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Research 2019年第1期2019卷 433-441页

作者： Xiao Yang Hao-Long Zhou Chun-Ting He Zong-Wen Mo Jia-Wen Ye Xiao-Ming Chen Jie-Peng Zhang MOE Key laboratory of bioinorganic and Synthetic Chemistry School of ChemistrySun Yat-Sen UniversityGuangzhou 510275China

Understanding,controlling,and utilizing the flexibility of adsorbents are of great importance and *** with conventional solid materials,downsizing to the nanoscale is emerging as a possible strategy for controlling the flexibility of porous coordination polymers(or metal-organic frameworks).We report a unique flexibility controllable by crystal size at the micrometer to submillimeter *** removal transforms[Cu_(2)(pypz)_(2)]·0.5p-xylene(MAF-36,Hpypz=4-(1H-pyrazol-4-yl)pyridine)with one-dimensional channels toα-[Cu_(2)(pypz)_(2)]with discrete small cavities,and further heating gives a nonporous isomerβ-[Cu_(2)(pypz)_(2)].Both isomers can adsorb p-xylene to give[Cu_(2)(pypz)_(2)]·0.5p-xylene,meaning the coexistence of guest-driven flexibility and shape-memory *** phase transition temperature fromα-[Cu_(2)(pypz)_(2)]toβ-[Cu_(2)(pypz)_(2)]decreased from~270℃ to~150℃ by increasing the crystal size from the micrometer to the submillimeter scale,ca.2-3 orders larger than those of other size-dependent ***-crystal X-ray diffraction showed coordination bond reconstitution and chirality inversion mechanisms for the phase transition,which provides a sufficiently high energy barrier to stabilize the metastable phase without the need of downsizing to the *** virtue of the crystalline molecular imprinting and gate-opening effects,α-[Cu_(2)(pypz)_(2)]andβ-[Cu_(2)(pypz)_(2)]show unprecedentedly high p-xylene selectivities of 16 and 51,respectively,as well as ultrafast adsorption kinetics(<2 minutes),for xylene isomers.

关键词： isomers coordination adsorbent

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 *** 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

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

Polypyrrole@NiCo hybrid nanotube arrays as high performance electrocatalyst for hydrogen evolution reaction in alkaline solution

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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

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 ***,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 *** 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 *** 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 *** 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

A novel pillared-layer-type porous coordination polymer featuring three-dimensional pore system and high methane storage capacity

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Science China Chemistry 2016年第8期59卷 970-974页

作者： Jiao-Min Lin Chun-Ting He Pei-Qin Liao Dong-Dong Zhou Jie-Peng Zhang Xiao-Ming Chen Key laboratory of bioinorganic and Synthetic Chemistry Ministry of EducationSchool of Chemistry and Chemical Engineering Sun Yat-Sen University Guangzhou 510275 China

Solvothermal reaction of Zn（NO3）2, 4-（1H-pyrazol-4-yl）pyridine （Hpypz） and 1,3,5-benzenetricarboxylic acid （H3btc） in N,N-dimethylacetamide （DMA） produced a new porous coordination polymer [Zns（pypz）4（btc）2] （1）. Single-crystal X-ray diffraction study of 1 showed that deprotonated pypz^- ligands served as 1,2,4-triazolate-like ligands, linking Zn（II） ^＋ ions to form porous two-dimensional （2-D） sql-a layers {Zn（pypz）} , which were further connected by eight-legged pillars {Zn2（btc）4（H2O）2}8- based on the typical paddlewheel dinuclear Zn2（RCOO）4（H20）2 cluster to form a novel type of non-interpenetrated pillared-layer framework with 3-D intersecting pore system and large pore volume. Gas sorption measurements revealed that 1 possesses large BET surface area of 2061 m^2g^-1 and very high methane total uptake of 245 cm^3（STP） cm^-3 at 298 K and 65 bar.

关键词： metal-organic framework network topology eight-legged pillar methane storage

Controlling flexibility of metal–organic frameworks

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National Science Review 2018年第6期5卷 907-919页

作者： Jie-Peng Zhang Hao-Long Zhou Dong-Dong Zhou Pei-Qin Liao Xiao-Ming Chen MOE Key laboratory of bioinorganic and Synthetic Chemistry School of ChemistrySun Yat-Sen University Department of Chemistry and Key laboratory for Preparation and Application of Ordered Structural Materials of Guangdong Province Shantou University

Framework flexibility is one of the most important characteristics of metal–organic frameworks(MOFs),which is not only interesting, but also useful for a variety of applications. Designing, tailoring or controlling framework flexibility of MOFs is much more difficult than for static structural features such as the framework topology and pore size/shape. Nevertheless, with in-depth understanding of the relationship between framework flexibility and the host framework structure, guest loading and other aspects such as the crystal size/morphology and external physical environment, some strategies have been developed for controlling the flexibility of MOFs and the corresponding properties, which are summarized and discussed in this review.

关键词： porous coordination polymers metal–organic frameworks flexibility dynamism adsorption structural transformation

High-stability spherical lanthanide nanoclusters for magnetic resonance imaging

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National Science Review 2023年第4期10卷 123-132页

作者： Hai-Ling Wang Donglin Liu Jian-Hua Jia Jun-Liang Liu Ze-Yu Ruan Wei Deng Shiping Yang Si-Guo Wu Ming-Liang Tong Key laboratory of bioinorganic and Synthetic Chemistry of Ministry of Education School of Chemistry Sun Yat-sen University College of Chemistry and Materials Science Shanghai Normal University

High-nuclear lanthanide clusters have shown great potential for the administration of high-dose mononuclear gadolinium chelates in magnetic resonance imaging(MRI). The development of high-nuclear lanthanide clusters with excellent solubility and high stability in water or solution has been challenging and is very important for expanding the performance of MRI. We used N-methylbenzimidazole-2-methanol(HL) and LnCl3·6H2O to synthesize two spherical lanthanide clusters, Ln32(Ln = Ho, Ho32; and Ln =Gd, Gd32), which are highly stable in solution. The 24 ligands L-are all distributed on the periphery of Ln32and tightly wrap the cluster core, ensuring that the cluster is stable. Notably, Ho32can remain highly stable when bombarded with different ion source energies in HRESI-MS or immersed in an aqueous solution of different pH values for 24 h. The possible formation mechanism of Ho32was proposed to be Ho(Ⅲ),(L)-and H2O → Ho3(L)3/Ho3(L)4→ Ho4(L)4/Ho4(L)5→ Ho6(L)6/Ho6(L)7→ Ho16(L)19→Ho28(L)15→ Ho32(L)24/Ho32(L)21/Ho32(L)23. To the best of our knowledge, this is the first study of the assembly mechanism of spherical high-nuclear lanthanide clusters. Spherical cluster Gd32, a form of highly aggregated Gd(Ⅲ), exhibits a high longitudinal relaxation rate(1 T, r1= 265.87 mM-1·s-1). More notably, compared with the clinically used commercial material Gd-DTPA, Gd32has a clearer and higher-contrast T1-weighted MRI effect in mice bearing 4T1 tumors. This is the first time that high-nuclear lanthanide clusters with high water stability have been utilized for MRI. High-nuclear Gd clusters containing highly aggregated Gd(Ⅲ) at the molecular level have higher imaging contrast than traditional Gd chelates; thus, using large doses of traditional gadolinium contrast agents can be avoided.

关键词： T1-weighted MRI lanthanide clusters high stability low toxicity assembly mechanism

Four-step spin-crossover in an oxamide-decorated metal-organic framework

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Chinese Chemical Letters 2022年第3期33卷 1381-1384页

作者： Siguo Wu Sukhen Bala Zeyu Ruan Guozhang Huang Zhaoping Ni Mingliang Tong Key laboratory of bioinorganic and Synthetic Chemistry of Ministry of Education School of ChemistrySun Yat-Sen UniversityGuangzhou 510275China

Spin-crossover(SCO)complexes with multiple spin states are promising candidates for high-order magnetic storage and multiple ***,by employing the N,N'-4-dipyridyloxalamide(dpo)ligand,we synthesize two Hofmann-type metal-organic frameworks(MOFs)[Fe(dpo){Ag(CN)_(2)}_(2)]·3DMF(1)and[Fe(dpo){Ag(CN)_(2)}_(2)]·0.5MeCN·2DEF(2),which exhibit guest dependent four-step SCO behaviors with the sequences of LS→~LS_(2/3)HS_(1/3)→LS_(1/2)HS_(1/2)→~LS_(3/10)HS_(7/10)→HS and LS→~LS_(2/3)HS_(1/3)→LS_(1/2)HS_(1/2)→~LS_(1/4)HS_(3/4)→HS,***,the incorporation of hydrogen-donating/hydrogen-accepting groups into the Hofmann-type MOFs may effectively explore the multi-step SCO materials by tuning hydrogen-bonding interactions.

关键词： Spin crossover Oxamide Metal-organic framework Hofmann-type Host-guest interaction

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 *** the films with nanostructures were successfully synthesized by electrodeposition at room *** 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 *** energy dispersive spectrometer （EDS） indicated that the five elements were *** result of XRD suggested that the film was *** 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