Wang, X.*; Tang, X.*; Zhang, P.*; Wang, Y.*; Gao, D.*; Liu, J.*; Hui, K.*; Wang, Y.*; Dong, X.*; Hattori, Takanori; et al.
Journal of Physical Chemistry Letters (Internet), 12(50), p.12055 - 12061, 2021/12
Substituted polyacetylene is expected to improve the chemical stability, physical properties, and additional functions of the polyacetylene backbones, but its diversity is very limited. Here, by applying external pressure on solid acetylenedicarboxylic acid, we report the first crystalline poly-dicarboxylacetylene with every carbon on the trans-polyacetylene backbone bonded to a carboxyl group, which is very hard to synthesize by traditional methods. This unique structure combines the extremely high content of carbonyl groups and high conductivity of a polyacetylene backbone, which exhibits a high specific capacity and excellent cycling/rate performance as a Li-ion battery (LIB) anode. We present a completely functionalized crystalline polyacetylene and provide a high-pressure solution for the synthesis of polymeric LIB materials and other polymeric materials with a high content of active groups.
Yan, S. Q.*; Li, X. Y.*; Nishio, Katsuhisa; Lugaro, M.*; Li, Z. H.*; Makii, Hiroyuki; Pignatari, M.*; Wang, Y. B.*; Orlandi, R.; Hirose, Kentaro; et al.
Astrophysical Journal, 919(2), p.84_1 - 84_7, 2021/10
Gao, D.*; Tang, X.*; Wang, X.*; Yang, X.*; Zhang, P.*; Che, G.*; Han, J.*; Hattori, Takanori; Wang, Y.*; Dong, X.*; et al.
Physical Chemistry Chemical Physics, 23(35), p.19503 - 19510, 2021/09
Pressure-induced phase transition and polymerization of nitrogen-rich molecules are widely focused due to its extreme importance for the development of green high energy density materials. Here, we present a study of the phase transition and chemical reaction of 1H-tetrazole up to 100 GPa by using Raman, IR, X-ray diffraction, neutron diffraction techniques and theoretical calculation. A phase transition above 2.6 GPa was identified and the high-pressure structure was determined with one molecule in a unit cell. The 1H-tetrazole polymerizes reversibly below 100 GPa, probably through a carbon-nitrogen bonding instead of nitrogen-nitrogen bonding. Our studies updated the structure model of the high pressure phase of 1H-tetrazole, and presented the possible intermolecular bonding route for the first time, which gives new insights to understand the phase transition and chemical reaction of nitrogen-rich compounds, and benefit for designing new high energy density materials.
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
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.
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
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.
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
Chen, L.-M.; Kotaki, Hideyuki; Nakajima, Kazuhisa*; Koga, J. K.; Bulanov, S. V.; Tajima, Toshiki; Gu, Y. Q.*; Peng, H. S.*; Wang, X. X.*; Wen, T. S.*; et al.
Physics of Plasmas, 14(4), p.040703_1 - 040703_4, 2007/04
An experiment for the laser self-guiding studies has been carried out with 100 TW laser pulse interaction with the long underdense plasma. Formation of extremely long plasma channel with its length, about 10 mm, 20 times above the Rayleigh length is observed. The self-focusing channel features such as the laser pulse significant bending and the electron cavity formation are demonstrated experimentally for the first time.
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.
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.