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Multifunction-oriented high-mobility polymer semiconductors

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National Science Review 2024年第3期11卷 16-19页

作者： Mingliang Zhu Yunlong Guo Yunqi Liu Beijing National Laboratory for molecular sciences Organic Solids Laboratory Institute of Chemistry Chinese Academy of Sciences school of Chemical sciences University of Chinese Academy of Sciences

The discovery of conductive polyacetylene has initiated interdisciplinary research into condensed matter physics and synthetic chemistry in organic electronics. Unlike their inorganic and small-molecule counterparts, polymer semiconductors possess the inherent advantages of facile solution processing,large-area manufacturing, excellent mechanical strength and intrinsic flexibility.

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Pathogenic contribution of cholesteryl ester accumulation in the brain to neurodegenerative disorders

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Neural Regeneration Research 2024年第10期19卷 2099-2100页

作者： Michiko Shirane Department of molecular Biology Graduate School of Pharmaceutical SciencesNagoya City UniversityNagoyaJapan

Cholesteryl esters(CEs) have been increasingly implicated in neurodegenerative disorders such as Alzheimer's disease(AD).Alois Alzheimer noted three prominent neuropathologic features in his original analysis of the AD brain:senile plaques,neurofibrillary tangles,and lipid granule *** plaques,which are aggregates of amyloid-beta(Aβ),and neurofibrillary tangles,which are aggregates of phosphorylated tau,have been regarded as more consistent characteristics of the AD brain compared with lipid granule accumulation and thus have been studied more intensively(Foley,2010).

关键词： esters ester cholesteryl

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

Axial enantiomers with donor-regulated TADF feature for multicolor circularly polarized electroluminescence

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Science China Chemistry 2024年第6期67卷 2039-2045页

作者： Chen-Hao Guo Wen-Long Zhao Ke-Ke Tan Wei-Chen Guo Liheng Feng Chuan-Feng Chen Meng Li school of Chemistry and Chemical Engineering Shanxi UniversityTaiyuan030006China Beijing National Laboratory for molecular sciences CAS Key Laboratory of Molecular Recognition and FunctionInstitute of ChemistryChinese Academy of SciencesBeijing100190China University of Chinese Academy of sciences Beijing100049China

This study optimized the TADF feature of axial chiral enantiomers through precise donor engineering,and multicolor CP-TADFwas achieved in the axial chiral *** pairs of axial enantiomers with donor-regulated TADF feature,namely(R/S)-TPCBD,(R/S)-DPCBD,and(R/S)-DPACBD,were synthesized by introducing carbazole donors with different substituents onto biphenyl cyanide *** the electron-donating ability of donors increases,the emission of these axial enantiomers ranges from 455,476 to 552 nm,their singlet-triplet energy gaps(ΔE_(ST))gradually decrease from 0.30,0.22 to 0.02 e V,accompanied by an increasement in the transition rate(k_(RISC))of RISC process,and the k_(RISC)of DPACBD could reach up to 7.16×10^(5)s^(-1).These axial enantiomers also exhibit mirror-image CD and circularly polarized luminescence(CPL)***,OLEDs based on TPCBD,DPCBD,and DPACBD as emitter were then fabricated,which displayed blue,green,and orange electroluminescence with EQE_(max)of 13.0%,16.4%,and 25.0%,*** results also exhibited a phenomenon of device efficiency increasing with the enhancement of donor ***,the CP-OLEDs using(R/S)-TPCBD,(R/S)-DPCBD and(R/S)-DPACBD as emitters displayed intense CPEL signals with g_(EL)values of 3.4×10^(-3)/-4.1×10^(-3),3.2×10^(-3)/-3.1×10^(-3)and2.3×10^(-3)/-2.1×10^(-3),*** convenient molecular engineering of donor regulation in the same molecular skeleton,CP-TADF materials with multicolor CPEL and improved device performance could be conveniently achieved.

关键词： axial chirality thermally activated delayed fluorescence circularly polarized luminescence electroluminescence organic light-emitting diodes

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

Efficient nitrate electroreduction over Mn-doped Cu catalyst via regulating N-containing intermediates adsorption configuration

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Science China Chemistry 2024年第6期67卷 1969-1975页

作者： Limin Wu Shunhan Jia Libing Zhang Ruhan Wang Jiaqi Feng Xiaofu Sun Buxing Han Beijing National Laboratory for molecular sciences CAS Laboratory of Colloid and Interface and ThermodynamicsCAS Research/Education Center for Excellence in Molecular SciencesCenter for Carbon Neutral ChemistryInstitute of ChemistryChinese Academy of SciencesBeijing100190China school of Chemical sciences University of Chinese Academy of SciencesBeijing100049China College of Chemical Engineering and Environment China University of PetroleumBeijing102249China Shanghai Key Laboratory of Green Chemistry and Chemical Processes School of Chemistry and Molecular EngineeringEast China Normal UniversityShanghai200062China

The electrochemical reduction of NO_(3)^(-)to NH_(3)holds promise for economic and environmental benefits,presenting an energyefficient alternative to the traditional Haber-Bosch ***,challenges exist due to its sluggish kinetics,multiple intermediates,and various reaction *** this study,Mn-doped-Cu catalyst was synthesized and employed for electrochemical NO_(3)^(-)-to-NH_(3)*** doping of Mn into Cu resulted in exceptional performance,achieving a FE of 95.8%and an NH_(3)yield rate of 0.91 mol g^(-1)h^(-1)at-0.6 V in a neutral electrolyte at low NO_(3)^(-)*** experimental studies and theoretical calculations revealed that the Mn dopant enhanced the kinetic rate of NO_(2)~--to-NH_(3)and induced a distinct configuration of**** alteration decreased the energy barrier of*NO-to-*NOH,consequently promoting the conversion of NO_(3)^(-)-to-NH_(3).

关键词： nitrate reduction electrocatalysis ammonia synthesis N-intermediate green chemistry

Bionic immunoactivator copresenting autophagy promoting and costimulatory molecules for synergistic cancer immunotherapy

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Nano Research 2024年第3期17卷 1710-1724页

作者： Yiwei Peng Yiliang Yang Zhenzhen Yang Datong Gao Jiajia Li Qi Sun Yitian Du Meng Lin Xianrong Qi Beijing Key Laboratory of molecular Pharmaceutics and New Drug Delivery System School of Pharmaceutical SciencesPeking UniversityBeijing 100191China

Immunotherapy has great promise in improving malignant tumor ***,the efficacy of existing strategies is often limited by the immunosuppressive ***,we demonstrate an in situ bionic immunoactivator,PLT-Bec1/DTA-1,with possessed natural advantages of platelets for tumor recruitment and activation,on which DTA-1(CD357 monoclonal antibody)and Bec1 were tethered as combined immune ***-Bec1/DTA-1,as a self-triggered release repository,can deliver the pre-tethered Bec1 and DTA-1 deeply through the secretion of platelet microparticles(PMPs),thereby cooperate tacitly and exhibit superiority in immune activation of dendritic cells(DCs)and T cells via autophagy inducibility,coupled with glucocorticoid-induced tumor necrosis factor receptor(GITR)-triggered T_(Reg) suppression,remodeled the immunosuppressive network of tumor ***-Bec1/DTA-1 promoted antigen presentation and T cell proliferation,and alleviated the low activity state of bone marrow-derived dendritic cells(BMDCs)in tumor suppressive ***-Bec1/DTA-1 inhibited tumor recurrence(5-and 13-fold lower of control group in tumor volume)and CD8^(+)T/T_(Reg) ratio(6.3-and 8.8-fold *** group)in mouse tumor model after intravenous or subcutaneous ***,PLT-Bec1/DTA-1 prevented tumor colonization in lung through in situ immune activation,and was slightly superior to the combined of Bec1 and *** findings highlight the promise of delivering immunostimulatory payloads via bionic carriers,eliciting automatic in situ activation of effector immune cells in tumor microenvironment for tumor *** these results provide promising prospects into the application of immunoactivator in improving cancer synergistic immunotherapy to overcome the bottlenecks in clinic.

关键词： in situ bionic immunoactivator autophagy glucocorticoid-induced tumor necrosis factor receptor(GITR)agonist platelets and platelet microparticles cancer immunotherapy

Structural transition,electric transport,and electronic structures in the compressed trilayer nickelate La4Ni3O10

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Science China(Physics,Mechanics & Astronomy) 2024年第11期Mechanics & Astronomy) .卷 13-19页

作者： Jingyuan Li Cui-Qun Chen Chaoxin Huang Yifeng Han Mengwu Huo Xing Huang Peiyue Ma Zhengyang Qiu Junfeng Chen Xunwu Hu Lan Chen Tao Xie Bing Shen Hualei Sun Dao-Xin Yao Meng Wang Center for Neutron Science and Technology Guangdong Provincial Key Laboratory of Magnetoelectric Physics and Devices School of Physics Sun Yat-sen University Center for Materials of the Universe School of Molecular Sciences Arizona State University school of sciences Sun Yat-sen University

Atomic structure and electronic band structure are fundamental properties for understanding the mechanism of superconductivity. Motivated by the discovery of pressure-induced high-temperature superconductivity at 80 K in the bilayer Ruddlesden-Popper nickelate La3Ni2O7, the atomic structure and electronic band structure of the trilayer nickelate La4Ni3O10under pressure up to 44.3 GPa are investigated. A structural transition from the monoclinic P21/a space group to the tetragonal I4/mmm around 12.6-13.4 GPa is identified, accompanied by a drop of resistance below 7 K. Density functional theory calculations suggest that the bonding state of Ni 3dz2orbital rises and crosses the Fermi level at high pressures, which may give rise to possible superconductivity observed in resistance under pressure in La4Ni3O10. The trilayer nickelate La4Ni3O10shows some similarities with the bilayer La3Ni2O7and has unique properties, providing a new platform to investigate the underlying mechanism of superconductivity in nickelates.

关键词： La4Ni3O10 high pressure synchrotron X-ray diffraction structural transition DFT calculations

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