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贵金属原子在CeO2(111)表面吸附的密度泛函理论研究

袁金焕,  滕波涛,  赵越,  赵云,  罗孟飞

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文章导航 > 燃料化学学报（中英文）  > 2012 >  40(01): 124-128
袁金焕, 滕波涛, 赵越, 赵云, 罗孟飞. 贵金属原子在CeO2(111)表面吸附的密度泛函理论研究[J]. 燃料化学学报（中英文）, 2012, 40(01): 124-128.
引用本文: 袁金焕, 滕波涛, 赵越, 赵云, 罗孟飞. 贵金属原子在CeO2(111)表面吸附的密度泛函理论研究[J]. 燃料化学学报（中英文）, 2012, 40(01): 124-128.
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YUAN Jin-huan, TENG Bo-tao, ZHAO Yue, ZHAO Yun, LUO Meng-fei. A density functional theory study of the noble metal adsorption on the CeO2(111) surface[J]. Journal of Fuel Chemistry and Technology, 2012, 40(01): 124-128.
Citation: YUAN Jin-huan, TENG Bo-tao, ZHAO Yue, ZHAO Yun, LUO Meng-fei. A density functional theory study of the noble metal adsorption on the CeO2(111) surface[J]. Journal of Fuel Chemistry and Technology, 2012, 40(01): 124-128.
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贵金属原子在CeO2(111)表面吸附的密度泛函理论研究

  • 浙江师范大学 化学与生命科学学院, 浙江 金华 321004

基金项目: 国家自然科学基金(20903081);浙江省自然科学基金(Y407163)。
详细信息
    通讯作者:

    滕波涛、罗孟飞, E-mail:tbt@zjnu.cn, mengfeiluo@zjnu.cn; Tel:86-579-82282234; Fax:+86-579-82282595。

  • 中图分类号: O643

A density functional theory study of the noble metal adsorption on the CeO2(111) surface

  • College of Chemistry and Life Sciences, Zhejiang Normal University, Jinhua 321004, China

    摘要
  • 摘要: 利用密度泛函理论系统研究了贵金属原子(Au、Pd、Pt和Rh)在CeO2(111)表面的吸附行为。结果表明,Au吸附在氧顶位最稳定,Pd、Pt倾向吸附于氧桥位,而Rh在洞位最稳定。当金属原子吸附在氧顶位时,吸附强度依次为Pt > Rh > Pd > Au。Pd、Pt与Rh吸附后在Ce 4f、O 2p电子峰间出现掺杂峰;Au未出现掺杂电子峰,其d电子峰与表面O 2p峰在-4～-1 eV重叠。态密度分析表明,Au吸附在氧顶位、Pd与Pt吸附在桥位、Rh吸附在洞位时,金属与CeO2(111)表面氧原子作用较强,这与Bader电荷分析结果相一致。
    Abstract: Adsorption behaviors of four typical noble metals (Au, Pd, Pt, and Rh) on the CeO2(111) surface were systematically investigated by using density functional theory method. The results indicated that Au prefers to be adsorbed on the atop site, while Pd and Pt on the O-bridge site. Rh adsorbed on the 3-fold hollow site is the most stable configurations. When the noble metals are adsorbed on the atop site, the adsorption strength is in the order of Pt > Rh > Pd > Au. New electronic peaks are present between the Ce 4f and O 2p peaks when Pd, Pt, and Rh atoms are adsorbed on the CeO2(111) surface, while no peak is found for the adsorption of Au; the d electronic peak of Au overlaps with the O 2p peaks at-4 to-1 eV. According to the density of states (DOS) analysis, when Au is adsorbed on the atop site, Pd and Pt on the bridge site, and Rh on the 3-fold hollow site, their interactions with surface oxygen atoms on the CeO2(111) surface are stronger than other configurations, which is in good agreement with the results of Bader charge population.
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    • 参考文献(26)
  • TROVARELLI A. Catalytic properties of ceria and CeO2-containing materials[J]. Catal Rev Sci Eng, 1996, 38(4):439-509.
    MONTE R D, KASPAR J. On the role of oxygen storage in three-way catalysis[J]. Top Catal, 2004, 28(1/4):47-57.
    ZHOU H-P, WU H-S, SHEN J, YIN A-X, SUN L-D, YAN C-H. Thermally stable Pt/CeO2 hetero-nanocomposites with high catalytic activity[J]. J Am Chem Soc, 2010, 132(14):4998-4999.
    ETSELL T H, FLENGAS S N. The electrical properties of solid oxide electrolytes[J]. Chem Rev, 1970, 70(3):339-376.
    KASïPAR J, FORNASIERO P, GRAZIANI M. Use of CeO2-based oxides in the three-way catalysis[J]. Catal Today, 1999, 50(2):285-298.
    YEE A, MORRISON S J, IDRISS H. A study of the reactions of ethanol on CeO2 and Pd/CeO2 by steady state reactions, temperature programmed desorption, and in situ FT-IR[J]. J Catal, 1999, 168(2):279-295.
    YEE A, MORRISON S J, IDRISS H. A study of ethanol reactions over Pt/CeO2 by temperature-programmed desorption and in situ FT-IR spectroscopy:Evidence of benzene formation[J]. J Catal, 2000, 191(1):30-45.
    YEE A, MORRISON S J, IDRISS H. The reactions of ethanol over M/CeO2 catalysts:Evidence of carbon-carbon bond dissociation at low temperatures over Rh/CeO2[J] Catal Today, 2000, 63(2/4):327-335.
    FU Q, SALTSBURG H, FLYTZANI-STEPHANOPOULOS M. Active nonmetallic Au and Pt species on ceria-based water-gas shift catalysts[J] Science, 2003, 301(5635):935-938.
    TABAKOVAT T, BOCCUZZI F, MANZOLI M, ANDREEVA D. FTIR study of low-temperature water-gas shift reaction on gold/ceria catalyst[J] Appl Catal A, 2003, 252(2):385-397.
    滕波涛, 蒋仕宇, 赵雷洪, 罗孟飞. 铈基催化剂的密度泛函理论研究进展[J]. 中国稀土学报, 2010, 28(2):129-140. (TENG Bo-tao, JIANG Shi-yu, ZHAO Lei-hong, LUO Meng-fei. Density functional theory of ceria-based catalyst[J]. Journal of the Chinese Rare Earth Society, 2010, 28(2):129-140.)
    (a) YANG Z X, LU Z S, LUO G X, HERMANSSON K. Oxygen vacancy formation energy at the Pd/CeO2(111) interface[J]. Phy Lett A, 2007, 369 (1/2):132-139; (b) 路战胜, 罗改霞, 杨宗献. Pd与CeO2(111)面的相互作用的第一性原理研究[J]. 物理学报, 2007, 56(9):5382-5388. (LU Zhan-sheng, LUO Gai-xia, YANG Zong-xian. The interaction between Pd and CeO2 (111) surface:A first principle study[J]. Acta Phys Sinica, 2007, 56(9):5382-5388.)
    YANG Z, LU Z, LUO G. First-principles study of the Pt/CeO2(111) interface[J]. Phys Rev B, 2007, 76(7):075421.
    CHEN Y, HU P, LEE M-H, WANG H-F. Au on (111) and (110) surfaces of CeO2:A density functional theory study[J]. Surf Sci, 2008, 602(10):1736-1741.
    (a) KRESSE G, HAFNER J. Ab initio molecular-dynamics simulation of the liquid-metal-amorphous-semiconductor transition in germanium[J]. Phys Rev B, 1994, 49(20):14251-14269; (b) KRESSE G, FURTHMIILLER J. Efficiency of ab-initio total energy calculations for metals and semiconductors using a plane-wave basis set[J]. Comput Mater Sci, 1996, 6 (1):15-50.
    PERDEW J P, BURKE K, ERNZERHOF M. Generalized gradient approximation made simple[J]. Phys Rev Lett, 1996, 77(18):3865-3868.
    KRESSE G, JOUBERT D. From ultrasoft pseudopotentials to the projector augmented-wave method[J]. Phys Rev B, 1999, 59(3):1758-1775.
    MONKHORST H J, PACK J D. Special points for Brillouin-zone integrations[J]. Phys Rev B, 1976, 13(12):5188-5192.
    FABRIS S, de GIRONCOLI S, BARONI S, VICARIO G, BALDUCCI G. Taming multiple valency with density functionals:A case study of defective ceria[J]. Phys Rev B, 2005, 71(4):041102.
    NOLAN M, GRIGOLEIT S, SAYLE D C, PARKER S C, WATSON G W. Density functional theory studies of the structure and electronic structure of pure and defective low index surfaces of ceria[J]. Surf Sci, 2005, 576(1/3):217-229.
    KÜVMMERLE E A, HEGER G. The structures of C-Ce2O3+δ, Ce7O12, and Ce11O20[J]. J Solid State Chem, 1999, 147(2):485-500.
    蒋仕宇, 滕波涛, 鲁继青, 刘雪松, 杨培芳, 杨飞勇, 罗孟飞. 甲醛在CeO2(111)表面吸附的密度泛函理论研究[J]. 物理化学学报,2008, 24(11):2025-2031. (JIANG Shi-yu, TENG Bo-tao, LU Ji-qing, LIU Xue-song, YANG Pei-fang, YANG Fei-yong, LUO Meng-fei. A density functional theory study of formaldehyde adsorption on CeO2(111) surface[J]. Acta Phys Chim Sinica, 2008, 24(11):2025-2031.)
    TENG B-T, JIANG S-Y, YANG Z-X, LUO M-F, LAN Y-Z. A density functional theory study of formaldehyde adsorption[J]. Surf Sci, 2010, 604(1):68-78.
    HERNÀNDEZ N C, GRAU-CRESPO R, de LEEUW N H, SANZ J F. Electronic charge transfer between ceria surfaces and gold adatoms:A GGA+U investigation[J]. Phys Chem Chem Phys, 2009, 11(26):5246-5252.
    JUNG C, ISHIMOTO R, TSUBOI H, KOYAMA M, ENDOU A, KUBO M, del CARPIO C A, MIYAMOTO A. Interfacial properties of ZrO2 supported precious metal catalysts:A density functional study[J]. Appl Catal A, 2006, 305(1):102-109.
    BRANDA M M,HERNÀNDEZ N C, SANZ J F, ILLAS F. Density functional theory study of the interaction of Cu, Ag, and Au atoms with the regular CeO2 (111) surface[J]. J Phys Chem C, 2010, 114(4):1934-1941.
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出版历程
  • 收稿日期:  2011-02-13
  • 修回日期:  2011-05-26
  • 刊出日期:  2012-01-31

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