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The TiC(111) surface has been studied with synchrotron-based, angle-resolved photoemission spectroscopy, where the results showed the surface to be polar with the Ti layer on top

Surface chemistry of transition metal carbides.

CHEMICAL REVIEWS, no. 1.0 (2005): 185-212

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186 Chemical Reviews, 2005, Vol. 105, No. 1 properties.[<a class="ref-link" id="c1" href="#r1">1</a>,<a class="ref-link" id="c2" href="#r2">2</a>,<a class="ref-link" id="c3" href="#r3">3</a>,<a class="ref-link" id="c4" href="#r4">4</a>,<a class="ref-link" id="c5" href="#r5">5</a>,<a class="ref-link" id="c6" href="#r6">6</a>] For example, ...更多

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简介
  • 186 Chemical Reviews, 2005, Vol 105, No 1 properties.[1,2,3,4,5,6] For example, TMC compounds combine the physical properties of three different classes of materials: covalent solids, ionic crystals, and transition metals.
  • Oxidation at 1300 K resulted in the formation of a thin WOx surface layer.[89] Synchrotron-based CLPES investigations by Johansson and co-workers showed the W 4f components to be shifted and strongly attenuated upon relatively high oxygen exposures.[90] HREELS and UPS studies following room-temperature exposure of oxygen on WC(101h0) were consistent with molecular adsorption; the O-O bond order was considerably reduced to a value between 1.05 and 1.25.91
重点内容
  • 186 Chemical Reviews, 2005, Vol 105, No 1 properties.[1,2,3,4,5,6] For example, TMC compounds combine the physical properties of three different classes of materials: covalent solids, ionic crystals, and transition metals
  • Ever since the landmark paper by Levy and Boudart regarding the Pt-like properties of tungsten carbides,[7] the catalytic properties of TMCs have been the subject of many investigations in the fields of catalysis and surface science
  • In reactions involving the transformation of C-H bonds of hydrocarbons, such as dehydrogenation, hydrogenation, and hydrogenolysis, the catalytic performances of TMCs are approaching or surpassing those of Pt-group metals.[2,5,6]
  • Johansson reviewed the electronic properties of bulk single-crystal TMCs in 1995.12 The chemical and catalytic properties of powder and supported TMC catalysts were reviewed by Oyama in 1996.5 The preparation, characterization, and reactivities of TMC surfaces were reviewed by Chen in 1996.6 The characterization of the local structural and electronic properties of single-crystal and polycrystalline TMCs was reviewed by Chen in 1997.13
  • The TiC(111) surface has been studied with synchrotron-based, angle-resolved photoemission spectroscopy (ARPES), where the results showed the surface to be polar with the Ti layer on top.[21]
  • Additional atomic force microscopy (AFM) studies of ethanol adsorbed on VC(100) showed approximately 40% reduction in the frictional forces when compared to the case of the unmodified VC(100) surface.[194]
  • high-resolution electron energy loss spectroscopy (HREELS) and ultraviolet photoelectron spectroscopy (UPS) studies following room-temperature exposure of oxygen on WC(101h0) were consistent with molecular adsorption; the O-O bond order was considerably reduced to a value between 1.05 and 1.25.91
结果
  • Previous theoretical studies by Jansen and Hoffmann revealed a significant reduction in the ability of the TiC(100) substrate to donate electrons into the 2π* antibonding orbitals of CO when compared with that of Ti(0001).[20] Experimentally, the adsorption of CO on TiC(100) was studied by Didziulis et al using TPD, HREELS, UPS, and XPS.[99] The authors observed that a majority of the CO bonded weakly to
  • On both W(211) and C/W(211), acetylene decomposed to surface carbon and gas-phase hydrogen.[130] TPD results showed that, upon carbide modification, the hydrogen desorption feature shifted to higher temperatures and broadened significantly.
  • Additional vibrational spectra obtained for CH2I2 and C2H5I on the Mo2C/Mo(111) surface were consistent with the presence of di-σ bonded ethylene at low temperatures and ethylidyne at higher temperatures.[137] Lastly, TPD results following the reaction of CH3I on Mo2C/Mo(111) showed that methane, ethylene, and hydrogen were the gas-phase products.[136]
  • On Pt(111), the only desorption products detected following the reaction of cyclohexene adsorption were H2 and benzene.[148,149] Vibrational studies have revealed that adsorbed cyclohexene molecules were completely converted to adsorbed benzene on Pt(111) at 300 K.148-150 the selectivity for converting cyclohexene to surface benzene was nearly 100% at 300 K, a significant fraction of surface benzene underwent subsequent thermal dissociation instead of desorbing to the gas-phase.
结论
  • The values presented in Table 5 were derived by first correlating the carbon signal from AES to the hydrogen desorption peak area from TPD on the clean metal surfaces, on which only the complete decomposition of cyclohexene was observed (m‚c-C6H10 f 6m‚C + 5m‚H2).
  • Several research groups have reported that the catalytic properties of powder carbides can be significantly modified by the presence of oxygen.[158,159,160,161] As discussed earlier, the adsorption of oxygen on C/Mo(110) at 600 and 900 K led to oxygen residing in different bonding environments,[55] which was confirmed in the dissociation of oxygen on C/W(111) at 600 and 900 K.95 Correspondingly, thermal desorption studies following cyclohexene adsorption on the 600 K O/C/Mo(110) and O/C/W(111) surfaces showed only reversible molecular desorption.
总结
  • 186 Chemical Reviews, 2005, Vol 105, No 1 properties.[1,2,3,4,5,6] For example, TMC compounds combine the physical properties of three different classes of materials: covalent solids, ionic crystals, and transition metals.
  • Oxidation at 1300 K resulted in the formation of a thin WOx surface layer.[89] Synchrotron-based CLPES investigations by Johansson and co-workers showed the W 4f components to be shifted and strongly attenuated upon relatively high oxygen exposures.[90] HREELS and UPS studies following room-temperature exposure of oxygen on WC(101h0) were consistent with molecular adsorption; the O-O bond order was considerably reduced to a value between 1.05 and 1.25.91
  • Previous theoretical studies by Jansen and Hoffmann revealed a significant reduction in the ability of the TiC(100) substrate to donate electrons into the 2π* antibonding orbitals of CO when compared with that of Ti(0001).[20] Experimentally, the adsorption of CO on TiC(100) was studied by Didziulis et al using TPD, HREELS, UPS, and XPS.[99] The authors observed that a majority of the CO bonded weakly to
  • On both W(211) and C/W(211), acetylene decomposed to surface carbon and gas-phase hydrogen.[130] TPD results showed that, upon carbide modification, the hydrogen desorption feature shifted to higher temperatures and broadened significantly.
  • Additional vibrational spectra obtained for CH2I2 and C2H5I on the Mo2C/Mo(111) surface were consistent with the presence of di-σ bonded ethylene at low temperatures and ethylidyne at higher temperatures.[137] Lastly, TPD results following the reaction of CH3I on Mo2C/Mo(111) showed that methane, ethylene, and hydrogen were the gas-phase products.[136]
  • On Pt(111), the only desorption products detected following the reaction of cyclohexene adsorption were H2 and benzene.[148,149] Vibrational studies have revealed that adsorbed cyclohexene molecules were completely converted to adsorbed benzene on Pt(111) at 300 K.148-150 the selectivity for converting cyclohexene to surface benzene was nearly 100% at 300 K, a significant fraction of surface benzene underwent subsequent thermal dissociation instead of desorbing to the gas-phase.
  • The values presented in Table 5 were derived by first correlating the carbon signal from AES to the hydrogen desorption peak area from TPD on the clean metal surfaces, on which only the complete decomposition of cyclohexene was observed (m‚c-C6H10 f 6m‚C + 5m‚H2).
  • Several research groups have reported that the catalytic properties of powder carbides can be significantly modified by the presence of oxygen.[158,159,160,161] As discussed earlier, the adsorption of oxygen on C/Mo(110) at 600 and 900 K led to oxygen residing in different bonding environments,[55] which was confirmed in the dissociation of oxygen on C/W(111) at 600 and 900 K.95 Correspondingly, thermal desorption studies following cyclohexene adsorption on the 600 K O/C/Mo(110) and O/C/W(111) surfaces showed only reversible molecular desorption.
表格
  • Table1: Characterization of TMC Surfaces techniques
  • Table2: Summary of Surface Chemistry on TMC Surfaces surface molecule(s)
  • Table3: Comparison of CO Desorption Temperature from Carbide- and Oxycarbide-Modified Mo(110), W(110), and W(111), Pt, and Ru surface
  • Table4: Vibrational Frequencies of Ethylidyne on C/V(110), C/Mo(110), C/Ti(0001), C/W(110), and Pt(111)
  • Table5: Benzene Selectivity from C/Ti(0001), C/Mo(110), C/W(111), and Corresponding Oxycarbide Surfaces surface
  • Table6: Comparison of Activity and Selectivity of CH3OH on C/Ti(0001), C/V(110), C/Mo(110), C/W(111), and C/W(110)
Download tables as Excel
基金
  • We acknowledge financial support from Basic Energy Sciences of the Department of Energy (DOE/ BES Grant No DE-FG02-04ER15501)
  • H.H.H. acknowledges financial support from the Presidential Fellowship at the University of Delaware
研究对象与分析
pairs: 6
First principles calculations on TiC(001) showed that the surface C atoms moved slightly outward and Ti atoms inward,[39,42] consistent with experimental observation for the TiC(100) surface.18,19. Rodriguez and co-workers recently determined that the structure of the T8C12 “metcar” consisted of metal atoms occupying the low-coordination inner positions and highcoordination outer positions, as well as the presence of six pairs of short C-C bonds. The presence of the C2 groups increased the stability of the “metcar” T8C12 structure

adsorbed species: 3
Perry and co-workers observed four molecular desorption states of deuterated water at 188, 233, 263, and 308 K on TiC(100) at saturation exposure.179. XPS studies showed the formation of three adsorbed species at low temperatures: atomic O, partially dissociated hydroxyl groups, and molecular water.178. Heating the surface resulted in the desorption of D2, CO, and CO2 species

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