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Lewis-base ligand-reshaped interfacial hydrogen-bond network boosts CO2 electrolysis

National science Review 2024年第8期11卷 264-274页

作者： Wangxin Ge Haolan Tao Lei Dong Yu Fan Yanpu Niu Yihua Zhu Cheng Lian Honglai Liu Hongliang Jiang Chunzhong Li Key Laboratory for Ultrafine Materials of Ministry of Education School of Chemical Engineering East China University of Science and Technology Shanghai Engineering Research Center of Hierarchical Nanomaterials School of Materials Science and Engineering East China University of Science and Technology State Key Laboratory of Chemical Engineering Shanghai Engineering Research Center of Hierarchical NanomaterialsSchool of Chemistry and Molecular Engineering East China University of Science and Technology Department of Chemical Engineering School of Chemistry and Chemical Engineering Shanghai Jiao Tong University

Both the catalyst and electrolyte strongly impact the performance of *** substantial progress in catalysts,it remains highly challenging to tailor electrolyte compositions and understand their functions at the catalyst ***,we report that the ethylenediaminetetraacetic acid（EDTA） and its analogs,featuring strong Lewis acid-base interaction with metal cations,are selected as electrolyte additives to reshape the catalyst-electrolyte interface for promoting *** studies reveal that EDTA molecules are dynamically assembled toward interface regions in response to bias potential due to strong Lewis acid-base interaction of EDTA4--K+.As a result,the original hydrogen-bond network among interfacial H2O is disrupted,and a hydrogen-bond gap layer at the electrified interface is *** EDTA-reshaped K+solvation structure promotes the protonation of*CO2to*COOH and suppressing*H2O dissociation to*H,thereby boosting the co-electrolysis of CO2and H2O toward carbon-based *** particular,when 5 mM of EDTA is added into the electrolytes,the Faradaic efficiency of CO on the commercial Ag nanoparticle catalyst is increased from 57.0% to 90.0% at an industry-relevant current density of 500 mA *** importantly,the Lewis-base ligand-reshaped interface allows a range of catalysts（Ag,Zn,Pd,Bi,Sn,and Cu） to deliver substantially increased selectivity of carbon-based products in both H-type and flow-type electrolysis cells.

关键词： CO2 electrolysis electrode-electrolyte interface Lewis acid-base interaction hydrogen-bonding interaction AIMD simulation

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Exploring halide perovskite nanocrystal decomposition:Insight by insitu electron paramagnetic resonance spectroscopy

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Nano Research 2025年第3期18卷 322-332页

作者： Anastasiya Sedova Philip N.Immanuel Raanan Carmieli Hila Shalom Achiad Goldreich Alen S.Thomas Jonathan Prilusky Akshay Puravankara Ido Bar-On Lena Yadgarov Department of Chemical Engineering Ariel UniversityAriel 4076414Israel Department of Molecular Chemistry and Materials Science Weizmann Institute of ScienceRehovot 7610001Israel Department of Chemical Research Support Weizmann Institute of ScienceRehovot 7610001Israel

Zero-dimensional(0D)and three-dimensional(3D)halide perovskite nanocrystals(HP-NCs),owing to their unique optoelectronic properties,are extensively studied for photocatalytic ***,HPs are highly sensitive to light,humidity,and other environmental factors,which accelerate their *** the decomposition process is crucial for gaining insights into how to stabilize ***,we investigate the radical-driven decomposition process and dynamics of the 0D Cs_(4)PbBr_(6)and 3D CsPbBr_(3)NCs under the influence of visible light and a polar solvent by electron paramagnetic resonance(EPR)*** findings indicate that light accelerates radical formation over time,making the decomposition of HP-NCs a self-sustaining *** illumination of the NCs,hydroperoxyl radicals are formed first,followed by unconventional Br,Cs,and Pb-related radicals,indicating the initiation of NC *** decomposition of CsPbBr_(3)NCs starts after 3 min of light exposure,while Cs_(4)PbBr_(6)NCs take 18 min,indicating the greater stability of the ***,we evaluated the photocatalytic activity of the HPs toward degrading organic *** 3D CsPbBr_(3)NCs performed as superior photocatalysts compared to their 0D Cs_(4)PbBr_(6)NCs ***,linking the results of EPR measurements with the photocatalytic efficacy suggests that the CsPbBr_(3)NCs undergo degradation during the photocatalytic process,thereby serving as a sacrificial agent to enhance photocatalytic *** understanding derived from EPR spectroscopy in tracking radical formation and dynamics can be extended to enhance the stability and efficiency of various nanomaterials in optoelectronic and photocatalytic applications,thus contributing to advancements beyond the HP family.

关键词： halide perovskites electron paramagnetic resonance spectroscopy photocatalysis degradation stability

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Encapsulating perovskite quantum dots into 3D COF for visible light-driven CO_(2) reduction

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science China Chemistry 2025年第4期68卷 1478-1485页

作者： Xinxin Wang Yucheng Jin Xiya Yang Qingyu Luan Tianyu Wang Dongdong Qi Kang Wang Jianzhuang Jiang College of Chemistry and Materials Science Anhui Normal UniversityWuhu 241002China Beijing Advanced Innovation Center for Materials Genome Engineering Beijing Key Laboratory for Science and Application of Functional Molecular and Crystalline MaterialsDepartment of Chemistry and Chemical EngineeringSchool of Chemistry and Biological EngineeringUniversity of Science and Technology BeijingBeijing 100083China

Lead halide perovskite quantum dots(LHP QDs)have been revealed to possess great potential in photocatalytic applications including CO_(2)reduction;which however suffer from poor ***;a high crystalline hydrazine-linked three-dimensional(3D)covalent organic framework;USTB-17;was fabricated from the reaction between 12-connected building block and 4-connected 3,5,7-tetrakis(4-aldophenyl)-***-modification with Ni^(2+) affords the metallic framework USTB-17(Ni)followed by sequential deposition of the CH_(3)NH_(2)PbI_(3)(MAPbI_(3))perovskite QDs into its pores;generating the USTB-17(Ni)@MAPbI_(3) *** X-ray diffraction analysis together with theoretical simulations and transmission electron microscopy discloses the crystalline nature of USTB-17;USTB-17(Ni);and USTB-17(Ni)@MAPbI_(3) with an unprecedented noninterpenetrated hpt *** close contact of QDs inside the COF pores with the Ni catalytic site locating at the pore surface of COF allows a rapid transfer of the photogenerated electrons in QDs to the Ni catalytic sites;enhancing the photocatalytic activity for CO_(2)*** endows USTB-17(Ni)@MAPbI_(3) with efficient photocatalysis performance for photocatalytic CO_(2)reduction with CO generation rate of 365μmol g^(-1)h^(-1)and CO selectivity up to 96%under visible-light irradiation;7 times higher than that of USTB-17(Ni).After four cycles of reactions;the photocatalytic CO generation rate remains almost unchanged;demonstrating its excellent cycle stability.

关键词： lead halide perovskite quantum dots 3D covalent organic frameworks hpt topology photocatalytic CO_(2)reduction

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Hydrothermal synthesis of polyimide-linked covalent organic frameworks towards ultrafast and stable cathodic sodium storage

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science China Chemistry 2024年第4期67卷 1300-1310页

作者： Xiya Yang Lei Gong Zhixin Liu Qianjun Zhi Baoqiu Yu Xin Chen Kang Wang Xiaofeng Li Dongdong Qi Jianzhuang Jiang Beijing Advanced Innovation Center for Materials Genome Engineering Beijing Key Laboratory for Science and Application of Functional Molecular and Crystalline MaterialsDepartment of Chemistry and Chemical EngineeringSchool of Chemistry and Biological EngineeringUniversity of Science and Technology BeijingBeijing 100083China State Key Laboratory of Organic-Inorganic Composites College of Materials Science and EngineeringBeijing University of Chemical TechnologyBeijing 100029China

Redox-active organic materials are capturing growing attention as cathode materials for sustainable alkaline metal ion ***,the storage of Na+in most organic materials-based cathodes is plagued by low capacity and unsatisfying rate performance due to their low active site densities and limited exposed active ***,two polyimide-linked covalent organic frameworks(COFs),namely HATN-PD-COF and HATN-TAB-COF,were fabricated from hydrothermal synthesis with redoxactive triphenylene-2,3,6,7,10,11-hexacarboxylic acid and aromatic amines as starting *** X-ray diffraction and electron microscopy analysis indicate the high crystalline nature of these COFs with AA stacking configuration and orderly mesoporous tunnel.N_(2) sorption measurement discloses the permanent porosity of these two COFs with a Brunauer-EmmettTeller surface area of 1,065-1,200 m^(2)g^(-1)and a large pore size of 2.0-3.1 *** intermittent titration technique and density functional theory calculations reveal the facile Na+ion diffusion along the mesoporous tunnel of these COFs with a small energy barrier of 0.13-0.40 e *** particular,the as-prepared COFs based-cathodes show ultrafast and stable Na+storage associated with their conjugated electronic structure,highly ordered mesoporous tunnel,robust structure,and redox-active C=N/C=O-rich framework as exemplified by the high reversible capacity of 210 m A h g^(-1)at 200 m A g^(-1),record-high rate performance(195 m A h g^(-1)at a high current density of 10,000 m A g^(-1))among organic electrodes and the capacity retention of nearly 91%at 10,000 m A g^(-1)after 7,000 cycles for HATN-PD-COF.

关键词： covalent organic framework sodium ion battery cathode high rate organic electrode

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An activated fluorescent probe to monitor NO fluctuation in Parkinson’s disease

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Chinese chemical Letters 2025年第3期36卷 341-344页

作者： Tao Liu Xuwei Han Xueyi Sun Weijie Zhang Ke Gao Runan Min Yuting Tian Caixia Yin Department of Chemical and Materials Engineering Lvliang UniversityLvliang 033001China Key Laboratory of Chemical Biology and Molecular Engineering of Ministry of Education Institute of Molecular ScienceShanxi UniversityTaiyuan 030006China School of Chemistry and Chemical Engineering Shanxi UniversityTaiyuan 030006China

The imbalance of nitric oxide(NO)homeostasis in the brain is closely related to the occurrence of Parkinson’s disease(PD).Therefore,revealing the fluctuation of NO in brain is crucial for understanding the pathophysiological ***,currently developed NO probes are unsuitable for this purpose due to their poor blood-brain barrier ***,a fluorescent probe(PO-NH)with blood-brain barrier crossing capability and high selectivity for NO was *** the NO mediation,the photoinduced electron transfer(PET)process of the probe was blocked,giving an intensive fluorescence enhancement(F/F_(0)=15).Moreover,PO-NH can be used to effectively monitor changes in intracellular NO ***,due to excellent blood-brain barrier crossing ability and near-infrared(NIR)emission,PO-NH is suitable for in vivo imaging of NO in the brain and illustrating with the deterioration of PD,the level of NO gradually increased in the brain of PD *** believe that PO-NH may provide a beneficial tool for understanding the biological function of NO in the brain and revealing the complex connection between NO and PD.

关键词： Blood brain barrier Nitric oxide Fluorescent probe Turn off/on Parkinson’s disease

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A tetraaldehyde-derived porous organic cage and covalent organic frameworks:Syntheses,structures,and iodine vapor capture

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Chinese chemical Letters 2024年第9期35卷 426-431页

作者： Xinyi Cao Yucheng Jin Hailong Wang Xu Ding Xiaolin Liu Baoqiu Yu Xiaoning Zhan Jianzhuang Jiang Beijing Advanced Innovation Center for Materials Genome Engineering Beijing Key Laboratory for Science and Application of Functional Molecular and Crystalline MaterialsDepartment of Chemistry and Chemical EngineeringSchool of Chemistry and Biological EngineeringUniversity of Science and Technology BeijingBeijing 100083China

Dynamic covalent imine reactions between 2,3-dimethoxy-[1,1:4,1-terphenyl]-3,3,5,5-tetracarbaldehyde(DMTT)and cyclohexanediamine,p-phenylenediamine,and benzidine,respectively,generate a porous organic cage(DMPOC)and two covalent organic frameworks(COFs),USTB-29,and *** shows a[3+6]topological cage-like structure according to single crystal X-ray diffraction *** contrast,both microcrystalline USTB-29 and USTB-30 exhibit two-dimensional monoporous structures in an eclipsed AA stacking style based on powder X-ray diffraction and theoretical *** addition,DMPOC is capable of efficiently absorbing the iodine vapor with an outstanding uptake of 5.10 g/g,much higher than that of USTB-29(3.07 g/g)and USTB-30(3.16 g/g).Cage to COFs transformations have been realized from DMPOC to USTB-29 and USTB-30 via the imine bond exchange with slightly increased iodine vapor *** investigations uncover that both nitrogen and oxygen atoms of POC and COFs contribute to iodine vapor capture due to the formation of charge transfer matter,and loose interaction introducing adaptive expanding voids of DMPOC is suggested to capture more iodine vapor than that of COFs with strongπ-πinteractions.

关键词： Porous organic cage Crystal structure Covalent organic framework Transformation Iodine vapor adsorption

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Topochemical polymerization of hydrogen-bonded organic framework for supporting ultrafine palladium nanoparticles

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science China Chemistry 2023年第7期66卷 2019-2027页

作者： Xu Ding Bin Han Baoqiu Yu Hailong Wang Jianzhuang Jiang Beijing Advanced Innovation Center for Materials Genome Engineering Beijing Key Laboratory for Science and Application of Functional Molecular and Crystalline MaterialsDepartment of Chemistry and Chemical EngineeringSchool of Chemistry and Biological EngineeringUniversity of Science and Technology BeijingBeijing 100083China

Topochemical polymerization of molecular crystals into porous materials is of significance due to their promising applications in the field of adsorption and catalysis,yet rarely reported due to the synthesis ***,a hydrogen-bonded organic framework(HOF-45)has been fabricated by the crystallization of a cage-like building block containing three alkynyl *** exhibits almost mesoporous structure demonstrated by single crystal X-ray diffraction ***-driven topochemical polymerization of HOF-45 with ethanedithiol covalently links alkynyl groups in HOF-45,generating a hydrogen-bond and covalentbond cross-linked material(HOF-45C).In contrast to HOF-45,cross-linked HOF-45C retains the crystalline nature and displays improved solution resistence according to the powder X-ray diffraction *** particular,HOF-45C is able to support the growth of ultrafine palladium nanoparticles with the average size of ca.1.9 nm for rapidly promoting the degradation of nitrophenol,methyl orange,and congo red with the help of NaBH_(4)as well as Suzuki-Miyaura coupling *** work inputs a new idea on the HOFs application in preparing covalent-linked porous organic materials.

关键词： hydrogen-bonded organic frameworks topochemical polymerization palladium nanoparticles nitrophenol degradation organic dyes degradation Suzuki-Miyaura coupling reaction

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

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science China Chemistry 2025年第5期68卷 1642-1702页

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 School of Materials Science and Engineering Nankai University School of Physical Science and Technology Shanghai Tech University MOE Key Laboratory of Bioinorganic and Synthetic Chemistry GBRCE for Functional Molecular EngineeringSchool of ChemistryIGCMESun 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 SciencesSoochow 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 & EngineeringZhejiang University Institute for New Energy Materials and Low Carbon Technologies School of Materials Science and EngineeringTianjin University of Technology School of Chemistry and Chemical Engineering Yangzhou 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 MOFs-related fields are also discussed.

关键词： metal-organic frameworks storage and separation sensing and detection multitype catalysis energy storage

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A multifunctional electrolyte additive for zinc-ion capacitors with low temperature resistant and long lifespan

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Journal of Energy Chemistry 2024年第7期94卷 477-485页

作者： Ming Sun Zekai Zhang Shuqing Fu Yifan Zhang Ruoyu Wang Hongchun Mu Cheng Lian Wenqiang Wang Gengchao Wang Shanghai Engineering Research Center of Hierarchical Nanomaterials Shanghai Key Laboratory of Advanced Polymeric MaterialsSchool of Materials Science and EngineeringEast China University of Science and TechnologyShanghai 200237China State Key Laboratory of Chemical Engineering Shanghai Engineering Research Center of Hierarchical NanomaterialsFrontiers Science Center for Materiobiology and Dynamic Chemistryand School of Chemistry and Molecular EngineeringEast China University of Science and TechnologyShanghai 200237China State Key Laboratory of Molecular Engineering of Polymers Department of Macromolecular ScienceFudan UniversityShanghai 200438China

Aqueous zinc-ion capacitors (ZICs) are considered as potential candidates for next generation electrochemical energy storage devices due to their high safety and low ***,the existing aqueous ZICs usually have the problems of zinc dendrite growth and unsatisfactory performance at low ***,an erythritol (Eryt) additive with inhibition of zinc dendrites and anti-freezing capability was introduced into the *** experimental characterization and theoretical calculation confirm that the Eryt adsorbed on the surface of zinc anodes regulates the deposition orientation of Zn^(2+) and inhibits the formation of *** also reconstructs the solvation structure in the electrolyte to reduce water activity,enabling the electrolyte to have a lower freezing point for operation at low *** the assistance of Eryt,the Zn||Zn symmetric cell exhibits a long cycle life of 2000 h,while the ZIC assembled with activated carbon (AC) cathode and zinc anode (Zn||AC) maintains a capacity retention of 98.2% after 30,000 cycles at a current density of 10 A g^(-1)(even after 10,000 cycles at-20°C,the capacity retention rate reached 94.8%.).This work provides a highly scalable,low-cost and effective strategy for the protection of the anodes of low-temperature aqueous ZICs.

关键词： Zinc-ioncapacitors Electrolyte additive Dendrite-free Freeze-resistant electrolyte

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High-work-function transparent electrode with an enhanced air-stable conductivity based on AgNiCu core-shell nanowires for Schottky photodiode

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材料科学技术（英文版） 2025年第6期209卷 95-102页

作者： Tingting Yan Wei Yang Limin Wu Xiaosheng Fang Department of Materials Science State Key Laboratory of Molecular Engineering of PolymersFudan UniversityInstitute of OptoelectronicsShanghai 200438China SINOMACH Intelligence Technology Co. Ltd.Guangzhou 510700China Department of Materials Science State Key Laboratory of Molecular Engineering of PolymersFudan UniversityInstitute of OptoelectronicsShanghai 200438China College of Chemistry and Chemical Engineering Inner Mongolia UniversityHohhot 010021China

Silver nanowires(Ag NWs)have promising application potential in electronic displays because of their superior flexibility and *** Ni in Ag NWs has proven to be an effective strategy to im-prove its work ***,AgNi NWs-based electrodes suffer from poor electrical conductivity under air exposure due to the low-conductivity NiO generated on its ***,Cu was further doped in AgNi NWs to form AgNiCu NWs and regulate its surface oxide under long-term air ***,it is demonstrated that the conductivity of AgNiCu NWs can acquire an improved tolerable tempera-ture(over 240 ℃)and prolonged high-temperature tolerance time(over 150 min)by finely regulating the doping content Cu,indicating an enhanced air-stable *** optimized AgNiCu NWs also achieve superior transparent conductivity as pure Ag NWs and high work function as AgNi NWs,which has been successfully applied in constructing an n-type photodiode with an effective rectification effect.

关键词： Mental nanowires Cu-doping Air-stable conductivity Transparent electrode Photodiode

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