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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

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

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

Bi nanoparticles in situ encapsulated by carbon film as high-performance anode materials for Li-ion batteries

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Journal of Energy chemistry 2022年第6期31卷 524-530,I0015页

作者： Jun Yang Jiahui Xian Qinglin Liu Yamei Sun Guangqin Li MOE Laboratory of Bioinorganic and Synthetic Chemistry Lehn Institute of Functional MaterialsSchool of ChemistrySun Yat-Sen UniversityGuangzhou 510006GuangdongChina

Bismuth (Bi) has indeed inspired great interests in lithium-ion batteries (LIBs) due to the high capacity,but was still limited by the low electrical conductivity and large volume variation.Herein,a composite material based on Bi nanoparticles in situ encapsulated by carbon film (Bi@CF) is prepared successfully through a facile metal–organic framework (MOF)-engaged approach.As anode materials for LIBs,the Bi@CF composites achieved high reversible capacities of 705 and 538 mAh g^(-1)at 0.2 and 0.5 A g^(-1) after200 cycles,and long cycling performance with a stable capacity of 306 mAh g^(-1)at 1.0 A g^(-1) even after 900 cycles.In situ X-ray diffraction (XRD) measurements clearly revealed the conversion between Bi and Li_(3)Bi during the alloying/dealloying process,confirming the good electrochemical reversibility of Bi@CF for Li-storage.The reaction kinetics of this Bi@CF composite was further studied by galvanostatic intermittent titration technique (GITT).This work may provide an inspiration for the elaborate design and facile preparation of alloy-type anode materials for high-performance rechargeable batteries.

关键词： Bi nanoparticles Carbon film Anode materials Lithium-ion batteries In situ XRD

Thermal expansion-quench of nickel metal-organic framework into nanosheets for efficient visible light CO_(2) reduction

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Chinese Chemical Letters 2023年第2期34卷 249-253页

作者： Liuyong Chen Qinglin Liu Jun Yang Yinle Li Guangqin Li MOE Laboratory of Bioinorganic and Synthetic Chemistry Lehn Institute of Functional MaterialsSchool of ChemistrySun Yat-sen UniversityGuangzhou 510275China

Metal-organic framework nanosheets (MOF NNs) offer potential opportunities for many applications,but an efficient strategy for the scalable preparation of few-layered two-dimensional (2D) MOF NNs are still a major challenge.Herein,we present an efficient top-down method for the synthesis of the Ni-BDC(Ni_(2)(OH)_(2)(1,4-BDC);1,4-BDC=1,4-benzenedicarboxylate) nanosheets utilizing a novel thermal expansionquench method of the flowerlike bulky MOFs in liquid N2.The obtained Ni-BDC nanosheets exhibit significantly enhanced photocatalytic performance of reductive CO_(2)deoxygenation (7.0μmol h^(-1)mg^(-1)) under visible light illumination compared with the bulky MOFs,due to much higher surface area for CO_(2)adsorption,more abundant active sites exposed and stronger electron transport ability of the nanosheets.More importantly,this synthetic strategy can be extended to fabricate other MOF nanosheets which also exhibit significantly improved performance for deoxygenative CO_(2)reduction compared to their bulky counterparts.This work may provide a guideline for preparing other 2D layered photocatalysts materials to realize energy conversion applications.

关键词： Thermal expansion-quench Metal-organic framework(MOF) Two-dimensional Ni-BDC nanosheets Visible light CO_(2)photoreduction

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