Evidence for Ambient-Temperature Reversible Catalytic Hydrogenation in Pt-doped Carbons

被引：34

作者：

Liu, Xiao Ming ^{[1
]}

Tang, Youjian ^{[2
]}

Xu, En Shi ^{[2
]}

Fitzgibbons, Thomas C. ^{[3
]}

Larsen, Gregory S. ^{[1
]}

Gutierrez, Humberto R. ^{[2
]}

Tseng, Huan-Hsiung ^{[8
]}

Yu, Ming-Sheng ^{[8
]}

Tsao, Cheng-Si ^{[8
]}

Badding, John V. ^{[3
]}

Crespi, Vincent H. ^{[2
,4
,5
]}

Lueking, Angela D. ^{[1
,6
,7
]}

机构：

[1] Penn State Univ, Mat Res Lab, University Pk, PA 16802 USA

[2] Penn State Univ, Dept Phys, University Pk, PA 16802 USA

[3] Penn State Univ, Dept Chem, University Pk, PA 16802 USA

[4] Penn State Univ, Dept Mat Sci & Engn, University Pk, PA 16802 USA

[5] Penn State Univ, Mat Res Inst, University Pk, PA 16802 USA

[6] Penn State Univ, Dept Chem Engn, Dept Energy & Mineral Engn, University Pk, PA 16802 USA

[7] Penn State Univ, EMS Energy Inst, University Pk, PA 16802 USA

[8] Inst Nucl Energy Res, Tao Yuan 32546, Taiwan

来源：

NANO LETTERS | 2013年 / 13卷 / 01期

关键词：

Graphene; graphane; Pt nanoparticles; hydrogen; spillover; catalysis; SPILLOVER; ADSORPTION; SCATTERING; GRAPHITE; GRAPHENE; STORAGE; SURFACE;

D O I：

10.1021/nl303673z

中图分类号：

O6 [化学];

学科分类号：

0703 ;

摘要：

In situ high-pressure Raman spectroscopy, with corroborating density functional calculations, is used to probe C-H chemical bonds formed when dissociated hydrogen diffuses from a platinum nanocatalyst to three distinct graphenic surfaces. At ambient temperature, hydrogenation and dehydrogenation are reversible in the combined presence of an active catalyst and oxygen heteroatoms. Hydrogenation apparently occurs through surface diffusion in a chemisorbed state, while dehydrogenation requires diffusion of the chemisorbed species back to an active catalyst.

引用

页码：137 / 141

页数：5

共 25 条

[1] Hydrogen Spillover in Pt-Single-Walled Carbon Nanotube Composites: Formation of Stable C-H Bonds [J].

Bhowmick, Ranadeep ;

Rajasekaran, Srivats ;

Friebel, Daniel ;

Beasley, Cara ;

Jiao, Liying ;

Ogasawara, Hirohito ;

Dai, Hongjie ;

Clemens, Bruce ;

Nilsson, Anders .

JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 2011, 133 (14) :5580-5586

[2] SPECTROSCOPIC INVESTIGATION OF ELECTRONIC AND VIBRONIC PROPERTIES OF ION-BEAM-DEPOSITED AND THERMALLY TREATED ULTRATHIN C-H FILMS [J].

BIENER, J ;

SCHENK, A ;

WINTER, B ;

SCHUBERT, UA ;

LUTTERLOH, C ;

KUPPERS, J .

PHYSICAL REVIEW B, 1994, 49 (24) :17307-17318

[3] A new route towards uniformly functionalized single-layer graphene [J].

Boukhvalov, D. W. ;

Katsnelson, M. I. .

JOURNAL OF PHYSICS D-APPLIED PHYSICS, 2010, 43 (17)

[4] Hydrogen spillover in the context of hydrogen storage using solid-state materials [J].

Cheng, Hansong ;

Chen, Liang ;

Cooper, Alan C. ;

Sha, Xianwei ;

Pez, Guido P. .

ENERGY & ENVIRONMENTAL SCIENCE, 2008, 1 (03) :338-354

[5] PREPARATION OF PLATINUM SUPPORTED ON PREGRAPHITIZED CARBON-BLACKS [J].

COLOMA, F ;

SEPULVEDAESCRIBANO, A ;

FIERRO, JLG ;

RODRIGUEZREINOSO, F .

LANGMUIR, 1994, 10 (03) :750-755

[6] SPILLOVER IN HETEROGENEOUS CATALYSIS [J].

CONNER, WC ;

FALCONER, JL .

CHEMICAL REVIEWS, 1995, 95 (03) :759-788

[7] Detection of Hydrogen Spillover in Palladium-Modified Activated Carbon Fibers during Hydrogen Adsorption [J].

Contescu, Cristian I. ;

Brown, Craig M. ;

Liu, Yun ;

Bhat, Vinay V. ;

Gallego, Nidia C. .

JOURNAL OF PHYSICAL CHEMISTRY C, 2009, 113 (14) :5886-5890

[8] INFRARED-SPECTRA FOR CO ISOTOPES CHEMISORBED ON PT[111] - EVIDENCE FOR STRONG ABSORBATE COUPLING INTERACTIONS [J].

CROSSLEY, A ;

KING, DA .

SURFACE SCIENCE, 1977, 68 (01) :528-538

[9] Monitoring dopants by Raman scattering in an electrochemically top-gated graphene transistor [J].

Das, A. ;

Pisana, S. ;

Chakraborty, B. ;

Piscanec, S. ;

Saha, S. K. ;

Waghmare, U. V. ;

Novoselov, K. S. ;

Krishnamurthy, H. R. ;

Geim, A. K. ;

Ferrari, A. C. ;

Sood, A. K. .

NATURE NANOTECHNOLOGY, 2008, 3 (04) :210-215

[10] Control of Graphene's Properties by Reversible Hydrogenation: Evidence for Graphane [J].

Elias, D. C. ;

Nair, R. R. ;

Mohiuddin, T. M. G. ;

Morozov, S. V. ;

Blake, P. ;

Halsall, M. P. ;

Ferrari, A. C. ;

Boukhvalov, D. W. ;

Katsnelson, M. I. ;

Geim, A. K. ;

Novoselov, K. S. .

SCIENCE, 2009, 323 (5914) :610-613

← 1 2 3 →