaxy were also investigated,resulting in the successful illumination of LED devices.This work presents an effective synthesis strategy for the preparation of nitrogen-doped graphene,and provides a foundation for designing graphene functional layers in optoelectronic devices.
文摘High-quality antiferromagnetic(AFM)θ-phase manganese nitride(MnN)films were successfully grown on MgO(001)substrates by plasma-assisted molecular beam epitaxy.Structural analysis confirms the high-quality MnN film has a tetragonal distortion with a c/a ratio of~0.98.The film exhibits exceptional stability in both aqueous and ambient conditions,which is a crucial factor for practical applications.Electrical transport reveals its metallic behavior with an upturn at low temperatures,which could be attributed to the Kondo effect originated from nitrogen vacancy-induced magnetic impurities.Room temperature exchange bias has been demonstrated in a MnN/CoFeB heterostructure,verifying the AFM ordering of MnN.Considering its high Néel temperature~650 K,superior stability,and low-cost,this work highlights the epitaxial MnN films as a promising candidate for AFM spintronic applications.
文摘We introduce our state-of-the art of“vacuum consistent electrochemistry”to an investigation of the interfaces between oxides and ionic liquid(IL).Pulsed laser deposition(PLD)has been one of the powerful and sophisticated techniques to realize nanoscale preparation of high-quality epitaxial oxide thin films.On the other hand,electrochemistry is a simple,very sensitive,and non-destructive analysis technique for solid-liquid interfaces.To ensure the reproducibility in experiment of the interfaces of such epitaxial oxide films,as well as bulk oxide single-crystals,with IL,we employ a home-built PLD-electrochemical(EC)system with IL as an electrolyte.The system allows one to perform all-in-vacuum experiments during the preparation of well-defined oxide electrode surfaces to their electrochemical analyses.The topics include electrochemical evaluations of the oxide’s own properties,such as carrier density and relative permittivity,and the interfacial properties of oxides in contact with IL,such as flat band potential and electric double layer(EDL)capacitance,ending with future perspectives in all-solid-state electrochemistry.
基金Supported by the Natural Science Basic Research Program of Shaanxi Province(2023-JC-QN-0758)Shaanxi University of Science and Technology Research Launch Project(2020BJ-26)Doctoral Research Initializing Fund of Hebei University of Science and Technology,China(1181476).
文摘This paper discusses the influence of Sb/In ratio on the transport properties and crystal quality of the 200 nm InAs_(x)Sb_(1-x)thin film.The Sb content of InAs_(x)Sb_(1-x)thin film in all samples was verified by HRXRD of the symmetrical 004 reflections and asymmetrical 115 reflections.The calculation results show that the Sb component was 0.6 in the InAs_(x)Sb_(1-x)thin film grown under the conditions of Sb/In ratio of 6 and As/In ratio of 3,which has the highest electron mobility(28560 cm^(2)/V·s)at 300 K.At the same time,the influence ofⅤ/Ⅲratio on the transport properties and crystal quality of Al_(0.2)In_(0.8)Sb/InAs_(x)Sb_(1-x)quantum well heterostructures also has been investigated.As a result,the Al_(0.2)In_(0.8)Sb/InAs_(0.4)Sb_(0.6)quantum well heterostructure with a channel thickness of 30 nm grown under the conditions of Sb/In ratio of 6 and As/In ratio of 3 has a maximum electron mobility of 28300 cm^(2)/V·s and a minimum RMS roughness of 0.68 nm.Through optimizing the growth conditions,our samples have higher electron mobility and smoother surface morphology.
基金Project supported by the Innovation Program for Quantum Science and Technology(Grant No.2021ZD0303400)the National Key Research and Development Program of China(Grant Nos.2022YFB3605602 and 2024YFE0205000)+1 种基金the Natural Science Foundation of Jiangsu Province,China(Grant No.BK20243037)the Jiangsu Special Professorship,Collaborative Innovation Center of Solid-state Lighting and Energy-saving Electronics,Postdoctoral Fellowship Program of CPSF(Grant No.GZC20231098)。
文摘We have investigated homoepitaxy of Al N films grown by molecular beam epitaxy(MBE)on Al N/sapphire templates.The MBE epitaxy of Al N at the low temperature range,which is suitable for Al Ga N,encounters significant challenge in preventing Al droplet and pits,since the migration and desorption rate of Al atom are very low.In contrast,by elevating the growth temperature,such a difficulty can be effectively overcome,and we were able to grow Al N films with much improved surface morphology and obtained step flow growth mode without any Al droplets and pits.The cathodoluminescence spectroscopy indicate that the impurity incorporation and defect generation in the Al N epilayers was suppressed by elevating the growth temperature.A systematic investigation on the influence of Al beam flux and growth temperature in a very wide range on the Al N films has been conducted,and a comprehensive growth diagram of MBE Al N has been obtained.
基金supported by the National Key Research and Development Program of China(No.2022YFA1603902)the National Natural Science Foundation of China(No.12175235,No.62271462,and No.12004407)。
文摘Nickel oxide(NiO)based gas sensors have at-tracted intense attention due to its high re-sponse to hydrogen sulfide(H_(2)S)gas.It has been demonstrated that the NiO sensors with exposed(111)facet exhibit excellent perfor-mance,but the single-orientation NiO sensors with exposed(111)facet have rarely been studied.In this work,high quality(111)-ori-ented NiO epitaxial films were fabricated by pulsed laser deposition.Detailed crystalline structural information was revealed by using synchrotron based X-ray diffraction(XRD)technology.These NiO thin films show good se-lectivity for H_(2)S gas detection.Without further modification,the highest response to 100 ppm H_(2)S was measured to be 13.07 at 300℃,and limit of detection(LOD)could be as low as 186 ppb.Fitting of the electrical response curves during adsorption and desorption of H_(2)S gas indicates the two-site Langmuir kinetic processes.Combining with XPS and XAS measure-ments,the mechanism was discussed.Density functional theory(DFT)calculations show that NiO with exposed(111)facets has the most negative adsorption energy,indicating more sen-sitive to H_(2)S.These results could inspire more studies of metal oxide semiconductor-based gas sensors with specific surface.
基金supported by the National Natural Science Foundation of China(Grant Nos.12374196,92165201,and 11634011)the Innovation Program for Quantum Science and Technology(Grant No.2021ZD0302800)+2 种基金the CAS Project for Young Scientists in Basic Research(Grant No.YSBR-046)the Fundamental Research Funds for the Central Universities(Grant Nos.WK3510000006 and WK3430000003)the Initiative Project in Quantum Information Technologies of Anhui Province,China(Grant No.AHY170000)。
文摘Confining particles in one-dimensional(1D)systems profoundly modifies their electronic behaviors,which have been extensively demonstrated in carbon nanotubes and atomic chains.Structural instabilities and electron localizations often dominate the conductivity of 1D nanowires.Here,we successfully grew Bi single nanowires and nanowire arrays on Pb-√7×√3substrates via molecular beam epitaxy,both of which exhibit metallic behavior.Using scanning tunneling microscopy and first-principles density functional theory calculations,the interwire coupling and the correlation between nanowire bundles and electronic properties are investigated.A characteristic peak at 0.75 e V is observed on single wires and wire bundles of up to four nanowires,whereas interwire coupling weakens it and makes it disappear for wire bundles of five and above.These findings illustrate that the interwire coupling plays a critical role in the electronic structure of the1D system,which provides insights for the design of nano-electronics materials.
基金supported by the National Natural Science Foundation of China(Grant Nos.12374459,61974138,and 92065106)the Innovation Program for Quantum Science and Technology(Grant No.2021ZD0302400)+1 种基金the Strategic Priority Research Program of Chinese Academy of Sciences(Grant No.XDB0460000)the support from the Youth Innovation Promotion Association,Chinese Academy of Sciences(Grant Nos.2017156 and Y2021043)。
文摘Anti-phase domain defects easily form in the in-plane GaAs nanowires(NWs)grown on CMOS-compatiblegroup IV substrates,which makes it difficult to obtain GaAs NWs with a designed length and also leads to asignificant limitation in the growth of high-quality in-plane GaAs NW networks on such substrates.Here,wereport on the selective area growth of anti-phase domain-free in-plane GaAs NWs and NW networks on Ge(111)substrates.Detailed structural studies confirm that the GaAs NW grown using a large pattern period and GaAsNW networks grown by adding the Sb are both high-quality pure zinc-blende single crystals free of stackingfaults,twin defects,and anti-phase domain defects.Room-temperature photoluminescence measurements show asubstantial improvement in crystal quality and good consistency and uniformity of the GaAs NW networks.Ourwork provides useful insights into the controlled growth of high-quality anti-phase domain-defects-free in-planeIII-V NWs and NW networks.
基金supported by the National Natural Science Foundation of China(grant Nos.52073290 and 51927803)the Liaoning Province Science and Technology Plan Project(No.2022-MS-011)the Shenyang science and technology plan project(23-407-3-23).
文摘Intermetallic Pt-based nanoparticles have displayed excellent activity for the oxygen reduction reaction(ORR)in fuel cells.However,it remains a great challenge to synthesize highly atomically ordered Pt-based nanoparticle catalysts because the formation of an atomically ordered structure usually requires high-temperature annealing accompanied by grain sintering.Here we report the direct epitaxial growth of well-aligned,highly atomically ordered Pt3 Fe and PtFe nanoparticles(<5 nm)on single-walled carbon nanotube(SWCNT)bundles films.The long-range periodically symmetric van der Waals(vdW)interac-tions between SWCNT bundles and Pt-Fe nanoparticles play an important role in promoting not only the alignment ordering of inter-nanoparticles but also the atomic ordering of intra-nanoparticles.The ordered Pt_(3)Fe/SWCNT catalyst showed enhanced ORR catalytic performance of 2.3-fold higher mass activity and 3.1-fold higher specific activity than commercial Pt/C.Moreover,the formation of an interlocked inter-face and strong vdW interaction endow the Pt-Fe/SWCNT catalysts with extreme long-term stability in potential cycling and excellent anti-thermal sintering ability.
基金supported by the Key Laboratory of Fine Chemicals,Jiangsu Provincefinancially supported by the Jiangsu Province Science and Technology Support Program (BE2011651)the Key University Science Research Project of Jiangsu Province (11KJA610002)
文摘MnSAPO-34 molecular sieves were synthesized by vapor-phase transport （VPT） method using triethylamine （Et3N） as a structure directing agent （SDA）, and were characterized by XRD, BET, SEM, UV-Vis, FT-IR, and TG analy- ses. The influence of the zeolite crystallization conditions and the dry-gel composition were investigated. The results showed that the synthesis conditions had an effect on the crystalline phase. Pure MnSAPO-34 had been obtained when it was crystallized at 140 C for 18 hours. The ratio of MnO/A1203 in the starting gel ranging from 0.1 to 0.2 resulted in pure MnSAPO-34 with a CHA topology. Beyond this scope, MnSAPO-5 with an AFI topology structure was obtained as an impurity substance. UV-Vis spectroscopy and FT-IR spectroscopy study indicated that manganese was incorporated into the framework of the molecular sieve. The catalytic performance of MnSAPO-34 molecular sieve was tested by ketalization reaction of l, 2-propanediol with cyclohexanone. High yield of cyclohexanone-1, 2-propanediol ketal was obtained.
文摘Kinetic regularities of 4-phenyl-o-tolunitrile ammoxidation on V-Sb-Bi-Zr/γ-Al2O3 oxide catalyst in the temperature interval 633 - 673 K have been studied. It has been established that rates of conversion of 4-phenyl-o-tolu- nitrile into the aimed 4-phenylphthalonitrile and CO2 are described by half-order equation on concentration of substratum and to be independent of the oxygen and ammonia partial pressures. It has been revealed that formation of 4-phenylphthalimide from byproducts is due to hydrolysis of 4-phenylphthalonitrile;carbon dioxide is produced by oxidation of 4-phenyl-o-tolunitrile and decarboxylation of 4-phenylphthalimide, and 4-phenylben- zonitrile is produced from 4-phenyl-o-tolunitrile and 4-phenylphthalimide.
基金Supported by the National Natural Science Foundation of China under Grant Nos 50572053 and 10234010, and NCET of the Ministry of Education of China under Grant No 040634.
文摘High quality Co-doped ZnO thin films are grown on single crystalline Al2O3（0001） and ZnO（0001） substrates by oxygen plasma assisted molecular beam epitaxy at a relatively lower substrate temperature of 450℃. The epitaxial conditions are examined with in-situ reflection high energy electron diffraction （RHEED） and ex-situ high resolution x-ray diffraction （HRXRD）. The epitaxial thin films are single crystal at film thickness smaller than 500nm and nominal concentration of Co dopant up to 20%. It is indicated that the Co cation is incorporated into the ZnO matrix as Co^2＋ substituting Zn^2＋ ions. Atomic force microscopy shows smooth surfaces with rms roughness of 1.9 nm. Room-temperature magnetization measurements reveal that the Co-doped ZnO thin films are ferromagnetic with Curie temperatures Tc above room temperature.
基金supported by the National Key R&D Program of China(Grant No.2021YFB2206503)National Natural Science Foundation of China(Grant No.62274159)+1 种基金CAS Project for Young Scientists in Basic Research(Grant No.YSBR-056)the“Strategic Priority Research Program”of the Chinese Academy of Sciences(Grant No.XDB43010102).
文摘Ex situ characterization techniques in molecular beam epitaxy(MBE)have inherent limitations,such as being prone to sample contamination and unstable surfaces during sample transfer from the MBE chamber.In recent years,the need for improved accuracy and reliability in measurement has driven the increasing adoption of in situ characterization techniques.These techniques,such as reflection high-energy electron diffraction,scanning tunneling microscopy,and X-ray photoelectron spectroscopy,allow direct observation of film growth processes in real time without exposing the sample to air,hence offering insights into the growth mechanisms of epitaxial films with controlled properties.By combining multiple in situ characterization techniques with MBE,researchers can better understand film growth processes,realizing novel materials with customized properties and extensive applications.This review aims to overview the benefits and achievements of in situ characterization techniques in MBE and their applications for material science research.In addition,through further analysis of these techniques regarding their challenges and potential solutions,particularly highlighting the assistance of machine learning to correlate in situ characterization with other material information,we hope to provide a guideline for future efforts in the development of novel monitoring and control schemes for MBE growth processes with improved material properties.
文摘In order to obtain bi epitaxial 45° grain boundary YBa 2Cu 3O 7 (YBCO) junctions, the in plane epitaxy of CeO 2 films on both MgO films and SrTiO 3 substrates was studied. Using magnetron sputtering technique and decreasing the substrate temperature, 100% CeO 2∥MgO in plane orientation for bi epitaxial grain boundary junction can be obtained.
基金funded by the UM’s research funds(MYRG2020-00283-IAPME,MYRG2022-00266-IAPME,and MYRG-GRG2023-00224-IAPME-UMDF)the Science and Technology Development Fund,Macao SAR(FDCT 0006/2021/AKP,FDCT 0096/2020/A2,0013/2021/AMJ,and 0082/2022/A2)City University of Hong Kong(Project No.9020002)
文摘Two-dimensional materials have been widely used to tune the growth and energy-level alignment of perovskites.However,their incomplete passivation and chaotic usage amounts are not conducive to the preparation of highquality perovskite films.Herein,we succeeded in obtaining higher-quality CsPbBr_(3)films by introducing large-area monolayer graphene as a stable physical overlay on top of TiO_(2)substrates.Benefiting from the inert and atomic smooth graphene surface,the CsPbBr_(3)film grown on top by the van der Waal epitaxy has higher crystallinity,improved(100)orientation,and an average domain size of up to 1.22μm.Meanwhile,a strong downward band bending is observed at the graphene/perovskite interface,improving the electron extraction to the electron transport layers(ETL).As a result,perovskite film grown on graphene has lower photoluminescence(PL)intensity,shorter carrier lifetime,and fewer defects.Finally,a photovoltaic device based on epitaxy CsPbBr_(3)film is fabricated,exhibiting power conversion efficiency(PCE)of up to 10.64%and stability over 2000 h in the air.
基金Supported by the Key Basic Research of Science and Technology Commission of Shanghai Municipality(10JC1405900)and Shanghai Leading Academic Disciplines(S30107)。
文摘The Si overlayers are grown by molecular beam epitaxy on atomically smllth Er_(2)O_(3)(111)films prepared on Si(111)substrates.Single crystalline Si overlayers are achieved and are evident due to the spot-like reflective high energy electron diffraction(RHEED)patterns and x-ray diffraction patterns.The epitaxial relationship of the Si overlayer along the surface with respect to the orientation of Er_(2)O_(3)and the Si substrate is as follows:overgrown Si(111)//Er_(2)O_(3)(111)//Si(111).The rough surface of Si overlayers,as identified by both RHEED patterns and atomic force microscopy images,indicates a three-dimensional growth mode.The reason for this is based on the interfacial energy argument.Further growth of Er_(2)O_(3)films on this rough Si overlayer leads to the polycrystalline nature of the topmost Er2O3 layer.
文摘Vapor-phase nitration of benzene over solid acid catalyst is expected to be a clean process with no sulfuric acid waste. We investigated this process over solid acidic catalysts utilizing diluted nitric acid (60-70%) as nitrating agent, and found that supported sulfuric acid catalyst exhibited a very high catalytic activity. Under the conditions of reaction temperature 160-170℃, space velocity (SV) 1200 h-1, the yield and the space-time yield (STY) of nitrobenzene (NB) based on HNO3 were more than 98% and 0.75 kg穔gcat-1穐-1 over 10% H2SO4/SiO2 (by weight) catalyst respectively.
