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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

An assessment of the CMIP6 performance in simulating Arctic sea ice volume flux via Fram Strait

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Advances in Climate Change Research 2024年第4期15卷 584-595页

作者： Hui-Yan KUANG Shao-Zhe sun Yu-Fang YE Shao-Yin WANG Hai-Bo BI Zhuo-Qi CHEN Xiao CHENG School of Geospatial Engineering and Science Sun Yat-sen UniversitySouthern Marine Science and Engineering Guangdong Laboratory(Zhuhai)Zhuhai 519082China Key Laboratory of Comprehensive Observation of Polar Environment(sun yat-sen university) Ministry of EducationZhuhai 519082China CAS Key Laboratory of marine geology and Environment Institute of OceanologyChinese Academy of Sciences(CAS)Qingdao 266071China Laboratory for marine geology Qingdao National Laboratory for Marine Science and Technology Qingdao 266237China

Numerical models serve as an essential tool to investigate the causes and effects of Arctic sea ice *** the simulation capabilities of the most recent CMIP6 models in sea ice volume flux provides references for model applications and ***,reliable long-term simulation results of the ice volume fux contribute to a deeper understanding of the sea ice response to global climate *** this study,the sea ice volume flux through six Arctic gateways over the past four decades(1979-2014)were estimated in combination of satellite observations of sea ice concentration(SIC)and sea ice motion(SIM)as well as the Pan-Arctic Ice-Ocean Modeling and Assimilation System(PIOMAS)reanalysis sea ice thickness(SIT)*** simulation capability of 17 CMIP6 historical models for the volume flux through Fram Strait were quantitatively *** ice volume flux simulated from the ensemble mean of 17 CMIP6 models demonstrates better performance than that from the individual model,yet IPSL-CM6A-LR and EC-Earth3-Veg-LR outperform the ensemble mean in the annual volume flux,with Taylor scores of 0.86 and 0.50,***6 models display relatively robust capability in simulating the seasonal variations of volume *** them,CESM2-WACCM performs the best,with a correlation coefficient of 0.96 and a Taylor score of ***,NESM3 demonstrates the largest devi-ation from the observation/reanalysis data,with the lowest Taylor score of *** variability of sea ice volume flux is primarily influenced by SIM and SIT,followed by *** extreme large sea ice export through Fram Strait is linked to the occurrence of anomalously low air temperatures,which in turn promote increased SIC and SIT in the corresponding ***,the intensified activity of Arctic cyclones and Arctic dipole anomaly could boost the southward sea ice velocity through Fram Strait,which further enhance the sea ice outflow.

关键词： Sea ice volume flux CMIP6 models Fram Strait Attribution analysis

Intermolecular Acid-Base-Pairs Containing Poly(p-Terphenyl-co-Isatin Piperidinium) for High Temperature Proton Exchange Membrane Fuel Cells

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Energy & Environmental Materials 2024年第3期7卷 410-418页

作者： Xiaofeng Hao Zhen Li Min Xiao Zhiheng Huang Dongmei Han Sheng Huang Wei Liu Shuanjin Wang Yuezhong Meng The Key Laboratory of Low-carbon chemistry & Energy Conservation of Guangdong Province State Key Laboratory of Optoelectronic Materials and TechnologiesSchool of Materials Science and EngineeringSun Yat-sen University School of Chemical Engineering and Technology Sun Yat-sen University institute of chemistry Henan Provincial Academy of Sciences Research Center of Green Catalysts College of ChemistryZhengzhou University

How to optimize and regulate the distribution of phosphoric acid in matrix,and pursuing the improved electrochemical performance and service lifetime of high temperature proton exchange membrane （HT-PEMs） fuel cell are significant ***,bifunctional poly （p-terphenyl-co-isatin piperidinium） copolymer with tethered phosphonic acid （t-PA） and intrinsic tertiary amine base groups are firstly prepared and investigated as *** distinctive architecture of the copolymer provides a well-designed platform for rapid proton *** not only transports through the hydrogen bond network formed by the adsorbed free phosphoric acid （f-PA）anchored by the tertiary amine base groups,but also rely upon the proton channel constructed by the ionic cluster formed by the t-PA *** the design of the structure,the bifunctional copolymers with lower PA uptake level （<100%） display prominent proton conductivities and peak power densities (99 mS cm-1,812 mW cm-2at 160℃),along with lower PA leaching and higher voltage stability,which is a top leading result in disclosed *** results demonstrate that the design of intermolecular acid-base-pairs can improve the proton conductivity without sacrificing the intrinsic chemical stability or mechanical property of the thin membrane,realizing win-win demands between the mechanical robustness and electrochemical properties of HT-PEMs.

关键词： bifunctional copolymer high temperature proton exchange membrane intermolecular acid–base-pairs phosphonic acid retention phosphonic acid uptake level

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

Activity promotion of Rh_(1)Ca_(x)/Al_(2)O_(3) single-atom catalyst in 1-octene hydroformylation:a volcano curve exists between Ca adding ratio and catalytic activity

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Science China chemistry 2024年第4期67卷 1187-1192页

作者： Hao Zhang Xingcong Zhang Xilun Wang Qingdi sun Hao Liu Hongbing Ji Xiaohui He Key Laboratory of Bioinorganic and Synthetic chemistry of Ministry of Education Fine Chemical Industry Research InstituteSchool of ChemistryIGCMESun Yat-sen UniversityGuangzhou 510275China Huizhou Research institute Sun Yat-sen UniversityHuizhou 516081China State Key Laboratory Breeding Base of Green-Chemical Synthesis Technology Institute of Green Petroleum Processing and Light Hydrocarbon ConversionCollege of Chemical EngineeringZhejiang University of TechnologyHangzhou 310014China

Single-atom catalysts(SACs)are considered the best candidates for olefin hydroformylation due to their combined advantages of homogeneous and heterogeneous *** conventional organo-phosphine modification,Rh SAC is modified by introducing Ca,resulting in a significant increase in activity(maximum~5.7-fold)and ***,a volcano curve between Ca addition ratio and catalytic activity is *** Ca significantly increases activity by decreasing the energy barrier,but excessive Ca decreases activity due to hindering substrate adsorption and reaction.

关键词： hydroformylation bimetallic single-atom catalysts rhodium heterogeneous catalyst

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

Employing pH-responsive RNA triplex to control CRISPR/Cas9-mediated gene manipulation in mammalian cells

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Chinese Chemical Letters 2024年第9期35卷 219-222页

作者： Yan Liu Yang Wang Jiayi Zhu Xuxian Su Xudong Lin Liang Xu Xiwen Xing Guangdong Provincial Key Laboratory of sensor Technology and Biomedical Instrument School of Biomedical EngineeringShenzhen Campus of Sun Yat-sen UniversitySun Yat-sen UniversityShenzhen 518107China MOE Key Laboratory of Bioinorganic and Synthetic chemistry School of ChemistrySun Yat-sen UniversityGuangzhou 510275China Department of Cardiology the first people’s hospital of FoshanFoshan 528000China Department of Biotechnology College of Life Science and TechnologyJinan UniversityGuangzhou 510632China

The clustered regularly interspersed short palindromic repeats/CRISPR-associated protein 9(CRISPR/Cas9)system is an RNA-guided platform for highly efficient and specific genome targeting in diverse organisms,which has been exploited for various applications in gene *** with the constantly active CRISPR/Cas9 function,conditional control of its activity can improve the performance of the system with reduced side effects and high spatiotemporal *** pH-responsive triplex RNA was successful used in CRISPR-derived RNA/trans-activating crRNA(crRNA/tracrRNA)of CRISPR/Cas9,thus affecting RNA/dead Cas9(dCas9)complex to target DNA in vitro and in *** design of triplex RNA opens a new window towards the broad involvement of eukaryotic cells for conditional control of CRISPR/Cas9function.?2024 Published by Elsevier *** behalf of Chinese Chemical Society and institute of Materia Medica,Chinese Academy of Medical Sciences.

关键词： RNA triplex pH-responsive CRISPR/Cas9 Gene manipulation Eukaryotic cells

Challenges and opportunities in Quaternary palynology

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Science China Earth Sciences 2024年第7期67卷 2148-2161页

作者： Qinghai XU Houyuan LU Zhuo ZHENG College of Geographical Sciences Hebei Key Laboratory of Environmental Change and Ecological ConstructionHebei Normal UniversityShijiazhuang 050024China Key Laboratory of Cenozoic geology and Environment Institute of Geology and GeophysicsChinese Academy of SciencesBeijing 100029China School of Earth Sciences and Engineering Sun Yat-sen UniversityZhuhai 519082China

Quaternary palynology plays a pivotal role in investigating global climate change and various other research fields,serving as an essential tool for the quantitative analysis of paleoenvironment ***,due to the vast diversity of terrestrial ecosystems and intricate interactions between vegetation,climate,and human activities,further advancements are required in the following aspects within this discipline.(1)The accuracy of classification in pollen morphology and fossil pollen identification needs improvement,particularly at the species *** represents a significant challenge in present Quaternary ***-aided intelligent recognition holds promise as a solution for species identification based on more detail pollen morphology.(2)Most pollen-based vegetation and climate reconstructions overlook the significance of bare *** bare ground can lead to substantial inaccuracies when quantitatively reconstructing past vegetation and climate.(3)While pollen records provide reliable information on paleoclimate changes,current quantitative climate reconstruction models heavily rely on modern pollen datasets derived from present-day vegetation disturbed more or less by human *** introduces bias and uncertainties into paleoclimate reconstruction.(4)Although pollen can serve as an indicator of human activities,accurately quantifying the intensity of human influence remains *** accurate identification of crop pollen,reconstructing reliable land cover/use data,and integrating multidisciplinary data may enhance the identification and quantification of signals related to human activity in pollen records.

关键词： Quaternary palynology Paleoclimate Paleovegetation Human activity

Dynamic Spacer Installation of Multifunctionalities into Metal-Organic Frameworks for Spontaneous One-Step Ethylene Purification from a Ternary C_(2)-Hydrocarbons Mixture

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CCS chemistry 2024年第1期6卷 241-254页

作者： Yang-Yang Xiong Cheng-Xia Chen Tony Pham Zhang-Wen Wei Katherine A.Forrest Mei Pan Cheng-Yong Su MOE Laboratory of Bioinorganic and Synthetic chemistry Lehn Institute of Functional MaterialsSchool of ChemistrySun Yat-sen UniversityGuangzhou 510275 Department of chemistry University of South FloridaTampaFlorida 33620

Simultaneous ethane and acetylene removal from a C_(2)-gases mixture(C_(2)H_(6),C_(2)H_(4),and C_(2)H_(2))through a one-step separation process for ethylene purification is of great importance yet challenging in petrochemical industry,owing to their similar molecule sizes and physical ***,a series of multifunctionalized metal–organic frameworks(MOFs),LIFM-XYY-1∼8(LIFM stands for Lehn institute of Functional Materials,and XYY are the initials of the first author),are constructed via a dynamic spacer installation(DSI)approach to optimize the pore-nanospaces for efficient C_(2)H_(4) isolation from the ternary C_(2)-gases *** of variable organic-spacers into the prototypical MOFs,LIFM-28 or PCN-700,results in dramatically improved pore volume/surface area,contracted pore size,and functionalized pore surface,which in turn bring out high C_(2)-gases uptake capacities,enhanced C_(2)H_(6) and C_(2)H_(2) adsorption selectivities over C_(2)H_(4),and fast adsorption kinetics,providing an effective strategy to achieve delicate trade-off among these indexes for adequate separation ***,optimized LIFM-XYY-7 presents four-times C_(2)H_(6) and C_(2)H_(2) adsorption capacities than *** breakthrough experiments reveal that poly-grade C_(2)H_(4)(>99.9%)can be obtained from binary or ternary C_(2)-hydrocarbon mixtures through a single separation *** with themolecular simulations,this work demonstrates a promising protocol of porenanospace engineering via multi-functional optimization by the DSI approach to screen out MOFs for a formidable task.

关键词： metal-organic frameworks dynamic spacer installation C_(2)H_(6)/C_(2)H_(2)/C_(2)H_(4)gases separation pore nanospace engineering multi-functional optimization

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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