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Science China Chemistry 2025年第2期68卷 679-686页

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 ChemistrySun Yat-sen UniversityGuangzhou 510006China Guangzhou National laboratory Guangzhou 510005China Bioland laboratory Guangzhou 510005China

Herein,we report a novel and highly efficient method for the synthesis ofα-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 *** 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 ***,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.

关键词： α-phosphoryloxy ketones high-throughput experimentation machine learning P(O)O-H insertion sulfoxonium ylides

Dual atom-bridge effect promoting interfacial charge transfer in 2D/2D Cs3Bi2Br9/BiOBr epitaxial heterojunction for efficient photocatalysis

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Chinese Chemical Letters 2025年第2期36卷 218-223页

作者： Yuan Teng Zichun Zhou Jinghua Chen Siying Huang Hongyan Chen Daibin Kuang MOE Key laboratory of bioinorganic and Synthetic Chemistry LIFM GBRCE for Functional Molecular Engineering School of Chemistry IGCME Sun Yat-sen University National Experimental Teaching Demonstration Center for Chemistry College of Chemistry and Chemical Engineering Jishou University

Optimizing the interfacial quality of halide perovskites heterojunction to promote the photogenerated charge separation is of great significance in photocatalytic ***,the delicately regulation of interfacial structure and properties of halide perovskites hybrid is still a big challenge owing to the growth uncontrollability and incompatibility between different *** we use Bi OBr nanosheets as the start-template to in situ epitaxially grow Cs3Bi2Br9nanosheets by“cosharing”Bi and Br atoms strategy for designing a 2D/2D Cs3Bi2Br9/BiOBr *** studies show that the epitaxial heterojunction can optimize the synergistic effect of Bi OBr and Cs3Bi2Br9via the formation of tight-contact interfaces,strong interfacial electronic coupling and charge redistribution,which can not only drive the Z-scheme charge transfer mechanism to greatly promote the spatial separation of electronhole pairs,but also modulate the interfacial electronic structure to facilitate the adsorption and activation of toluene *** heterojunction exhibited 62.3 and 2.4-fold photoactivity improvement for toluene oxidation to benzaldehyde than parental Bi OBr and Cs3Bi2Br9,*** study not only proposed a novel dual atom-bridge protocol to engineer high-quality perovskite heterojunctions,but also uncovered the potential of heterojunction in promoting electron-hole separation as well as the application in photocatalytic organic synthesis.

关键词： Bismuth oxyhalide Bismuth-based perovskite Direct Z-scheme heterojunction Dual atom-bridge effect Photocatalytic C(sp3)-H bond activation

Photo-controllable multiple and orthogonal regulation of gene expression by chemically modified oligonucleotides

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Science China Chemistry 2025年第2期68卷 694-704页

作者： Yang Wang Qiu-Long Zhang Yan Liu Liang-Liang Wang Chao-Qun Wu Ming Shao Xiwen Xing Juan Du Liang Xu Key laboratory of Tropical Biological Resources of Ministry of Education and One Health Institute School of Pharmaceutical SciencesHainan UniversityHaikou 570228China Central laboratory Department of The Second Affiliated Hospital School of MedicineThe Chinese University of Hong KongShenzhen&Longgang District People’s Hospital of ShenzhenShenzhen 518172China MOE Key laboratory of bioinorganic and Synthetic Chemistry School of ChemistrySun Yat-sen UniversityGuangzhou 510275China Department of Biotechnology College of Life Science and TechnologyJinan University InstitutionGuangzhou 510632China School of Pharmacy and Medical Technology Putian UniversityPutian 351100China

Gene expression must be precisely regulated in cells and functional nucleic acids are the most widely utilized tools for gene *** of how these nucleic acid tools work in the cellular environment can precisely manipulate gene expression through a non-invasive *** we report a methodology on multiplex photocontrol of functional nucleic acids to achieve totally temporal and orthogonal regulation of gene expression in living *** select two functional nucleic acid systems as examples,DNAzyme and CRISPR/Cas9,and demonstrate the power of light control for precise gene manipulation by rational design of chemically modified oligonucleotides through introduction of two photocleavable *** the previous modulation of functional nucleic acids by simply activating or deactivating,we successfully achieve versatile controlling patterns using light as the governing *** design represents a generalized pathway towards the photo-controllable functional nucleic acids,which greatly enriches the toolbox for optogenetic studies.

关键词： functional nucleic acids optogenetics modified oligonucleotides gene technology

Deciphering Water Oxidation Catalysts:The Dominant Role of Surface Chemistry over Reconstruction Degree in Activity Promotion

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Nano-Micro Letters 2025年第3期17卷 340-354页

作者： Li An Jianyi Li Yuanmiao Sun Jiamin Zhu Justin Zhu Yeow Seow Hong Zhang Nan Zhang Pinxian Xi Zhichuan J.Xu Chun‑Hua Yan State Key laboratory of Applied Organic Chemistry Key Laboratory of Nonferrous Metal Chemistry and Resources Utilization of Gansu ProvinceFrontiers Science Center for Rare IsotopesCollege of Chemistry and Chemical EngineeringLanzhou UniversityLanzhou 730000People’s Republic of China School of Materials Science and Engineering Nanyang Technological UniversitySingapore 639798Singapore Faculty of Materials Science and Energy Engineering Institute of Technology for Carbon NeutralityShenzhen Institute of Advanced TechnologyChinese Academy of SciencesShenzhen 518055People’s Republic of China Key laboratory of Electromagnetic Materials and Devices National Center for International Research On Photoelectric and Energy MaterialsSchool of Materials and EnergyElectron Microscopy CenterYunnan UniversityKunming 650091People’s Republic of China State Key laboratory of Baiyunobo Rare Earth Resource Researches and Comprehensive Utilization Baotou Research Institute of Rare EarthsBaotou 014030People’s Republic of China Beijing National laboratory for Molecular Sciences State Key Laboratory of Rare Earth Materials Chemistry and ApplicationsPKU‑HKU Joint Laboratory in Rare Earth Materials and Bioinorganic ChemistryPeking UniversityBeijing 100871People’s Republic of China

Water splitting hinges crucially on the availability of electrocatalysts for the oxygen evolution *** surface reconstruction has been widely observed in perovskite catalysts,and the reconstruction degree has been often correlated with the activity ***,a systematic study on the roles of Fe substitution in activation of perovskite LaNiO_(3)is *** substituting Fe content influences both current change tendency and surface reconstruction ***_(0.9)Fe_(0.1)O_(3)is found exhibiting a volcano-peak intrinsic activity in both pristine and reconstructed among all substituted perovskites in the LaNi_(1-x)Fe_(x)O_(3)(x=0.00,0.10,0.25,0.50,0.75,1.00)*** reconstructed LaNi_(0.9)Fe_(0.1)O_(3)shows a higher intrinsic activity than most reported NiFe-based ***,density functional theory calculations reveal that Fe substitution can lower the O 2p level,which thus stabilize lattice oxygen in LaNi0.9Fe0.1O3 and ensure its long-term ***,it is vital interesting that activity of the reconstructed catalysts relied more on the surface chemistry rather than the reconstruction *** effect of Fe on the degree of surface reconstruction of the perovskite is decoupled from that on its activity enhancement after surface *** finding showcases the importance to customize the surface chemistry of reconstructed catalysts for water oxidation.

关键词： Oxygen evolution reaction Perovskite oxides Doping Activation and reconstruction

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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 2025年第2期 679-686页

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 ChemistrySun 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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Isolation and single-molecule magnetism of neutral rare-earth(III) sandwich complexes supported by compact aromatic rings

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Science China Chemistry 2025年

作者： Ming Liu Yan-Cong Chen Jieyu Zheng Xiao-Han Peng Ming-Liang Tong Akseli Mansikkam?ki Fu-Sheng Guo Institute of Fundamental and Frontier Sciences University of Electronic Science and Technology of China Key laboratory of bioinorganic and Synthetic Chemistry of Ministry of Education School of Chemistry Institute of Green Chemistry and Molecular Engineering (IGCME) Guangdong Basic Research Center of Excellence (GBRCE) for Functional Molecular EngineeringSun Yat-sen University NMR Research Unit University of Oulu

Over the past few decades,various types of metal-sandwich structures have been synthesized and reported,which significantly advanced organometallic chemistry and contributed to numerous ***,charge-neutral rare-earth（III） sandwich structures based on compact aromatic ligands still remained unexplored due to the challenges in their ***,the immense potential of this type of structure in building high-performance single-molecule magnets （SMMs） has compelled us to overcome these synthetic ***,we aimed to isolate such complexes in a general formula of[（Ring1）REIII（Ring2）].[（CE4B）t4Me2NREIII(Cpi Pr5)](3-RE,RE=Y,Dy;（C4B）Et4Me2N=1-（N,N-dimethylamino）-2,3,4,5-tetraethylborolyl;Cpi Pr5=pentaisopropylcyclopentadienyl) were successfully obtained via the salt-metathesis reaction of the precursor[REIII(CpiPr5)（BH4）2-（THF）]（,RE=Y,Dy;THF=tetrahydrofuran） and the new aminoborolide ligand[Na2（C4B）Et4Me2N1-RE（THF）2]2（2）,which represent the first neutral rare-earth（III）-sandwich complexes ligated by compact aromatic *** complexes 3-RE were characterized by single-crystal X-ray diffraction,elemental analysis,UV-Vis-NIR and *** 3-Y was studied by NMR *** and dynamic magnetic properties of 3-Dy were investigated by SQUID magnetometry,showing a high anisotropy barrier of 785（12） cm-1and open hysteresis loops up to 12 *** bonding of nitrogen to dysprosium（III） near the equatorial plane lowers the anisotropy,and a bulkier ligand in the future should be able to avoid *** work not only demonstrates that such type of neutral rare-earth（III）-sandwich complexes is totally synthetically feasible,but also paves the way for the development of high-performance SMMs.

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Enhancing negative thermal quenching in green-emitting perovskite microspheres via shallow trap state modulation

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Science China Materials 2025年第1期68卷 149-155页

作者： Zhenxu Lin Rui Huang Jie Song Yi Zhang Zewen Lin Hongliang Li Haixia Wu Dejian Hou Yanqing Guo Jing Wang Paul K.Chu School of Materials Science and Engineering Hanshan Normal UniversityChaozhou 521041China Ministry of Education Key laboratory of bioinorganic and Synthetic Chemistry State Key Laboratory of Optoelectronic Materials and TechnologiesSun Yat-Sen UniversityGuangzhou 510275China Department of Physics Department of Materials Science and Engineeringand Department of Biomedical EngineeringCity University of Hong KongTat Chee AvenueKowloonHong KongChina

For luminescent materials,negative thermal quenching(NTQ),characterized by an increase in the luminescent intensity with temperature,has a large potential in lighting and display ***,leveraging NTQ in metal halide perovskites is challenging,and the mechanism is not well ***,by utilizing low-temperature photoluminescence,persistent luminescence and thermoluminescence,the origins of NTQ in CsPbBr_(3) microspheres are systematically studied,which pertain to the liberation of carriers from shallow trap *** and theoretical investigations reveal that the energy of these shallow defect states is approximately 0.135 eV beneath the conduction band.A rapid thermal treatment increases the density of these shallow traps and amplifies the NTQ effect,resulting in an enhancement of room-temperature photoluminescence by more than 60%compared to that at 150 *** process also reduces the threshold for amplified spontaneous emission to about 45 W/cm^(2).Our findings not only provide a deeper understanding of the NTQ phenomenon in CsPbBr3 microspheres but also open new avenues for enhancing the performance of perovskite optoelectronic devices through energy state regulation.

关键词： negative thermal quenching photoluminescence CsPbBr3 microsphere amplified spontaneous emission low threshold

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Optimizing luminescence sensitivity and moisture stability of porous coordination frameworks by varying ligand side groups

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Science China Chemistry 2019年第3期62卷 341-346页

作者： Jia-Wen Ye Xu-Yu Li Hao-Long Zhou Jie-Peng Zhang MOE Key laboratory of bioinorganic and Synthetic Chemistry School of Chemistry Sun Yat-Sen University

Hydrophobic ethyl, butyl or hexyl groups were introduced into the dicarboxylate ligand in the fluorescent porous coordination framework [Zn_2(fda)_2(bpy)](LMOF-202, H_2fda=9H-fluorene-2,7-dicarboxylic acid, bpy=4,4′-bipyridine) for improving water stability and tuning oxygen sensitivity. The long hexyl groups gave satisfactory water stability but its oxygen sensitivity is low(70.8% fluorescence quenched at 1 bar O_2(1 bar=105 Pa)). In contrast, the shorter side groups gave high oxygen sensitivity(93.9% fluorescence quenched at 1 bar O_2) and low water stability. The derivation of the Stern-Volmer curves of the O_2 luminescence quenching data from the linear form can be used for detecting trace impurities in the luminescent framework, being much more sensitive than conventional methods such as powder X-ray diffraction. Mixing the ethyl and hexyl groups in the solid-solution manner brought high oxygen sensitivity(96.4% fluorescence quenched at 1 bar O_2) and high water stability simultaneously in the same coordination framework.

关键词： metal-organic framework water stability oxygen fluorescence sensor

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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 *** 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,***-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 ***-9 exhibits very large N2-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 N2uptakes,*** contrast,MAF-2 F is quite rigid and does not show the inversed temperature-dependent N2adsorption and large guest-induced expansion like ***,despite the higher molecular weight and larger volume,MAF-2 F possesses 6% and 25%higher gravimetric and volumetric CO2uptakes,*** 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

Recent progress in metal-organic frameworks(Part II—material application)

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Science China Chemistry 2025年

作者： Jiandong Pang Wentao Jiang Xue-Wen Zhang Hao-Long Zhou Yuxiu Sun Wei Gong Bin Wang Fuyin Ma Linwei He Long Chen Qiang Chen He-Qi Zheng Yuanjing Cui Wen-Jie Shi Chao Zhang Mei Wang Yue-Biao Zhang Jie-Peng Zhang Chongli Zhong Yong Cui Shuao Wang Jian-Rong Li Guodong Qian Tong-Bu Lu Huan Pang Xian-He Bu Institute for New Energy Materials and Low Carbon Technologies School of Materials Science and Engineering Tianjin University of Technology School of Chemistry and Chemical Engineering Yangzhou University School of Materials Science and Engineering Nankai University School of Physical Science and Technology ShanghaiTech University MOE Key laboratory of bioinorganic and Synthetic Chemistry GBRCE for Functional Molecular Engineering School of Chemistry IGCMESun Yat-sen University Department of Chemistry Shantou University School of Chemical Engineering and Technology Tiangong University School of Chemistry and Chemical Engineering Shanghai Jiao Tong University State Key laboratory of Radiation Medicine and Protection School for Radiological and Interdisciplinary Sciences Soochow University College of Materials Science & Engineering Beijing University of Technology State Key laboratory of Silicon and Advanced Semiconductor Materials Cyrus Tang Center for Sensor Materials and ApplicationsSchool of Materials Science & Engineering Zhejiang University

As a class of functional crystalline porous materials, metal-organic frameworks(MOFs) gained rapid development in the past three decades and a large number of MOFs with ordered structures, high surface areas, and functionalized channels have been investigated. MOFs and MOF-derived/composite materials show great potential in many application fields. In this review, we discussed the main applications of MOFs and MOF-derived/composite materials in small molecule storage, separation, luminescence, sensing, multitype catalysis, and energy storage. In addition, challenges and problems in the future research of MOFsrelated fields are also discussed.

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