The unique chemistry of hydrogen beneath the surface: Catalytic hydrogenation of hydrocarbons

被引:123
作者
Ceyer, ST [1 ]
机构
[1] MIT, Dept Chem, Cambridge, MA 02139 USA
关键词
D O I
10.1021/ar970030f
中图分类号
O6 [化学];
学科分类号
0703 ;
摘要
Hydrogen atoms emerging from the bulk of Ni metal to the surface are observed to be the reactive species in the hydrogenation of adsorbed methyl radical, ethylene, and acetylene to gas-phase products. Surface-bound H atoms are unreactive. The distinctive chemistry of a bulk H atom arises largely from its significantly higher energy as compared to that of a surface-bound H atom. These results demonstrate that bulk H is not solely a source of surface-bound H in catalytic hydrogenation as proposed 50 years ago, but rather, a reactant with a chemistry of its own.
引用
收藏
页码:737 / 744
页数:8
相关论文
共 56 条
[1]   Collision induced desorption and dissociation of O2 on Pt(111) [J].
Åkerlund, C ;
Zoric, I ;
Kasemo, B .
JOURNAL OF CHEMICAL PHYSICS, 1998, 109 (02) :737-745
[2]  
ALEFELD G, 1978, HYDROGEN METALS 1 2
[3]   The role of bulk H and C species in the chain lengthening of Fischer-Tropsch synthesis over nickel [J].
Barbier, A ;
Pereira, EB ;
Martin, GA .
CATALYSIS LETTERS, 1997, 45 (3-4) :221-226
[4]   OBSERVATION AND MECHANISM OF COLLISION-INDUCED DESORPTION - CH4 ON NI(111) [J].
BECKERLE, JD ;
JOHNSON, AD ;
CEYER, ST .
PHYSICAL REVIEW LETTERS, 1989, 62 (06) :685-688
[5]   COLLISION-INDUCED DESORPTION OF PHYSISORBED CH4 FROM NI(111) - EXPERIMENTS AND SIMULATIONS [J].
BECKERLE, JD ;
JOHNSON, AD ;
CEYER, ST .
JOURNAL OF CHEMICAL PHYSICS, 1990, 93 (06) :4047-4065
[6]   COLLISION-INDUCED DISSOCIATIVE CHEMISORPTION OF CH4 ON NI(111) BY INERT-GAS ATOMS - THE MECHANISM FOR CHEMISTRY WITH A HAMMER [J].
BECKERLE, JD ;
JOHNSON, AD ;
YANG, QY ;
CEYER, ST .
JOURNAL OF CHEMICAL PHYSICS, 1989, 91 (09) :5756-5777
[7]   KINETICS OF THE ACTIVATED DISSOCIATIVE ADSORPTION OF METHANE ON THE LOW INDEX PLANES OF NICKEL SINGLE-CRYSTAL SURFACES [J].
BEEBE, TP ;
GOODMAN, DW ;
KAY, BD ;
YATES, JT .
JOURNAL OF CHEMICAL PHYSICS, 1987, 87 (04) :2305-2315
[8]   Synthesis and spectroscopic identification of ethylidyne adsorbed on Ni(111) [J].
Bürgi, T ;
Trautman, TR ;
Haug, KL ;
Utz, AL ;
Ceyer, ST .
JOURNAL OF PHYSICAL CHEMISTRY B, 1998, 102 (25) :4952-4965
[9]   EFFECT OF TRANSLATIONAL AND VIBRATIONAL-ENERGY ON ADSORPTION - THE DYNAMICS OF MOLECULAR AND DISSOCIATIVE CHEMISORPTION [J].
CEYER, ST ;
BECKERLE, JD ;
LEE, MB ;
TANG, SL ;
YANG, QY ;
HINES, MA .
JOURNAL OF VACUUM SCIENCE & TECHNOLOGY A-VACUUM SURFACES AND FILMS, 1987, 5 (04) :501-507
[10]   NEW MECHANISMS FOR CHEMISTRY AT SURFACES [J].
CEYER, ST .
SCIENCE, 1990, 249 (4965) :133-139