Ordered graphane nanoribbons synthesized via high-pressure diels-alder polymerization of 2,2'-bipyrazine

Li, F.*; Tang, X.*; Fei, Y.*; Zhang, J.*; Liu, J.*; Lang, P.*; Che, G.*; Zhao, Z.*; Zheng, Y.*; Fang, Y.*; et al.

Journal of the American Chemical Society, 147(17), p.14054 - 14059, 2025/04

https://doi.org/10.1021/jacs.5c03116

We synthesized a crystalline graphane nanoribbon (GANR) via pressure-induced polymerization of 2,2'-bipyrazine (BPZ). By performing Rietveld refinement of in situ neutron diffraction data, nuclear magnetic resonance spectroscopy, infrared spectra, and theoretical calculation, we found that BPZ experienced Diels-Alder polymerization between the stacked aromatic rings, and formed extended boat-GANR structures with exceptional long-range order. The unreacted -C=N- groups bridge the two ends of the boat, and ready for further functionalization. The GANR has a bandgap of 2.25 eV, with booming photoelectric response (/ =18.8). Our work highlights that the high-pressure topochemical polymerization is a promising method for the precise synthesis of graphane with specific structure and desired properties.

Concurrent neutron imaging and diffraction analysis revealing spatial lithiation phase evolution in an ultra-thick graphite electrode

Strobl, M.*; Baur, M. E.*; Samothrakitis, S.*; Molamud, F.*; Zhang, X.*; Tung, P. K. M.*; Schmidt, S.*; Woracek, R.*; Lee, J.*; Kiyanagi, Ryoji; et al.

Advanced Energy Materials, p.2405238_1 - 2405238_9, 2025/01

https://doi.org/10.1002/aenm.202405238

Solid-state Alder-ene reaction of 1-hexene under high pressure

Xu, J.*; Lang, P.*; Liang, S.*; Zhang, J.*; Fei, Y.*; Wang, Y.*; Gao, D.*; Hattori, Takanori; Abe, Jun*; Dong, X.*; et al.

Journal of Physical Chemistry Letters (Internet), p.2445 - 2451, 2025/00

https://doi.org/10.1021/acs.jpclett.4c03696

The Alder-ene reaction is a chemical reaction between an alkene with an allylic hydrogen, and it provides an efficient method to construct the C-C bond. Traditionally, this reaction requires catalysts, high temperatures, or photocatalysis. In this study, we reported a high-pressure-induced solid-state Alder-ene reaction of 1-hexene at room temperature without a catalyst. 1-Hexene crystallizes at 4.3 GPa and polymerizes at 18 GPa, forming olefins. By exploring gas chromatography-mass spectrometry, we discovered that 1-hexene generates dimeric products through the Alder-ene reaction under high pressures. The in situ neutron diffraction shows that the reaction process did not obey the topochemical rule. A six-membered ring transition state including one C-H bond and two alkene bonds was evidenced by the theoretical calculation, whose energy obviously decreased when compressed to 20 GPa. Our work offers a novel and promising method to realize the Alder-ene reaction at room temperature without a catalyst, expanding the application of this important reaction.

Gradient residual strain measurement procedure in surface impacted railway steel axles by using neutron scattering

Zhou, L.*; Zhang, H.*; Qin, T. Y.*; Hu, F. F.*; Xu, P. G.; Ao, N.*; Su, Y. H.; He, L. H.*; Li, X. H.*; Zhang, J. R.*; et al.

Metallurgical and Materials Transactions A, 55(7), p.2175 - 2185, 2024/07

https://doi.org/10.1007/s11661-024-07352-5

Crystal-liquid duality driven ultralow two-channel thermal conductivity in -MgAgSb

Li, J.*; Li, X.*; Zhang, Y.*; Zhu, J.*; Zhao, E.*; Kofu, Maiko; Nakajima, Kenji; Avdeev, M.*; Liu, P.-F.*; Sui, J.*; et al.

Applied Physics Reviews (Internet), 11(1), p.011406_1 - 011406_8, 2024/03

https://doi.org/10.1063/5.0173680

Pressure engineering of van der Waals compound RhI; Bandgap narrowing, metallization, and remarkable enhancement of photoelectric activity

Fang, Y.*; Kong, L.*; Wang, R.*; Zhang, Z.*; Li, Z.*; Wu, Y.*; Bu, K.*; Liu, X.*; Yan, S.*; Hattori, Takanori; et al.

Materials Today Physics (Internet), 34, p.101083_1 - 101083_7, 2023/05

https://doi.org/10.1016/j.mtphys.2023.101083

The layered van der Waals halides are particularly sensitive to external pressure, suggesting a feasible route to pinpoint their structure with extraordinary behavior. However, a very sensitive pressure response usually lead to a detrimental phase transition and/or lattice distortion, making the approach of materials manipulation in a continuous manner remain challenging. Here, the extremely weak interlayer coupling and high tunability of layered RhI crystals are observed. A pressure-driven phase transition occurs at a moderate pressure of 5 GPa, interlinking to a change of layer stack mode. Strikingly, such a phase transition does not affect the tendency of quasi-linear bandgap narrowing, and a metallization with an ultra-broad tunability of 1.3 eV redshift is observed at higher pressures. Moreover, the carrier concentration increases by 4 orders of magnitude at 30 GPa, and the photocurrent enhances by 5 orders of magnitude at 7.8 GPa. These findings create new opportunities for exploring, tuning, and understanding the van der Waals halides by harnessing their unusual feature of a layered structure, which is promising for future devices based on materials-by-design that are atomically thin.

Heat-induced structural changes in magnesium alloys AZ91 and AZ31 investigated by in situ synchrotron high-energy X-ray diffraction

Liu, X. J.*; Xu, P. G.; Shiro, Ayumi*; Zhang, S. Y.*; Shobu, Takahisa; Yukutake, Eitaro*; Akita, Koichi*; Zolotoyabko, E.*; Liss, K.-D.*

Journal of Materials Science, 57(46), p.21446 - 21459, 2022/12

https://doi.org/10.1007/s10853-022-07917-y

Fine structure in the decay of the 8 isomer in U

Zhang, M. M.*; Tian, Y. L.*; Wang, Y. S.*; Zhang, Z. Y.*; Gan, Z. G.*; Yang, H. B.*; Huang, M. H.*; Ma, L.*; Yang, C. L.*; Wang, J. G.*; et al.

Physical Review C, 106(2), p.024305_1 - 024305_6, 2022/08

https://doi.org/10.1103/PhysRevC.106.024305

Crystalline fully carboxylated polyacetylene obtained under high pressure as a Li-ion battery anode material

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

https://doi.org/10.1021/acs.jpclett.1c03734

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.

Phase transition and chemical reactivity of 1H-tetrazole under high pressure up to 100 GPa

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

https://doi.org/10.1039/D1CP02913D

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.