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Inherently Chiral and Symmetrical Heteroatom-Doped Zigzag-Type Hydrocarbon Belts

CCS chemistry 2024年第5期6卷 1198-1210页

作者： Xue-Yuan wang Xin-Yu Zhang Shuo Tong Qing-Hui Guo mei-Ling Tan Cheng-Jun Li mei-{3. wang key laboratory of Bioorganic Phosphorous {2. and {3. biology(Ministry of Education) Department of ChemistryTsinghua UniversityBeijing 100084

hydrocarbon belts due to their potential applications in carbon *** contrast,heteroatomembedded zigzag hydrocarbon belts as advanced design strategies with fascinating structures and desirable,unique properties have remained largely unexplored,and inherently chiral ones are ***,we report the synthesis of a diversity of symmetric and highly enantiopure inherently chiral O-and N-doped zigzag-type hydrocarbon belts starting from strainless macrocycles based on fjord-stitching *** readily available pertriflated resorcin[6]arene underwent partial hydrolyses and intramolecular S_(N)Ar reactions to form a calix[3.(9H-xanthene)derivative and a prochiral half-belt *** transformations of calix[3.(9H-xanthene)into C_(3.)-symmetric molecular belts were achieved by closing the rest of the fjords with triple intramolecular S_(N)Ar reactions and Yamamoto homo coupling reactions,as well as palladiumcatalyzed intermolecular acridination reactions with primary *** prochiral half-belt underwent enantioselective desymmetrizative mono-acridination to afford an inherently chiral N,O_(4)-bridged pseudo-belt with an enantiomeric excess(ee)value of>99%under the catalysis of Pd(OAc)_(2.and(R)-*** closure reactions of the pseudo-belt produced diverse heteroatom-inlayed zigzag-type hydrocarbon belts of inherent ***,we showed the unique cavity structures of the belts and demonstrated interesting chiroptic properties of the inherently enantiopure chiral *** research opens the door for the exploration of novel and sophisticated symmetric and inherently chiral molecular nanobelt structures with outstanding physical and chemical properties,as well as potential applications.

关键词： zigzag-type molecular belt heterocycle chiroptical property fjord-stitching strategy resorcinarene

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Graphdiyne(C_(n)H_(2.-2.)as an"electron transfer bridge"boosting photocatalytic hydrogen evolution over Zn_(0.5)Co_(0.5)S/MoS_(2.S-scheme heterojunction

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Rare Metals 2024年第5期43卷 1999-2014页

作者： mei Li Jing-Zhi wang Zhi-Liang Jin School of chemistry and chemical Engineering North Minzu UniversityYinchuan 750021China School of chemistry and chemical Engineering Ningxia Key Laboratory of Solar Chemical Conversion TechnologyKey Laboratory for Chemical Engineering and TechnologyState Ethnic Affairs CommissionNorth Minzu UniversityYinchuan 750021China

In the process of photocatalytic water cracking,the migration rate and utilization rate of photogenerated charges determine the hydrogen evolution performance of the *** this paper,a carbon isotope superconducting material graphdiyne(GDY)is prepared by mechanical ball milling and introduced into the S-scheme heterojunction Zn_(0.5)Co_(0.5)S/MoS_(2.inorganic *** terms of hydrogen evolution kinetics,GDY acts as an electron bridge,not only accelerating the migration of photogenerated carriers but also improving the utilization of photogenerated ***,the large twodimensional layer provides more loading and anchoring points for Zn_(0.5)Co_(0.5)S/MoS_(2.,which increases the number of active *** ternary composite catalyst 2.%GDY/Zn_(0.5)Co_(0.5)S/MoS_(2.(2.-GCSM)generates 69.94μmol of hydrogen(5 h)in triethanolamine *** is 2.97 and1.80 times higher than Zn_(0.5)Co_(0.5)S and Zn_(0.5)Co_(0.5)S/MoS_(2.,*** the cyclic experiment,it still has stable hydrogen evolution performance after standing for2. h(under dark conditions).In addition,the potential mechanism of photocatalytic hydrogen evolution is demonstrated through in-situ X-ray photoelectron *** work provides a reference for further research in the field of introducing carbon materials into photocatalytic systems and improving the utilization of photogenerated charges.

关键词： Graphdiyne S-scheme heterojunction Electron transfer bridge Hydrogen production

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Synthesis, Crystal Structures and Catalysis of Dinuclear Cd(Ⅱ) Complexes Bridged by Unusual (N,O,O′)-Coordinated α-Amino Acids

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chemical Research in Chinese Universities 2012年第1期28卷 73-78页

作者： DENG Dong-sheng1,2. wang Li1, PEI Ya-mei1, FENG Lu2.and LIU Chang-lin1 1. {2. laboratory of Pesticide & chemical biology, Ministry of Education, School of chemistry, Central china Normal university, Wuhan 43.079, P. R. china 2. College of chemistry and chemical Engineering, Luoyang Normal university, Luoyang 47102., P. R. china School of chemistry Central China Normal University Key Laboratory of Pesticide & Chemical Biology Ministry of Education Wuhan 430079 College of chemistry and chemical Engineering Luoyang Normal University Luoyang 471022

Four dinuclear amino acid cadmium（II） complexes [Cd2.tren）2.dl-alaninato）]（ClO4）3.H2.（I）, [Cd2.tren）2. （l-alaninato）]（ClO4）3.H2.（II）, [Cd2.tren）2.dl-phenylalaninato）]（ClO4）3.III） and [Cd2.tren）2.l-phenylalaninato）]· （ClO4）3.IV）, constructed from mixed ligands of tris（2.aminoethyl）amine（tren） and racemic or natural amino ac ids（amino acids=dl or l-alanine, and dl or l-phenylalanine）, have been synthesized and characterized by X-ray crys tallography. The structural analysis of complexes I and III reveals that the cadmium centers are coordinated by one tren ligand and one amino acid molecule with the unusual （N,O,O′）-bridged mode, resulting in asymmetric chromo phores of CdN4O and CdN5O in complex I, CdN4O2.and CdN5O in complex III, respectively. The utility of the four complexes as efficient water-compatible Lewis acid catalysts for the direct aldol reaction in water was examined. The reaction proceeded smoothly to afford the corresponding β-hydroxy ketones in up to 99% yield. Moreover, the dias tereoselectivity of the reaction favors the formation of the syn-isomers.

关键词： Dinuclear cadmium(II) complex Amino acid Aldol reaction

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Facet-dependent transformation and toxicity of nanoscale zinc oxide in the synthetic saliva

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Journal of Environmental Sciences 2024年第5期139卷 170-181页

作者： xiang Zhang Yunpeng Huang Jikun wang Jie Tang Yang{2. Nali Zhu Zhigang Li Lingxiangyu Li Yaweiwang School of Environment Hangzhou Institute for Advanced StudyUniversity of Chinese Academy of SciencesHangzhou 310024China College of Resources and Environment University of Chinese Academy of SciencesBeijing 100049China State key laboratory of Environmental {2. and Ecotoxicology Research Center for Eco-Environmental SciencesChinese Academy of SciencesBeijing 100085China key laboratory of Systems Health Science of Zhejiang Province Hangzhou Institute for Advanced StudyUniversity of Chinese Academy of SciencesHangzhou 310024China department of chemistry University of PennsylvaniaPhiladelphia 19104USA

The nanoscale zinc oxide(n-ZnO)was used in food packages due to its superior antibac terial activity,resulting in potential intake of n-ZnO through the digestive system,wherein n-ZnO interacted with *** recent,facet engineering,a technique for controlling the exposed facets,was applied to n-ZnO,whereas risk of n-ZnO with specific exposed facets in saliva was *** nanoflakes(ZnO-0001)and nanoneedles(ZnO-1010)with the pri mary exposed facets of{0001}and{1010}respectively were prepared in this study,investigat ing stability and toxicity of ZnO-0001 and ZnO-1010 in synthetic *** ZnO-0001 and ZnO-1010 partially transformed into amorphous Zn_(3.(PO_(4))_(2.within 1 hr in the saliva even containing orgnaic components,forming a ZnO-Zn_(3.(PO_(4))_(2.core-shell *** less,ZnO-1010 relative to ZnO-0001 would likely transform into Zn_(3.(PO_(4))_(2.,being attributed to superior dissolution of{1010}facet due to its lower vacancy formation energy(1.15 eV than{0001}facet(3.90 eV)).The toxicity of n-ZnO to Caco-2.cells was also dependent on the primary exposed facet;ZnO-0001 caused cell toxicity through oxidative stress,whereas ZnO-1010 resulted in lower cells viability than ZnO-0001 through oxidative stress and mem brane *** functional theory calculations illustrated that·O_(2.^(-)was formed and released on{1010}facet,yet O_(2.^(2.)instead of·O_(2.^(-)was generated on{0001}facet,leading to low oxidative stress from *** findings demonstrated that stability and toxicity of n-ZnO were dependent on the primary exposed facet,improving our understanding o health risk of nanomaterials.

关键词： The exposed facet Nanoscale ZnO chemical transformation Synthetic salica Nanotoxicity

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Inducing mitochondriopathy-like damages by transformable nucleopeptide nanoparticles for targeted therapy of bladder cancer

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National Science Review 2024年第4期11卷 216-227页

作者： Da-Yong Hou Ni-Yuan Zhang Lu wang mei-Yu Lv {2.-Peng Li Peng Zhang Yue-Ze wang Lei Shen Xiu-Hai Wu Bo Fu Peng-Yu Guo Zi-Qi wang Dong-Bing Cheng Hao wang Wanhai Xu NHC and CAMS key laboratory of Molecular Probe and Targeted Theranostics Heilongjiang Key Laboratory of Scientific Research in Urology Harbin Medical University department of Urology Harbin Medical University Cancer Hospital CAS key laboratory for Biomedical Effects of Nanomaterials and Nanosafety CAS Center for Excellence in NanoscienceNational Center for Nanoscience and Technology(NCNST) School of chemistry Chemical Engineering & Life Science Hubei Key Laboratory of Nanomedicine for Neurodegenerative Diseases Wuhan University of Technology

Mitochondriopathy inspired adenosine triphosphate(ATP) depletions have been recognized as a powerful way for controlling tumor growth. Nevertheless, selective sequestration or exhaustion of ATP under complex biological environments remains a prodigious challenge. Harnessing the advantages of in vivo self-assembled nanomaterials, we designed an Intracellular ATP Sequestration(IAS) system to specifically construct nanofibrous nanostructures on the surface of tumor nuclei with exposed ATP binding sites,leading to highly efficient suppression of bladder cancer by induction of mitochondriopathy-like ***, the reported transformable nucleopeptide(NLS-FF-T) self-assembled into nuclear-targeted nanoparticles with ATP binding sites encapsulated inside under aqueous conditions. By interaction with KPNA2. the NLS-FF-T transformed into a nanofibrous-based ATP trapper on the surface of tumor nuclei,which prevented the production of intracellular energy. As a result, multiple bladder tumor cell lines(T2.,EJ and RT-112. revealed that the half-maximal inhibitory concentration(IC50) of NLS-FF-T was reduced by approximately 4-fold when compared to NLS-T. Following intravenous administration, NLS-FF-T was found to be dose-dependently accumulated at the tumor site of T2. xenograft mice. More significantly, this IAS system exhibited an extremely antitumor efficacy according to the deterioration of T2. tumors and simultaneously prolonged the overall survival of T2. orthotopic xenograft mice. Together, our findings clearly demonstrated the therapeutic advantages of intracellular ATP sequestration-induced mitochondriopathy-like damages, which provides a potential treatment strategy for malignancies.

关键词： self-assembly nucleopeptide nanomaterial bladder cancer mitochondriopathy

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Simultaneous integration of Fe clusters and NiFe dual single atoms in nitrogen-doped carbon for oxygen reduction reaction

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Nano Research 2024年第4期17卷 2291-2297页

作者： Jirong Bai Yuebin Lian Yaoyao Deng mei xiang Peng Xu Quanfa Zhou Yawen Tang Yaqiong Su Research Center of Secondary Resources and Environment School of Chemical Engineering and MaterialsChangzhou Institute of TechnologyChangzhou 213022China Jiangsu key laboratory of New Power Batteries School of Chemistry and Materials ScienceNanjing Normal UniversityNanjing 210023China School of chemistry Engineering Research Center of Energy Storage Materials and Devices of Ministry of EducationNational Innovation Platform(Center)for Industry-Education Integration of Energy Storage TechnologyXi’an Jiaotong UniversityXi’an 710049China

Atomically-dispersed iron-based electrocatalysts are promising substitutes for noble metal electrocatalysts because of excellent performance in oxygen reduction reaction(ORR).Rationally modulating the local coordination environment of the Fe site and optimizing the binding energy of oxygen reduction intermediates are effective strategies to optimize ORR ***,we report a new method in which Ni is introduced to construct NiFe dual single atoms and iron nanoclusters loaded on the nitrogen-doped carbon with a highly porous *** design plays a synergistic role of dual single atoms and clusters,optimizes the 3. orbital and Fermi level of Fe,breaks the symmetrical structure of Fe-N_(4),and effectively improves the adsorption/desorption behavior of the oxygen-containing *** tests show FeNCs/NiFeSAs-NC has an excellent intrinsic *** calculations show the oxygen-containing species on the Ni active site will move to the middle of NiFe(bridge site connection)after optimization and that the key step is OH desorption,with a reaction energy of 0.2. *** electron exchange between NiFe-N6 and Fe-cluster is very strong,further indicating the introduction of Ni species and Fe clusters has a regulatory effect on the electronic structure of Fe-N_(4).

关键词： NiFe dual single atoms Fe clusters OH*adsorption energy oxygen reduction reaction

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Engineering the Interface Between Au Nanoparticles and CoO-Ov to Enhance the Catalytic Performance of 5-Hydroxymethylfurfural(HMF)to 2.5-Dimethylfuran(DMF)

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chemical Research in Chinese Universities 2024年第1期40卷 47-54页

作者： xiang Shuang GUO Yong LIU Xiaohui wang Yanqin key laboratory for Advanced Materials and Joint International Research laboratory of Precision {3. and Molecular Engineering Feringa Nobel Prize Scientist Joint Research CenterResearch Institute of Industrial CatalysisSchool of Chemistry and Molecular EngineeringEast China University of Science and TechnologyShanghai 200237P.R.China

The interface between Au and support has attracted extensive interest because of its unique catalytic ability for hydrogen activation in catalytic hydrogenation/hydrogenolysis ***,we create the Au-CoO-OV interface in the 1.0%Au/Co3.4-Rod-2.0 catalyst,which could dissociate H2.via the heterolytic way to yield rich hydride species and achieve excellent catalytic performance in the hydrogenolysis of biomass-derived 5-hydroxymethylfurfural(HMF)to 2.5-dimethylfuran(DMF).The XRD and HRTEM analyses show that Au nanoparticles are uniformly dispersed on CoO-OV surface and in situ DRIFTS spectra show the enhancement of heterolytic dissociation of hydrogen(signals of Au-D and O-D vibration)compared with bare CoO(Co3.4-Rod-2.0).This work provides insights for fabricating highly active Au-support catalysts for catalytic hydrogenation/hydrogenolysis reactions.

关键词： Au-CoO-OV interface Hydride species Heterolytic dissociation 5-Hydroxymethylfurfural(HMF) 2 5-Dimethylfuran(DMF)

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Control of aluminum distribution in ZSM-5 zeolite for enhancement of its catalytic performance for propane aromatization

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Frontiers of chemical Science and Engineering 2024年第8期18卷 15-24页

作者： Zhao Ma Dezhi Shi Sen wang mei Dong Weibin Fan State key laboratory of Coal Conversion Institute of Coal ChemistryChinese Academy of SciencesTaiyuan 030001China university of Chinese Academy of Sciences Beijing 100049China

Regulation of aluminum distribution in zeolite framework is an effective method for improving its catalytic performance for propane ***,we found that recrystallization and post-realuminization of ZSM-5 cannot only create hollow structures to enhance the diffusion ability,but also adjust the content and position of paired aluminum species in its *** characterizations results confirmed that increase of paired aluminum content and inducement of more aluminum atoms sited in the intersection cavity are beneficial to the formation of aromatic products in propane *** a result,the hollow-structured ZSM-5 zeolite with more paired aluminum(H-2.0-hollow)showed higher propane conversion and aromatics selectivity than other samples at the same *** catalytic performance of H-2.0-hollow can be further improved by ion-exchanging with a small amount of Ga(III)*** propane conversion and aromatics selectivity of Ga-2.0-hollow reached as high as 95%and 70%,respectively,at 540°C and 1 atm.

关键词： propane aromatization zeolite aluminum distribution recrystallization and post-realuminization

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Metal-organic framework hybrid materials of ZIF-8/RGO for immobilization of D-amino acid dehydrogenase

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Nano Research 2024年第1期17卷 290-296页

作者： Hangbin Lei Qian Zhang Xiaoyan xiang Liang Jiang Shiyan wang Lingxuan Duan Shizhen wang department of chemical and Biochemical Engineering College of Chemistry and Chemical EngineeringXiamen UniversityXiamen 361005China Xiamen key laboratory of Synthetic Biotechnology Xiamen UniversityXiamen 361005China

Immobilization of D-amino acid dehydrogenase(DAADH)by the assembly of peptide linker was studied for the biosynthesis of *** material of zeolitic imidazolate framework-8(ZIF-8)combined with reduced graphene oxide(RGO)was applied for the immobilization of DAADH from Ureibacillus *** recovery rate of DAADH/ZIF-8/RGO was 165.6%.DAADH/ZIF-8/RGO remained 53.4%of its initial activity at 50°C for 10 h while the free enzyme was ***/ZIF-8/RGO maintained 70.5%activity in hyperalkaline solution with pH *** parameters indicated that DAADH/ZIF-8/RGO had greater affinity of phenylpyruvate as V_(max)/K_(m)of DAADH/ZIF-8/RGO was 1.2.-fold than free *** seven recycles,the activity of DAADH/ZIF-8/RGO remained 64.3..Furthermore,one-step separation and in situ immobilization of DAADH by ZIF-8/RGO/Ni was carried out with 1.5-fold activity *** peptide linker and metal-organic framework(MOF)immobilization,thermostability and activity of the immobilized DAADH were significantly improved.

关键词： D-Amino acid dehydrogenase immobilization metal-organic frameworks zeolitic imidazolate framework-8(ZIF-8) reduced graphene oxide

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A Simple-Prepared and Multi-Reusable Adhesive Based on Epoxy Vitrimer

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Chinese Journal of Polymer Science 2024年第10期42卷 1589-1594,I0015页

作者： Yu-Ting wang Huan Liang Yen Wei Jian-Long wang {2.-Ming He Yang Yang Institute of Nuclear and New Energy Technology Tsinghua UniversityBeijing100084China The key laboratory of Bioorganic Phosphorus {2.&{3. biology(Ministry of Education) Department of ChemistryTsinghua UniversityBeijing100084China

Adhesives play an important role in modern society's production and daily *** robust and sustainable adhesives remains a great *** we report a sustainable epoxy-vitrimer adhesive with high adhesive strength(about 10 MPa)and reusability(82.strength after 3.times).This adhesive can be fabricated from commercially available products through a straightforward hot-pressing method without the need of *** adhesive process is also simple,requiring only 3. min at 180℃.In addition,the vitrimer adhesive has the advantages of both erasability for reuse and excellent water *** work provides a facile strategy to fabricate high-strength adhesive that ensures reusability,recyclability,low cost of raw materials,and simple processing ***,it expands the range of potential applications for epoxy vitrimers.

关键词： Epoxy Vitrimer Adhesive Reusable Sustainable

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