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Frontiers of Chemical Science and Engineering 2018年第3期12卷 473-480页

作者： Shenghua Ye Gaoren Li moe laboratory of bioinorganic and synthetic chemistry KLGHEI of Environment and Energy Chemistry School of Chemistry and Chemical Engineering Sun Yat-sen University Guangzhou 510275 China

Abstract The polypyrrole（PPy）@NiCo hybrid nanotube arrays have been successfully fabricated as a high performance electrocatalyst for hydrogen evolution reaction （HER） in alkaline solution. The strong electronic interactions between PPy and NiCo alloy are confirmed by X-ray photoelectron spectroscopy and Raman spectra. Because these interations can remarkably reduce the apparent activation energy （Ea） for HER and enhance the turnover frequency of catalysts, the electrocatalytic performance of PPy@NiCo hybrid nanotube arrays are significantly improved. The electrochemical tests show that the PPy@NiCo hybrid catalysts exhibit a low overpotential of-186 mV at 10.0 mA·cm^-2 and a small tafel slope of 88.6 mV·deg^-1 for HER in the alkaline solution. The PPy@NiCo hybrid nanotubes also exhibit high catalytic activity and high stability for HER.

关键词： NiCo alloy polypyrrole hybrid nanotube electrocatalyst hydrogen evolution reaction

The development of an iridium(Ⅲ) complex functionalized G-quadruplex probe for the stability of G-quadruplex and lifetime image in cytoplasm

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中国化学快报：英文版 2023年第2期34卷 397-402页

作者： Shaokang Jia Wenjin Wang Shanshan Qin Shengjie Xie Lisi Zhan Qi Wei Ziang Lu Xiaolu Zhou Cong Chen Kun Chen Shen Yan Caiping Tan Zongwan Mao Xiang Zhou College of chemistry and Molecular Sciences Key Laboratory of Biomedical Polymers-Ministry of EducationWuhan UniversityWuhan 430072China moe Key laboratory of bioinorganic and synthetic chemistry School of ChemistrySun Yat-sen UniversityGuangzhou 510275China

G-quadruplex(G4) is widely known as a non-classical secondary structure of nucleic acid. With the indepth study of G4, it is an urgent need for a phosphorescent probe with a high G4 binding ability to evaluate the level of G4 in the cytoplasm. Thus, this study designed and synthesized Ir-PDP where an Ir(Ⅲ)complex was used as a phosphorescent emitter. Meanwhile, two installed PDPs(pyridostatin derivatives)were used to improve the combination ability with G4 and reduced the cytotoxicity of the Ir(Ⅲ) complex.Compared with other nucleic acid secondary structures, Ir-PDP produced a higher phosphorescence lifetime after interacting with G4. Ir-PDP was distributed in the cytoplasm of living cells, and two-photon phosphorescence lifetime imaging can detect the binding events of the probe in the cytoplasm. The addition of G4 binder PDS significantly regulated cytoplasmic phosphorescence lifetime. The project explored a new sensing pathway to observe the binding manners of probes in the cytoplasm through the phosphorescence lifetime of probes.

关键词： G-quadruplex Pyridostatin derivatives Iridium(Ⅲ)complex Phosphorescent probe Phosphorescence lifetime Cell imaging

Spherical lanthanide nanoclusters toward white-light emission and cell membrane imaging

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Nano Research 2023年第8期16卷 11495-11502页

作者： Hai-Ling Wang Zhiqiang Ni Ze-Yu Ruan Zhong-Hong Zhu Pei-Yu Liao Guangxue Feng Jian-Hua Jia Ming-Liang Tong Key laboratory of bioinorganic and synthetic chemistry of Ministry of Education School of ChemistrySun Yat-Sen UniversityGuangzhou 510006China State Key laboratory of Luminescent Materials and Devices Guangdong Provincial Key Laboratory of Luminescence from Molecular AggregatesSchool of Materials Science and EngineeringSouth China University of TechnologyGuangzhou 510640China

Lanthanide doping is an effective strategy for modulating the emission of emitters.Herein,by changing the cluster composition to control the energy transfer pathway,the application potential of high-nuclearity lanthanide cluster(HLC)as white-light emitter has been confirmed for the first time.Specifically,by precisely controlling the proportion of GdIII,TbIII,and EuIII ions in reactants,we obtained a spherical heterotrimetallic nanocluster Gd_(10)Tb_(12)Eu_(10),a white-light emitter with quantum yield(QY)of 12.58%and lifetime of 327.14μs.High-resolution electrospray ionization mass spectrometry(HRESI-MS)demonstrates that homometallic nanoclusters Ln_(32)(Ln=Gd,Tb,and Eu)are tetracationic clusters and are highly stable in solution.The peripheral dense organic ligands provide a protective layer for the cluster core,which improves the stability of Ln_(32) in aqueous solution,avoids the contact between metal centers and bioactive molecules,and greatly reduces the biological toxicity.In cell imaging experiments,cationic clusters Ln_(32) are mainly localized on the cell membrane with negative charge distribution.As far as we know,this is the first time that spherical lanthanide nanoclusters have been used for membrane imaging of living cell,opening the door for the application of HLCs in biological imaging.

关键词： spherical lanthanide clusters white-light emission high stability low toxicity cell membrane imaging

Layered-stacking of titania films for solar energy conversion:Toward tailored optical,electronic and photovoltaic performance

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Journal of Energy chemistry 2018年第3期27卷 690-702页

作者： Wu-Qiang Wu Jin-Feng Liao Dai-Bin Kuang moe Key laboratory of bioinorganic and synthetic chemistry School of ChemistrySun Yat-sen University.Guangzhou 510275Guangdong.China

Nanostructured TiO2 with differentiate morphologies has attracted tremendous attention due to its wide band-gap nature as well as outstanding optical and electric properties for solar-driven light-toelectricity conversion application. Layered-stacking TiO2 film such as double-layer, tri-layer, quadrupleor quintuplicate-layer, is highly desirable to the design of high-performance semiconductor material photoanodes and the development of advanced photovoltaic devices. In this minireview, we will summarize the recent progress and achievements on proof-of-concept of layered-stacking TiO2 films（LTFs） for solar cells with emphasis on the tailored properties and synergistic functionalization of LTFs, such as optimized sensitizer adsorption, broadened light confinement as well as facilitated electron transport characteristics.Various demonstrations of LTFs photovoltaic systems provide lots of possibilities and flexibilities for more efficient solar energy utilization that a wide variety of TiO2 with distinguished morphologies can be integrated into differently structured photoanodes with synergistic and complementary advantages. This key structure engineering technology will also pave the way for the development of next generation state-ofthe-art electronics and optoelectronics. Finally, from our point of view, we conclude the future research interest and efforts for constructing more efficient LTFs as photoelectrode, which will be highly warranted to advance the solar energy conversion process.

关键词： TiO2 Charge transport Light scattering Power conversion efficiency Solar cells

Calibration of local chemical pressure by optical probe

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National Science Review 2023年第9期10卷 258-269页

作者： Xiao Zhou Mei-Huan Zhao Shan-Ming Yao Hongliang Dong Yonggang Wang Bin Chen Xianran Xing Man-Rong Li Key laboratory of bioinorganic and synthetic chemistry of Ministry of Education School of ChemistrySun Yat-sen University Center for High Pressure Science and Technology Advanced Research School of Materials Science and Engineering Peking University Beijing Advanced Innovation Center for Materials Genome Engineering Institute of Solid State Chemistry University of Science and Technology Beijing School of Science Hainan University

Chemical stabilization of a high-pressure metastable state is a major challenge for the development of advanced materials.Although chemical pressure(Pchem) can effectively simulate the effect of physical pressure(Pphy)) experimental calibration of the pressure passed to local structural motifs,denoted as local chemical pressure(Pchem-△) which significantly governs the function of solid materials,remains absent due to the challenge of probing techniques.Here we establish an innovative methodology to experimentally calibrate the Pchem-△and build a bridge between Pchemand Pphyvia an optical probe strategy.Site-selective Bi3+-traced REVO4(RE=Y,Gd) is adopted as a prototype to introduce Bi3+optical probes and on-site sense of the Pchem-△experienced by the REO8motif.The cell compression of RE0.9gBi0.02VO4under Pphyis chemically simulated by smaller-ion substitution(Sc3+→RE3+) in RE0.98-xScxBi0.02VO4.The consistent red shift(△λ) of the emission spectra of Bi3+,which is dominated by locally pressure-induced REO8dodecahedral variation in RE0.98Bi0.02VO4(Pphy) and RE0.98-xScxBi0.02VO4(Pchem-△),respectively,is evidence of their similar pressure-dependent local structure evolution.This innovative △λ-based experimental calibration of Pchem-△in the crystal-field dimension portrays the anisotropic transmission of Pchemto the local structure and builds a bridge between Pchem-△and Pphyto guide a new perspective for affordable and practical interception of metastable states.

关键词： chemical pressure high pressure ion substitution optical parameter spectra shift pressure calibration

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),respectively.Single-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 bottle.Guest-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

Structural tuning of coordination polymers by 4-connecting metal node and secondary building process

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Chinese Chemical Letters 2019年第6期30卷 1297-1301页

作者： Chaojie Li Zhangwen Wei Mei Pan Haiying Deng Jijun Jiang Chengyong Su moe laboratory of bioinorganic and synthetic chemistry Lehn Institute of Functional Materials School of ChemistrySun Yat-sen University

Five transition metal coordination polymers,{[Cu(4-pmntd)2(NO3)2]·2CHCl3}n (1),{[Cu(4-pmntd)2(NO3)2]· 3C7H8}n (2),{[Cu(4-pmntd)2(CF3SO3)(H2O)]·CF3SO3·H2O·CH3OH}n (3),[Cd(4-pmntd)2]n·nSiF6·x(CH3OH)· y(CHCl3)(4), and [Zn(4-pmntd)2(CF3SO3)2]n·x(solvent)(5), have been obtained from a ditopic ligand, N,N'-bis(4-pyridylmethyl)naphthalene diimide (4-pmntd). Either sql-or dia-structures are generated from four connecting coordination nodes of the metal centers. While delicate interpenetration and structural tuning in these complexes is achieved by the different conformations and spatially extending geometries adopted by the ligand and"secondary building process"induced by pillar-like anions.

关键词： Coordination polymer Structural tuning Interpenetration Pillar anions Secondary building process

A facile method to fabricate high-quality perovskite nanocrystals based on single crystal powder

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Nano Research 2019年第10期12卷 2640-2645页

作者： Jin-Feng Liao Yi-Xin Chen Jun-Hua Wei Ya-Ting Cai Xu-Dong Wang Yang-Fan Xu Dai-Bin Kuang moe Key laboratory of bioinorganic and synthetic chemistry Lehn Institute of Functional MaterialsSchool of ChemistrySun Yat-sen UniversityGuangzhou 510275China

Although great advancements have been successfully achieved in ligand-assisted reprecipitation strategy(LARP)towards lead halide perovskite nano crystals(NCs)syn thesis,it still remains challe nging to develop bright and stable iodide-based perovskite NC via facile LARP.Herein,striki ngly bright MAPbl3 NCs with photoluminesce nee qua ntum yield(PLQY)as high as 79%are synthesized via replacing the raw material(MAI and Pbh)with MAPbl3 crystal powder during LARP procedure.It has been found that crystal powder derived MAPbl3 NCs are more iodide-rich compared with that based on raw material,which is favorable to passivate the surface trap state.Accordingly,femtosecond transient absorption spectroscopies and space charge limited current measurements have corroborated that the trap density is much less in crystal powder resulted MAPbl3 NCs.Further analyses indicate stronger solvation with reduced precursor colloid size has been observed in crystal powder derived precursor solution probably due to the formation of MAPbl3-DMF.This work has provided a facile but valid method to enhance the photoluminesce nee of perovskite NC via modulati ng the beginning precursor solution.

关键词： MAPbh nanocrystal perovskite transient absorption light emitting

Facile preparation and magnetic study of amorphous Tm-Fe-Co-Ni-Mn multicomponent alloy nanofilm

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Journal of Rare Earths 2011年第2期29卷 133-137页

作者：姚陈忠卫博慧张鹏卢锡洪刘鹏童叶翔 moe of Key laboratory of bioinorganic and synthetic chemistry/School of chemistry and Chemical Engineering Sun Yat-Sen University Department of Applied chemistry Yuncheng University

A facile and efficient synthesis route for the preparation of Tm-Fe-Co-Ni-Mn multicomponent alloy films was reported.Here the films with nanostructures were successfully synthesized by electrodeposition at room temperature.By changing the electrodeposition parameters,such as the deposition potential,deposition time,and the substrates,the styles of the nanostructures and surface morphologies of the deposits could be well controlled.The energy dispersive spectrometer （EDS） indicated that the five elements were co-deposited.The result of XRD suggested that the film was amorphous.The as-deposited alloys showed soft magnetic and superparamagnetic behavior,and the magnetic particles were frozen step by step in the freezing process.

关键词： electrodeposition nano-film multicomponent alloy magnetic properties rare earths

Thermal expansion behaviors of Mn(Ⅱ)-pyridylbenzoate frameworks based on metal-carboxylate chains

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Science China chemistry 2014年第3期57卷 365-370,1-3页

作者： ZHOU HaoLong Li Mian LI Dan ZHANG JiePeng CHEN XiaoMing moe Key laboratory of bioinorganic and synthetic chemistry School of Chemistry and Chemical Engineering Sun Yat-Sen University Department of chemistry Shantou University

Solvothermal reactions of MnCl2with pyridylbenzoic acids gave three-dimensional metal-carboxylate frameworks(MCFs),named MCF-34,MCF-43,and MCF-44,based on one-dimensional Mn-carboxylate chains.The crystal structure,stability,porosity,and framework flexibility of the new compound MCF-44 were studied in detail and compared with its analogs.Depending on their shapes and the bridging angles of the ligands,these compounds possess different network connectivities and porosities.Considering the pyridylbenzote ligands and Mn(II)ions as,respectively,3-and 6-connected nodes,they resemble either the anatase(ant)or rutile(rtl)polymorph of TiO2.Variable-temperature single-crystal X-ray diffraction studies revealed large thermal expansion coefficients for these compounds,which are probably related to the relatively flexible edge-sharing polyhedral structure of their Mn-carboxylate chains.Interestingly,the new compound MCF-44,with its highly porous rtl structure exhibits the largest thermal expansion coefficienct among the coordination polymers reported so far.

关键词：热膨胀行为羧酸甲酯框架金属 Mn 金红石型二氧化钛单晶X-射线衍射链