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Real-time tracking of ER turnover during ERLAD by a rhenium complex via lifetime imaging

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National Science Review 2022年第7期9卷 80-87页

作者： Liang Hao Yu-Yi Ling Zhi-Xin Huang Zheng-Yin Pan Cai-Ping Tan Zong-Wan Mao moe key laboratory of bioinorganic and synthetic chemistry School of ChemistryState Key Laboratory of Oncology in South China Sun Yat-Sen University

Endoplasmic reticulum(ER) degradation by autophagy(ER-phagy) is a recently revealed selective autophagy pathway that plays important roles in organelle turnover and protein degradation,but the biological functions of ER-phagy are largely unknown.Here,we present an ER-targeting Re(I) tricarbonyl complex(Re-ERLAD) that can accumulate in the ER,induce ER-to-lys osome-associated degradation(ERLAD) upon visible light irradiation,and label ER buds and track their morphological alterations during ER-phagy.The emission of Re-ERLAD is sensitive to viscosity,which is a key parameter reflecting the amount of unfolded protein in the ER.Quantitative detection using two-photon fluorescence lifetime imaging microscopy shows that ER viscosity initially increases and then decreases during ERLAD,which reveals that ERLAD is a pathway for alleviating ER stress caused by unfolded proteins.In conclusion,our work presents the first specific photoinducer and tracker of ERLAD,which can be used in studying the regulatory mechanism and function of this process.

关键词： rhenium ER-phagy viscosity TPFLIM

A partially fluorinated ligand for two super-hydrophobic porous coordination polymers with classic structures and increased porosities

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National Science Review 2021年第3期8卷 99-107页

作者： Chao Wang Dong-Dong Zhou You-Wei Gan Xue-Wen Zhang Zi-Ming Ye Jie-Peng Zhang moe key laboratory of bioinorganic and synthetic chemistry School of ChemistrySun Yat-Sen University

3-Ethyl-5-trifluoromethyl-1,2,4-triazole is synthesized by a one-pot reaction.Using this asymmetric triazole ligand bearing one trifluoromethyl and one ethyl as side groups,we construct two new porous coordination polymers,MAF-9 and MAF-2 F,being isostructural with the classic hydrophobic and flexible materials,FMOF-1 and MAF-2,based on symmetric triazole ligands bearing two trifluoromethyl groups or two ethyl groups,respectively.MAF-9 and MAF-2 F can adsorb large amounts of organic solvents but completely exclude water,showing superhydrophobicity with water contact angles of 1520 in between those of FMOF-1 and MAF-2.MAF-9 exhibits very large N-induced breathing and colossal positive and negative thermal expansions like FMOF-1,but the lower molecular weight and smaller volume of MAF-9 give 16%and 4% higher gravimetric and volumetric Nuptakes,respectively.In contrast,MAF-2 F is quite rigid and does not show the inversed temperature-dependent Nadsorption and large guest-induced expansion like MAF-2.Further,despite the higher molecular weight and larger volume,MAF-2 F possesses 6% and 25%higher gravimetric and volumetric COuptakes,respectively.These results can be explained by the different pore sizes and side group arrangements in the two classic framework prototypes,which demonstrate the delicate roles of ligand side groups in controlling porosity,surface characteristic and flexibility.

关键词： porous coordination polymers metal-organic frameworks super-hydrophobicity flexibility

Local Weak Hydrogen Bonds Significantly Enhance CO_(2)Electroreduction Performances of a Metal-Organic Framework

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CCS chemistry 2023年第1期5卷 145-151页

作者： Yu Wang Ning-Yu Huang Hao-Yu Wang Xue-Wen Zhang Jia-Run Huang Pei-Qin Liao Xiao-Ming Chen Jie-Peng Zhang moe key laboratory of bioinorganic and synthetic chemistry School of ChemistrySun Yat-Sen UniversityGuangzhou 510275

Technological application of the electrochemical reduction of CO_(2)relies on efficient electrocatalysts.We demonstrate that the introduction of amino groups alongside the porphyrin cobalt centers in a metal-organic framework(MOF)can dramatically accelerate the electrochemical CO_(2)reduction performance.A classic cobalt porphyrin-based MOF showing moderate CO_(2)-to-CO electroreduction performance(turnover frequency[TOF]=0.20 s^(−1),Faradic efficiency[FE]=47.4%)is modified.By molecular design of the porphyrin-based ligand,amino groups are introduced alongside the cobalt center,giving remarkably enhanced CO_(2)-to-CO electroreduction performance as high as FE 99.4%,current density 7.2 mA cm^(−2),and TOF 21.17 s^(−1),in a nearneutral aqueous solution at a low overpotential of 525 mV.Density functional theory calculations showed that the prepositioned amino groups,although located not sufficiently close to the active center,serve as hydrogen-bonding donors to stabilize the intermediate Co-CO_(2)adduct and impede the formation of Co-H_(2)O adduct,which not only promotes the CO_(2)reduction reaction but also restrains the hydrogen evolution reaction.

关键词： CO_(2)electroreduction metal-organic frameworks hydrogen bond porphyrin amino groups

Crystal structures and phase transitions in two new hybrid crystals: (Me_(3)NCH_(2)CH_(2)X)_(4)[Ni(NCS)_6](X=Cl and Br)

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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 materials.Herein,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 transitions.Specifically,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 0.0475.Whereas the Br-substituted cations with larger steric effect prevent the solid-solid phase transition but give a solid-liquid phase transition at above 419 K.The 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

一例具有高低温双铁弹性的新型杂化晶体:(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：刘德轩陈晓娴叶子铭张伟雄陈小明 moe key laboratory of bioinorganic and synthetic chemistry School of ChemistrySun Yat-Sen UniversityGuangzhou 510275China

本文报道了一例具有反XeF4结构的新型杂化晶体(Me_(3)NCH_(2)-CH_(2)OH)_(4)[Ni(NCS)_(6)],其分子组分的较复杂有序-无序转变使得该化合物在269和360 K发生两步可逆相变.这两步相变伴随着P2_(1)/n-P4/mnc-Bmab的空间群变化,即分别属于... 详细信息

本文报道了一例具有反XeF4结构的新型杂化晶体(Me_(3)NCH_(2)-CH_(2)OH)_(4)[Ni(NCS)_(6)],其分子组分的较复杂有序-无序转变使得该化合物在269和360 K发生两步可逆相变.这两步相变伴随着P2_(1)/n-P4/mnc-Bmab的空间群变化,即分别属于正常的降温对称性破缺和反常的升温对称性破缺现象,因此使得该化合物可在低温和高温均展现出铁弹性(自发极化强度分别为0.0603和0.0073).这种不同寻常的高低温双铁弹性的发现和研究,有助于加深对反常对称性破缺相变的理解,并为今后在分子杂化晶体中探索高温铁性材料提供重要线索.

关键词：对称性破缺可逆相变铁弹性高低温杂化 NCS

构建三元WO_(3)/CsPbBr_(3)/ZIF-67异质结用于高效光催化CO_(2)还原

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Science China Materials 2022年第6期65卷 1550-1559页

作者：董玉杰江勇廖金凤陈洪燕匡代彬苏成勇 moe key laboratory of bioinorganic and synthetic chemistry Lehn Institute of Functional MaterialsSchool of ChemistrySun Yat-sen UniversityGuangzhou 510006China

近年来,卤素钙钛矿纳米材料以其优异的光电性能在光催化等领域引起了关注.然而,光生载流子严重的复合反应和较差的反应动力学也极大地限制了其光催化性能.本论文设计合成了一种三元WO_(3)/CsPbBr_(3)/ZIF-67异质光催化剂,并将其应用于... 详细信息

近年来,卤素钙钛矿纳米材料以其优异的光电性能在光催化等领域引起了关注.然而,光生载流子严重的复合反应和较差的反应动力学也极大地限制了其光催化性能.本论文设计合成了一种三元WO_(3)/CsPbBr_(3)/ZIF-67异质光催化剂,并将其应用于有效的CO_(2)光还原反应.研究表明,WO_(3)与CsPbBr_(3)之间构建的Z型电荷转移路径能够保证光生载流子的有效转移和分离.此外,在表面修饰具有活性Co中心的ZIF-67壳层作为助催化剂有利于改善复合材料的CO_(2)的吸附和活化能力.因此,电荷分离和CO_(2)吸附性能的增强大大提高了WO_(3)/CsPbBr_(3)/ZIF-67的光催化活性,还原产物中CO产率达到99.38μmol g_(−1),是单一CsPbBr_(3)的6.8倍.这项工作有望为开发高效的卤素钙钛矿基光催化剂及其在CO_(2)还原和其他复杂光催化反应中的应用提供参考.

关键词： Z-scheme heterojunction halide perovskite CO_(2)photoreduction heterostructure charge separation

Te^(4+)掺杂Cs_(2)InCl_(5)·H_(2)O单晶的光学测温应用

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Science China Materials 2022年第3期65卷 764-772页

作者：魏俊华罗健彬廖金凤区维韬匡代彬 moe key laboratory of bioinorganic and synthetic chemistry Lehn Institute of Functional MaterialsSchool of ChemistrySun Yat-sen UniversityGuangzhou 510275China

本文设计合成了一种Te^(4+)离子掺杂的Cs_(2)InCl_(5)·H_(2)O单晶,该单晶在紫外光激发下发射明亮橙光.未掺杂的Cs_(2)InCl_(5)·H_(2)O单晶几乎没有发光现象,但Te^(4+)掺杂的Cs_(2)InCl_(5)·H_(2)O单晶,发射峰位于660 nm,并伴随着大的Stokes位移和宽的发光半峰宽(180 nm).结合变温荧光光谱以及飞秒瞬态吸收光谱等表征,揭示了其发光机理为自陷激子发光.零维结构中的强电声耦合以及软晶格有利于形成并稳定自陷激子.特别地,由于Te^(4+)离子的最外层电子结构为5s^(2),对温度变化较为灵敏,Te^(4+)离子掺杂的Cs_(2)InCl_(5)·H_(2)O单晶的发光寿命表现出了非常强的温度依赖性,发光寿命从80 K下的6μs缩短至380 K下的19 ns,320 K处的相对灵敏度达到0.062 K^(-1),可以与传统稀土基光学测温材料相媲美.据我们所知,这是首次将铟基金属卤化物钙钛矿单晶应用于光学测温,将为设计合成新型多功能响应的金属卤化物钙钛矿发光材料提供借鉴意义.

关键词：金属卤化物温度依赖性相对灵敏度发光现象发光材料紫外光激发设计合成离子掺杂

Catalytic Enantioselective Construction of Chiral Benzo-Fused N-Heterocycles through Friedel-Crafts-Type Electrophilic Chlorination

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CCS chemistry 2022年第5期4卷 1486-1498页

作者： Jie Luo Yuanyuan Zhang Fuming Zhong Xiaodan Zhao Institute of Organic chemistry and moe key laboratory of bioinorganic and synthetic chemistry School of ChemistrySun Yat-sen UniversityGuangzhou 510275

Chiral benzo-fused N-heterocycles are frequently found in natural and synthetic products.However,their synthesis usually suffers from different limitations such as difficulty in accessing appropriate starting materials and unsatisfactory stereoselectivities.In this work,an unprecedented chiral sulfide-catalyzed enantioselective Friedel-Crafts-type electrophilic chlorination is shown to construct various 3,4-functionalized tetrahydroquinolines with excellent enantio-and diastereoselectivities from readily available aniline derivatives.Interestingly,employing N-allyl 1-naphthanilides as substrates,divergent reactions via chlorocarbocyclization and dearomatization occurred to afford two chiral polycyclic benzo-fused N-heterocycles.The system that we developed extends the scope of asymmetric chlorination to general substrateswithout the need of a N-H group,and significantly promotes the synthesis of enantioenriched benzo-fused N-heterocycles.

关键词： benzo-fused N-heterocycles asymmetric synthesis chiral sulfide catalysis electrophilic chlorination dearomatization divergent reactions

以NH3OH^+/NH2NH3^+作为B位阳离子的无金属六方钙钛矿含能材料

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Engineering 2020年第9期6卷 1144-1150页

作者：尚宇余志鸿黄瑞康陈劭力刘德轩陈晓娴张伟雄陈小明 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