Liang, Tian; Zhu, Xiaoming; Zeng, Xiaojun
doi: 10.1039/d4dt03215bpmid: 39869084
Due to a lack of spatially resolved characterization studies on statistical and individual particle microstructure at multiple scales, a knowledge gap exists in understanding the mechanistic link between rapid performance failure and atomic-scale structure degradation in single-crystalline Ni-rich battery cathodes. In a recent publication in Science, Huang et al. developed a multi-crystal rocking curve technique (combining X-ray and electron microscopy to capture both statistical and individual lattice distortions), which enables multiscale observations and further proves that the accumulation of the unrecoverable lattice rotation in cathodes upon repeated cycling exacerbates mechanical failure and electrochemical decay. The elucidation of failure mechanisms in single-crystalline cathodes offers valuable insights into the development of long-lasting and high-energy-density cathodes in next-generation batteries, encompassing strategies to mitigate lattice rotation and enhance lattice structure tolerance against lattice distortion within individual particles.
Kroitor, Andrey P.; Martynov, Alexander G.; Gorbunova, Yulia G.; Tsivadze, Aslan Yu.; Sorokin, Alexander B.
doi: 10.1039/d4dt03263bpmid: 39937538
The novel ruthenium octa-n-butoxy-naphthalocyanine complex was shown to retain an essentially monomeric state in dilute solutions. It was successfully applied as a homogeneous catalyst for carbene insertion into N–H bonds of amines with various substitution patterns, providing high yields of glycine derivatives.
Gao, Zhixia; Li, Ke; Du, Hong; Baiheti, Tuohetijiang
doi: 10.1039/d4dt03580apmid: 39996382
Herein, four molybdophosphates, AxB4−xMo5P2O22 (A = Na, K and B = Rb, Cs), were synthesized by cation substitution. Compared with the parent compound A4Mo5P2O22 (A = Rb, Cs), the different cations result in different polarities of the structural-functional unit, ultimately influencing the nonlinear optical properties of AxB4−xMo5P2O22 (x = 1–4).
Münster, Katharina; Kudo, Shunsuke; Kuwabara, Takuya; Shimamura, Eriko; Furukawa, Shunsuke; Yoshida, Yusuke; Ishida, Shintaro; Iwamoto, Takeaki; Tanifuji, Kazuki; Ohki, Yasuhiro; Minoura, Mao; Saito, Masaichi
Yang, Wei; Wang, Wenqing; Huang, Shidi; Gao, Mengluan; Weng, Fuming; Zou, Rujia
doi: 10.1039/d4dt03381gpmid: 39910916
An effective way to improve the cycling performance of metal sulfide materials is to blend them with conductive materials. In this paper, three-dimensional (3D) hollow MXene/ZnS heterostructures (ZnSMX) were prepared via a two-step process involving hydrothermal and template methodologies. The formation of Ti–O–Zn bonds enables the firm bonding between ZnS nanoparticles and the MXene substrate at heterogeneous interfaces, which can act as “electron bridges” to facilitate electron and charge transfer. Additionally, 3D hollow ZnSMX not only enhances the conductivity of ZnS, enabling rapid charge transfer, but also effectively show restacking of MXene nanosheets to maintain structural stability during the charge/discharge process. More importantly, the 3D porous structure provides ultrafast interfacial ion transport pathways and extra surficial and interfacial storage sites, thus boosting excellent storage performances in lithium-ion battery applications. The 3D ZnSMX exhibited a high capacity of 782.1 mA h g−1 at 1 A g−1 current, excellent cycling stability (providing a high capacity of 1027.8 mA h g−1 after 350 cycles at 2 A g−1), and excellent rate performance. This indicates that 3D ZnS/MXene heterostructures can potentially be highly promising anode materials for high-multiplication lithium-ion batteries.
Gujarati, Akash V.; Patel, Divyesh K.
doi: 10.1039/d4dt03509gpmid: 39927843
In this work, 4-((4-methylbenzyl)oxy)benzaldehyde resin-supported Pd(II)-Schiff base PS@Pd(OAc)2 was synthesized. FT-IR, XPS, TGA, ICP-MS, and powder XRD established the structure of PS@Pd(OAc)2. The morphology and distribution of elements on PS@Pd(OAc)2 were determined using SEM, TEM, and elemental mapping analysis. The heterogenized PS@Pd(OAc)2 catalyst was found to be efficient in promoting three-component Mizoroki–Heck coupling via an in situ Witting reaction, where (E)-1,2-diphenylethenes were efficiently synthesized from the Witting salt. In this one-pot reaction, this catalyst exhibits a distinct synergistic effect. The significant mass-transfer limitation results from a nonsignificant distribution of active sites amalgamated with the crumpling of catalysts, which facilitates the smooth, easy movement of the reactants and products toward the well-spaced active catalytic sites on the catalyst's surface. These characteristics increase the catalytic activity of PS@Pd(OAc)2. Moreover, the catalyst was found to be quite robust for this reaction with very little metal leaching; thus, it can be efficiently recycled. Hence, multiple uses were established, and its reusability was proven in this important reaction.
Xu, Yuchen; Dong, Wenxiao; Song, Shaoli; He, Huichao; Jiang, Hanmei; Jia, Bi; Liu, Xiaoyan; Qiu, Jianbei; Han, Tao
doi: 10.1039/d4dt03247kpmid: 39873642
Achieving multicolor emission is a fascinating goal that remains challenging for zero-dimensional (0D) hybrid halides. We successfully obtained a three-millimeter-scale 0D (MXDA)2CdBr6 (MXDA = C8H14N22+) single crystal (SC) by the solvothermal method. It serves as an outstanding host for doping with various valence activators, such as Cu+, Mn2+ and Sb3+, and these doped single crystals emit blue (470 nm), yellow (580 nm) and red (618 nm) fluorescence, which accurately cover a large visible region and achieve efficient multicolor emission. (MXDA)2CdBr6:8%Cu+ exhibits a high photoluminescence quantum yield (PLQY) of 60.31% under 320 nm UV excitation, while (MXDA)2CdBr6:10%Mn2+ shows a PLQY of 50.52%. Density functional theory calculations indicate that the hybrid 0D (MXDA)2CdBr6 halide is an indirect bandgap semiconductor with a bandgap value of 3.33 eV. This work expands the new material space for organic–inorganic hybrid halide materials and provides insights for tuning their optical properties.
Showing 1 to 10 of 40 Articles
The synthesis and full characterization of 1,4-dilithio-1,4-bis(triisopropylsilyl)-2,3-diphenylbuta-1,3-diene (1b) are reported. This molecule featuring extremely bulky silyl groups at the 1- and 4-positions serves as a precursor for the synthesis of 2,5-bis(triisopropylsilyl)-3,4-diphenyl-1-silacyclopenta-1,3-dienes (siloles) bearing various substituents at the silicon atom (SiR2 = SiH2 (4), SiH(OMe) (5), SiF2 (6), SiBr2 (7), SiBr(OMe) (8)). Importantly, compounds 6 and 7 reacted with lithium to afford 2,5-bis(triisopropylsilyl)-3,4-diphenyldilithiosilole (9). The solid-state molecular structure and solution NMR spectra reveal the formation of an aromatic ring system, as opposed to the precursors 6 and 7, with two Li cations coordinated by the silacycle in η5-fashions. The sterically bulky dilithiosilole 9 can be applied as an important starting material in the pursuit of low-valent silicon species without donor stabilization.