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Strong metal-support interactions between highly dispersed Cu^(+) species and ceria via mix-MOF pyrolysis toward promoted water-gas shift reaction

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Journal of Energy Chemistry 2024年第4期91卷 475-483页

作者： Xiao-Chen Sun Xing-Chi Li Ze-Wei Xie Chen-Yue Yuan De-Jiu Wang Qian Zhang Xiao-Yu Guo Hao Dong Hai-Chao Liu Ya-Wen Zhang beijing national laboratory for molecular sciences(bnlms) State Key Laboratory of Rare Earth Materials Chemistry and ApplicationsPKU-HKU Joint Laboratory in Rare Earth Materials and Bioinorganic ChemistryCollege of Chemistry and Molecular EngineeringPeking UniversityBeijing 100871China beijing national laboratory for molecular sciences(bnlms) College of Chemistry and Molecular EngineeringPeking UniversityBeijing 100871China beijing national laboratory for molecular sciences(bnlms) State Key Laboratory for Structural Chemistry of Stable and Unstable SpeciesCollege of Chemistry and Molecular EngineeringPeking UniversityBeijing 100871China

The modulation of metal-support interfacial interaction is significant but challenging in the design of high-efficiency and high-stability supported ***,we report a synthetic strategy to upgrade Cu-CeO_(2)interfacial interaction by the pyrolysis of mixed metal-organic framework(MOF)*** obtained highly dispersed Cu/CeO_(2)-MOF catalyst via this strategy was used to catalyze water-gas shift reaction(WGSR),which exhibited high activity of 40.5μmolCOgcat^(-1).s^(-1)at 300℃and high stability of about 120 *** on comprehensive studies of electronic structure,pyrolysis strategy has significant effect on enhancing metal-support interaction and then stabilizing interfacial Cu^(+)species under reaction *** Cu^(+)species and generated oxygen vacancies over Cu/CeO_(2)-MOF catalyst played a key role in CO molecule activation and H2O molecule dissociation,*** collaborated closely and then promoted WGSR catalytic performance in comparison with traditio nal supported *** study shall offer a robust approach to harvest highly dispersed catalysts with finely-tuned metal-support interactions for stabilizing the most interfacial active metal species in diverse heterogeneous catalytic reactions.

关键词： Cu-based catalyst MOF derivative Water-gas shift reaction Metal-support interaction

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An unprecedented synthesis of axially chiral biaryls by rearrangement and aromatization of carbocations with central-to-axial conversion of chirality

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Science China Chemistry 2024年第9期67卷 2998-3003页

作者： Qi Liu Xue-Dong Li Liang Cheng Li Liu beijing national laboratory for molecular sciences(bnlms) CAS Key Laboratory of Molecular Recognition and FunctionCAS Research/Education Center for Excellence in Molecular SciencesInstitute of ChemistryChinese Academy of SciencesBeijing 100190China University of Chinese Academy of sciences Beijing 100049China

The central-to-axial chirality conversion represents a fascinating class of chemical processes consisting of the destruction of stereogenic centers and the simultaneous installation of axial chiral elements,which provides efficient methods for the preparation of axially chiral ***,developing catalytic asymmetric approaches for constructing these central chirality precursors and the efficient central-to-axial chirality conversion remains a challenge due to the requirement of aromatization or elimination *** this work,we have developed an unprecedented enantioselective intramolecular FriedelCrafts alkylation with unactivated-ketone carbonyls from which a chiral tertiary alcohol was generated with high efficiency and excellent *** addition,the central-to-axial chirality conversion strategy has been successfully applied to the synthesis of enantioenriched biaryls via a less-explored carbocation-initiated rearrangement and aromatization under the promotion of Lewis *** methodology provided a straightforward and sustainable access to a broad range of biaryl-2-carboxylic acid and in excellent yields(up to 92%)and excellent central-to-axial chirality conversion(up to 99%conversion percentage).This work could be a great model for developing new methods for synthesizing axially chiral biaryls and a general protocol for the rearrangement and aromatization of carbocations for further functionalization.

关键词： br?nsted acid catalysis desymmetrization phosphoric acid axially chiral biaryls central-to-axial conversion

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Solid-state lithium-ion batteries for grid energy storage:opportunities and challenges

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Science China Chemistry 2024年第1期67卷 43-66页

作者： Xin Chang Yu-Ming Zhao Boheng Yuan Min Fan Qinghai Meng Yu-Guo Guo Li-Jun Wan CAS Key laboratory of molecular Nanostructure and Nanotechnology CAS Research/Education Center for Excellence in Molecular SciencesBeijing National Laboratory for Molecular Sciences(BNLMS)Institute of ChemistryChinese Academy of Sciences(CAS)Beijing 100190China University of Chinese Academy of sciences Beijing 100049China

The energy crisis and environmental pollution drive more attention to the development and utilization of renewable *** the capricious nature of renewable energy resource,it has difficulty supplying electricity directly to consumers stably and efficiently,which calls for energy storage systems to collect energy and release electricity at peak *** to their flexible power and energy,quick response,and high energy conversion efficiency,lithium-ion batteries stand out among multiple energy storage technologies and are rapidly deployed in the *** superior performance and ensuring the safety of energy storage systems,intrinsically safe solid-state electrolytes are expected as an ideal alternative to liquid *** this review,we systematically evaluate the priorities and issues of traditional lithium-ion batteries in grid energy *** lithium-ion batteries containing liquid electrolytes,solid-state lithium-ion batteries have the potential to play a more significant role in grid energy *** challenges of developing solid-state lithium-ion batteries,such as low ionic conductivity of the electrolyte,unstable electrode/electrolyte interface,and complicated fabrication process,are discussed in ***,the safety of solid-state lithium-ion batteries is *** the obtained insights,inspiring prospects for solid-state lithium-ion batteries in grid energy storage are depicted.

关键词： lithium-ion batteries grid energy storage solid-state electrolytes interface stability

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Hydrogen generation from NaBH_(4) for portable proton exchange membrane fuel cell

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Materials Reports(Energy) 2024年第1期4卷 69-78页

作者： Bingxue Sun Xingguo Li Jie Zheng beijing national laboratory for molecular sciences(bnlms) College of Chemistry and Molecular EngineeringPeking UniversityBeijing100871PR China

Sodium borohydride(NaBH_(4)) is considered as the most potential hydrogen storage material for portable proton exchange membrane fuel cells(PEMFC)because of its high theoretical hydrogen ***,the slow and poor kinetic stability of hydrogen generation from NaBH_(4) hydrolysis limits its *** are two main factors influencing the kinetics stability of hydrogen generation from NaBH_(4).One factor is that the alkaline byproducts(NaBO_(2)) of the hydrolysis reaction can increase the pH of the solution,thus inhibiting the reaction *** mainly happens in the NaBH_(4) solution hydrolysis *** factor is that the monotonous increase in reaction temperature leads to uncontrollable and unpredictable hydrolysis rates in the solid NaBH_(4) hydrolysis *** is due to the excess heat generated from this exothermic reaction in the initial reaction of NaBH_(4) *** this perspective,we summarize the latest research progress in hydrogen generation from NaBH_(4) and emphasize the design principles of catalysts for hydrogen generation from NaBH_(4) solution and solid state NaBH_(4).The importance of carbon as catalyst support material for NaBH_(4) hydrolysis is also highlighted.

关键词： NaBH_(4)hydrolysis Hydrogen generation Catalyst Kinetics Carbon support materials

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Reduction of dinitrogen to ammonia on doped three-atom clusters Nb_(2)M(M=Sc to Cu & Y to Ag)

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Rare Metals 2024年第8期43卷 3810-3818页

作者： Ran Cheng Chao-Nan Cui Zhi-Xun Luo beijing national laboratory for molecular Science(bnlms) State Key Laboratory for Structural Chemistry of Unstable and Stable SpeciesInstitute of ChemistryChinese Academy of SciencesBeijing 100190China School of Chemical Science University of Chinese Academy of SciencesBeijing 100049China

Catalytic reduction of dinitrogen to ammonia under mild conditions remains an attractive topic for the purpose of lowering energy ***-atom metal clusters have been proved an ideal model to explore highly efficient catalysts taking advantage of unique geometric/electronic structures and cooperative active *** a study of N2 activation and reduction on seventeen bimetallic Nb_2M(M=Sc to Cu,and Y to Ag) clusters was *** key processes for ammonia fixation(namely nitrogen activation,hydrogenation,and ammonia desorption) are fully studied,and three preferred systems(Nb_2Ni,Nb_2Rh and Nb_2Pd) are highlighted with outstanding catalytic *** d-σ and d-π~* orbital hybridizations between these metal clusters and N_(2) were demonstrated and the internal association with the N≡N bond activation was *** examining the ammonia synthesis on four chosen Nb_(2)M clusters(M=Fe,Ni,Rh and Pd),it can be elucidated that the distal pathway is more favorable than the alternative pathway in these *** work not only clarifies the N_(2) reduction on the bimetallic Nb_(2)M clusters,but also guides efficient bimetallic catalyst design.

关键词： Three-atom cluster catalysis Three-criteria strategy Nitrogen fixation Ammonia synthesis Theoretical calculations

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Natural products inspired[3+2]cycloaddition enables efficient construction of hydroxylated tetrahydrofuran acetals and concise syntheses of lignans

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Science China Chemistry 2024年第7期67卷 2306-2313页

作者： Dong-Yue Cai Weiming Shi Zhao-Hui Jin Zhi-Xiang Yu Jin-Xin Zhao Jian-Min Yue State Key laboratory of Drug Research Shanghai Institute of Materia MedicaChinese Academy of SciencesShanghai 201203China University of Chinese Academy of sciences Beijing 100049China beijing national laboratory for molecular sciences(bnlms) Key Laboratory of Bioorganic Chemistry and Molecular Engineering of Ministry of EducationCollege of ChemistryPeking UniversityBeijing 100871China

Mimicking biosynthetic pathways of hongkonoids led to the development of a new Cu(Ⅰ)-catalyzed[3+2]cycloaddition ofα-hydroxyketone andβ-keto enol ethers,affording tetrahydrofuran acetals in a highly diastereoselective manner and 100%atom *** studies on the mechanism disclosed a concerted but asynchronous Michael addition/aldol *** the same importance,this methodology provides a practical biomimetic approach for one-step construction of the dibenzylbutyrolactol lignan backbone starting from two phenyl propane derivatives,opening up a powerful new approach for lignan synthesis,which is showcased by succinct total syntheses of two biologically important aryltetralin-type lignans,β-apopicropodophyllin and *** the mild and operationally simple conditions,the developed chemistry might have a promising prospect in potential industrial applications.

关键词： [3+2]cycloaddition transition-metal catalysis tetrahydrofuran lignans natural products

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Advances of graphdiyne-supported metal catalysts in thermocatalytic reactions

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Nano Research 2024年第4期17卷 2223-2233页

作者： Jia Yu Yida Yang Yuliang Li Changyan Cao Weiguo Song beijing national laboratory for molecular sciences CAS Research/Education Center for Excellence in Molecular SciencesLaboratory of Molecular Nanostructures and NanotechnologyInstitute of ChemistryChinese Academy of SciencesBeijing 100190China School of Chemical sciences University of Chinese Academy of SciencesBeijing 100049China beijing national laboratory for molecular sciences CAS Research/Education Center for Excellence in Molecular SciencesLaboratory of organic solidsInstitute of ChemistryChinese Academy of SciencesBeijing 100190China

Supported metal catalysts are widely used in the modern chemical *** electronic interaction between supports and active components is of great significance for heterogeneous ***(GDY),a new type of carbon allotrope with sp-hybridized carbon atoms,πconjugate structure,and electron transmission capability,is a promising candidate as catalyst *** years have witnessed the rapid progress of GDY-supported metal catalysts for different catalysis *** that most processes in the current chemical industry are thermocatalytic reactions,we herein give an overview about the advances and particular characteristics of GDY-supported catalysts in these *** geometric structure and electronic properties of GDY are first ***,the synthesis methods for GDY-supported metal catalysts and their applications in thermocatalytic reactions are discussed,in which the effect of electronic interaction on catalytic performance is ***,the current challenges and future directions of GDY-supported metal catalysts for thermocatalysis are *** is expected that this review will enrich our understanding of the advances of GDY as a superior support for metal catalysts in thermocatalytic reactions.

关键词： graphdiyne metal catalysts thermocatalytic reactions heterogeneous catalysis

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A star-like photodetector for angle-based light sensing in 3D space

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Nano Research 2024年第8期17卷 7567-7573页

作者： Qi Pan Sisi Chen Hongfei Xie Qiling Xu Meng Su Yanlin Song College of Chemistry Zhengzhou UniversityZhengzhou 450051China Key laboratory of Green Printing CAS Research/Education Center for Excellence in Molecular SciencesInstitute of ChemistryChinese Academy of Sciences(ICCAS)Beijing Engineering Research Center of Nanomaterials for Green Printing TechnologyBeijing National Laboratory for Molecular Sciences(BNLMS)Beijing 100190China University of Chinese Academy of sciences Beijing 100049China

The development of three-dimensional(3D)space light angle detection is vital in optical technology for applications such as 3D imaging,computer vision,and augmented *** methods involve advanced sensors and algorithms,including time-offlight cameras,which need multiple cameras and light sources to improve ***,it is a great challenge to integrate these complex components into compact *** semiconductor structures offer optical resonance characteristics,enabling precise light–matter interaction regulation.A 3D star-like photodetector,fabricated using a template assistant printing strategy,demonstrates optical resonances of the subwavelength facade and the shielding effect of spatial *** achieves light angle detection with the resolution of 10°in vertical space and the resolution of 36°in horizontal space,making it a promising prototype for various applications.

关键词： photodetector light angle detection printing subwavelength structure shielding effect

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Self-assembly Induced by Complexation of Diblock Copolyelectrolytes and Oppositely Charged Homopolymers

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Chinese Journal of Polymer Science 2024年第9期42卷 1321-1332,I0006页

作者： Ling Zhao Zhi-Yuan Yin Jia-Di Jiang Er-Qiang Chen Shuang Yang beijing national laboratory for molecular sciences Key Laboratory of Polymer Chemistry and Physics of Ministry of EducationCenter for Soft Mater Science and EngineeringCollege of Chemistry and Molecular EngineeringPeking UniversityBeijing100871China beijing national laboratory for molecular sciences College of Chemistry and Molecular EngineeringPeking UniversityBeijing100871China

We investigate the solution self-assembly of a mixture of positively charged homopolymers and AB diblock copolymers,in which the A blocks are negatively charged,and the B blocks are *** electrostatic complexation between oppositely charged polymers drives the formation of many ordered *** microstructures and phase diagrams are calculated using self-consistent field theory(SCFT)based on an ion-pair model with an equilibrium constant K to characterize the strength of binding between positively and negatively charged *** effects of the charge ratio,representing the ratio of charges from the homopolymer over all charges from polymers in the system,on the ordered structure are systematically studied,both for hydrophobic and hydrophilic A *** charge ratio plays an important role in determining the phase boundaries in the phase diagram of salt concentration versus polymer *** also provide information about the varying tendency of the domain spacing and core size of the spherical phase when the charge ratio is changed,and the results are in good agreement with *** studies provide a deep understanding of the self-assembled microstructures of oppositely charged diblock copolymer-homopolymer systems.

关键词： Self-assembly Polyelectrolyte complexation Self-consistent field theory Ion-pair

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C_(Ar)-Br bond cleavage via cooperative EnT/NHC catalysis: mild access to indolines

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Science China Chemistry 2024年第3期67卷 922-927页

作者： Yi-Xiong Dong Cao-Bo Li Ming-Lei Jin Zhong-Hua Gao Song Ye beijing national laboratory for molecular sciences CAS Key Laboratory of Molecular Recognition and FunctionCAS Research/Education Center for Excellence in Molecular SciencesInstitute of ChemistryChinese Academy of SciencesBeijing 100190China University of Chinese Academy of sciences Beijing 100049China

The cooperative visible-light mediated and NHC-catalyzed dearomative arylation-acylation of N-(2-bromobenzoyl)indoles with aldehydes was developed, affording the corresponding highly functionalized polycyclic indolines in moderate to good yields with exclusive diastereoselectivities. Mechanism investigations support the activation of CAr-Br bond via visible-light mediated energy transfer(EnT) and the following single-electron-transfer(SET) with Breslow intermediate under NHC catalysis to give key aryl radical and ketyl radical. This protocol demonstrates the cleavage of CAr-Br bond under mild cooperative EnT/NHC catalysis.

关键词： energy transfer N-heterocyclic carbenes photocatalysis aryl radicals indolines

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