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Carbon Energy 2024年第3期6卷 118-131页

作者： Jia-Ni Lu Yunze Huang Yuan-Sheng Xia long-zhang dong Lei zhang Jing-Jing Liu Lan-Gui Xie Jiang Liu Ya-Qian Lan Jiangsu Key Laboratory of New Power Batteries School of Chemistry and Materials ScienceJiangsu Collaborative Innovation Centre of Biomedical Functional MaterialsNanjing Normal UniversityNanjingChina School of Chemistry South China Normal UniversityGuangzhouChina

The semi-hydrogenation of alkyne to form Z-olefins with high conversion and high selectivity is still a huge challenge in the chemical ***,flammable and explosive hydrogen as the common hydrogen source of this reaction increases the cost and danger of industrial ***,we connect the photocatalytic hydrogen evolution reaction and the semihydrogenation reaction of alkynes in series and successfully realize the high selective production of Z-alkenes using low-cost,safe,and green water as the proton *** the cascade reaction,a series of isomorphic metal–organic cage catalysts(Co_(x)Zn_(8−x)L_(6),x=0,3,4,5,and 8)are designed and synthesized to improve the yield of the photocatalytic hydrogen *** them,Co_(5)Zn_(3)L_(6) shows the highest photocatalytic activity,with a H_(2) generation rate of 8.81 mmol g^(−1) h^(−1).Then,Co_(5)Zn_(3)L_(6) is further applied in the above tandem reaction to efficiently reduce alkynes to Z-alkenes under ambient conditions,which can reach high conversion of>98%and high selectivity of>99%,and maintain original catalytic activity after multiple ***“one-pot”tandem reaction can achieve a highly selective and safe stepwise conversion from water into hydrogen into Z-olefins under mild reaction conditions.

关键词： alkyne semi-hydrogenation hydrogen evolution reaction metal-organic cages photocatalysis Z-olefins

用于实现高性能热催化氧化还原反应的二茂铁功能化锆氧簇

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Science Bulletin 2024年第10期69卷 1418-1426页

作者：姚苏娟林焦敏董龙章李颖霖李宁刘江兰亚乾 School of Chemistry South China Normal UniversityGuangzhou 510006China

The Zr(Ⅳ)ions are easily hydrolyzed to form oxides,which severely limits the discovery of new structures and applications of Zr-based *** this work,three ferrocene(Fc)-functionalized Zr-oxo clusters(ZrOCs),Zr_(9)Fc_(6),Zr_(10)Fc_(6) and Zr_(12)Fc_(8) were synthesized through inhibiting the hydrolysis of Zr(Ⅳ)ions,which show increased nuclearity and regular structural *** importantly,these Fc-functionalized ZrOCs were used as heterogeneous catalysts for the transfer hydrogenation of levulinic acid(LA)and phenol oxidation reactions for the first time,and displayed outstanding catalytic *** particular,Zr_(12)Fc_(8) with the largest number of Zr active sites and Fc groups can achieve>95% yield for LAto-c-valerolactone within 4 h(130℃)and>98% yield for 2,3,6-trimethylphenol-to-2,3,5-trimethyl-pbenzoquinone within 30 min(80℃),showing the best catalytic *** characterization combined with theory calculations reveal that in the Fc-functionalized ZrOCs,the Zr active sites could serve as substrate adsorption sites,while the Fc groups could act as hydrogen transfer reagent or Fenton reagent,and thus achieve effectively intramolecular metal-ligand synergistic *** work develops functionalized ZrOCs as catalysts for thermal-triggered redox reactions.

关键词： Zirconium-oxo cluster Metal-ligand synergitic thermalcatalysis Crystalline coordination compound Hydrogen transfer Fenton reagent

Porous copper cluster-based MOF with strong cuprophilic interactions for highly selective electrocatalytic reduction of CO_(2) to CH4

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Nano Research 2022年第12期15卷 10185-10193页

作者： long-zhang dong Yun-Feng Lu Rui Wang Jie Zhou Yu zhang Lei zhang Jiang Liu Shun-Li Li Ya-Qian Lan National and Local Joint Engineering Research Center of MPTES in High Energy and Safety LIBs Engineering Research Center of MTEES(Ministry of Education)Key Lab.of ETESPG(GHEI)School of ChemistrySouth China Normal UniversityGuangzhou510006China Jiangsu Collaborative Innovation Centre of Biomedical Functional Materials Jiangsu Key Laboratory of New Power BatteriesSchool of Chemistry and Materials ScienceNanjing Normal UniversityNanjing210023China

It is well known that the low-valent Cu species are important catalytically active centers in the reduction of CO_(2) to hydrocarbon ***,the Cu(l)-based catalysts are easily reduced during the electroreduction of CO_(2),which causes phase transformation of catalysts and leads to a decrease of intrinsic catalytic ***,it is of great significance to synthesize Cu(l)-based catalysts with specific interactions that can keep the catalytically active Cu sites stable in the electrocatalytic *** on the above considerations,a hexanuclear Cu cluster with strong cuprophilic interactions has been designed and utilized as a secondary building unit(SBU)to construct a stable metal-organic framework(MOF)electrocatalyst(NNU-50).As expected,the NNU-50 has served as an effective electrocatalyst for the CO_(2)-to-CH4 conversion by exhibiting a high Faradaic efficiency for CH4(FEcH4)of 66.40%and a large current density of~400 mA·cm-2 at-1.0 V *** hydrogen electrode(RHE),which is one of the best catalytic performances among the stable MOF electrocatalysts until *** work contributes more ideas for the design of stable and efficient MOF-based electrocatalysts for CO_(2) reduction reaction.

关键词： metal-organic framework cuprophilic interactions carbon dioxide electroreduction

Uncovering the synergistic photocatalytic behavior of bimetallic molecular catalysts

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Chinese Chemical Letters 2023年第1期34卷 487-492页

作者： Lin Yuan Lei zhang Xiao-Xin Li Jiang Liu Jing-Jing Liu long-zhang dong dong-Sheng Li Shun-Li Li Ya-Qian Lan Jiangsu Collaborative Innovation Centre of Biomedical Functional Materials Jiangsu Key Laboratory of New Power BatteriesCollege of Chemistry and Materials ScienceNanjing Normal UniversityNanjing 210023China School of Chemistry South China Normal UniversityGuangzhou 510006China School of Chemistry and Chemical Engineering Southeast UniversityNanjing 211189China Key Laboratory of Inorganic Nonmetallic Crystalline and Energy Conversion Materials China Three Gorges UniversityYichang 443002China

Bimetallic catalysts usually exhibit better performance than monometallic catalysts due to synergistic ***,there is a lack of exploring the synergistic effect on catalytic performance caused by the introduction of inactive metal *** this work,we design a molecular model system that can precisely regulate the metal site number and catalytic *** these molecular metal compounds are used as homogeneous catalysts for photocatalytic CO_(2)reduction,the dinuclear heterometallic CuNi-L2shows the highest CO_(2)-to-CO conversion,which is 2.1 and 3.0 times higher than that of dinuclear homometallic Ni2-L2and mononuclear *** functional theory calculations demonstrate that,in CuNi-L2,the introduction of inactive CuⅡis easier to promote the photo-generated electrons transferring to the coupled active NiⅡsite to achieve the highest *** addition,this work also provides insights to design and construct more efficient bimetallic catalysts in future.

关键词： Dinuclear metal compounds Crystalline photocatalyst Synergistic effect Photocatalytic CO_(2)RR Artificial photosynthesis

Three-in-one Fe-porphyrin based hybrid nanosheets for enhanced CO_(2)reduction and evolution kinetics in Li-CO_(2)battery

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Chinese Chemical Letters 2023年第6期34卷 471-475页

作者： Shan Li Jian-Hui Wang long-zhang dong Yu zhang Xiao-Man Yao Yifa Chen Shun-Li Li Ya-Qian Lan Jiangsu Collaborative Innovation Centre of Biomedical Functional Materials Jiangsu Key Laboratory of New Power BatteriesSchool of Chemistry and Materials ScienceNanjing Normal UniversityNanjing 210023China National and Local Joint Engineering Research Center of MPTES in High Energy and Safety LIBs Engineering Research Center of MTEES(Ministry of Education)Key Lab.of ETESPG(GHEI)School of ChemistrySouth China Normal UniversityGuangzhou 510006China

Efficient cathode-catalysts with multi-functional properties are essential for Li-CO_(2)battery,while the construction of them with simultaneously enhanced CO_(2)reduction and evolution kinetics is still ***,a kind of hybrid nanosheets based on Ru nanoparticles,Fe-TAPP and grapheme oxide(GO)has been designed through a one-pot self-assembly *** Ru,Fe-porphyrin and GO based hybrid nanosheets(denoted as Ru/Fe-TAPP@GO)with integrated multi-components offer characteristics of ultrathin thickness(~4 nm),high electro-redox property,uniformly dispersed morphology,and high electrical conductivity,*** features endow Ru/Fe-TAPP@GO with ultra-low overpotential(0.82 V)and fully reversible discharge/charge property with a high specific-capacity of 39,000 m Ah/g within 2.0-4.5 V at 100 m A/g,which are much superior to Ru@GO and Fe-TAPP@*** achieved performance was presented as one of the best cathode-catalysts reported to *** synergistically enhanced activity originated from the integrated hybrid nanosheets may provide a new pathway for designing efficient cathode-catalysts for Li-CO_(2)batteries.

关键词： Single-metal sites Porphyrin Li-CO_(2)battery Cathode catalyst Ru nanoparticles

Green synthesis of bifunctional phthalocyanine-porphyrin COFs in water for efficient electrocatalytic CO2 reduction coupled with methanol oxidation

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National Science Review 2023年第11期10卷 160-170页

作者： Mi zhang Jia-Peng Liao Run-Han Li Sheng-Nan Sun Meng Lu long-zhang dong Pei Huang Shun-Li Li Yue-Peng Cai Ya-Qian Lan South China Normal University School of Chemistry

Electrocatalytic CO2reduction(ECR) coupled with organic oxidation is a promising strategy to produce high value-added chemicals and improve energy efficiency. However, achieving the efficient redox coupling reaction is still challenging due to the lack of suitable electrocatalysts. Herein, we designed two bifunctional polyimides-linked covalent organic frameworks(PI-COFs) through assembling phthalocyanine(Pc) and porphyrin(Por) by non-toxic hydrothermal methods in pure water to realize the above catalytic *** to the high conductivity and well-defined active sites with different chemical environments, Ni Pc-Ni Por COF performs efficient ECR coupled with methanol oxidation reaction(MOR)(Faradaic efficiency of CO(FECO) = 98.12%, partial current densities of CO(j CO) = 6.14 m A cm-2for ECR, FEHCOOH = 93.75%,j HCOOH = 5.81 m A cm-2for MOR at low cell voltage(2.1 V) and remarkable long-term stability).Furthermore, experimental evidences and density functional theory(DFT) calculations demonstrate that the ECR process mainly conducts on Ni Pc unit with the assistance of Ni Por, meanwhile, the MOR prefers Ni Por conjugating with Ni Pc. The two units of Ni Pc-Ni Por COF collaboratively promote the coupled oxidation-reduction reaction. For the first time, this work achieves the rational design of bifunctional COFs for coupled heterogeneous catalysis, which opens a new area for crystalline material catalysts.

关键词： hydrothermal synthesis phthalocyanine-porphyrin COFs bifunctional electrocatalysts electrocatalytic CO2 reduction methanol oxidation reaction

Mechanism of Diabatic Heating on Precipitation and the Track of a Tibetan Plateau Vortex over the Eastern Slope of the Tibetan Plateau

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Advances in Atmospheric Sciences 2024年第1期41卷 155-172页

作者： Yuanchang dong Guoping LI Xiaolin XIE long YANG Peiwen zhang Bo ZENG Institute of Plateau Meteorology China Meteorological Administration(CMA)/Heavy Rain and Drought-Flood Disaster in Plateau and Basin Key Laboratory of Sichuan ProvinceChengdu 610072China School of Atmospheric Sciences Chengdu University of Information TechnologyChengdu 610225China Meteorological Observation Data Center of Sichuan Province Chengdu 610072China Sichuan Branch of Meteorologist Training Institute CMAChengdu 610072China

Existing studies contend that latent heating(LH)will replace sensible heating(SH)to become the dominant factor affecting the development of the Tibetan Plateau vortex(TPV)after it moves off the Tibetan Plateau(TP).However,in the process of the TPV moving off the TP requires that the airmass traverse the eastern slope of the Tibetan Plateau(ESTP)where the topography and diabatic heating(DH)conditions rapidly *** LH gradually replaces SH to become the dominant factor in the development of the TPV over the ESTP is still not very *** this paper,an analysis of a typical case of a TPV with a long life history over the ESTP is performed by using multi-sourced meteorological data and model *** results show that SH from the TP surface can change the TPV-associated precipitation distribution by temperature advection after the TPV moves off the *** LH can then directly promote the development of the TPV and has a certain guiding effect on the track of the *** SH can control the active area of LH by changing the falling area of the TPV-associated precipitation,so it still plays a key role in the development and tracking of the TPV even though it has moved out of the main body of the TP.

关键词： eastern slope of the Tibetan Plateau diabatic heating Tibetan Plateau vortex precipitation distribution track

The energy-free purification of trace thallium(I)-contaminated potable water using a high-selective filter paper with multi-layered Prussian blue decoration

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Frontiers of Chemical Science and Engineering 2024年第2期18卷 1-12页

作者： Jiangyan Lu Zhu Xiong Yuhang Cheng Qingwu long Kaige dong Hongguo zhang Dinggui Luo Li Yu Wei zhang Gaosheng zhang Key Laboratory for Water Quality and Conservation of the Pearl River Delta(Ministry of Education) School of Environmental Science and EngineeringGuangzhou UniversityGuangzhou 510006China College of Light Chemical Industry and Materials Engineering Shunde PolytechnicFoshan 528333China

Thallium is a highly toxic metal,and trace amount of thallium(I)(Tl+)in potable water could cause a severe water crisis,which arouses the exploitation of highly-effective technology for purification of Tl+contaminated *** report proposes the multi-layered Prussian blue(PB)-decorated composite membranes(PBx@PDA/PEI-FP)based on the aminated filter papers for Tl+*** characterization by Fourier transform infrared spectrometer-attenuated total reflectance,scanning electron microscope,thermogravimetric analysis,X-ray photoelectron spectroscopy and X-ray diffraction were performed to confirm the in situ growth of cubic PB crystals on filter paper membrane surfaces via the aminated layers,and the successful fabrication of multi-layered PB overcoats via the increasing of aminated *** effect of PB layers on Tl+removal by PBx@PDA/PEI-FP from simulated drinking water was evaluated as well as the influence of different experimental conditions.A trade-off between PB decoration layer number and PB distribution sizes is existed in Tl+uptake by PBx@PDA/*** double-layered PB2@PDA/PEI-FP membrane showed the maximum sorption capacity,but its Tl+uptake performance was weakened by the acid,coexisting ions(K+and Na+)and powerful operation pressure,during filtrating a large volume of low-concentrated Tl+-containing ***,the negative effect of coexisting ions on the Tl+uptake could be effectively eliminated in weak alkaline water,and the Tl+removal was increased up to 100%without any pressure driving for PB2@PDA/PEI-FP *** importantly,PB2@PDA/PEI-FP displayed the high-efficiency and high-selectivity in purifying the Tl+-spiked Pearl River water,in which the residual Tl+in filtrate was less than 2μg·L^(–1) to meet the drinking water standard of United States Environmental Protection *** work provides a feasible avenue to safeguard the drinking water in remote and underdeveloped area via the energy-free operation.

关键词： membrane adsorption Prussian blue energy-free filtration potable water trace thallium(I)

Rapid and chemoselective imidation of sulfides in aqueous buffer enabled by a novel guanidine-derived N-O reagent

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Science China Chemistry 2024年第6期67卷 1929-1934页

作者： Hanzheng Li long Xu Jiajia dong Key Laboratory of Organofluorine Chemistry Center for Excellence in Molecular SynthesisShanghai Institute of Organic ChemistryUniversity of Chinese Academy of SciencesChinese Academy of SciencesShanghai200032China Institute of Translational Medicine National Facility for Translational Medicine(Shanghai)Shanghai Jiao Tong UniversityShanghai200240China School of Chemistry and Chemical Engineering Zhangjiang Institute for Advanced StudyShanghai Jiao Tong UniversityShanghai200240China Shanghai Artificial Intelligence Laboratory Shanghai200232China

Herein we report the facile synthesis of a series of novel N-O reagents and identify N′-di-Boc-N′′-[(mesitylsulfonyl)oxy]-guanidine as an efficient imidating *** reagent is synthetically scalable and bench-stable,yet it shows unprecedented reactivity and chemoselectivity towards S(II)in buffer/hexafluoroisopropanol(HFIP)system,to generate a new class of Nguanyl *** transformation of N-guanyl sulfilimines to N-guanyl sulfoximines provides us a chance to investigate these rarely reached compounds,which are shown to be versatile precursors to a variety of N-heterocyclic and *** work provides an addition to the tool box of both sulfur imidation and guanidine synthesis,especially for the need of rapid and selective modifications of sulfur(II)center under biocompatible conditions.

关键词： sulfur imidation N-O reagent

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Metallurgy and Solidification Microstructure Control of Fusion-Based Additive Manufacturing Fabricated Metallic Alloys:A Review

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Acta Metallurgica Sinica(English Letters) 2024年第1期37卷 29-53页

作者： Qiang Li Xing-Ran Li Bai-Xin dong Xiao-long zhang Shi-Li Shu Feng Qiu Lai-Chang zhang Zhi-Hui zhang Key Laboratory of Bionic Engineering(Ministry of Education) and College of Bionic Science and EngineeringJilin UniversityChangchun130022China Institute of Structured and Architected Materials Liaoning Academy of MaterialsShenyang110167China Key Laboratory of Automobile Materials Ministry of Education and Department of Materials Science and EngineeringJilin UniversityChangchun130025China School of Mechanical and Aerospace Engineering Jilin UniversityChangchun130025China School of Engineering Edith Cowan University270 Joondalup DriveJoondalupPerthWA6027Australia

The metal-based additive manufacturing(AM),also referred to as metal 3D printing,has drawn particular interest because it enables direct creation,aided by computationally-directed path design,of intricate components with site-specific compositions and geometrical requirements as well as low buy-to-fly *** the last two decades,the objective of this revolutionary technology has been shifting from only“rapid prototyping”to advanced manufacturing of special high-end products or devices,which,in many aspects,outperform conventional manufacturing *** fusion-based AM,significant progress has been achieved in understanding the processing window of macroscopic scales,non-equilibrium metallurgy of mesoscale scales,and grain evolution of microscopic *** the versatile capacity of AM facilitates new avenues for discovering advanced materials and structures,their potential has still not been fully *** the unique non-equilibrium solidification during the AM process,coarse columnar grains with strong textures are usually developed along the build direction,which downgrades the mechanical *** push the limits of this digital manufacturing,this review attempts to provide in-depth and comprehensive overviews of the recent progress in understanding the evolution and control of the as-built microstructure that has been made recently and the challenges encountered during the AM process.

关键词： Additive manufacturing Temperature field Microstructure control Nanoparticles Functionally graded materials