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Hierarchical Self-Assembly Promoted Circularly Polarized Luminescence Enhancement and Handedness Inversion of Metal–Organic Helicate

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CCS Chemistry 2024年第9期6卷 2198-2209页

作者： Shuyuan Zheng Guofeng Liu School of chemical Science and Engineering Advanced Research InstituteTongji UniversityShanghai 200092

In-depth studies of hierarchical self-assembly with chirality inversion and asymmetry amplification are indispensable for understanding the chiral transfer rule in assembly systems and construction of circularly polarized luminescence(CPL)active ***,a coordination-driven primary assembly of pyrene-based chiral ligand and Zn(OTf)2 was employed for the construction of homochiral metal–organic helicate with a triple helix structure,tunable emission color,and significant chirality *** excitingly,the metal–organic helicate further assembled into well-ordered hierarchical nanoarchitectures with the aid of C–H⋯πinteraction andπ–πstacking,showing significant CPL enhancement and unexpected handedness ***,the|glum|increased from 5.20×10^(−5) to 5.60×10^(−2),and the|gabs|rose from 3.80×10^(−4) to 1.04×10^(−2) over the entire hierarchical self-assembly *** multiple supramolecular interactions not only endowed the resultant metal–organic helicate with efficient chirality transmission and tunable emission color but also guided the(supra)molecular building block of metal–organic helicate organizing into the hierarchically chiral nanoarchitecture in a directional *** work provides insight into the metal–organic helicate-mediated hierarchical self-assembly and aids the development of CPLactive materials with dynamic chirality modulation and enhanced chiroptical performance.

关键词： supramolecular chirality inversion circularly polarized luminescence metal-organic helicate hierarchically chiral assembly chirality amplification

Advances in selective conversion of carbohydrates into 5-hydroxymethylfurfural

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Green Energy & Environment 2024年第9期9卷 1384-1406页

作者： Jie Liang Jianchun Jiang Tingting Cai Chao Liu Jun Ye Xianhai Zeng Kui Wang institute of chemical Industry of Forest Products Chinese Academy of Forestry National Engineering Lab.for Biomass Chemical Utilization Co-Innovation Center of Efficient Processing and Utilization of Forest Resources Nanjing Forestry University College of Energy State Key Laboratory of Physical Chemistry of Solid Surfaces Xiamen University

Converting carbohydrates into 5-hydroxymethylfurfural(5-HMF) is an attractive and promising route for value-added utilization of agricultural and forestry biomass resource. As an important platform compound, 5-HMF possesses high active furan structure with hydroxymethyl and aldehyde group for production of various bio-chemicals and materials, meanwhile, which suffer from low stability and poor yield during the industrial biorefinery process. Hence, selective production of 5-HMF with high-yield and low-cost has attracted extensive attention from scientific and industrial researchers. This review sorted and described the latest advanced research on solvent and catalyst system, as well as energy field effect for production of 5-HMF with different feedstock in detail, emphatically discussing the solvent effect and its synergistic effect with other aspects. Besides, the future prospects and challenges for production of 5-HMF from carbohydrates were also presented, which provide a profound insight into industrial 5-HMF process with economic and environmental feature.

关键词： 5-Hydroxymethylfurfural Biorefinery Solvent Selectivity Carbohydrate

Copper-catalyzed enantioselective desymmetrizing C(sp^(2))-H functionalization of azide-ynamides via α-imino copper carbenes

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Science China Chemistry 2024年第9期67卷 2982-2988页

作者： En-He Huang Li-Gao Liu You-Wei Yin Hao-Xuan Dong Ji-Jia Zhou Xin Lu Bo Zhou Long-Wu Ye Key Laboratory for chemical Biology of Fujian Province and State Key Laboratory of physical Chemistry of Solid Surfaces College of Chemistry and Chemical EngineeringXiamen UniversityXiamen 361005China State Key Laboratory of Organometallic Chemistry Shanghai Institute of Organic ChemistryChinese Academy of SciencesShanghai 200032China

α-Imino metal carbenes are versatile intermediates in organic synthesis,and have broad applications in the assembly of divergent ***,the catalytic enantioselective desymmetrization based onα-imino metal carbenes has not been developed to ***,we disclose an enantioselective desymmetrizing C(sp^(2))-H functionalization of azide-ynamides viaα-imino copper carbenes,leading to the efficient assembly of divergent chiral indoloazepines in generally moderate to excellent yields with high ***,this reaction represents the first enantioselective desymmetrization based onα-imino metal *** synthetic transformations and biological tests show the potential utility of this ***,computational studies are employed to elucidate the reaction mechanism and the origin of enantioselectivity.

关键词： enantioselective desymmetrization metal carbenes copper catalysis nitrene transfer alkynes

Two-Dimensional Metallophthalocyanine Nanomaterials for Electrocatalytic Energy Conversion

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Energy & Environmental Materials 2024年第4期7卷 364-385页

作者： Xinqi Wang Shaohui Sun Jiahao Yao Hao Wan Renzhi Ma Wei Ma School of chemical Engineering and Zhongyuan Critical Metals Laboratory Zhengzhou University research Center for Materials Nanoarchitectonics (MANA) National Institute for Materials Science (NIMS)

Crowing energy demand drives the rapid development of clean and reliable energy *** the past years,the exploration of novel materials with considerable efficiency and durability has drawn attention in the area of elec... 详细信息

关键词： conjugated nanostructure electrocatalysis 2D metallophthalocyanines

Preliminary discussion on the ignition mechanism of exploding foil initiators igniting boron potassium nitrate

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Defence Technology（防务技术） 2024年第2期32卷 222-231页

作者： Haotian Jian Guoqiang Zheng Lejian Chen Zheng Ning Guofu Yin Peng Zhu Ruiqi Shen School of Chemistry and chemical Engineering Nanjing University of Science and TechnologyNanjing 210094China Micro-Nano Energetic Devices Key Laboratory of MIIT Nanjing University of Science and TechnologyNanjing 210094China Anhui Province Key Laboratory of Microsystem the 43rd Research Institute of CETCHefei 230088China Science and Technology on Applied physical and Chemistry Laboratory Shanxi Applied Physics and Chemistry Research Institute Xi'an 710061China

Exploding foil initiator(EFI)is a kind of advanced device for initiating explosives,but its function is unstable when it comes to directly igniting *** solve the problem,this research aims to reveal the ignition mechanism of EFIs directly igniting *** oscilloscope,a photon Doppler velocimetry,and a plasma spectrum measurement system were employed to obtain information of electric characteristics,impact pressure,and plasma *** results of the electric characteristics and the impact pressure were inconsistent with ignition *** only thing that the ignition success tests had in common was that their plasma all had a relatively long period of high-temperature duration(HTD).It eventually concludes that the ignition mechanism in this research is the microconvection heat transfer rather than the shock initiation,which differs from that of exploding foil initiators detonating ***,the methods for evaluating the ignition success of semiconductor bridge initiators are not entirely applicable to the tests mentioned in this *** HTD is the critical parameter for judging the ignition success,and it is influenced by two factors:the late time discharge and the energy of the electric *** longer time of the late time discharge and the more energy of the electric explosion,the easier it is to expand the HTD,which improves the probability of the ignition success.

关键词： Exploding foil initiator PDV Plasma spectrum Ignition mechanism Boron potassium nitrate

Constructing high-toughness polyimide binder with robust polarity and ion-conductive mechanisms ensuring long-term operational stability of silicon-based anodes

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Journal of Energy Chemistry 2024年第6期93卷 580-591,I0014页

作者： Yongjun Kang Nanxi Dong Fangzhou Liu Daolei Lin Bingxue Liu Guofeng Tian Shengli Qi Dezhen Wu State Key Laboratory of chemical Resource Engineering Beijing University of Chemical TechnologyBeijing 100029China ENFI R&D institute China ENFI Engineering CorporationBeijing 100038China China Automotive Battery research institute Co. Ltd.Beijing 101407China Changzhou institute of Advanced Materials Beijing University of Chemical TechnologyChangzhou 213164JiangsuChina

Silicon-based materials have demonstrated remarkable potential in high-energy-density batteries owing to their high theoretical ***,the significant volume expansion of silicon seriously hinders its utilization as a lithium-ion ***,a functionalized high-toughness polyimide(PDMI) is synthesized by copolymerizing the 4,4'-Oxydiphthalic anhydride(ODPA) with 4,4'-oxydianiline(ODA),2,3-diaminobenzoic acid(DABA),and 1,3-bis(3-aminopropyl)-tetramethyl disiloxane(DMS).The combination of rigid benzene rings and flexible oxygen groups(-O-) in the PDMI molecular chain via a rigidness/softness coupling mechanism contributes to high *** plentiful polar carboxyl(-COOH) groups establish robust bonding *** ionic transport is achieved by incorporating the flexible siloxane segment(Si-O-Si),which imparts high molecular chain motility and augments free volume holes to facilitate lithium-ion transport(9.8 × 10^(-10) cm^(2) s^(-1) vs.16 × 10^(-10) cm^(2) s~(-1)).As expected,the SiO_x@PDMI-1.5 electrode delivers brilliant long-term cycle performance with a remarkable capacity retention of 85% over 500 cycles at 1.3 A g^(-1).The well-designed functionalized polyimide also significantly enhances the electrochemical properties of Si nanoparticles ***,the assembled SiO_x@PDMI-1.5/NCM811 full cell delivers a high retention of 80% after 100 *** perspective of the binder design strategy based on polyimide modification delivers a novel path toward high-capacity electrodes for high-energy-density batteries.

关键词： Polyimide binder High toughness Robust ionic transport Silicon-based anodes Lithium-ion batteries

Enhanced stability of nitrogen-doped carbon-supported palladium catalyst for oxidative carbonylation of phenol

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Chinese Journal of chemical Engineering 2024年第1期65卷 19-28页

作者： Xiaojing Liu Ruohan Zhao Hao Zhao Zhimiao Wang Fang Li Wei Xue Yanji Wang Hebei Provincial Key Laboratory of Green chemical Technology and High Efficient Energy Saving School of Chemical Engineering and TechnologyHebei University of TechnologyTianjin 300130China Tianjin Key Laboratory of chemical Process Safety Tianjin 300130China Hebei Industrial Technology research institute of Green chemical Industry Huanghua 061100China

Enhancing the stability of supported noble metal catalysts emerges is a major challenge in both science and ***,a heterogeneous Pd catalyst(Pd/NCF)was prepared by supporting Pd ultrafine metal nanoparticles(NPs)on nitrogen-doped carbon;synthesized by using F127 as a stabilizer,as well as chitosan as a carbon and nitrogen *** Pd/NCF catalyst was efficient and recyclable for oxidative carbonylation of phenol to diphenyl carbonate,exhibiting higher stability than Pd/NC prepared without F127 *** hydrogen bond between chitosan(CTS)and F127 was enhanced by F127,which anchored the N in the free amino group,increasing the N content of the carbon material and ensuring that the support could provide sufficient N sites for the deposition of Pd *** process helped to improve metal *** increased metal-support interaction,which limits the leaching and coarsening of Pd NPs,improves the stability of the Pd/NCF ***,density functional theory calculations indicated that pyridine N stabilized the Pd^(2+)species,significantly inhibiting the loss of Pd^(2+)in Pd/NCF during the reaction *** work provides a promising avenue towards enhancing the stability of nitrogen-doped carbon-supported metal catalysts.

关键词： Supported Pd catalyst N-doped carbon Amphiphilic triblock copolymer Pyridinic nitrogen Stability

Regulated reaction pathway of CO_(2)photoreduction into CH_(4)by metal atom pair sites

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Rare Metals 2024年第9期43卷 4620-4627页

作者： Dong-Po He Guang-Bing Huang Jun Hu Yang Wu Xiao-Dong Li Qing-Xia Chen Shan Zhu Wen-Sheng Yan Jun-Fa Zhu Yang Pan Xing-Chen Jiao Key Laboratory of Synthetic and Biological Colloids Ministry of EducationSchool of Chemical and Material EngineeringJiangnan UniversityWuxi 214122China Hefei National research Center for physical Sciences at Microscale National Synchrotron Radiation LaboratoryUniversity of Science and Technology of ChinaHefei 230026China Max Planck institute of Microstructure Physics Weinberg 206120 HalleGermany State Grid Anhui Electric Power research institute Hefei 230601China

The carbon dioxide(CO_(2))reduction process involves complex protonation,making the resulting product often *** achieve the desired product,it is crucial to manipulate the reaction ***,we build the metal atom pair sites for selective CO_(2)photoreduction into *** a prototype,Ni atom pair sites loaded on the Mo S_(2)nanosheets were synthesized and verified by highresolution transmission electron microscopy(HRTEM),X-ray photoelectron spectroscopy(XPS)and X-rayabsorption near edge structure spectra(XANES).In-situ Fourier transform infrared spectroscopy(FTIR)monitors the*CHO group,a crucial intermediate in CH_(4)production,during CO_(2)photoreduction on the Ni-Mo S_(2)nanosheets,whereas this monitoring is not observed for the Mo S_(2)***,theoretical calculations disclose that over the Ni-Mo S_(2)nanosheet slab,the formation energy of*CHO intermediates is determined to be lower(0.585 e V)than the desorption energy of*CO intermediates for CO production(0.64 e V),implying the higher selectivity of CH_(4)production.

关键词： steps dioxide desired

Coordination-environment regulation of atomic Co-Mn dual-sites for efficient oxygen reduction reaction

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Nano research 2024年第8期17卷 6841-6848页

作者： Caiting Sun Yarong Liu Zunhang Lv Rui Liu Changli Wang Liuhua Li Jinming Wang Yu Zhang Wenxiu Yang Bo Wang Key Laboratory of Cluster Science(Ministry of Education) Beijing Key Laboratory of Photoelectronic/Electrophotonic Conversion MaterialsAdvanced Technology Research Institute(Jinan)Advanced Research Institute of Multidisciplinary ScienceSchool of Chemistry and Chemical EngineeringBeijing Institute of TechnologyBeijing 100081China Beijing institute of Technology Library Beijing Institute of TechnologyBeijing 100081China

Precisely designing atomic metal-nitrogen-carbon(M-N-C)catalysts with asymmetric diatomic configurations and studying their structure–activity relationships for oxygen reduction reaction(ORR)are important for zinc-air batteries(ZABs).Herein,a dualatomic-site catalyst(DASC)with CoN_(3)S-MnN_(2)S_(2) configuration was prepared for the cathodes of *** with Co-N-C(Mn-free)and CoMn-N-C(S-free doping),CoMn-N/S-C exhibits excellent half-wave potential(0.883 V)and turnover frequency(1.54 e·s^(−1)·site^(−1)),surpassing most of the reported state-of-the-art Pt-free ORR *** CoMn-N/S-C-based ZABs achieve extremely high specific capacity(959 mAh·g^(−1))and good stability(350 h@5 mA·cm^(−2)).Density functional theory(DFT)calculation shows that the introduction of Mn and S can break the electron configuration symmetry of the original Co 3d orbital,lower the dband center of the Co site,and optimize the desorption behavior of*OH intermediate,thereby increasing the ORR activity.

关键词： metal organic frameworks oxygen reduction reaction dual-atom catalyst coordination-environment regulation zinc-air batteries