In 2023,the majority of the Earth witnessed its warmest boreal summer and autumn since 1850.Whether 2023 will indeed turn out to be the warmest year on record and what caused the astonishingly large margin of warming ...In 2023,the majority of the Earth witnessed its warmest boreal summer and autumn since 1850.Whether 2023 will indeed turn out to be the warmest year on record and what caused the astonishingly large margin of warming has become one of the hottest topics in the scientific community and is closely connected to the future development of human society.We analyzed the monthly varying global mean surface temperature(GMST)in 2023 and found that the globe,the land,and the oceans in 2023 all exhibit extraordinary warming,which is distinct from any previous year in recorded history.Based on the GMST statistical ensemble prediction model developed at the Institute of Atmospheric Physics,the GMST in 2023 is predicted to be 1.41℃±0.07℃,which will certainly surpass that in 2016 as the warmest year since 1850,and is approaching the 1.5℃ global warming threshold.Compared to 2022,the GMST in 2023 will increase by 0.24℃,with 88%of the increment contributed by the annual variability as mostly affected by El Niño.Moreover,the multidecadal variability related to the Atlantic Multidecadal Oscillation(AMO)in 2023 also provided an important warming background for sparking the GMST rise.As a result,the GMST in 2023 is projected to be 1.15℃±0.07℃,with only a 0.02℃ increment,if the effects of natural variability—including El Niño and the AMO—are eliminated and only the global warming trend is considered.展开更多
Twisted bilayer graphene(TBG) has been extensively studied because of its novel physical properties and potential application in electronic devices.Here we report the synthesis and characterization of 300 TBG naturall...Twisted bilayer graphene(TBG) has been extensively studied because of its novel physical properties and potential application in electronic devices.Here we report the synthesis and characterization of 300 TBG naturally grown on Cu_(0.75)Ni_(0.25)(111) film and investigate the electronic structure by angle-resolved photoemission spectroscopy.Compared with other substrates,our TBG with a wafer scale is acquired with a shorter growth time.The Fermi velocity and energy gap of Dirac cones of TBG are comparable with those of a monolayer on Cu_(0.85)Ni_(0.15)(111).The signature of moré lattices has not been observed in either the low-energy electron diffraction patterns or the Fermi surface map within experimental resolution,possibly due to different Cu and Ni contents in the substrates enhancing the different couplings between the substrate and the first/second layers and hindering the formation of a quasiperiodic structure.展开更多
For laser cladding a large temperature gradient easily weakened the surface quality by generating cracks and irregular coating surfaces,which in turn affected the bearing capacity and corrosion resistance of coatings ...For laser cladding a large temperature gradient easily weakened the surface quality by generating cracks and irregular coating surfaces,which in turn affected the bearing capacity and corrosion resistance of coatings in the rapid heating and cooling process.The response surface methodology(RSM)was used to predict coating cracks by changing the powder ratio,energy density,and preheating temperature,which obtained the relevant mathematical model.After that,the sensitivity of the crack length to process parameters was analyzed based on the sensitivity analysis method.The effect of Ni60/WC composite powder process parameters on the surface quality was revealed in laser cladding.The crack length first decreased and then increased,and the Smooth decreased with the increased powder ratio.The crack length and Smooth increased with the increased energy density.The crack length decreased and Smooth increased with the increased preheating temperature.Sensitivity analysis showed that the crack length and Smooth were the most sensitive to the powder ratio.Therefore,the process parameters were reasonably selected to control the surface quality.The mathematical model and sensitivity analysis method in the work could improve the surface quality,which provided a theoretical basis for the prediction and control of laser cladding cracks.展开更多
The adsorption behavior of methyl nitrite (MN) on the closed-packed Pd(111) sur- face has been investigated in detail by using density functional theory (DFT). MN binds to the surface in two alternative forms, u...The adsorption behavior of methyl nitrite (MN) on the closed-packed Pd(111) sur- face has been investigated in detail by using density functional theory (DFT). MN binds to the surface in two alternative forms, using the nitrogen atom attached to the surface. An overall net charge transfer from the substrate to the cis-MN molecule is also confirmed. In addition, the reaction mechanism for the dissociation of MN on the Pd(111) surface has been identified and compared with the methanol decomposition via O-H scission. The results demonstrate that MN is a more active reactant than methanol for the oxidative addition to the Pd catalyst. The possible reason has been analyzed from the adsorption behaviors and reaction barriers, that is, MN is chemically absorbed on the Pd(111) surface; the CHaO-NO bond scission, leading to the formation of adsorbed methoxy species, is much more favorable than that of the O-H bond scission and has a large exothermic behavior.展开更多
To elucidate feasible routes of producing CO from CH 3 and unravel the eff ect of adsorbed O on CH x transformation, the reactivity of CH x ( x = 1-3) with and without the assistance of adsorbed atomic O on Ni(111) wa...To elucidate feasible routes of producing CO from CH 3 and unravel the eff ect of adsorbed O on CH x transformation, the reactivity of CH x ( x = 1-3) with and without the assistance of adsorbed atomic O on Ni(111) was explored using density functional theory calculations. The adsorption energies of CH x ( x = 0-3) were found to be signifi cantly reduced on an O-preadsorbed Ni(111) surface compared to a pure surface. Furthermore, O-assisted one-step dehydrogenation of CH x ( x = 1-3) features energy barriers and thus is diffi cult to proceed. In terms of energy, the direct dissociation of CH 3 is favorable, except for the last CH dehydrogenation, which is energy intensive. Interestingly, in O-assisted two-step CH transformation to CO via CHO intermediate, the barrier is dramatically lowered. The successive dehydrogenations of CH x O ( x = 1-3) were also found to be a route for CO formation. Finally, two possible pathways from CH 3 to CO are proposed:(a) CH 3 → CH 2 → CH → CHO → CO;(b) CH 3 → CH 3 O → CH 2 O → CHO → CO.展开更多
The interaction of cyanide (CN) with different sites on Ni(111) surface is studied by using density functional theory (DFT). Ni19 cluster is used to simulate the surface. The present calculations show that the end-o...The interaction of cyanide (CN) with different sites on Ni(111) surface is studied by using density functional theory (DFT). Ni19 cluster is used to simulate the surface. The present calculations show that the end-on bonded (through C atom) configuration is much more preferable than the side-on bonded CN or other configurations on the same adsorption site. For all adsorption modes, adsorption energies at the top, bridge, and three-fold sites on Ni(111) are comparable, with the bridge site of the end-on bonded CN (through C atom) more favorable than other adsorption sites. CN vibrational frequencies are red-shifted at all cases, except that the end-on CN bonded (through C atom) on the top site is blue-shifted. The bonding of CN on the Ni(111) surface is large- ly ionic.展开更多
Adsorption behavior of Fe atoms on a metal-free naphthalocyanine(H2Nc) monolayer on Ag(111) surface at room temperature has been investigated using scanning tunneling microscopy combined with density functional th...Adsorption behavior of Fe atoms on a metal-free naphthalocyanine(H2Nc) monolayer on Ag(111) surface at room temperature has been investigated using scanning tunneling microscopy combined with density functional theory(DFT)based calculations. We found that the Fe atoms were adsorbed on the centers of H2Nc molecules and formed Fe–H2Nc complexes at low coverage. DFT calculations show that Fe sited in the center of the molecule is the most stable configuration, in good agreement with the experimental observations. After an Fe–H2Nc complex monolayer was formed, the extra Fe atoms self-assembled to Fe clusters of uniform size and adsorbed dispersively at the interstitial positions of Fe–H2Nc complex monolayer. Therefore, the H2Nc monolayer grown on Ag(111) could be a good template to grow dispersed magnetic metal atoms and clusters at room temperature for further investigation of their magnetism-related properties.展开更多
We report the formation and local electronic structure of Ge clusters on the Si(111)-7×7 surface studied by using variable temperature scanning tunnelling microscopy (VT-STM) and low-temperature scanning tunn...We report the formation and local electronic structure of Ge clusters on the Si(111)-7×7 surface studied by using variable temperature scanning tunnelling microscopy (VT-STM) and low-temperature scanning tunnelling spectroscopy (STS). Atom-resolved STM images reveal that the Ce atoms are prone to forming clusters with 1.0 nm in diameter for coverage up to 0.12 ML. Such Ce clusters preferentially nucleate at the centre of the faulted-half unit cells, leading to the 'dark sites' of Si centre adatoms from the surrounding three unfaulted-half unit cells in filled-state images. Biasdependent STM images show the charge transfer from the neighbouring Si adatoms to Ce clusters. Low-temperature STS of the Ce clusters reveals that there is a band gap on the Ce cluster and the large voltage threshold is about 0.9 V.展开更多
The adsorption of CH3CN and CH3NC on the Pt(111)surface at the 1/4 monolayer(ML)coverage has been carried out at the level of density functional theory for understanding hydrogenation processes of nitriles.The most fa...The adsorption of CH3CN and CH3NC on the Pt(111)surface at the 1/4 monolayer(ML)coverage has been carried out at the level of density functional theory for understanding hydrogenation processes of nitriles.The most favored adsorption structure for CH3CN is the C-N bond almost parallel to the surface with the C-N bond interaction with adjacent surface Pt atoms.For CH3NC,the most stable configuration is the CH3NC locates at the face center cubic(fcc)site with the C-atom bonded to three Pt atoms.In addition,the HCN and HNC adsorption has been computed,and the adsorption pattern is nearly similar to the CH3CN and CH3NC,respectively.The adsorbed molecules rehybridize on the surface,becoming non-linear with a bent C-C-N or C-N-C angle.Furthermore,the binding mechanism of these molecules on the Pt(111)surface is also analyzed.展开更多
We applied periodic density-functional theory to investigate the adsorption of HCN on x Ni@Pt(111) bimetallic surfaces(x = 1~4). The results have been compared with those obtained on pure Ni(111) and Pt(111) s...We applied periodic density-functional theory to investigate the adsorption of HCN on x Ni@Pt(111) bimetallic surfaces(x = 1~4). The results have been compared with those obtained on pure Ni(111) and Pt(111) surfaces. For all bimetallic surfaces,HCN is preferentially tilted with the CN bond parallel to the surface,and adsorption energies increase with an increasing number of layer Ni atoms on the surface. The adsorption energies of HCN on all bimetallic surfaces are larger than that on the Pt(111) surface,whereas the adsorption energies of HCN on 3Ni@Pt(111) and 4Ni@Pt(111) are larger than that on the Ni(111) surface,indicating that the introduction of Ni to the Pt catalyst could increase the activity of bimetallic catalyst in the hydrogenation reaction for nitriles. Larger adsorption energy of HCN leads to a longer C–N bond length and a smaller CN vibrational frequency. The analysis of Bader charge and vibrational frequencies showed obvious weakening of the adsorbed C–N bond and an indication of sp2 hybridization of both carbon and nitrogen atoms.展开更多
Surface preparation is potentially important to the corrosion and biomedical properties of NiTi shape memory alloys. The effect of surface preparation on corrosion properties and nickel release of a Ti-56 wt.%Ni alloy...Surface preparation is potentially important to the corrosion and biomedical properties of NiTi shape memory alloys. The effect of surface preparation on corrosion properties and nickel release of a Ti-56 wt.%Ni alloy has been studied. Surface of the NiTi coupons were prepared by four methods, namely, chemical etching, electropolishing, mechanical polishing and oxidizing, and then examined by corrosion test system. Furthermore, the Ni ion releases from NiTi samples with different surface preparations dipped in 1% HCl solution were analysed. Compared with the surface after chemical treatment, mechanical polishing and thermal oxidation, electropolished surface has better corrosion resistance and less nickel release for not only its lower surface roughness, but also the composition and property of its surface film.展开更多
Adsorption of CH3O at four sites (top, bridge, hcp, fcc) on Au(111) surface has been investigated by density functional theory method at the generalized gradient approximation level. We have performed calculations...Adsorption of CH3O at four sites (top, bridge, hcp, fcc) on Au(111) surface has been investigated by density functional theory method at the generalized gradient approximation level. We have performed calculations on adsorption energies, structures, Mulliken charges and vibrational frequencies of CH3O on Au(111) surface with full-geometry optimization. The predicted results are compared with the available experimental observation. The calculated CH3O adsorption structure and stretching vibrational frequencies agree well with experimental ones, and precise determinations of adsorption sites are carded out. The most favorite adsorption on Au(111) occurs at the bridge site, and O-C axis is tilted to the surface. However, on hollow sites (hcp, fcc) the species is adsorbed in an upright geometry (pseudo-C3v local symmetry).展开更多
Thiophene adsorption on the(111) surfaces of Pd and Pt have been investigated by density functional theory.The results indicate that the adsorption at the hollow sites is the most stable.To our interest,the molecula...Thiophene adsorption on the(111) surfaces of Pd and Pt have been investigated by density functional theory.The results indicate that the adsorption at the hollow sites is the most stable.To our interest,the molecular plane of thiophene ring is distorted with C=C bond being elongated to 1.450 and C–C bond being shortened to 1.347 ,and the C–H bonds tilt 13.91~44.05o away from this plane.Furthermore,analysis on population and density of states verified the calculated adsorption geometries.Finally,charge analysis suggests that thiophene molecule is an electron acceptor,reflecting the interaction between the lone pair of sulfur and the d-orbitals of metal.展开更多
The surface infiltrated composite (Ni/WC) layers on gray iron substrate were fabricated through a vacuum infiltration casting technique (VICT) using Ni-based composite powder with different WC particles content as...The surface infiltrated composite (Ni/WC) layers on gray iron substrate were fabricated through a vacuum infiltration casting technique (VICT) using Ni-based composite powder with different WC particles content as raw materials.The microstructures of surface infiltrated composite layer,the interface structures between surface composite layer and the substrate,the changes of macro-hardness with the increasing of WC content and the micro-hardness distribution are investigated.The infiltrated composite layer includes a surface composite layer and a transition layer,and the thickness of the transition layer decreases with the increasing content of WC.The thickness of transition layer with 20%WC content in the surface infiltrated composite layer was 170 μm which was the thickest for all transition layers with different WC content.The surface composite layer was mainly composed of WC,W2C,FeB and NiB,along with Ni-Cr-Fe,Ni (Cr) solid solution,Ni (Si) solid solution and Ni (Fe) solid solution.The transition layer was composed of Ni (Cr) solid solution,Ni (Fe) solid solution,Ni (Si) solid solution,Fe (Ni) solid solution and eutectic.The surface macro-hardness and micro-hardness of the infiltrated layer had been evaluated.The macro-hardness of the surface composite layer decreases with the WC content increasing,and the average macro-hardness is HRC60.The distribution of micro-hardness presents gradient change.The average micro-hardness of the infiltrated layer is about HV1000.展开更多
Laser multiple processing, i.e. laser surface texturing and then Laser Shock Processing (LSP), is a new surface processing technology for the preparation of bionic non-smooth surfaces. Based on engineering bionics, sa...Laser multiple processing, i.e. laser surface texturing and then Laser Shock Processing (LSP), is a new surface processing technology for the preparation of bionic non-smooth surfaces. Based on engineering bionics, samples of bionic non-smooth surfaces of stainless steel 0Crl 8Ni9 were manufactured in the form of reseau structure by laser multiple processing. The mechanical properties (including microhardness, residual stress, surface roughness) and microstructure of the samples treated by laser multiple processing were compared with those of the samples without LSP The results show that the mechanical properties of these samples by laser multiple processing were clearly improved in comparison with those of the samples without LSP The mechanisms underlying the improved surface microhardness and surface residual stress were analyzed, and the relations between hardness, comnressive residual stress and roughness were also presented.展开更多
The density functional theory(DFT) and self-consistent periodic calculation were used to investigate the methanol adsorption on the Pt-Mo(111)/C surface.The adsorption energies,equilibrium geometries and vibration...The density functional theory(DFT) and self-consistent periodic calculation were used to investigate the methanol adsorption on the Pt-Mo(111)/C surface.The adsorption energies,equilibrium geometries and vibration frequencies of CH3OH on nine types of sites on the Pt-Mo(111)/C surface were predicted and the favorite adsorption site for methanol is the top-Pt site.Both sites of valence and conduction bands of doped system have been broadened,which are favorable for electrons to transfer to the cavity.The possible decomposition pathway was investigated with transition state searching and the calculation results indicate that the O-H bond is first broken,and then the methanol decomposes into methoxy.The activation barrier of O-H bond breaking with Pt-Mo catalyst is only 104.8 kJ mol-1,showing that carbon supported Pt-Mo alloys have promoted the decomposition of methanol.Comparing with the adsorption energies of CH3OH on the Pt(111)/C surface and that of CO,the adsorption energies of CO are higher,and Pt(111)/C is liable to be oxidized and loses the activity,which suggests that the catalyst Pt-Mo(111)/C is in favor of decomposing methanol and has better anti-poisoning ability than Pt(111)/C.展开更多
This study assesses the reproducibility of 31 historical simulations from 1850 to 2014 in the Coupled Model Intercomparison Project phase 6(CMIP6) for the subsurface(Sub-IOD) and surface Indian Ocean Dipole(IOD) and t...This study assesses the reproducibility of 31 historical simulations from 1850 to 2014 in the Coupled Model Intercomparison Project phase 6(CMIP6) for the subsurface(Sub-IOD) and surface Indian Ocean Dipole(IOD) and their association with El Ni?o-Southern Oscillation(ENSO). Most CMIP6 models can reproduce the leading east-west dipole oscillation mode of heat content anomalies in the tropical Indian Ocean(TIO) but largely overestimate the amplitude and the dominant period of the Sub-IOD. Associated with the much steeper west-to-east thermocline tilt of the TIO, the vertical coupling between the Sub-IOD and IOD is overly strong in most CMIP6 models compared to that in the Ocean Reanalysis System 4(ORAS4). Related to this, most models also show a much tighter association of Sub-IOD and IOD events with the canonical ENSO than observations. This explains the more(less) regular Sub-IOD and IOD events in autumn in those models with stronger(weaker) surface-subsurface coupling in TIO. Though all model simulations feature a consistently low bias regarding the percentage of the winter–spring Sub-IOD events co-occurring with a Central Pacific(CP) ENSO, the linkage between a westward-centered CP-ENSO and the Sub-IOD that occurs in winter–spring, independent of the IOD, is well reproduced.展开更多
Haiyang-2A(HY-2A) is China's first ocean dynamic environment satellite and the radar altimeter is one of its main payloads. One of the main purposes of the radar altimeter is to measure the sea surface height(SSH...Haiyang-2A(HY-2A) is China's first ocean dynamic environment satellite and the radar altimeter is one of its main payloads. One of the main purposes of the radar altimeter is to measure the sea surface height(SSH). The SSH determined from the altimeter range measurements includes some range and geophysical corrections. These corrections largely affect the accuracy of the SSH measurements. The range and the geophysical corrections are reprocessed and the altimeter waveforms in HY-2A sensor interim geophysical data set records(S-IGDR) are retracked from June 1, 2014 to June 14, 2014, and the accuracy of the reprocessed SSH measurements is evaluated.The methods of the range and geophysical corrections used to reprocess HY-2A altimeter data are validated by using these methods to reprocess the Jason-2 range and geophysical corrections and comparing the results with the range and geophysical corrections in Jason-2 geophysical dataset records(GDR) product. A crossover analysis is used to evaluate the accuracy of the reprocessed HY-2A SSH measurements. The standard deviation(STD) of the crossover SSH differences for HY-2A is around 4.53 cm while the STD of the SSH differences between HY-2A and Jason-2 is around 5.22 cm. The performance of the reprocessed HY-2A SSH measurements is significantly improved with respect to the SSH measurements derived from HY-2A interim geophysical dataset records(IGDR)product. The 2015–2016 El Ni?o has been the strongest El Ni?o event since 1997–1998. The range and the geophysical corrections in HY-2A IGDR are reprocessed and sea level anomalies are used to monitor the2015–2016 El Ni?o. The results show that the HY-2A altimeter can well observe the 2015–2016 El Ni?o.展开更多
This paper describes the electroless Ni or Cu plating of some fiuoropolymer substrates through a tin-free activation process. Materials subjected to surface metallization are commercial Teflon() FEP, Nafion(), ACLAR()...This paper describes the electroless Ni or Cu plating of some fiuoropolymer substrates through a tin-free activation process. Materials subjected to surface metallization are commercial Teflon() FEP, Nafion(), ACLAR() and LaRCTM-CP1 thin films which have recently gained a large scientific and technological interest due to their excellent thermal, chemical, mechanical and dielectric properties. The original approach implemented in the present work involves: (i)the grafting of nitrogen-containing functionalities on the polymer surfaces through plasma treatments in ammonia, (ii) the direct catalysis of the so-modified surfaces via their immersion in a simple acidic PdCl2 solution (i.e. without using a prior surface sensitization in an acidic SnCl2 solution), and finally (iii) the electroless metallization itself. However, prior to the immersion in the industrial plating baths, the chemical reduction of the Pd+2 species (species covalently tethered on the nitrogen-containing groups) to metallic palladium (PdO) is shown to be a key factor in catalyzing the electroless deposition initiation. This is made by immersion in an hypophosphite (H2PO2-) solution. Wettability measurements and X-ray photoelectron spectroscopy (XPS) experiments are used to characterize every surface modification step of the developed process. A cross-hatch tape test was used to asses the adhesion strength of the electroless films that is shown qualitatively good. In addition, a fragmentation test was developed in combination with electrical measurements. Its use allows to distinguish different adhesion levels at the metal/polymer interface and to evidence the influence of some processing parameters.展开更多
基金supported by the Key Research Program of Frontier Sciences,Chinese Academy of Sciences(Grant No.ZDBS-LY-DQC010)the National Natural Science Foundation of China(Grant No.42175045).
文摘In 2023,the majority of the Earth witnessed its warmest boreal summer and autumn since 1850.Whether 2023 will indeed turn out to be the warmest year on record and what caused the astonishingly large margin of warming has become one of the hottest topics in the scientific community and is closely connected to the future development of human society.We analyzed the monthly varying global mean surface temperature(GMST)in 2023 and found that the globe,the land,and the oceans in 2023 all exhibit extraordinary warming,which is distinct from any previous year in recorded history.Based on the GMST statistical ensemble prediction model developed at the Institute of Atmospheric Physics,the GMST in 2023 is predicted to be 1.41℃±0.07℃,which will certainly surpass that in 2016 as the warmest year since 1850,and is approaching the 1.5℃ global warming threshold.Compared to 2022,the GMST in 2023 will increase by 0.24℃,with 88%of the increment contributed by the annual variability as mostly affected by El Niño.Moreover,the multidecadal variability related to the Atlantic Multidecadal Oscillation(AMO)in 2023 also provided an important warming background for sparking the GMST rise.As a result,the GMST in 2023 is projected to be 1.15℃±0.07℃,with only a 0.02℃ increment,if the effects of natural variability—including El Niño and the AMO—are eliminated and only the global warming trend is considered.
基金Project supported by the National Key R&D Program of China (Grant Nos. 2022YFB3608000 and 2022YFA1204900)the National Natural Science Foundation of China (Grant Nos. 12222413 and 12074205)+2 种基金the Natural Science Foundation of Shanghai (Grant Nos. 23ZR1482200 and 22ZR1473300)the Natural Science Foundation of Zhejiang Province (Grant No. LQ21A040004)the funding of Ningbo University (Grant No. LJ2024003)。
文摘Twisted bilayer graphene(TBG) has been extensively studied because of its novel physical properties and potential application in electronic devices.Here we report the synthesis and characterization of 300 TBG naturally grown on Cu_(0.75)Ni_(0.25)(111) film and investigate the electronic structure by angle-resolved photoemission spectroscopy.Compared with other substrates,our TBG with a wafer scale is acquired with a shorter growth time.The Fermi velocity and energy gap of Dirac cones of TBG are comparable with those of a monolayer on Cu_(0.85)Ni_(0.15)(111).The signature of moré lattices has not been observed in either the low-energy electron diffraction patterns or the Fermi surface map within experimental resolution,possibly due to different Cu and Ni contents in the substrates enhancing the different couplings between the substrate and the first/second layers and hindering the formation of a quasiperiodic structure.
基金supported by Science and Technology Major Project of Fujian Province(Grant No.2020HZ03018).
文摘For laser cladding a large temperature gradient easily weakened the surface quality by generating cracks and irregular coating surfaces,which in turn affected the bearing capacity and corrosion resistance of coatings in the rapid heating and cooling process.The response surface methodology(RSM)was used to predict coating cracks by changing the powder ratio,energy density,and preheating temperature,which obtained the relevant mathematical model.After that,the sensitivity of the crack length to process parameters was analyzed based on the sensitivity analysis method.The effect of Ni60/WC composite powder process parameters on the surface quality was revealed in laser cladding.The crack length first decreased and then increased,and the Smooth decreased with the increased powder ratio.The crack length and Smooth increased with the increased energy density.The crack length decreased and Smooth increased with the increased preheating temperature.Sensitivity analysis showed that the crack length and Smooth were the most sensitive to the powder ratio.Therefore,the process parameters were reasonably selected to control the surface quality.The mathematical model and sensitivity analysis method in the work could improve the surface quality,which provided a theoretical basis for the prediction and control of laser cladding cracks.
基金supported by the National Natural Science Foundation of China (21171039)
文摘The adsorption behavior of methyl nitrite (MN) on the closed-packed Pd(111) sur- face has been investigated in detail by using density functional theory (DFT). MN binds to the surface in two alternative forms, using the nitrogen atom attached to the surface. An overall net charge transfer from the substrate to the cis-MN molecule is also confirmed. In addition, the reaction mechanism for the dissociation of MN on the Pd(111) surface has been identified and compared with the methanol decomposition via O-H scission. The results demonstrate that MN is a more active reactant than methanol for the oxidative addition to the Pd catalyst. The possible reason has been analyzed from the adsorption behaviors and reaction barriers, that is, MN is chemically absorbed on the Pd(111) surface; the CHaO-NO bond scission, leading to the formation of adsorbed methoxy species, is much more favorable than that of the O-H bond scission and has a large exothermic behavior.
文摘To elucidate feasible routes of producing CO from CH 3 and unravel the eff ect of adsorbed O on CH x transformation, the reactivity of CH x ( x = 1-3) with and without the assistance of adsorbed atomic O on Ni(111) was explored using density functional theory calculations. The adsorption energies of CH x ( x = 0-3) were found to be signifi cantly reduced on an O-preadsorbed Ni(111) surface compared to a pure surface. Furthermore, O-assisted one-step dehydrogenation of CH x ( x = 1-3) features energy barriers and thus is diffi cult to proceed. In terms of energy, the direct dissociation of CH 3 is favorable, except for the last CH dehydrogenation, which is energy intensive. Interestingly, in O-assisted two-step CH transformation to CO via CHO intermediate, the barrier is dramatically lowered. The successive dehydrogenations of CH x O ( x = 1-3) were also found to be a route for CO formation. Finally, two possible pathways from CH 3 to CO are proposed:(a) CH 3 → CH 2 → CH → CHO → CO;(b) CH 3 → CH 3 O → CH 2 O → CHO → CO.
基金This work was supported by the National Natural Science Foundation of China (20273013 20303002)+1 种基金 the Fujian Province Key Foundation (K02012) the State Key Laboratory of Structural Chemistry (020051) and Fuzhou University (2004XY04)
文摘The interaction of cyanide (CN) with different sites on Ni(111) surface is studied by using density functional theory (DFT). Ni19 cluster is used to simulate the surface. The present calculations show that the end-on bonded (through C atom) configuration is much more preferable than the side-on bonded CN or other configurations on the same adsorption site. For all adsorption modes, adsorption energies at the top, bridge, and three-fold sites on Ni(111) are comparable, with the bridge site of the end-on bonded CN (through C atom) more favorable than other adsorption sites. CN vibrational frequencies are red-shifted at all cases, except that the end-on CN bonded (through C atom) on the top site is blue-shifted. The bonding of CN on the Ni(111) surface is large- ly ionic.
基金supported by the National Natural Science Foundation of China(Grant Nos.61390501,51325204,and 11204361)the National Basic Research Program of China(Grant Nos.2011CB808401 and 2011CB921702)+1 种基金the National Key Scientific Instrument and Equipment Development Project of China(Grant No.2013YQ1203451)the National Supercomputing Center in Tianjin,China,and the Chinese Academy of Sciences
文摘Adsorption behavior of Fe atoms on a metal-free naphthalocyanine(H2Nc) monolayer on Ag(111) surface at room temperature has been investigated using scanning tunneling microscopy combined with density functional theory(DFT)based calculations. We found that the Fe atoms were adsorbed on the centers of H2Nc molecules and formed Fe–H2Nc complexes at low coverage. DFT calculations show that Fe sited in the center of the molecule is the most stable configuration, in good agreement with the experimental observations. After an Fe–H2Nc complex monolayer was formed, the extra Fe atoms self-assembled to Fe clusters of uniform size and adsorbed dispersively at the interstitial positions of Fe–H2Nc complex monolayer. Therefore, the H2Nc monolayer grown on Ag(111) could be a good template to grow dispersed magnetic metal atoms and clusters at room temperature for further investigation of their magnetism-related properties.
基金Project supported by the National Natural Science Foundation of China (Grant Nos 90406022 and 10674159).
文摘We report the formation and local electronic structure of Ge clusters on the Si(111)-7×7 surface studied by using variable temperature scanning tunnelling microscopy (VT-STM) and low-temperature scanning tunnelling spectroscopy (STS). Atom-resolved STM images reveal that the Ce atoms are prone to forming clusters with 1.0 nm in diameter for coverage up to 0.12 ML. Such Ce clusters preferentially nucleate at the centre of the faulted-half unit cells, leading to the 'dark sites' of Si centre adatoms from the surrounding three unfaulted-half unit cells in filled-state images. Biasdependent STM images show the charge transfer from the neighbouring Si adatoms to Ce clusters. Low-temperature STS of the Ce clusters reveals that there is a band gap on the Ce cluster and the large voltage threshold is about 0.9 V.
基金Natural Science Foundation of Shanxi Province(No. 2009011014)
文摘The adsorption of CH3CN and CH3NC on the Pt(111)surface at the 1/4 monolayer(ML)coverage has been carried out at the level of density functional theory for understanding hydrogenation processes of nitriles.The most favored adsorption structure for CH3CN is the C-N bond almost parallel to the surface with the C-N bond interaction with adjacent surface Pt atoms.For CH3NC,the most stable configuration is the CH3NC locates at the face center cubic(fcc)site with the C-atom bonded to three Pt atoms.In addition,the HCN and HNC adsorption has been computed,and the adsorption pattern is nearly similar to the CH3CN and CH3NC,respectively.The adsorbed molecules rehybridize on the surface,becoming non-linear with a bent C-C-N or C-N-C angle.Furthermore,the binding mechanism of these molecules on the Pt(111)surface is also analyzed.
基金supported by the National Natural Science Foundation of China(21203027,21373048,21371034)Scientific Development Fund of Fuzhou University(2012-XQ-11)
文摘We applied periodic density-functional theory to investigate the adsorption of HCN on x Ni@Pt(111) bimetallic surfaces(x = 1~4). The results have been compared with those obtained on pure Ni(111) and Pt(111) surfaces. For all bimetallic surfaces,HCN is preferentially tilted with the CN bond parallel to the surface,and adsorption energies increase with an increasing number of layer Ni atoms on the surface. The adsorption energies of HCN on all bimetallic surfaces are larger than that on the Pt(111) surface,whereas the adsorption energies of HCN on 3Ni@Pt(111) and 4Ni@Pt(111) are larger than that on the Ni(111) surface,indicating that the introduction of Ni to the Pt catalyst could increase the activity of bimetallic catalyst in the hydrogenation reaction for nitriles. Larger adsorption energy of HCN leads to a longer C–N bond length and a smaller CN vibrational frequency. The analysis of Bader charge and vibrational frequencies showed obvious weakening of the adsorbed C–N bond and an indication of sp2 hybridization of both carbon and nitrogen atoms.
文摘Surface preparation is potentially important to the corrosion and biomedical properties of NiTi shape memory alloys. The effect of surface preparation on corrosion properties and nickel release of a Ti-56 wt.%Ni alloy has been studied. Surface of the NiTi coupons were prepared by four methods, namely, chemical etching, electropolishing, mechanical polishing and oxidizing, and then examined by corrosion test system. Furthermore, the Ni ion releases from NiTi samples with different surface preparations dipped in 1% HCl solution were analysed. Compared with the surface after chemical treatment, mechanical polishing and thermal oxidation, electropolished surface has better corrosion resistance and less nickel release for not only its lower surface roughness, but also the composition and property of its surface film.
文摘Adsorption of CH3O at four sites (top, bridge, hcp, fcc) on Au(111) surface has been investigated by density functional theory method at the generalized gradient approximation level. We have performed calculations on adsorption energies, structures, Mulliken charges and vibrational frequencies of CH3O on Au(111) surface with full-geometry optimization. The predicted results are compared with the available experimental observation. The calculated CH3O adsorption structure and stretching vibrational frequencies agree well with experimental ones, and precise determinations of adsorption sites are carded out. The most favorite adsorption on Au(111) occurs at the bridge site, and O-C axis is tilted to the surface. However, on hollow sites (hcp, fcc) the species is adsorbed in an upright geometry (pseudo-C3v local symmetry).
基金Supported by the National Natural Science Foundation of China (No 20273013)the Important Special Foundation of Fujian Province (No 2005HZ01-2-6)the Natural Education Department Foundation of PhD Unit (No 20050386003)
文摘Thiophene adsorption on the(111) surfaces of Pd and Pt have been investigated by density functional theory.The results indicate that the adsorption at the hollow sites is the most stable.To our interest,the molecular plane of thiophene ring is distorted with C=C bond being elongated to 1.450 and C–C bond being shortened to 1.347 ,and the C–H bonds tilt 13.91~44.05o away from this plane.Furthermore,analysis on population and density of states verified the calculated adsorption geometries.Finally,charge analysis suggests that thiophene molecule is an electron acceptor,reflecting the interaction between the lone pair of sulfur and the d-orbitals of metal.
基金Funded by"Xi-Bu-Zhi-Guang" Foundation of Chinese Academy of Sciences(No.XBZG-2007-5)Gansu Natural Science Foundation of China(No.0806RJYA004)Outstanding Youngth of Lanzhou University of Technology (No.Q200910)
文摘The surface infiltrated composite (Ni/WC) layers on gray iron substrate were fabricated through a vacuum infiltration casting technique (VICT) using Ni-based composite powder with different WC particles content as raw materials.The microstructures of surface infiltrated composite layer,the interface structures between surface composite layer and the substrate,the changes of macro-hardness with the increasing of WC content and the micro-hardness distribution are investigated.The infiltrated composite layer includes a surface composite layer and a transition layer,and the thickness of the transition layer decreases with the increasing content of WC.The thickness of transition layer with 20%WC content in the surface infiltrated composite layer was 170 μm which was the thickest for all transition layers with different WC content.The surface composite layer was mainly composed of WC,W2C,FeB and NiB,along with Ni-Cr-Fe,Ni (Cr) solid solution,Ni (Si) solid solution and Ni (Fe) solid solution.The transition layer was composed of Ni (Cr) solid solution,Ni (Fe) solid solution,Ni (Si) solid solution,Fe (Ni) solid solution and eutectic.The surface macro-hardness and micro-hardness of the infiltrated layer had been evaluated.The macro-hardness of the surface composite layer decreases with the WC content increasing,and the average macro-hardness is HRC60.The distribution of micro-hardness presents gradient change.The average micro-hardness of the infiltrated layer is about HV1000.
基金supported by the National Natural Science Foundation of China (Grant No.50705038,50735001 and 10804037)the Foundation of Jiangsu Province (Grant No.06-D-023,BK2007512 and BG2007033)+2 种基金The 8th Student Research Train Program of Jiangsu University (Grant No.08A172)the Innovation Program of Graduated Student of Jiangsu Province (Grant No.XM2006-45)the Open Foundation of Jiangsu Key Laboratory of Advanced Numerical Control Technology (Grant No.KXJ07126)
文摘Laser multiple processing, i.e. laser surface texturing and then Laser Shock Processing (LSP), is a new surface processing technology for the preparation of bionic non-smooth surfaces. Based on engineering bionics, samples of bionic non-smooth surfaces of stainless steel 0Crl 8Ni9 were manufactured in the form of reseau structure by laser multiple processing. The mechanical properties (including microhardness, residual stress, surface roughness) and microstructure of the samples treated by laser multiple processing were compared with those of the samples without LSP The results show that the mechanical properties of these samples by laser multiple processing were clearly improved in comparison with those of the samples without LSP The mechanisms underlying the improved surface microhardness and surface residual stress were analyzed, and the relations between hardness, comnressive residual stress and roughness were also presented.
文摘The density functional theory(DFT) and self-consistent periodic calculation were used to investigate the methanol adsorption on the Pt-Mo(111)/C surface.The adsorption energies,equilibrium geometries and vibration frequencies of CH3OH on nine types of sites on the Pt-Mo(111)/C surface were predicted and the favorite adsorption site for methanol is the top-Pt site.Both sites of valence and conduction bands of doped system have been broadened,which are favorable for electrons to transfer to the cavity.The possible decomposition pathway was investigated with transition state searching and the calculation results indicate that the O-H bond is first broken,and then the methanol decomposes into methoxy.The activation barrier of O-H bond breaking with Pt-Mo catalyst is only 104.8 kJ mol-1,showing that carbon supported Pt-Mo alloys have promoted the decomposition of methanol.Comparing with the adsorption energies of CH3OH on the Pt(111)/C surface and that of CO,the adsorption energies of CO are higher,and Pt(111)/C is liable to be oxidized and loses the activity,which suggests that the catalyst Pt-Mo(111)/C is in favor of decomposing methanol and has better anti-poisoning ability than Pt(111)/C.
基金supported by the National Key R&D Program of China (Grant No. 2019YFA0606701)the Guangdong Major Project of Basic and Applied Basic Research (Grant No. 2020B0301030004)。
文摘This study assesses the reproducibility of 31 historical simulations from 1850 to 2014 in the Coupled Model Intercomparison Project phase 6(CMIP6) for the subsurface(Sub-IOD) and surface Indian Ocean Dipole(IOD) and their association with El Ni?o-Southern Oscillation(ENSO). Most CMIP6 models can reproduce the leading east-west dipole oscillation mode of heat content anomalies in the tropical Indian Ocean(TIO) but largely overestimate the amplitude and the dominant period of the Sub-IOD. Associated with the much steeper west-to-east thermocline tilt of the TIO, the vertical coupling between the Sub-IOD and IOD is overly strong in most CMIP6 models compared to that in the Ocean Reanalysis System 4(ORAS4). Related to this, most models also show a much tighter association of Sub-IOD and IOD events with the canonical ENSO than observations. This explains the more(less) regular Sub-IOD and IOD events in autumn in those models with stronger(weaker) surface-subsurface coupling in TIO. Though all model simulations feature a consistently low bias regarding the percentage of the winter–spring Sub-IOD events co-occurring with a Central Pacific(CP) ENSO, the linkage between a westward-centered CP-ENSO and the Sub-IOD that occurs in winter–spring, independent of the IOD, is well reproduced.
文摘Haiyang-2A(HY-2A) is China's first ocean dynamic environment satellite and the radar altimeter is one of its main payloads. One of the main purposes of the radar altimeter is to measure the sea surface height(SSH). The SSH determined from the altimeter range measurements includes some range and geophysical corrections. These corrections largely affect the accuracy of the SSH measurements. The range and the geophysical corrections are reprocessed and the altimeter waveforms in HY-2A sensor interim geophysical data set records(S-IGDR) are retracked from June 1, 2014 to June 14, 2014, and the accuracy of the reprocessed SSH measurements is evaluated.The methods of the range and geophysical corrections used to reprocess HY-2A altimeter data are validated by using these methods to reprocess the Jason-2 range and geophysical corrections and comparing the results with the range and geophysical corrections in Jason-2 geophysical dataset records(GDR) product. A crossover analysis is used to evaluate the accuracy of the reprocessed HY-2A SSH measurements. The standard deviation(STD) of the crossover SSH differences for HY-2A is around 4.53 cm while the STD of the SSH differences between HY-2A and Jason-2 is around 5.22 cm. The performance of the reprocessed HY-2A SSH measurements is significantly improved with respect to the SSH measurements derived from HY-2A interim geophysical dataset records(IGDR)product. The 2015–2016 El Ni?o has been the strongest El Ni?o event since 1997–1998. The range and the geophysical corrections in HY-2A IGDR are reprocessed and sea level anomalies are used to monitor the2015–2016 El Ni?o. The results show that the HY-2A altimeter can well observe the 2015–2016 El Ni?o.
文摘This paper describes the electroless Ni or Cu plating of some fiuoropolymer substrates through a tin-free activation process. Materials subjected to surface metallization are commercial Teflon() FEP, Nafion(), ACLAR() and LaRCTM-CP1 thin films which have recently gained a large scientific and technological interest due to their excellent thermal, chemical, mechanical and dielectric properties. The original approach implemented in the present work involves: (i)the grafting of nitrogen-containing functionalities on the polymer surfaces through plasma treatments in ammonia, (ii) the direct catalysis of the so-modified surfaces via their immersion in a simple acidic PdCl2 solution (i.e. without using a prior surface sensitization in an acidic SnCl2 solution), and finally (iii) the electroless metallization itself. However, prior to the immersion in the industrial plating baths, the chemical reduction of the Pd+2 species (species covalently tethered on the nitrogen-containing groups) to metallic palladium (PdO) is shown to be a key factor in catalyzing the electroless deposition initiation. This is made by immersion in an hypophosphite (H2PO2-) solution. Wettability measurements and X-ray photoelectron spectroscopy (XPS) experiments are used to characterize every surface modification step of the developed process. A cross-hatch tape test was used to asses the adhesion strength of the electroless films that is shown qualitatively good. In addition, a fragmentation test was developed in combination with electrical measurements. Its use allows to distinguish different adhesion levels at the metal/polymer interface and to evidence the influence of some processing parameters.