Low-temperature deformation mechanism in a work-hardenable body-centered cubic high-entropy alloy with a large uniform elongation

Zhu, L.*; Dong, W.*; Naeem, M.*; Kong, H.*; Hu, C.*; Fan, Z.*; Gong, W.; Harjo, S.; Lan, S.*; Wu, Y.*; et al.

Acta Materialia, 303, p.121734_1 - 121734_10, 2026/01

https://doi.org/10.1016/j.actamat.2025.121734

Pressure-driven solid-state radical polymerization toward carbon nanothread

Che, G.*; Tang, X.*; Liu, J.*; Lang, P.*; Fei, Y.*; Yang, X.*; Wang, Y.*; Gao, D.*; Wang, X.*; Ju, J.*; et al.

Nano Letters, 25(39), p.14467 - 14472, 2025/09

https://doi.org/10.1021/acs.nanolett.5c03977

Mechanochemical radical polymerization has unique advantages in the synthesis of polymer due to its reduced solvent consumption and adaptability of insoluble monomers. However, it suffers from the uncontrollable degradation of the formed polymers during reaction and new synthetic strategy with precise controllability needs to be developed. Here, by employing high static pressure up to 30 GPa, we found 1,3,5-trifluorobenzene undergoes radical polymerization by breaking the conjugated -bonds, and forms a carbon nanothread with high selectivity (Polymer-I polymorph). Based on the crystal structure at the threshold pressure and the calculated energy barriers for the bonding pathway, we concluded that the benzene-rings react via a 1-2 radical polymerization pathway. Our work highlights high pressure is a robust method to initiate the solid-state radical polymerization, even for very stable aromatics, and offers fresh insights for the synthesis of polymeric carbon-based materials with high selectivity.

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), 16(10), p.2445 - 2451, 2025/03

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.

Pressure-induced polymerization of 1,4-difluorobenzene towards fluorinated diamond nanothreads

Che, G.*; Fei, Y.*; Tang, X.*; Zhao, Z.*; Hattori, Takanori; Abe, Jun*; Wang, X.*; Ju, J.*; Dong, X.*; Wang, Y.*; et al.

Physical Chemistry Chemical Physics, 27(2), p.1112 - 1118, 2025/01

https://doi.org/10.1039/D4CP03751K

Pressure-induced polymerization (PIP) of aromatic molecules has emerged as an effective method for synthesizing various carbon-based materials. In this work, PIP of 1,4-difluorobenzene (1,4-DFB) was investigated. high-pressure investigations of 1,4-DFB reveal a phase transition at approximately 12.0 GPa and an irreversible chemical reaction at 18.7 GPa. Structural analysis of the product and the kinetics of the reaction uncovered the formation of pseudohexagonal stacked fluoro-diamond nanothreads with linear growth. Compared to the crystal structures of benzene under high pressure, 1,4-DFB exhibits higher compression along the [001] axis. The anisotropic compression is attributed to the stronger H interaction along the [01] axis and the potential compression-inhibiting HF interactions along the [100] and [010] axes, and it facilitates a possible reaction pathway along the [01] axis. This work emphasizes the crucial role of functionalization in modulating molecular stacking and influencing the reaction pathway.

Probing deformation behavior of a refractory high-entropy alloy using neutron diffraction

Zhou, Y.*; Song, W.*; Zhang, F.*; Wu, Y.*; Lei, Z.*; Jiao, M.*; Zhang, X.*; Dong, J.*; Zhang, Y.*; Yang, M.*; et al.

Journal of Alloys and Compounds, 971, p.172635_1 - 172635_7, 2024/01

https://doi.org/10.1016/j.jallcom.2023.172635

A One-third magnetization plateau phase as evidence for the Kitaev interaction in a honeycomb-lattice antiferromagnet

Shangguan, Y.*; Bao, S.*; Dong, Z.-Y.*; Xi, N.*; Gao, Y.-P.*; Ma, Z.*; Wang, W.*; Qi, Z.*; Zhang, S.*; Huang, Z.*; et al.

Nature Physics, 19(12), p.1883 - 1889, 2023/09

https://doi.org/10.1038/s41567-023-02212-2

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.

Evidence for magnon-phonon coupling in the topological magnet CuTeO

Bao, S.*; Cai, Z.*; Si, W.*; Wang, W.*; Wang, X.*; Shangguan, Y.*; Ma, Z.*; Dong, Z.-Y.*; Kajimoto, Ryoichi; Ikeuchi, Kazuhiko*; et al.

Physical Review B, 101(21), p.214419_1 - 214419_8, 2020/06

https://doi.org/10.1103/PhysRevB.101.214419

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.