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
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
Graphene with a Dirac cone-like electronic structure has been extensively studied because of its novel transport properties and potential application for future electronic devices.For epitaxially grown graphene,the pr...Graphene with a Dirac cone-like electronic structure has been extensively studied because of its novel transport properties and potential application for future electronic devices.For epitaxially grown graphene,the process conditions and the microstructures are strongly dependent on various substrate materials with different lattice constants and interface energies.Utilizing angle-resolved photoemission spectroscopy,here we report an investigation of the electronic structure of single-crystalline graphene grown on Cu/Ni(111)alloy film by chemical vapor deposition.With a relatively low growth temperature,graphene on Cu/Ni(111)exhibits a Dirac cone-like dispersion comparable to that of graphene grown on Cu(111).The linear dispersions forming Dirac cone are as wide as 2 e V,with the Fermi velocity of approximately 1.1×10^6 m/s.Dirac cone opens a gap of approximately 152 meV at the binding energy of approximately 304 meV.Our findings would promote the study of engineering of graphene on different substrate materials.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
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
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.
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Project supported by the National Natural Science Foundation of China(Grant Nos.51772317,11604356,and 11704394)
文摘Graphene with a Dirac cone-like electronic structure has been extensively studied because of its novel transport properties and potential application for future electronic devices.For epitaxially grown graphene,the process conditions and the microstructures are strongly dependent on various substrate materials with different lattice constants and interface energies.Utilizing angle-resolved photoemission spectroscopy,here we report an investigation of the electronic structure of single-crystalline graphene grown on Cu/Ni(111)alloy film by chemical vapor deposition.With a relatively low growth temperature,graphene on Cu/Ni(111)exhibits a Dirac cone-like dispersion comparable to that of graphene grown on Cu(111).The linear dispersions forming Dirac cone are as wide as 2 e V,with the Fermi velocity of approximately 1.1×10^6 m/s.Dirac cone opens a gap of approximately 152 meV at the binding energy of approximately 304 meV.Our findings would promote the study of engineering of graphene on different substrate materials.
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(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.
