Hydrogen absorption and diffusion behaviors in cube-shaped palladium nanoparticles revealed by ambient-pressure X-ray photoelectron spectroscopy

Tang, J.*; Seo, O.*; Rivera Rocabado, D. S.*; Koitaya, Takanori*; Yamamoto, Susumu*; Namba, Yusuke*; Song, C.*; Kim, J.*; Yoshigoe, Akitaka; Koyama, Michihisa*; et al.

Applied Surface Science, 587, p.152797_1 - 152797_8, 2022/06

https://doi.org/10.1016/j.apsusc.2022.152797

The hydrogen absorption and diffusion mechanisms on cube-shaped Pd nanoparticles (NPs) which are important hydrogen-storage materials were studied using X-ray photoelectron spectroscopy and DFT calculations. In the surface region, hydrogen absorption showed almost similar behavior regardless of the NPs size. It was found that the octahedral sites are more favorable than the tetrahedral sites for hydrogen occupation. We also clarified that the hydrogen atoms absorbing on the smaller-sized Pd NPs diffuse to the subsurface more actively because of the weakened Pd-H bond by the surface disordering, which plays an important role in hydrogen adsorption at a low H pressure.

Distance-selected topochemical dehydro-diels-alder reaction of 1,4-Diphenylbutadiyne toward crystalline graphitic nanoribbons

Zhang, P.*; Tang, X.*; Wang, Y.*; Wang, X.*; Gao, D.*; Li, Y.*; Zheng, H.*; Wang, Y.*; Wang, X.*; Fu, R.*; et al.

Journal of the American Chemical Society, 142(41), p.17662 - 17669, 2020/10

https://doi.org/10.1021/jacs.0c08274

Solid-state topochemical polymerization (SSTP) is a promising method to construct functional crystalline polymeric materials, but in contrast to various reactions that happen in solution, only very limited types of SSTP reactions are reported. Diels-Alder (DA) and dehydro-DA (DDA) reactions are textbook reactions for preparing six-membered rings in solution but are scarcely seen in solid-state synthesis. Here, using multiple cutting-edge techniques, we demonstrate that the solid 1,4-diphenylbutadiyne (DPB) undergoes a DDA reaction under 10-20 GPa with the phenyl as the dienophile. The crystal structure at the critical pressure shows that this reaction is "distance-selected". The distance of 3.2 between the phenyl and the phenylethynyl facilitates the DDA reaction, while the distances for other DDA and 1,4-addition reactions are too large to allow the bonding. The obtained products are crystalline armchair graphitic nanoribbons, and hence our studies open a new route to construct the crystalline carbon materials with atomic-scale control.

Pressure-induced Diels-Alder reactions in CH - CF cocrystal towards graphane structure

Wang, Y.*; Dong, X.*; Tang, X.*; Zheng, H.*; Li, K.*; Lin, X.*; Fang, L.*; Sun, G.*; Chen, X.*; Xie, L.*; et al.

Angewandte Chemie; International Edition, 58(5), p.1468 - 1473, 2019/01

https://doi.org/10.1002/anie.201813120

Pressure-induced polymerization (PIP) of aromatics is a novel method to construct sp-carbon frameworks, and nanothreads with diamond-like structures were synthesized by compressing benzene and its derivatives. Here by compressing benzene-hexafluorobenzene cocrystal(CHCF), we identified H-F-substituted graphane with a layered structure in the PIP product. Based on the crystal structure determined from the in situ neutron diffraction and the intermediate products identified by the gas chromatography-mass spectrum, we found that at 20 GPa CHCF forms tilted columns with benzene and hexafluorobenzene stacked alternatively, which leads to a [4+2] polymer, and then transfers to short-range ordered hydrogenated-fluorinated graphane. The reaction process contains [4+2] Diels-Alder, retro-Diels-Alder, and 1-1' coupling, and the former is the key reaction in the PIP. Our studies confirmed the elemental reactions of the CHCF for the first time, which provides a novel insight into the PIP of aromatics.

Elongation of plasma channel for electron acceleration

Chen, L.-M.; Nakajima, Kazuhisa; Hong, W.*; Hua, J. F.*; Kameshima, Takashi; Kotaki, Hideyuki; Sugiyama, Kiyohiro*; Wen, X.*; Wu, Y.*; Tang, C.*; et al.

Chinese Optics Letters, 5(S1), p.S133 - S135, 2007/05

Guiding of 100 TW Relativistic Laser Pulses by 10 mm Plasma Channels

Koga, J. K.; Chen, L.-M.; Kotaki, Hideyuki; Nakajima, Kazuhisa; Bulanov, S. V.; Tajima, Toshiki; Gu, Y. Q.*; Peng, H. S.*; Hua, J. F.*; An, W. M.*; et al.

no journal, , 

First experiments for electron acceleration with the laser-gas plasma interaction have been carried out with 30 fs, 100 TW relativistic Ti:Sapphier laser pulse into a long slit (1.2 10 mm) gas plasma. The 10 mm length plasma channel formed that was longer than 20 times the Rayleigh length. Plasma density was the key factor for this long channel stimulation under 100 TW laser pulse irradiation that was much higher than critical power for relativistic self-focusing. For the first time, channel characteristics such as laser bending, hosing and cavity formation were demonstrated experimentally. In case of long channel guiding, accelerated electron bunch was tightly collimated with low emmitance mm mrad and quasi-monoenergetic electron bunch ( 70 MeV) was obtained as well. Accelerated electron charge current with electron energy 1 MeV was 10 nC/shot which was highest value in laser accelerator, to our knowledge, and ascribed to the contribution of long plasma channel. These well controlled laser-driven acceleration is an important cornerstone of relativistic engineering.

Laser electron acceleration in cm-scale capillary-discharge plasma channel

Kameshima, Takashi; Kotaki, Hideyuki; Kando, Masaki; Daito, Izuru; Kawase, Keigo; Fukuda, Yuji; Chen, L. M.*; Homma, Takayuki; Kondo, Shuji; Esirkepov, T. Z.; et al.

no journal, , 

The acceleration method of laser plasma electron acceleration has very strong electric field, however, the acceleration length is veryshort. Hence, the energy gain of electron beams were confined to be approximately 100 MeV. Recently, this problem was solved by using discharge capillary. The feature of plasma was used that high dense plasma has low refractive index. Distributing plasma inside capillary as low dense plasma is in the center of capillary and high dense plasma is in the external side of capillary can make a laser pulse propaget inside capillary with initial focal spot size. Experiments with capillary were performed in China Academy of Engineering Physics (CAEP) and Japan Atomic Energy Agency (JAEA). We obtained the results of 4.4 J laser pulse optical guiding in 4 cm capillary and 0.56 GeV electron production in CAEP in 2006, and 1 J laser pulse optical guiding in 4 cm capillary and electron beams productions.