• Title/Summary/Keyword: Adsorbed hydrogen

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Spontaneously Adsorbed Mo Layers on Pt(111) and Pt(100) Single Crystal Electrode Surfaces

  • Han, Yoon-gu;Jung, Chang-hoon;Rhee, Choong-Kyun
    • Bulletin of the Korean Chemical Society
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    • v.23 no.3
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    • pp.395-399
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    • 2002
  • The voltammetric behavior of spontaneously adsorbing Mo layers on Pt(111) and Pt(100) electrodes has been studied to estimate the number of electrons involved in the electrochemical processes of spontaneously adsorbed Mo and the number of the bloc ked Pt sites for hydrogen adsorption. On Pt(111) and Pt(100) surfaces, the spontaneously adsorbed Mo layers showed redox peaks at 0.10 V and 0.15 V, respectively, and continuous current-potential waves in the conventional hydrogen region. Since the potential range of the Mo redox processes on both surfaces overlapped partially with the potential range of hydrogen adsorption, the variation in the ratio of the total charge of Mo and H ($Q_H$ +$Q_{MO}$) to the hydrogen charge of clean Pt electrode ($Q_H^0$) was analyzed. From the analysis, six electrons were estimated to be involved in the electrochemical processes of the spontaneously adsorbed Mo, and four Pt sites for hydrogen adsorption were calculated to be blocked by one adsorbed Mo atom. Based on these figures and the pH dependence of the Mo redox processes, we have proposed an electrochemical equation for the spontaneously adsorbed Mo. This electrochemical equation led us to conclude that the saturation coverage of the spontaneously adsorbed Mo is 0.25. The coverage of Mo less than 0.25, however, could not be determined voltammetrically due to the convolution of the charges of Mo and H.

Sticking and Desorption of Atomic Hydrogen on the Armchair Edges of Bilayer Graphene

  • Natividad, Michelle;Arboleda Jr., Nelson;Kasai, Hideaki
    • Journal of Electrochemical Science and Technology
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    • v.7 no.3
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    • pp.185-189
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    • 2016
  • The coupled channel method via the Local Reflection (LORE) matrix is employed to investigate the quantum mechanical behavior of the sticking or adsorption and desorption of hydrogen (H) atom on bilayer graphene via the armchair edge. The sticking and desorption probabilities of H are calculated and are plotted against the initial translational energy of H. The sticking probability plot shows a barrierless reaction indicating that hydrogen is easily adsorbed on the armchair edge of graphene. The desorption probability plot, however, shows that desorption of H from the graphene sheets is an activated process with a barrier height of 4.19 eV suggesting that a strong bond exists between the adsorbed H atom and the edge carbon atom. Thus, temperatures higher than the operating temperatures (300 - 1500 K) of conventional fuel cells are necessary to release the adsorbed H atom from the armchair edge of graphene.

Hydrogenation of Phenylacetylene to Styrene on Pre-CxHy- and C-Covered Cu(111) Single Crystal Catalysts

  • Sohn, Young-Ku;Wei, Wei;White, John M.
    • Bulletin of the Korean Chemical Society
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    • v.32 no.5
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    • pp.1559-1563
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    • 2011
  • Thermal hydrogenation of phenylacetylene (PA, $C_8H_6$) to styrene ($C_8H_8$) on pre-$C_xH_y$- and C-covered Cu(111) single crystal substrates has been studied using temperature-programmed desorption (TPD) mass spectrometry. Chemisorbed PA with an acetylene group has been proved to be associated with hydrogen of pre-adsorbed $C_xH_y$ to form styrene (104 amu) on Cu surface. For the parent (PA) mass (102 amu) TPD profile, the TPD peaks at 360 K and 410 K are assigned to chemisorbed vertically aligned PA and flat-lying cross-bridged PA, respectively (J. Phys. Chem. C 2007, 111, 5101). The relative $I_{360K}/I_{410K}$ TPD ratio dramatically increases with increasing pre-adsorbed $C_xH_y$ before dosing PA, while the ratio does not increase for pre-C-covered surface. For PA on pre-$C_xH_y$-covered Cu(111) surface, styrene desorption is enhanced relative to the parent PA desorption, while styrene formation is dramatically quenched on pre-C-covered (lack of adsorbed hydrogen nearby) surface. It appears that only cross-bridged PA associates with adsorbed hydrogen to form styrene that promptly desorbs at 410 K, while vertically aligned PA is less likely to participate in forming styrene.

Zundel- and Eigen-like Surface Hydrated Protons on Pt(111)

  • Kim, Youngsoon;Park, Youngwook;Shin, Sunghwan;Kang, Heon
    • Proceedings of the Korean Vacuum Society Conference
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    • 2016.02a
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    • pp.167.1-167.1
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    • 2016
  • The interaction between adsorbed water and hydrogen on metallic surfaces is important for fundamental understanding of heterogeneous catalysis and electrode surface reactions in acidic environment. Here, we explore a long-standing question of whether hydronium ion can exist or not on a Pt surface coadsorbed with atomic hydrogen and water. Studies based on mass spectrometry and infrared spectroscopy show clear evidence that hydrogen atoms are converted into hydrated protons on a Pt(111) surface. The preferential structures of hydrated protons are identified as multiply hydrated $H_5O_2{^+}$ and $H_7O_3{^+}$ species rather than as hydronium ions. The multiply hydrated protons may be regarded as two dimensional zundel ($H_5O_2{^+}$) and Eigen cation ($H_7O_3{^+}$) in water-metal interface. These surface-bound hydrated protons may be key surface intermediates of the electrochemical interconversion between adsorbed hydrogen atoms and solvated protons.

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Interplay between Defect Propagation and Surface Hydrogen in Silicon Nanowire Kinking Superstructures

  • Sin, Nae-Cheol
    • Proceedings of the Korean Vacuum Society Conference
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    • 2015.08a
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    • pp.221.1-221.1
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    • 2015
  • The vapor-liquid-solid (VLS) method, where the "liquid" catalytic droplets collecting atoms from vapor precursors build the solid crystal layers via supersaturation, is a ubiquitous technique to synthesize 1-dimensional nanoscale materials. However, the lack of fundamental understanding of chemical information governing the process inhibits the rational route to the structural programming. By combining the in situ or operando IR spectroscopy with post-growth high resolution electron microscopy, we show the strong correlation between the surface chemical species concentration and nanowire structures. More specifically, the critical role of surface adsorbed hydrogen, generated from the decomposition of Si2H6 precursor on the interplay between nanowire / kinking and the defect propagation is demonstrated. Our results show that adsorbed hydrogen atoms are responsible for selecting -oriented growth and indicate that a twin boundary imparts structural coherence. The twin boundary, only continuous at / kinks, reduces the symmetry of the trijunction and limits the number of degenerate directions available to the nanowire. These findings constitute a general approach for rationally engineering kinking superstructures and also provide important insight into the role of surface chemical bonding during VLS synthesis.

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Investigation of Cryogenic Breakthrough Curve Measurement System at 77 K for Hydrogen Isotopologue Separation (수소 동위원소 분리를 위한 77 K 극저온 파과 곡선 측정 시스템 제작)

  • Kim, Suhwan;Oh, Hyunchul
    • Korean Journal of Materials Research
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    • v.32 no.1
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    • pp.36-43
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    • 2022
  • Breakthrough analysis has widely been explored for the dynamic separation of gaseous mixtures in porous materials. In general, breakthrough experiments measure the components of a flowing gas when a gaseous mixture is injected into a column filled with an adsorbent material. In this paper, we report on the design and fabrication of a breakthrough curve measurement device to study the dynamic adsorptive separation of hydrogen isotopologues in porous materials. Using the designed system, an experiment was conducted involving a 1:1 mixture of hydrogen and deuterium passed through a column filled with zeolite 13X (1 g). At room temperature, both hydrogen and deuterium were adsorbed in negligible amounts; however, at a temperature of 77 K, deuterium was preferentially adsorbed over hydrogen. The selectivity was different from that in the existing literature due to the different sample shapes, measurement methods, and column structures, but was at a similar level to that of cryogenic distillation (1.5).

Hydrogen Storage Using Pd Doped Mesoporous Carbon Materials (팔라듐이 담지된 중형 기공성 탄소 재료를 이용한 수소 저장)

  • Kim, Wooyoung;Kim, Dongmin;Hong, Youngteak;Kang, Taegyun;Yi, Jongheop
    • Clean Technology
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    • v.12 no.2
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    • pp.107-111
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    • 2006
  • Two types of mesoporous carbons, CMK-3 and CMK-5, were prepared using mesoporous silica as a removable template, and their hydrogen storage capacities were evaluated. For the purpose of comparison, MWCNT (multi-walled carbon nanotubes) was selected and the adsorption of hydrogen was measured. The amount of hydrogen adsorbed on carbon materials was found to be closely related to the surface areas of carbon samples: The higher the surface area of the carbon material, the larger amount of hydrogen was adsorbed. The hydrogen storage capacity increased in the order of CMK-5 > CMK-3 > MWCNT. In addition, hydrogen storage capacity was greatly enhanced by the Pd-doping onto CMK-5. When the metallic Pd was doped on the carbon material, the adsorption amount of hydrogen via a hydrogen spill-over mechanism was crucial to the hydrogen storage capacity of Pd-doped CMK-5.

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Hydrogen-bonded clusters in transformed Lewis acid to new Brønsted acid over WOx/SiO2 catalyst

  • Boonpai, Sirawat;Wannakao, Sippakorn;Panpranot, Joongjai;Praserthdam, Supareak;Chirawatkul, Prae;Praserthdam, Piyasan
    • Advances in nano research
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    • v.12 no.3
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    • pp.291-300
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    • 2022
  • The behavior of hydrogen species on the surface of the catalyst during the Lewis acid transformation to form Brønsted acid sites over the spherical silica-supported WOx catalyst was investigated. To understand the structure-activity relationship of Lewis acid transformation and hydrogen bonding interactions, we explore the potential of using the in situ diffuse reflection infrared Fourier transform spectroscopy (DRIFTS) with adsorbed ammonia and hydrogen exposure. From the results of in situ DRIFTS measurements, Lewis acid sites on surface catalysts were transformed into new Brønsted acid sites upon hydrogen exposure. The adsorbed NH3 on Lewis acid sites migrated to Brønsted acid sites forming NH4+. The results show that the dissociated H atoms present on the catalyst surface formed new Si-OH hydroxyl species - the new Brønsted acid site. Besides, the isolated Si-O-W species is the key towards H-bond and Si-OH formation. Additionally, the H atoms adsorbed surrounding the Si-O-W species of mono-oxo O=WO4 and di-oxo (O=)2WO2 species, where the Si-O-W species are the main species presented on the Inc-SSP catalysts than that of the IWI-SSP catalysts.