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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

A novel structural variant of RET causes familial Hirschsprung's disease via nonsense-mediated mRNA decay

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Genes & Diseases 2024年第1期11卷 7-10页

作者： Qi Wang Siyu Pu Bo Xiang Jing Chen Department of Pediatric Surgery and Laboratory of Pediatric Surgery Rare Diseases CenterInstitute of Immunology and InflammationFrontiers Science Center for Disease-Related Molecular NetworkWest China HospitalSichuan UniversityChengduSichuan 610041China

Hirschsprung's disease(HsCR)is the most common type of developmental gastrointestinal malformation causing intestinal obstruction in children,with an incidence of 1/5000 in live births.1 it is characterized by the absence of intrinsic ganglion cells in the myenteric and submucosal plexuses of the distal gastrointestinal tract,leading to the dysregulation of smooth muscle contraction/relaxation and resulting in intestinal *** on the length of the aganglionic intestine,HSCR can be categorized into short-segmental HSCR(S-HSCR),which affects up to the sigmoid colon from the anus,and long-segmental HSCR(LHSCR),which affects beyond the sigmoid colon.1 In some rare conditions,aganglionic lesions can affect the full length of the colon or even the whole intestine.

关键词： intestine colon relaxation

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 Function CAS Research/Education Center for Excellence in Molecular Sciences Institute of Chemistry Chinese Academy of Sciences University of Chinese Academy of Sciences

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 compounds. However, 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 process. In 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 enantioselectivity. In 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 acid. This 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： brønsted acid catalysis desymmetrization phosphoric acid axially chiral biaryls central-to-axial conversion

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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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Neutrophils are shaped by the tumor microenvironment:novel possibilities for targeting neutrophils in cancer

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Signal Transduction and Targeted Therapy 2024年第5期9卷 1788-1790页

作者： Carlos Silvestre-Roig Lydia Kalafati Triantafyllos Chavakis Institute of Experimental Pathology(ExPat) Center for Molecular Biology of Inflammation(ZMBE)University of MünsterMünsterGermany Institute for Clinical Chemistry and Laboratory Medicine University Hospital and Faculty of MedicineTechnische Universität DresdenDresdenGermany

In a recent paper published in Science,Ng et *** seminal insights into the process through which neutrophils are reprogrammed by the tumor environment,leading to a convergent transition from different neutrophil states towards a unique end-stage differentiated pro-tumor phenotype.1 These findings have major translational implications as they provide potential neutrophil-related targets for tumor immunotherapy.

关键词： al. neutrophils tumor

Developing silicon-based photocathodes for CO_(2) conversion

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Science China Chemistry 2024年第6期67卷 1904-1921页

作者： Weijie Zhuang Miao Kan Tao Meng Jinlong Zhang Key Laboratory for Advanced Materials and Joint International research Laboratory of Precision Chemistry and molecular Engineering Feringa Nobel Prize Scientist Joint Research CenterSchool of Chemistry and Molecular EngineeringEast China University of Science and TechnologyShanghai200237China Shanghai Engineering research center for Multimedia Environmental Catalysis and Resource Utilization East China University of Science and TechnologyShanghai200237China

Photoelectrochemical(PEC)conversion of CO_(2) presents a promising avenue for solar-driven chemical fuel production,with silicon emerging as a cost-effective and high-light-absorbing material pivotal to this *** at exploring opportunities for industrializing PEC CO_(2) reduction(PEC-CO_(2)R)by minimizing reaction energy consumption,enhancing reaction efficiency and selectivity,this review summarizes recent advancements in developing Si-based photocathodes for PEC-CO_(2)*** outlines the fundamental principles,advantages,and limitations of Si photocathodes with key performance *** on this understanding,the strategies to enhance the performance of the PEC-CO_(2)R system,including light absorption,charge separation,and catalytic reactions are categorized as the interfacial modification,active site decoration,and protective layer *** design ideas of this advantageous three-layer structure in promoting the efficiency,stability,and selectivity have been ***,this review scrutinizes the influence of the photocathodic chemical *** review consolidates the mechanism insights and notable breakthroughs of various fuel generation processes within Si-based PEC-CO_(2)R *** this wealth of information offers an up-to-date perspective on the dynamic developments in silicon-based PEC-CO_(2) conversion and underscores the promising pathways toward the sustainable fuel synthesis from pollutant CO_(2).

关键词： photoelectrochemistry solar fuels silicon photocathodes carbon dioxide reduction microenvironment

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Bias distribution and regulation in photoelectrochemical overall water-splitting cells

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National Science Review 2024年第4期11卷 141-150页

作者： Kun Dang Siqin Liu Lei Wu Daojian Tang Jing Xue Jiaming Wang Hongwei Ji Chuncheng Chen Yuchao Zhang Jincai Zhao Key Laboratory of Photochemistry CAS ResearchEducation Center for Excellence in Molecular Sciences Institute of Chemistry Chinese Academy of Sciences University of Chinese Academy of Sciences

The water oxidation half-reaction at anodes is always considered the rate-limiting step of overall water splitting（OWS）,but the actual bias distribution between photoanodes and cathodes of photoelectro chemical（PEC） OWS cells has not been investigated *** this work,we find that,for PEC cells consisting of photoanodes（nickel-modified n-Si [Ni/n-Si] and α-Fe2O3） with low photovoltage(Vph 1V,the bias required for cathode activation can be significantly reduced,exhibiting a kinetics-controlled *** investigations show that the bias distribution can be regulated by tuning the electrolyte pH and using alternative half-reaction ***,a volcano plot is presented for the rational design of the overall reactions and unbiased PEC *** by this,an unbiased PEC cell consisting of a simple Ni/n-Si photoanode and Pt cathode is assembled,delivering a photo current density of 5.3±0.2 mA cm-2.

关键词： photoelectrochemistry overall reaction cell bias distribution photoanode water splitting

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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Going only half the way:cell cycle exit after the G1 restriction point

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Signal Transduction and Targeted Therapy 2024年第1期9卷 1-2页

作者： Lisa Muller Tony Gutschner Mechthild Hatzfeld Department of Pathobiochemistry Institute of Molecular MedicineMartin Luther University Halle-WittenbergCharles Tanford Protein Research CenterHalleGermany Department of RNA Biology and Pathogenesis Institute of Molecular MedicineMartin Luther University Halle-WittenbergCharles Tanford Protein Research CenterHalleGermany

In a recent article published in Nature,James *** et *** that cyclin A2 levels determine whether cells will make an entrance into mitosis or whether cells will leave the cell cycle after having passed the G1/restriction(R)-point implicating that the decision is fully reversible(Fig.1).This ground-breaking study could impact future approaches for cancer treatment by targeting the mitotic clock.

关键词： point cycle