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Journal of Rare Earths 2024年第7期42卷 1298-1303,I0004页

作者： Pei-Yu Liao Yu-Quan Qi Zhen Li Jian-Hua Jia Ming-Liang Tong Key laboratory of bioinorganic and Synthetic Chemistry of Ministry of Education School of ChemistrySun Yat-Sen UniversityGuangzhou510006China

On account of the complicated magnetic exchange interactions between lanthanide ions,binuclear lanthanide complexes have broad application prospect in the field of single-molecule ***,it is necessary to develop reasonable bridging ligands to manipulate the directional assembly of binuclear lanthanide ***,we selected the macrocyclic ligand L^(N_(8)O_(2))to build up two new dilanthanide complexes[Ln_(2)(LN_(8)O_(2))(OpyO)_(2)(H_(2)O)2](NO_(3))_(2)(1-Ln,Ln=Dy,Tb;LN_(8)O_(2)=hexamethyl-tetraaza-dioxe-dipyrazolacycloicosaphane-2,9,12,19-tetraene;OpyOH=2-pyridinol-1-oxide).Dynamic magnetic studies show that 1-Dy exhibits slow relaxation behavior under a 1 kOe applied *** fitting analysis of relaxation times gives the effective energy barrier of 38.2 cm^(−1),and reveals that the slow magnetic relaxation behavior is dominated by the Orbach and Raman ***-resolution luminescence emission spectrum indicates the energy gap of 36.8 cm^(−1)between the ground state and the first excited state,consistent with the magnetic measurement results.1-Tb exhibits brilliant characteristic green light emission under UV light *** absolute quantum yield of 1-Tb is 44.8%,and its first-order fitted decay lifetime is 779.21μs at room *** study provides the way for directional construction of high-performance molecular materials with magnetic and optical dual-function.

关键词： Dilanthanide complexes Single-molecule magnets Macrocyclic ligand Photoluminescence behavior Rare earths

Upgrading waste NO_(x) into amino acids via electrocatalysis on Co nanoparticles encapsulated in hollow carbon nanofibers

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Science China Chemistry 2024年第6期67卷 1946-1952页

作者： Jiahui Xian Kaixing Cai Peisen Liao Shihan Wang Guangqin Li Key laboratory of bioinorganic and Synthetic Chemistry of Ministry of Education LIFMIGCMESchool of ChemistrySun Yat-Sen UniversityGuangzhou510275China

Electrocatalytic conversion of waste nitrogen oxide(NO_(x))into value-added nitrogenous chemicals,especially amino acid,is an emerging strategy to alleviate NO_(x)***,this process suffers from the coexistence of multiple competitive reactions leading to complex product distribution and low efficiency,and thus the rational design and modulation of efficient catalysts remains a formidable ***,well-designed Co nanoparticles encapsulated in hollow carbon nanofiber(CoHCNF)were constructed to promote the amino acid electrosynthesis via dealing waste NO_(x)coupling with biomass-derived keto *** to the rapid reactant diffusion,electron transport and efficient contact with abundant accessible Co catalytic sites stemmed from the unique hollow nanotubular structure,Co-HCNF manifested impressive glycine synthesis performance in one-pot adopting NO as the nitrogen source with Faradaic efficiency(FE)of 41.7%and a corresponding yield rate of 222.3μmol h^(-1)as well as 120 h robust ***,it also demonstrates an excellent performance with the FE of 42.8%for NO_(3)~-solution as the nitrogen ***,this strategy displays a broad universality for the synthesis of other amino *** work not only highlights the importance of hollow-structuring electrocatalyst towards upgrading wasted NO_(x)species into amino acids,but also promotes the further development of electrosynthetic systems for high-valued N-containing organic chemicals.

关键词： electrocatalysis NO_(x)reduction amino acid porous materials hollow structure

Precise immobilization of metal single atoms into a porphyrinic metal-organic framework for an efficient alkene hydrosilylation

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Nano Research 2024年第7期17卷 5914-5921页

作者： Chun-Ying Chen Qi-Jie Mo Fu-Zhen Li Hai-Li Song Li Zhang MOE laboratory of bioinorganic and Synthetic Chemistry Lehn Institute of Functional MaterialsSchool of ChemistrySun Yat-Sen UniversityGuangzhou 510006China

Alkene hydrosilylation is one of the most concise and atom-economical methods to synthesize organosilicon ***,we reported the precise immobilization of metal single atoms(M-SAs;M=Ru,Rh,Ir,Pd,Pt,and Au)into a porphyrinic metalorganic framework(MOF)of PCN-222(PCN=porous coordination network),and then applied the resultant MOF composites of M-SAs@PCN-222 to alkene *** solvent-free conditions,Pt-SAs@PCN-222 displayed an especially high catalytic efficiency with the turnover frequency up to 119 s−1 and the maximum turnover number of 906,250 at room *** and theoretical studies revealed that there existed strong interactions between Pt-SAs@PCN-222 and the substrates,which helped to condense the substrates in the cavities of the porous *** density functional theory calculations and molecular dynamics simulations disclosed that PCN-222 could transfer electrons to Pt-SAs to enhance the silane oxidative addition and drive the reaction to proceed smoothly via Chalk–Harrod pathway.

关键词： alkene hydrosilylation single atom catalysts metal-organic frameworks precision chemistry synergistic catalysis

Structural phase transition in a new organic-inorganic hybrid post-perovskite:(N,N-dimethylpyrrolidinium)[Mn(N(CN)_(2))_(3)]

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Chinese Journal of Structural Chemistry 2024年第6期43卷 40-44页

作者： Le Ye Wei-Xiong Zhang MOE Key laboratory of bioinorganic and Synthetic Chemistry School of ChemistryIGCMESun Yat-Sen UniversityGuangzhou510275China

In the realm of molecular phase transition research,particularly for applications in sensors,data storage and switching technologies,the role of organic-inorganic hybrid perovskite materials has been increasingly recognized for their significant ***,hybrid post-perovskites,as a critical subclass of perovskites,have not been thoroughly studied and mainly limit in the instances based on polyatomic bridging agents like dicyanamide(dca^(-))and non-cyclic organic ***,a polar cyclic quaternary ammonium cation,N,N-dimethylpyrrolidinium(DMP^(+)),was used to assemble a new hybrid post-perovskite,(DMP)[Mn(dca)_(3)](1),which undergoes a phase transition from orthorhombic Bmmb to monoclinic P2_(1)/n space group at 249 *** employing multiple techniques such as differential scanning calorimetry,variable-temperature single-crystal X-ray analysis,dielectric measurements,and Hirshfeld surface analysis,we disclosed the role of polar cyclic quaternary ammonium DMP^(+)in elevating the phase-transition temperature by 48 K,generating significant dielectric switching effect and facilitating interlayer sliding of inorganic framework.

关键词： Structural phase transitions Dielectric switching Organic-inorganic hybrid crystals Post-perovskites

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

High-throughput experimentation and machine learning-promoted synthesis of α-phosphoryloxy ketones via Ru-catalyzed P(O)O–H insertion reactions of sulfoxonium ylides

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Science China Chemistry 2024年

作者： An Lin Jingyuan Liu Yougen Xu Haiting Wu Yating Chen Yan Zhang Lebin Su Xiaodan Zhao Kuangbiao Liao Institute of Organic Chemistry & MOE Key laboratory of bioinorganic and Synthetic Chemistry School of Chemistry Sun Yat-sen University Guangzhou National laboratory Bioland laboratory

Herein, we report a novel and highly efficient method for the synthesis of α-phosphoryloxy carbonyl compounds via Rucatalyzed P(O)O–H insertion reactions of sulfoxonium ylides and phosphinic acids, with the assistance of high-throughput experimentation(HTE) and machine learning(ML). A variety of P(O)O-H derivatives, including diarylphosphates, alkyl phosphates, and alkoxyphosphates, are competent candidates to react with sulfoxonium ylides in this transformation, and variousα-phosphoryloxy carbonyls and propylene phosphates are directly constructed. This approach utilizes readily available sulfoxonium ylide as a carbene precursor, and features mild conditions, operational simplicity, and broad functional groups tolerance, and could be used for late-stage functionalization of structurally complex bioactive molecules. Moreover, a conducive exploration of the reaction space is also conducted(756 reactions) and a machine learning model for reaction yield prediction has been developed and applied, showcasing the practical application of this newly workflow(HTE-ML) in the field of synthetic chemistry.

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Engineering a high-barrier d-f single-molecule magnet centered with hexagonal bipyramidal Dy(Ⅲ)unit

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Science China Chemistry 2024年第10期67卷 3291-3298页

作者： Wei Deng Chan-Ying Yao Yan-Cong Chen Ying-Qian Zhou Shan-Nan Du Jun-Liang Liu Ming-Liang Tong Key laboratory of bioinorganic and Synthetic Chemistry of Ministry of Education School of ChemistryInstitute of Green Chemistry and Molecular EngineeringGuangdong Basic Research Center of Excellence for Functional Molecular EngineeringSun Yat-sen UniversityGuangzhou 510006China

In the pursuit of high-performance single-molecule magnets(SMMs),incorporating intramolecular magnetic coupling emerges as a pivotal *** these,d-f SMMs have garnered significant attention due to their remarkable versatility,which lies in their ability to tune coordination environments and facilely substitute metal ***,achieving performance-centric d-f SMMs through the synergistic interplay between highly anisotropic f ions and d-f magnetic interactions remains a formidable *** mononuclear hexagonal bipyramidal(D_(6h))Dy^(Ⅲ)SMMs have been successfully isolated,the exploration of d-f SMMs featuring D_(6h)-lanthanide metal centers remains uncharted *** this study,we employed planar bipodal ligands in conjunction with“staple-like”axial phenoxide ligands to synthesize the first hexagonal bipyramidal d-f ***,this compound exhibits alternating-current magnetic susceptibilities peaking up to 68 K with an energy barrier surpassing 1,200 K,thus establishing a new benchmark within the heterometallic d-f SMM landscape inclusive of complexes with diamagnetic d metals and paramagnetic f ***,the ferromagnetic interaction at the d-f sites engenders oscillating relaxation times contingent on the magnetic field—a characteristic distinct from mononuclear *** findings shed light on a deliberate design approach for d-f SMMs,emphasizing the cooperative utilization of high-barrier lanthanide modules alongside d ions through magnetic *** synergy significantly enhances and diversifies the magnetic dynamics of these intriguing molecular systems.

关键词： single-molecule magnets magnetic coupling crystal engineering hexagonal bipyramid energy barrier

Light-induced stepped thermal relaxation in a Hofmann-type metal-organic framework

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Science China Chemistry 2024年第6期67卷 1983-1989页

作者： Wen Cui Wei-Wei Wu Ze-Yu Ruan Yan-Cong Chen Guang-Jun Zeng Guan-Xi Chen Si-Guo Wu Zhao-Ping Ni Ming-Liang Tong Key laboratory of bioinorganic and Synthetic Chemistry of Ministry of Education School of ChemistryInstitute of Green Chemistry and Molecular EngineeringGuangdong Basic Research Center of Excellence for Functional Molecular EngineeringSun Yat-sen UniversityGuangzhou510275China

Spin-crossover(SCO)materials with light-induced multistability have potential applications in multi-addressable opto-magnetic memory devices and multiple ***,we reported a three-dimensional Hofmann-type metal-organic framework(MOF)[Fe(bpy){Pt(CN)_(4)}]·coumarin(1·coumarin,bpy=4,4′-bipyridine),which exhibits an incomplete and hysteretic SCO *** importantly,the light-induced stepped thermal relaxation(LISTR)with obvious magnetic plateau for a hidden intermediate spin state is firstly *** hidden spin state is also observed for the first time in the thermal relaxation after light-assisted spin state annealing(LASSA).Meanwhile,an extremely rare bi-directional light-induced excited spin-state trapping(LIESST)with the highest reverse-LIESST temperature is ***,five spin states can be captured in 1·coumarin and the tristability can be modulated below 102 K through the excitation-relaxation ***,the light-and temperatureinduced multistability provides a new strategy for developing multistable materials.

关键词： light magnetic multistability iron metal-organic framework spin-crossover

A Stable Copper-based Metal-Azolate Framework for Efficient Electroreduction of CO_(2)to C_(2+)Products

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Chemical Research in Chinese Universities 2024年第4期40卷 664-669页

作者： LIU Yuan-Yuan ZHU Hao-Lin LIAO Pei-Qin CHEN Xiao-Ming Key laboratory of bioinorganic and Synthetic Chemistry Ministry of EducationGBRCE for Functional Molecular EngineeringSchool of ChemistryIGCMESun Yat-sen UniversityGuangzhou510275P.R.China Chemistry and Chemical Engineering Guangdong laboratory Shantou515031P.R.China

Driven by renewable or excess electrical energy,electrochemical CO_(2)reduction reaction(eCO_(2)RR)represents a promising carbon-neutral approach to generating valuable low-carbon fuels by consuming CO_(2)and H_(2)O.C_(2+)products are one of the most economically valuable products among the reduction species of eCO_(2)RR,but there are still some challenges,such as low selectivity or low current *** this work,we showed that a copper-based metal-azolate framework(MAF),denoted as MAF-203,exhibits the high performance of eCO_(2)RR to yield C_(2+)products with the Faradaic efficiency(C_(2+))of 52.5%and a current density of 660 mA/cm^(2)at-1.2 V *** in a flow cell device under alkaline *** experiment,in situ infrared spectroscopy and the density functional theory(DFT)calculations showed that the electron donating effect of methyl substituents on organic ligands of the copper-based MAF could enhance the ligand field and activation of key intermediates(*CO and*CHO species),thus promoting the coupling of*CO and*CHO for yielding C_(2+)products.

关键词： Metal-organic framework Carbon dioxide Electroreduction C_(2+)product Metal-azolate framework

Achieving tunable long persistent luminescence in metal organic halides based on pyridine solvent

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Chinese Chemical Letters 2024年第9期35卷 227-231页

作者： Jun-Ting Mo Zheng Wang College of Chemistry and Chemical Engineering Key Laboratory of Chemical Additives for China National Light IndustryShaanxi University of Science and TechnologyXi’an 710021China MOE laboratory of bioinorganic and Synthetic Chemistry Lehn Institute of Functional MaterialsSchool of ChemistrySun Yat-sen UniversityGuangzhou 510275China

The research of long persistent luminescence(LPL)materials has yield brilliant results in many ***,the efforts are still needed for the regulation of the LPL *** this work,a series of LPL metal organic halides with rich halogen-bond interactions,Py-CdX_(2)(X=Cl,Br,I)were synthesized through self-assembly by Cd X_(2)and pyridine *** steady-state emission redshifted and phosphorescence lifetime declined as the halogen atoms are *** halides exhibit adjustable emission from blue to green and multiple phosphorescence from green to yellow at room temperature by changing the excitation ***,Py-CdX_(2)can emit the visible color-tunable LPL from green to yellow after removing different excitation sources at ambient *** the results of theoretical calculation and experimental analysis,it is found that heavy atom effect and the rich intermolecular halogen bond help realize LPL and multiple triplet states originated from the pyridine ring and the halogens.

关键词： Metal organic halide Heavy atom effect Halogen bond Tunable long persistent luminescence Anti-counterfeiting