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Evolution of hollow nanosphere to microtube in the self-assembly of chiral dansyl derivatives and inversed circularly polarized luminescence

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Chinese chemical Letters 2024年第7期35卷 285-290页

作者： Sifan Du Yuan Wang Fulin Wang Tianyu Wang Li Zhang Minghua Liu Beijing Key Laboratory for Science and Application of Functional Molecular and Crystalline Materials Department of Chemistry and Chemical EngineeringSchool of Chemistry and Biological EngineeringUniversity of Science and Technology BeijingBeijing 100083China National Laboratory for Molecular Science(BNLMS) CAS Key Laboratory of ColloidInterface and Chemical ThermodynamicsInstitute of ChemistryChinese Academy of SciencesBeijing 100190China

Here,we designed asymmetric(m DS)and symmetrical(d DS)chiral V-shaped molecules by linking one or two dansyl groups to trans-1,2-cyclohexane diamine and investigated the solvent-regulated structural transformation and inversed circularly polarized luminescence(CPL)in the *** increasing water volume fraction(fw)in the mixed solvent of water/acetonitrile,asymmetric mDS selfassembled into hollow nanospheres and microtubes,while solid nanospheres and solid microplates were corresponding to symmetric d *** this transformation process,the emission of m DS and d DS was changed from yellow-green to blue and cyan color,which was ascribed to twisted intramolecular charge transfer(TICT)and locally excited(LE)fluorescence of V-shaped DS *** conformation of N,Ndimethyl groups with respect to naphthalene ring also led to the transformation of *** tubular and platelike structures had stronger and reversed CPL signals in comparison with spheroidal *** chiral information of DS assembly could be effective transferred to achiral Nile red via co-assembly strategy,which endowed Nile red exhibiting inversed induced CPL signal regulated by water *** work provides a method for achieving a variety of self-assembled structures with adjustable chiroptical properties.

关键词： CPL inversion Hollow structure Self-assembly Dansyl Chirality transfer

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Temperature-dependent microstructural evolution in a compositionally complex solid electrolyte:The role of a grain boundary transition

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Journal of Advanced Ceramics 2025年第3期14卷 163-176页

作者： Shu-Ting Ko Chaojie Du Huiming Guo Hasti Vahidi Jenna L.Wardini Tom Lee Yi Liu Jingjing Yang Francisco Guzman Timothy J.Rupert William J.Bowman Shen J.Dillon Xiaoqing Pan Jian Luo Aiiso Yufeng Li Family Department of Chemical and Nano Engineering University of California San DiegoLa JollaCalifornia 92093USA Program in Materials Science and Engineering University of California San DiegoLa JollaCalifornia 92093USA Department of Materials Science and Engineering University of California IrvineIrvineCalifornia 92697USA Department of Physics and Astronomy University of California IrvineIrvineCalifornia 92697USA Irvine Materials Research Institute University of California IrvineIrvineCalifornia 92697USA

Compositionally complex solid electrolyte(Li_(0.375)Sr_(0.4375))(Ta_(0.375)Nb_(0.375)Zr_(0.125)Hf_(0.125))O_(3)(LSTNZH)samples are synthesized using different sintering temperatures,durations,and cooling conditions(furnace cooling(FC)*** quenching(AQ)).The temperature-dependent grain growth has been examined to investigate the microstructural evolution and the origin of exaggerated(abnormal)grain *** moderate temperatures,the grain growth of LSTNZH follows a cubic root growth model with an Arrhenius temperature *** increasing temperature,bimodal microstructures develop,and the Arrhenius temperature dependence breaks ***,increasing the temperature induces increased Nb segregation at general grain boundaries(GBs),in contrast to classical GB segregation models but suggesting premelting-like GB disordering,which can explain the observed abnormal grain growth(AGG).In addition,the large grains become faceted with increasing temperature,which occurs concurrently with the temperature-induced transitions in GB segregation and grain growth,thereby further supporting the occurrence of a GB phase-like(complexion)*** impacts on the densification,ionic conductivity,and hardness are also *** work provides a new insight into the fundamental understanding of the grain growth mechanisms of the emergent class of medium-and high-entropy compositionally complex ceramics(CCCs),which is essential for tailoring microstructures and material properties.

关键词： compositionally complex ceramics(CCCs) solid electrolytes perovskite grain growth grain boundary(GB) electron backscatter diffraction(EBSD)

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Interfacial engineering of SnO_(2)/Bi_(2)O_(2)CO_(3)heterojunction on heteroatoms-doped carbon for high-performance CO_(2)electroreduction to formate

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Nano Research 2023年第2期16卷 2278-2285页

作者： Danni Wang Tingting Sun Lianbin Xu Lei Gong Baotong Chen Pianpian Zhang Tianyu Zheng Qingmei Xu Houhe Pan Yuexing Zhang 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 Beijing University of Chemical TechnologyBeijing 100029China College of Chemistry and Chemical Engineering Dezhou UniversityDezhou 253023China

Electrochemical CO_(2)reduction is a viable,economical,and sustainable method to transform atmospheric CO_(2)into carbon-based fuels and effectively reduce climate change and the energy *** robust catalysts through interface engineering is significant for electrocatalytic CO_(2)reduction(ECR)but remains a grand ***,SnO2/Bi_(2)O_(2)CO_(3)heterojunction on N,S-codoped-carbon(SnO_(2)/BOC@NSC)with efficient ECR performance was firstly constructed by a facile synthetic *** the SnO_(2)/BOC@NSC was utilized in ECR,it exhibits a large formic acid(HCOOH)partial current density(JHCOOH)of 86.7 mA·cm^(−2)at−1.2 V versus reversible hydrogen electrode(RHE)and maximum Faradaic efficiency(FE)of HCOOH(90.75%at−1.2 V versus RHE),***,the FEHCOOH of SnO_(2)/BOC@NSC is higher than 90%in the flow cell and the JHCOOH of SnO_(2)/BOC@NSC can achieve 200 mA·cm^(−2)at−0.8 V versus RHE to meet the requirements of industrialization *** comparative experimental analysis and in-situ X-ray absorption fine structure reveal that the excellent ECR performance can be ascribed to the synergistic effect of SnO_(2)/BOC heterojunction,which enhances the activation of CO_(2)molecules and improves electron *** work provides an efficient SnO_(2)-based heterojunction catalyst for effective formate production and offers a novel approach for the construction of new types of metal oxide heterostructures for other catalytic applications.

关键词： heterojunction charge transfer electrochemical CO_(2)reduction flow cell in-situ X-ray absorption fine structure

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Readily prepared and processed multifunctional MXene nanocomposite hydrogels for smart electronics

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SmartMat 2024年第2期5卷 103-114页

作者： Jiahui Huang Xianwu Huang Peiyi Wu State Key Laboratory for Modification of Chemical Fibers and Polymer Materials College of Chemistry and Chemical EngineeringCenter for Advanced Low-Dimension MaterialsDonghua UniversityShanghaiChina State Key Laboratory of Molecular Engineering of Polymers Department of Macromolecular Science and Laboratory of Advanced MaterialsFudan UniversityShanghaiChina

Booming sophisticated robotics and prosthetics put forward high requirements on soft conductive materials that can bridge electronics and biology,those soft conductive materials should imitate the mechanical properties of biological tissues and build information transmission *** now,it remains a great challenge to handle the trade-off among ease of preparation,high conductivity,processability,mechanical adaptability,and external stimuli ***,a kind of readily prepared and processed multifunctional MXene nanocomposite hydrogel is reported,which is prepared via the fast gelation of cationic monomer initiated by delaminated MXene *** gelation time can be adjusted(several seconds to minutes)based on the MXene *** adjusting the MXene ratio,the resulting nanocomposites are ultrastretchable(>5000%),three-dimensional(3D)printable,and show outstanding mechanical and electrical *** expected,the integration of multifunctional systems onto various substrates(e.g.,gloves and masks)is further demonstrated via 3D printing and could achieve diverse sensory capabilities toward strain,pressure,and temperature,showing great prospects as smart flexible electronics.

关键词： 3D printable electronics MXene polymeric hydrogels stretchable and conductive

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Metalphthalocyanine frameworks grown on TiO_(2)nanotubes for synergistically and efficiently electrocatalyzing urea production from CO_(2)and nitrate

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science China Chemistry 2023年第5期66卷 1417-1424页

作者： Ning Li Hui Gao Zhixin Liu Qianjun Zhi Bowen Li Lei Gong Baotong Chen Tao Yang Kang Wang Peng Jin 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 School of Materials Science and Engineering Hebei University of TechnologyTianjin 300130China Innovation Research Institute for Carbon Neutrality University of Science and Technology BeijingBeijing 100083China

Electrocatalytic synthesis of urea from CO_(2)and NO_(3)^(-)under ambient conditions provides an appealing alternative to the traditional energy-intensive urea synthetic *** active and selective electrocatalysts for efficient urea production are therefore urgently desired owing to the unsatisfactory performance of the thus far reported ***,a phthalocyaninebased(Pc-based)covalent organic framework(COF),namely Co Pc-COF,fabricated from the nucleophilic substitution reaction of hexadecafluorophthalocyaninato cobalt with octahydroxylphthalocyanine cobalt,in situ grew on the surface of multilayered Ti O_(2)nanotubes(NTs),generating the Co Pc-COF@Ti O_(2)NTs *** X-ray diffraction analysis in combination with electron microscopy measurements discloses the uniform coating of crystalline Co Pc-COF on the multilayered Ti O_(2)NTs in Co Pc-COF@Ti O_(2)***,electrochemical tests reveal the superior electrocatalytic activity of Co Pc-COF@Ti O_(2)NTs towards urea production from CO_(2)and NO3-with a record-high yield of 1,205μg h^(-1)cm^(-2)and an outstanding Faraday efficiency of 49%at-0.6 V versus reversible hydrogen electrode due to the significant synergistic catalysis *** situ attenuated total reflection infrared spectroscopic investigation and theoretical calculations unveil the efficient C–N coupling reaction between*CO intermediate derived from CO_(2)on Co Pc moieties and*NH2intermediate formed from NO_(3)^(-)on Ti O_(2)NTs during the urea formation process over Co Pc-COF@Ti O_(2)*** work should be helpful towards designing and fabricating high-performance electrocatalysts for sustainable synthesis of urea through efficient synergistic effect of multiactive centers.

关键词： covalent organic frameworks phthalocyanine TiO_(2) electrocatalytic urea synthesis C–N bond coupling

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Dual modifications of sensitizers and lanthanide ions on a two-dimensional zirconium-based metal-organic framework for photoluminescent detection

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CrystEngComm 2024年第22期26卷 2852-2861页

作者： Chang, Jhe-Wei Lin, Tzu-Chi Chen, You-Liang Han, Po-Chun Yang, Shang-Cheng Tsai, Meng-Dian Wu, Kevin C.-W. Kung, Chung-Wei Department of Chemical Engineering National Cheng Kung University Tainan City70101 Taiwan Department of Chemical Engineering National Taiwan University Taipei10617 Taiwan Ph. D. Program of Green Materials and Precision Devices College of Engineering National Taiwan University Taipei10617 Taiwan Department of Chemical Engineering and Materials Science Yuan Ze University Chung-Li Taoyuan320 Taiwan

A two-dimensional (2D) zirconium-based metal-organic framework (Zr-MOF) with abundant terminal -OH/-OH2 groups on its nodes, ZrBTB (BTB = 1,3,5-tris(4-carboxyphenyl)benzene), is utilized as a platform for dual post-synthetic modifications (PSM) to immobilize both the benzophenone-based photosensitizer (benzophenone-4,4′-dicarboxylate, bzpdc) and terbium ions onto the 2D Zr-MOF molecular sheets. Terbium ions are installed on the 2D Zr-MOF at various temperatures to adjust the loading of terbium ions on the 2D Zr-MOF while preserving the loading of the photosensitizer. The crystallinity, morphology, porosity, and loadings of both bzpdc ligands and terbium ions are characterized for each material, and the coordinating locations of terbium ions in the Zr-MOF structure are investigated. The photoluminescence (PL) properties of these materials are then examined. Since the installed bzpdc ligand can induce a highly efficient energy transfer to the neighbouring terbium ion upon excitation, the obtained material after dual PSM (ZrBTB-bzpdc-Tb-120) can show strong PL emissions of terbium ions upon the excitation of the bzpdc ligand at 355 nm, with a PL quantum yield of 5.04%. It is more advantageous than the 2D Zr-MOF solely functionalized with terbium ions, which can only exhibit similar emissions upon the excitation of the BTB linker at a less friendly wavelength of 310 nm, with a lower PL quantum yield of 2.94%. Owing to the high chemical stability as well as good dispersity of the luminescent ZrBTB-bzpdc-Tb-120 in water, its performances in selective PL sensing of Fe(iii) ions present in aqueous solutions are investigated. © 2024 The Royal Society of Chemistry.

关键词： Carboxylation

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Tuning the local coordination environment of silver(Ⅰ) coordination networks with counterions for enhanced electrocatalytic CO_(2) reduction

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science China Chemistry 2024年第5期67卷 1524-1530页

作者： Xiaofeng Cui Xueting Wang Cong Fu Bing Liu Mei-Yan Gao Tingting Kong Yujie Xiong Anhui Engineering Research Center of Carbon Neutrality The Key Laboratory of Functional Molecular SolidsMinistry of EducationAnhui Laboratory of Molecular-Based MaterialsCollege of Chemistry and Materials ScienceAnhui Normal UniversityWuhu 241002China Department of Chemical Sciences Bernal InstituteUniversity of LimerickLimerick V94 T9PXRepublic of Ireland School of Chemistry and Materials Science University of Science and Technology of ChinaHefei 230026China School of Chemical and Material Engineering Jiangnan UniversityWuxi 214122China

Very recently, the local coordination environment of active sites has been found to strongly influence their performance in electrocatalytic CO_(2) reduction by tuning the intrinsic kinetics of CO_(2) activation and intermediate stabilization. It is imperative to elucidate the mechanism for such an influence towards the rational design of efficient catalysts;however, the complex interactions between the multiple factors involved in the system make it challenging to establish a clear structure–performance relationship. In this work, we chose ion-intercalated silver(I)-based coordination networks(AgCNs) with a well-defined structure as a model platform, which enables us to understand the regulation mechanism of counterions as the counterions are the only tuning factor involved in such a system. We prepared two isostructural Ag CNs with different intercalation ions or counterions of BF_(4)^(-) and ClO_(4)^(-)(named as AgCNs-BF_(4) and AgCNs-ClO_(4)) and found that the former has a more competitive CO_(2) electroreduction performance than the latter. AgCNs-BF_(4) achieves the highest Faradaic efficiency for CO_(2) to CO of 87.1% at-1.0 V(vs. RHE) with a higher partial current density, while AgCNs-ClO_(4) exhibits only 77.2% at the same applied *** characterizations and theoretical calculation reveal that the presence of BF_(4)^(-)is more favorable for stabilizing the COOH^(*) intermediate by weakening hydrogen bonds, which accounts for the superior activity of Ag CNs-BF_(4).

关键词： electrocatalytic CO_(2) reduction coordination networks local environment counterions intercalation ions

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Au(Ⅰ)-BSA nanocomposites with assembling-induced excitation-dependent multicolor emission for dynamic cell imaging

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science China Chemistry 2023年第1期66卷 174-184页

作者： Xuejuan Wang Guofeng Liu Kuo Fu Xuping Li Mengting Yao Qinghua Lu Liangliang Zhu Xiang Ma Shanghai Key Laboratory of Chemical Assessment and Sustainability Advanced Research Institute School of Chemical Science and EngineeringTongjiUniversityShanghai200092China Key Laboratory for Advanced Materials and Joint International Research Laboratory of Precision Chemistry and Molecular Engineering Frontiers Science Center for Materiobiology and Dynamic ChemistrySchool of Chemistry and Molecular EngineeringEast China University of Scienceand TechnologyShanghai 200237China State Key Laboratory of Molecular Engineering of Polymers Department of Macromolecular ScienceFudan University Shanghai 200438China

Excitation wavelength dependent(Ex-De) luminescent materials have attracted intense attention due to their great potential in multicolor bioimaging,dynamic anti-counterfeiting,and light emitting ***,it remains a formidable challenge to construct an Ex-De luminescent biomaterial with green starting materials,excellent biocompatibility,good water solubility,and multiple color emission for dynamic cell *** this work,nanocomposites based on the facile self-assembly strategy of bovine serum albumin(BSA) and Au(Ⅰ)-complex are rationally designed and synthesized to simultaneously present Ex-De fluorescence(429–516 nm) and decent phosphorescence(~615 nm) in a dilute aqueous *** analyses of spectroscopic and microscopic results reveal that the luminescent mechanism of Au(Ⅰ)-BSA nanocomposites is cluster-induced Ex-De fluorescence and metal-to-ligand charge transition(MLCT) based ***,based on the excellent biocompatibility,water-solubility and color-tunable emission over the entire visible region(360–800 nm),the Au(Ⅰ)-BSA nanocomposites are successfully used for cell imaging with multiple and switchable colors on *** is more,the solid tablets of Au(Ⅰ)-BSA nanoparticles showed pressure-responsive luminescence and decent room temperature *** work provides an assembling-induced emission strategy for the design of water-soluble,non-cytotoxic,and color-tunable luminescent biomaterials based on the composite of protein and Au nanoparticles.

关键词： nanocomposites excitation wavelength-dependent emission room temperature phosphorescence assembling-induced emission dynamic cell imaging

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Intermittent oxidation kinetics and metal/oxide interfacial undulation

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Physical Review B 2024年第8期110卷 085402-085402页

作者： Dongxiang Wu Xianhu Sun Judith C. Yang Guangwen Zhou Department of Mechanical Engineering & Materials Science and Engineering Program Department of Chemical and Petroleum Engineering

The phenomenon of oxygen adsorption induced surface restructuring is widespread across various metal-oxygen systems, yet its impact on initiating bulk oxide formation remains largely unexplored. Through in situ atomic-resolution electron microscopy observations of surface oxidation of Cu(110) and Cu85Au15(110), we unveil intermittent oxide-film growth modulated by oxygen-induced surface restructuring. This modulation is evidenced by repeated pinning of the Cu2O growth front at isolated Cu columns of the c(6×2)-O reconstruction, owing to required long-range diffusion of Cu and O atoms to the Cu2O growth front. We reveal that Cu vacancies, generated at the Cu2O growth front, are injected into the Cu2O/Cu interface, inducing hill and valley undulation of the Cu2O film. In contrast, atomic vacancies produced during the Cu85Au15(110) oxidation preferentially migrate into interfaces between Au-rich and Au-poor regions in the bulk, resulting in a flat and adherent Cu2O film. These findings demonstrate the critical role of oxygen-induced surface restructuring in modulating oxide film growth kinetics and the manipulability of the fate of injected vacancies by alloying, thereby offering insights applicable to a broader range of metal-oxygen systems for fine-tuning oxidation kinetics and enhancing oxide/metal interfacial adhesion.

关键词： Surface & interfacial phenomena Surface reconstruction Surface growth Density functional theory Transmission electron microscopy

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High Performance Microwave Absorption Material Based on Metal-Backboned Polymer

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Chinese Journal of Polymer science 2024年第12期42卷 1881-1887,I0006页

作者： Jia-Ning Xu Kai-Wen Zeng Yi-Feng Zhang Yi-Bei Yang Zi-Wei Liu Yue Liu Jia-Jia Wang Kai-Lin Zhang Yan-Ru-Zhen Wu Hao Sun Hui-Sheng Peng State Key Laboratory of Molecular Engineering of Polymers Department of Macromolecular ScienceInstitute of Fiber Materials and Devicesand Laboratory of AdvancedMaterialsFudanUniversityShanghai200438China Frontiers Science Center for Transformative Molecules Schoolof Chemistry and Chemical Engineeringand Zhangjiang Institute for Advanced StudyShanghai JiaoTongUniversityShanghai200240China

Metal-backboned polymers with anisotropy microstructures are promising for conductive,optoelectronic,and magnetic functional ***,the structure-property relationships governing the interplay between the chemical structure and electromagnetic property of the metal-backboned polymer have been rarely *** we report a carbon/nickel hybrid from metal-backboned polymer to serve as electromagnetic wave-absorbing materials,which exhibit high microwave absorption capacity and tunable absorption *** presence of nickel backbones promote the generation of heterogeneous interfaces with carbon during calcination,thereby enhancing the wave-absorbing capacity of the carbon/nickel *** C/Ni hybrids show a minimal reflection loss of-49.1 dB at 13.04 GHz,and its frequency of the absorption band can be adjusted by controlling the thickness of the absorption layer.

关键词： Nickel Metal-backboned polymer Carbon Hybrid material

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