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Chinese Chemical Letters 2023年第3期34卷 486-489页

作者： De-Xuan Liu Zhi-Hong Yu xiao-xian chen Wei-Xiong Zhang xiao-Ming chen MOE Key Laboratory of Bioinorganic and Synthetic Chemistry School of ChemistrySun Yat-sen UniversityGuangzhou 510275China

Understanding phase transitions in multi-component crystals is of importance for regulating specified functional ***,we present two new organic-inorganic hybrid crystals,(Me_(3)NCH_(2)CH_(2)X)_(4)[Ni(NCS)_6](X=Cl and Br),revealing distinct phase ***,the Clsubstituted cations weakly interact with discrete inorganic part hence reveal step-wise dynamic changes upon heating,which result in multi-step solid-solid phase transitions (P1-P2_1/n-A2/a-Cmce) including a ferroelastic one with a spontaneous strain of *** the Br-substituted cations with larger steric effect prevent the solid-solid phase transition but give a solid-liquid phase transition at above 419 *** present instances well demonstrate the complicity for multi-component crystals arising from the delicate balance established by abundant weak intermolecular interactions,and inspire the design of novel phase-transition materials by judiciously assembling multi-component crystals.

关键词： Hybrid crystal Phase transition Ferroelasticity Intermolecular interaction Hirshfeld surface analysis

Solvent-Controlled Construction of Molecular Chains and Bowls/Sieves from a Bent Dipyridyl Ligand

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Chinese Journal of Chemistry 2021年第9期39卷 2523-2528页

作者： xiao-Yun Tian xiao-xian chen Chao Wang Zi-Ming Ye Dong-Dong Zhou Jie-Peng Zhang MOE Key Laboratory of Bioinorganic and Synthetic Chemistry School of ChemistrySun Yat-Sen UniversityGuangzhouGuangdong 510275China

Solvothermal reactions of 3,6-di(pyridin-4-yl)-9H-carbazole(dpc)with Cu(ll)yielded crystals of two new coordination complexes,namely[Cu(CH_(3)COO)_(2)(dpc)(H_(2)O)_(2)]n-xGuest(1)and[Cu_(13)(HCOO)_(16)(dpc)16(H_(2)O)6](HCOO)10-Guest(2),in which CH_(3)COO_and HCOO-were generated from the hydrolysis of the solvents A/zAZ-dimethylacetamide(DMA)and A/zA/-dimethylformamide(DMF),***-crystal X-ray diffraction showed that 1 possesses simple wavy coordination chains,while 2 possesses large molecular bowls/sieves with outer and inner effective sizes of 30.2 × 30.2 × 25.5 A^(3) and 15.0 × 15.0 × 18.6 A^(3),respectively,which consists of 4 linear Cu_(3)(HCOO)_(4)(H_(2)O)clusters and 12 dpc ligands as the square-shaped wall and a claw-like Cu(dpc)_(4) fragment as the ***-free 2 can adsorb considerable amounts of CO_(2)/H_(2)O and CH_(3)OH but completely exclude C2H4 and C3H6z which shows a potential application for olefin drying.

关键词： Self-assembly Crystal engineering Microporous materials Molecular sieve Olefin drying

A topology approach to overcome the pore size/volume trade-offs for autonomous indoor humidity control

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Science China Chemistry 2024年第9期67卷 2968-2974页

作者： Zhi-Shuo Wang Xue-Wen Zhang Kai Zheng xiao-xian chen Dong-Dong Zhou Jie-Peng Zhang MOE Key Laboratory of Bioinorganic and Synthetic Chemistry GBRCE for Functional Molecular EngineeringSchool of ChemistryIGCMESun Yat-Sen UniversityGuangzhou 510275China Chemistry and Chemical Engineering Guangdong Laboratory Shantou 515021China

Autonomous indoor humidity control is gaining more and more attention but is limited by the trade-offs among pore volume,pore size and water stability of water *** solve this problem by using a unique coordination network topology combined with hydrolytically stable M(Ⅲ)carboxylate *** extending the ligand length from 9.0 to 11.2 and 13.7?,the pore volume significantly increases from 0.99 to 1.40 and 1.78 cm^(3)g^(-1),which proportionally increases the saturated water adsorption ***,the pore size slightly increases from 10.4 to 11.0 and 13.5A,which restricts the isotherm inflection pressure and hysteresis width to meet the requirement of indoor humidity *** single-crystals suitable for Xray diffraction studies were obtained by using Fe(Ⅲ)salts,while isostructural frameworks with sufficiently high water stabilities were synthesized by using Cr(Ⅲ)salts,which offer record working capacity of 0.90 and 1.10 g g^(-1)for indoor humidity control.

关键词： metal-organic frameworks water adsorption indoor humidity control water stability pore engineering

Unique Freezing Dynamics of Flexible Guest Cations in the First Molecular Postperovskite Ferroelectric:(C_(5)H_(13)NBr)[Mn(N(CN)_(2))_(3)]

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CCS Chemistry 2019年第4期1卷 448-454页

作者： Sha-Sha Wang xiao-xian chen Bo Huang Rui-Kang Huang Wei-Xiong Zhang xiao-Ming chen MOE Key Laboratory of Bioinorganic and Synthetic Chemistry School of ChemistrySun Yat-Sen UniversityGuangzhou 510275China

Ferroelectricity is usually found in cubic and hexagonal perovskites consisting of corner-and faced-shared BX 6 octahedra,*** con-trast,another important branch of perovskites,postperovskites,which contain layers constructed by both edge-and corner-shared BX 6 octahedra,have been much more scarcely studied and virtually absent in the fields of ferroelectricity since the discovery of postperovskite structure in *** this study,we present for the first time a molec-ular postperovskite ferroelectric,(bromocholine)[Mn(N(CN)_(2))_(3)],and demonstrate how spontaneous polarization arises from the freezing dynamics of bromocholine cations in a unique space confined by postperovskite *** findings suggest that postperovskites could serve as a new type of host-guest model in controlling the molecular dynamics of abundant polar cations in the development of novel ferroelectric materials.

关键词： molecular postperovskite molecular ferroelectric host-guest compounds molecular dynamics

Multi-stimuli responsive behaviors in a new chiral hybrid nitroprusside salt（R-3-hydroxypyrrolidinium）2[Fe（CN）5（NO）]

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Chinese Chemical Letters 2024年第12期35卷 535-538页

作者： Mao-Fan Li Ming-Yu Guo De-Xuan Liu xiao-xian chen Wei-Jian Xu Wei-Xiong Zhang MOE Key Laboratory of Bioinorganic and Synthetic Chemistry School of ChemistryIGCMESun Yat-Sen University Department of Chemistry&CICECO-Aveiro Institute of Materials University of Aveiro

Multi-stimuli responsive materials controlled and coupled by two or more channels have a broad range of applications in the field of switches,memories,and molecular *** exploration of the material is currently focused on the pure organic system,which limits the development o such materials *** this work,we present a new chiral organic-inorganic hybrid salt,（R-3hydroxypyrrolidinium）2[Fe（CN）5（NO）]（1）,which exhibits rare multi-stimuli responsive behaviors in ther mal,mechanical and optical *** detail,1 undergoes a C2-P21221phase transition deriving from the thermal motion of organic cations with the increase of temperature,but the reverse transition can only be induced by mechanical ***,polycrystalline hybrid salt showed photo-responsive performance,i.e.,the ground-state N-bound nitrosyl ligand adopts two configurations in excited state caused by light in 532 nm irradiation,accompanying with a photo-induced structural transformation o the anionic ***,the thermal motion characteristics of organic cations,the photoresponse characteristics of anionic inorganic skeleton and the pressure characteristics from hydrogen bonds are si multaneously integrated in *** unprecedented coupling mechanism of multi-stimuli responses make1 a potential candidate for future multichannel data storage applications.

关键词： Phase transition Organic and inorganic hybrids Multi-stimuli responsive materials Nitroprusside Photoisomerization

High-and low-temperature dual ferroelasticity in a new hybrid crystal:(Me_(3)NCH_(2)CH_(2)OH)_(4)[Ni(NCS)_(6)]

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Science China Materials 2022年第1期65卷 263-267页

作者： De-Xuan Liu xiao-xian chen Zi-Ming Ye Wei-Xiong Zhang xiao-Ming chen MOE Key Laboratory of Bioinorganic and Synthetic Chemistry School of ChemistrySun Yat-Sen UniversityGuangzhou 510275China

Ferroelasticity,as a mechanical counterpart of ferroelectricity and ferromagnetism,describes the nonlinear response of strain to stress with a hysteresis loop[1].Ferroelastic phase features with two or more switchable orientation states of spontaneous strain[2,3],ensuring essential roles in shape memory,actuators,and mechanical switches[4].

关键词：对称性破缺可逆相变铁弹性高低温杂化 NCS

远程二烯的定向迁移驱动钯催化的不对称烯丙基化反应

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科学通报 2023年第26期68卷 3410-3412页

作者：陈先枭何智涛中国科学院上海有机化学研究所中国科学院天然产物有机合成化学重点实验室上海200032 国科大杭州高等研究院化学与材料科学学院杭州310024

手性是自然界的基本属性,例如天然存在的糖、蛋白质、核酸等生物活性分子均是手性的.众多药物和天然产物分子也包含手性片段,它们的生理活性往往同其手性特征密切相关.因此,利用催化不对称合成方法高效构建手性分子一直是有机合成化学... 详细信息

手性是自然界的基本属性,例如天然存在的糖、蛋白质、核酸等生物活性分子均是手性的.众多药物和天然产物分子也包含手性片段,它们的生理活性往往同其手性特征密切相关.因此,利用催化不对称合成方法高效构建手性分子一直是有机合成化学中广泛关注和深入研究的领域之一.2001和2021年两次诺贝尔化学奖正是表彰在不对称催化合成领域作出杰出贡献的科学家.

关键词：有机合成化学手性分子钯催化烯丙基化反应诺贝尔化学奖天然产物生物活性分子催化不对称合成

Metal-Free Hexagonal Perovskite High-Energetic Materials with NHOH/NHNH as B-Site Cations

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Engineering 2020年第9期6卷 1144-1150页

作者： Yu Shang Zhi-Hong Yu Rui-Kang Huang Shao-Li chen De-Xuan Liu xiao-xian chen Wei-Xiong Zhang xiao-Ming chen MOE Key Laboratory of Bioinorganic and Synthetic Chemistry School of ChemistrySun Yat-Sen UniversityGuangzhou 510275China

寻找可经由简单路线合成的高性能含能材料是发展先进实用含能材料的重要问题。文中通过合理地选择分子组分,经由易于规模放大的简单合成路线,以NH3OH^+和NH2NH3^+分别作为B位点阳离子构筑了两例无金属六方钙钛矿含能材料(H2dabco)B(ClO4... 详细信息

寻找可经由简单路线合成的高性能含能材料是发展先进实用含能材料的重要问题。文中通过合理地选择分子组分,经由易于规模放大的简单合成路线,以NH3OH^+和NH2NH3^+分别作为B位点阳离子构筑了两例无金属六方钙钛矿含能材料(H2dabco)B(ClO4)3(分别命名为DAP-6和DAP-7,其中,H2dabco2+是1,4-二氮杂双环[2.2.2]辛烷-1,4-二鎓离子)。与基于NH4^+阳离子构筑的立方钙钛矿类似物(H2dabco)(NH4)(ClO4)3相比,DAP-6和DAP-7有较高的晶体堆积密度和生成焓,从而具有更高的爆轰性能。特别地,DAP-7具有超高热稳定性(起始分解温度Td=375.3℃)、高爆速(D=8.883 km·s^-1)和高爆压(P=35.8 GPa),因此具有作为耐热炸药的应用潜力。计算表明,DAP-6不仅具有较高的热稳定性(Td=245.9℃)以及优异的爆轰性能(D=9.123 km·s^-1,P=38.1 GPa),而且其爆热值(Q=6.35 kJ·g^-1)和理论比冲值(Isp=265.3 s)均稍优于六硝基六氮杂异伍兹烷(CL-20:Q=6.23 k J·g^-1,Isp=264.8 s),在炸药和推进剂领域中具有很好的应用前景。

关键词：含能材料单质炸药固体推进剂无金属六方钙钛矿

Switchable K-O bonds unveiling anomalous ferroelastic transitions in a polar hybrid crystal

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Science China Materials 2024年第10期67卷 3408-3414页

作者： Yao-Bin Li Wei-Jian Xu xiao-xian chen De-Xuan Liu Zhi-Shuo Wang Wei-Xiong Zhang MOE Key Laboratory of Bioinorganic and Synthetic Chemistry School of ChemistryIGCMESun Yat-sen UniversityGuangzhou 510275China Department of Chemistry&CICECO-Aveiro Institute of Materials University of AveiroAveiro 3810-193Portugal

Hybrid ferroelastic crystals have garnered considerable interest due to their promising potential as mechanical switches and *** anomalous ferroelastic phase transitions,in which ferroelasticity occurs in the hightemperature phase rather than the low-temperature phase,are of particular interest,but they are sporadically-documented and none of them is involved in breaking of the chemical ***,a hydroxyl-containing cation,i.e.,Me_(3)NOH^(+),is employed to construct a three-dimensional hybrid crystal(Me_(3)NOH)_(2)KBiCl_(6)(1).This crystal undergoes distinct twostep structural phase transitions with space-group changes of Pna21–P112_(1)–P63mc,belonging to an anomalous temperaturereversed mm2F2 ferroelastic transition and a normal 6mmF2 ferroelastic transition,*** anomalous ferroelastic transition is entirely driven by switchable K–O coordination bonds involving breaking and ***,the dynamic behavior of Me_(3)NOH^(+)cations along with the distortion of inorganic framework enables the manifestation of unusual“high-low-medium”second-harmonic generation-switching *** study presents the enormous benefits of switchable coordination bonds for inducing anomalous ferroelastic phase transitions,offering valuable insight for the exploration of new multifunctional ferroelastic materials.

关键词： bond-switching transition ferroelastic phase transition hybrid crystal

Highly conductive and stable iodine doped argyrodite electrolyte for all-solid-state lithium batteries

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Journal of Energy Chemistry 2025年第1期100卷 50-58页

作者： Gaozhan Liu Jing Zhang Jing Yang Jinghui chen Xingyue xiao Xiayin Yao Ningbo Institute of Materials Technology and Engineering Chinese Academy of Sciences Center of Materials Science and Optoelectronics Engineering University of Chinese Academy of Sciences

Lithium argyrodites with high ionic conductivity and low cost are considered as one of the most prospective solid electrolytes for all-solid-state lithium ***,the poor chemical stability and compatibility with lithium metal limit their ***,Li5.4PS4.4Cl1.4I0.2solid electrolyte with high ionic conductivity of 11.49 m S cm-1and improved chemical stability is synthesized by iodine *** ultra-thin Li5.4PS4.4Cl1.4I0.2membrane with thickness of 10μm can be obtained by wet coating process,exhibiting a high ionic conductivity of 2.09 mS cm-1and low areal resistance of 1.17Ω***,iodine doping could in-situ form LiI at the lithium/electrolyte interface and improve the critical current density of Li5.4PS4.4Cl1.6from 0.8 to 1.35 mA *** resultant LiCoO2/Li5.4PS4.4Cl1.4I0.2/Li battery shows excellent cycling stability at 1 C,with a reversible specific capacity of 110.1 mA h g-1and a retention of 80.5% after 1000 *** addition,the assembled LiCoO2/Li5.4PS4.4Cl1.4I0.2membrane/Li pouch cell delivers an initial discharge capacity of 110.4 mA h g-1and 80.5% capacity retention after 100 cycles.

关键词： Argyrodite electrolytes Iodine doping Ionic conductivity Stability All-solid-state lithium battery