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Isolated diatomic Zn-Co metal–nitrogen/oxygen sites with synergistic effect on fast catalytic kinetics of sulfur species in Li-S battery

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Journal of Energy Chemistry 2023年第4期79卷 505-514页

作者： Chun-Lei Song Qiao-Tong He Zhongyi Zeng Jing-Yan Chen Tian Wen Yu-Xiao Huang Liu-Chun Zhuang Wei Yi Yue-Peng Cai Xu-Jia Hong School of Chemistry South China Normal UniversityGuangzhou 510006GuangdongChina guangzhou municipal and guangdong provincial key laboratory of molecular target&Clinical Pharmacology the NMPA and State Key Laboratory of Respiratory DiseaseSchool of Pharmaceutical Sciences&the Fifth Affiliated Hospital Guangzhou Medical UniversityGuangzhou 511436GuangdongChina

Lithium-sulfur batteries are severely restricted by low electronic conductivity of sulfur and Li_(2)S,shuttle effect,and slow conversion reaction of lithium polysulfides(LiPSs).Herein,we report a facile and highyield strategy for synthesizing dual-core single-atom catalyst(ZnCoN_(4)O_(2)/CN)with atomically dispersed nitrogen/oxygen-coordinated Zn-Co sites on carbon *** on density functional theory(DFT)calculations and LiPSs conversion catalytic ability,ZnCoN_(4)O_(2)/CN provides dual-atom sites of Zn and Co,which could facilitate Li^(+)transport and Li_(2)S diffusion,and catalyze LiPSs conversion more effectively than homonuclear bimetallic single-atom catalysts or their simple mixture and previously reported singleatom ***-S cell with ZnCoN_(4)O_(2)/CN modified separator showed excellent rate performance(789.4 mA h g^(-1)at 5 C)and stable long cycle performance(0.05%capacity decay rate at 6C with 1000cycles,outperforming currently reported single atomic catalysts for LiPSs *** work highlights the important role of metal active centers and provides a strategy for producing multifunctional dual-core single atom catalysts for high-performance Li-S cells.

关键词： Dual-core single-atom catalysts Lithium polysulfides Fast catalytic kinetics Li_(2)S diffusion Li-S battery

Regiocontrolled Rh(Ⅲ)-catalyzed C-C coupling/C-N cyclization mediated by distinctive 1,2-migratory insertion of gem-difluoromethylene allenes:Reaction development and mechanistic insight

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Chinese Chemical Letters 2023年第5期34卷 250-255页

作者： Zhi Zhou Kaifeng Chen Yi Wang Xiuhua Zhong Shuang Lin Hui Gao Wei Yi guangzhou municipal and guangdong provincial key laboratory of molecular target&Clinical Pharmacology NMPA and State Key Laboratory of Respiratory DiseaseSchool of Pharmaceutical Sciences and the Fifth Affiliated HospitalGuangzhou Medical UniversityGuangzhou 511436China

By developing gem-difluoromethylene allenes as viable partners,regiocontrolled Rh(Ⅲ)-catalyzed redoxneutral C-C coupling/C-N cyclization has been realized to build the pyridin-2(1H)-one motifs with the embedment of a Z-configured monofluoroalkene functionality,in which either(hetero)aromatic or vinylic amides were found to be *** experimental and computational mechanistic studies revealed that a tandem regioselective allene 1,2-insertion/β-H elimination/hydrogen transfer/oxidative addition/cyclization/cis-β-F elimination involving an unconventional Rh(Ⅲ)-Rh(I)-Rh(Ⅲ)catalytic cycle accounts for the established *** further FMO analysis and IGMH maps,a non-covalent weak interaction network between the gem-difluoromethylene part and the OPiv moiety was rationally defined for the unconventional and specific regioselectivity control.

关键词： Gem-difluoromethylene allenes C-H functionalization Regiocontrol Rhodium(Ⅲ)catalysis DFT calculations

Auto Machine Learning Assisted Preparation of Carboxylic Acid by TEMPO-Catalyzed Primary Alcohol Oxidation

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Chinese Journal of Chemistry 2023年第2期41卷 143-150页

作者： Jia Qiu Yougen Xu Shimin Su Yadong Gao Peiyuan Yu Zhixiong Ruan Kuangbiao Liao guangdong laboratory Animals Monitoring Institute Guangdong Provincial Key Laboratory of Laboratory AnimalsGuangzhouGuangdong 510663China guangzhou municipal and guangdong provincial key laboratory of molecular target&Clinical Pharmacology the NMPA and State Key Laboratory of Respiratory DiseaseSchool of Pharmaceutical Sciences and the Fifth Affiliated HospitalGuangzhou Medical UniversityGuangzhouGuangdong 511436China Bioland laboratory GuangzhouGuangdong 510005China Department of Chemistry Southern University of Science and TechnologyShenzhenGuangdong 518055China guangzhou laboratory GuangzhouGuangdong 510320China

Though alcohol oxidations were considered as well-established reactions,selecting productive conditions or predicting reaction yields for unseen alcohols remained as major ***,an auto machine learning(ML)model for TEMPO-catalyzed oxida-tion of primary alcohols to the corresponding carboxylic acids is disclosed.A dataset of 3444 data,consisting of 282 primary alco-hols and 45 conditions,were generated using high-throughput experimentation(HTE).With the HTE data and 105 descriptors,a multi-label prediction was performed with AutoGluon(an open-source auto machine learning framework)and KNIME(an open-source data analytics platform).For the independent test of 240 reactions(a full matrix of 20 unseen alcohols and 12 condi-tions),AutoGluon with multi-label prediction for yield prediction(AGMP)gave excellent *** external test of 1308 re-actions(consisting of 84 alcohols and 45 conditions),AGMP still afforded good results with R2 as 0.767 and MAE as 4.9%.The model also revealed that the newly generated descriptor(Y/N,classification of the reaction reactivity)was the most relevant descriptor for yield prediction,offering a new perspective to integrate HTE and ML in organic synthesis.

关键词： TEMPO Oxidation Primary alcohols Carboxylic acids AutoGluon

Enantioselective synthesis of indenopyrazolopyrazolones enabled by dual directing groups-assisted and rhodium(Ⅲ)-catalyzed tandem C-H alkenylation/[3+2] stepwise cycloaddition

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Chinese Chemical Letters 2022年第2期33卷 842-846页

作者： Min Wu Hui Gao Huiying Xu Wei Yi Zhi Zhou guangzhou municipal and guangdong provincial key laboratory of Protein Modiﬁcation and Degradation&molecular target and Clinical Pharmacology State Key Laboratory of Respiratory DiseaseSchool of Pharmaceutical SciencesGuangzhou Medical UniversityGuangzhou 511436China

The Cp;Rh(Ⅲ)-catalyzed asymmetric cascade C-H coupling/intramolecular cyclization of azomethine imines with propargyl carbonates has been developed, affording a variety of chiral tetracyclic indenopyrazolopyrazolone frameworks with good substrate/functional group tolerance and enantioselectivity(up to 97:3 er). Combined experimental studies and DFT calculations revealed the Rh(Ⅲ)-catalyzed stepwise annulation process and clarified the synergy coordination mode of dual directing groups in tuning the selectivity.

关键词： Indenopyrazolopyrazolone Azomethine imine Enantioselective synthesis DFT calculations Rhodium(Ⅲ)catalysis

Visualization of supramolecular assembly by aggregation-induced emission

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Aggregate

Aggregate 2023年第2期4卷 102-122页

作者： Wu-Jie Guo Tuokai Peng Wenping Zhu Shixiang Ma Guang Wang Ying Li Bin Liu Hui-Qing Peng Beijing Advanced Innovation Center for Soft Matter Science and Engineering State Key Laboratory of Chemical Resource EngineeringBeijing University of Chemical TechnologyBeijingChina Innovation Research Center for AIE Pharmaceutical Biology Guangzhou Municipal and Guangdong Provincial Key Laboratory of Molecular Target and Clinical PharmacologyThe NMPA and State Key Laboratory of Respiratory DiseaseSchool of Pharmaceutical Sciences and The Fifth Affiliated HospitalGuangzhou Medical UniversityGuangzhouChina guangdong provincial key laboratory of Luminescence from molecular Aggregates South China University of TechnologyGuangzhouChina

Supramolecular architectures are constructed by the self-assembly of small building blocks via the use of metal-ligand coordination,π–πstacking interactions,hydrogen bonding,host-guest interactions,and other noncovalent driving forces,which confer unique dynamic reversibility and stimulus responsiveness to the supramolecular materials and also lead to the demand of expensive and complex equipment for the characterization of supramolecular assembly ***,the self-assembly processes bring the monomeric chromophores together,offering possibilities to establish ties between the supramolecular assembly and aggregation-induced emission(AIE)*** to conventional luminescent molecules,AIE luminogens(AIEgens)exhibit significant fluorescence enhancement upon the restriction of molecular motions,thus displaying the advantages of signal amplification and low background *** the above,the real-time,sensitive,and in situ visualization of the formation of self-assemblies and their stimuli responsiveness based on AIE becomes ***,we review recent works that encompass the visualization of supramolecular assembly-related behaviors by means of AIE characteristics of *** organization of this review will be by different types of supramolecular architectures,including metallacycles/cages,micelles/vesicles,supramolecular polymers,and supramolecular *** overview of future opportunities and challenges for the real-time monitoring of supramolecular assembly by AIE is also provided.

关键词： aggregation-induced emission metallacycles/cages micelles/vesicles supramolecular gels supramolecular polymers visualization

Stabilization of MYC G-quadruplex DNA by ruthenium(II)complex overcomes imatinib resistance in chronic myeloid leukemia cells harboring T315I mutation

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Genes & Diseases 2023年第2期10卷 399-402页

作者： Yuening Sun Xin Chen Siyan Liao Aochu Liu Huan Zhou Liling Jiang Wa Ding Wenjie Mei Jinbao Liu Xianping Shi guangzhou municipal and guangdong provincial key laboratory of Protein Modification and Degradation State Key Laboratory of Respiratory DiseaseAffiliated Cancer Hospital of Guangzhou Medical University School of Basic Medical SciencesGuangzhou Medical UniversityGuangzhouGuangdong 510120China guangdong Province Engineering Technology Center for molecular Probe and Biomedicine Imaging Guangdong Pharmaceutical UniversityGuangzhouGuangdong 510006China

The key pathogenesis of chronic myeloid leukemia(CML)is the formation of BCR-ABL fusion gene,encoding a 210 kDa Bcr-Abl tyrosine kinase,which is crucial for the occurrence and development of ***(IM)is the first targeted anticancer drug approved by FDA for the treatment of CML;however,some patients,especially those in accelerated phase and blastic phase,develop primary or secondary drug resistance to ***,the most challenging resistance is caused by T315I mutation of Bcr-Abl,which represents approximately 15%–20%of all acquired mutations and renders cell resistant to a variety of tyrosine kinase inhibitors.1,2 Thus,there is an urgent need to develop novel strategies to overcome Bcr-Abl T315I-meidated IM resistance.

关键词： myeloid overcome resistance

Discovery of an enantiopure N-[2-hydroxy-3-phenyl piperazine propyl]-aromatic carboxamide derivative as highly selectiveα_(1D/1A)-adrenoceptor antagonist and homology modelling

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Chinese Chemical Letters 2024年第11期35卷 435-441页

作者： Junjun Huang Ran Chen Yajian Huang Hang Zhang Anran Zheng Qing Xiao Dan Wu Ruxia Duan Zhi Zhou Fei He Wei Yi The Fifth Affiliated Hospital Guangzhou Municipal and Guangdong Provincial Key Laboratory of Molecular Target&Clinical Pharmacologythe NMPA and State Key Laboratory of Respiratory DiseaseSchool of Pharmaceutical SciencesGuangzhou Medical UniversityGuangzhou 511436China Department of Pharmacy The Third Affiliated Hospital of Guangzhou Medical UniversityGuangzhou 510150China School of Traditional Chinese Medicine Southern Medical UniversityGuangzhou 510515China

α_(1)-Adrenergic receptor(AR)blockers can be effective for the treatment of benign prostatic hyperplasia/lower urinary tract symptoms(BPH/LUTS),their usage is limited by cardiovascular-related side effects that are caused by the subtype nonselective nature or low selectivity of many current *** previously reported that phenylpiperazine analogues with amide and propane linker were moderateα_(1D/1A)adrenoceptor antagonists and exhibited better anti-BPH effect than lead compound naftopidil(NAF)in vivo,however,with modestα_(1D/1A)-subtype ***,we replaced propane moiety with2-hydroxypropanol linker and synthesized twenty-seven racemic derivatives with modified aromatic and hetero aromatic *** these new compounds,quinoline surrogate 17 exhibited extremely weak antagonistic affinity onα_(1B)in both cell-based calcium assay and tissue-based functional assay,so that elicited significantα_(1A/1B)andα_(1D/1B)***,the R enantiomer of 17 preferentially displayed superior anti-BPH effect in rat model compared with S-17,supporting ligand regulates the receptor in a highly stereospecific ***,the computer-aided modelling research was also performed in order to deeply understand the unique binding mode of R-17 in complex withα_(1A)and the subtype receptor selectivity for R-17 was also rationalized in this *** together,our work enriched the diversity of phenylpiperazines for the treatment of BPH/LUTS,and provided a basis for discovery ofα_(1D/1A)-selective ligands.

关键词： Benign prostatic hyperplasia α_(1)-AR antagonist Phenylpiperazine Homology modelling Subtype selectivity

target chromosome-segment substitution: A way to breeding by design in rice

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The Crop Journal 2021年第3期9卷 658-668页

作者： Guiquan Zhang guangdong provincial key laboratory of Plant molecular Breeding State Key Laboratory for Conservation and Utilization of Subtropical Agro-BioresourcesSouth China Agricultural UniversityGuangzhou 510642GuangdongChina

Progress in plant breeding depends on the development of genetic resources,genetic knowledge,and breeding *** core of plant breeding is the use of naturally occurring *** the beginning of the post-genomic era,a new concept of"breeding by design"was proposed,which aims to control all allelic variation for all genes of agronomic *** the past two decades,we have applied a three-step strategy for research on rice breeding by *** the first step,we constructed a singlesegment substitution line(SSSL)library using Huajingxian 74(HJX74),an elite xian(indica)rice cultivar,as the recipient in which to assemble genes from the rice AA *** the second step,we identified a series of desirable genes in the SSSL *** the third step,we designed new rice lines,and achieved the breeding goals by pyramiding target genes in the HJX74-SSSL *** review introduces the background,concept,and strategy of breeding by design,as well as our achievements in rice breeding by design using the HJX74-SSSL *** practice shows that target chromosome-segment substitution is a way to breeding by design.

关键词： Gene pool Chromosome-segment substitution Breeding by design Breeding platform Rice

Metal-coordinated oxidative stress amplifier to suppress tumor growth combined with M2 macrophage elimination

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Chinese Chemical Letters 2024年第12期35卷 220-225页

作者： Chuyu Huang Zhishan Liu Linping Zhao Zuxiao Chen Rongrong Zheng Xiaona Rao Yuxuan Wei Xin Chen Shiying Li The Fifth Affiliated Hospital Guangdong Provincial Key Laboratory of Molecular Target & Clinical Pharmacologythe NMPA and State Key Laboratory of Respiratory Diseasethe School of Pharmaceutical SciencesGuangzhou Medical University Department of Pulmonary and Critical Care Medicine Zhujiang HospitalSouthern Medical University

The anti-oxidative characteristic and immunosuppressive microenvironment contribute to a high resistance of tumor to many treatments. In this work, a glutathione(GSH)-responsive metal-coordinated oxidative stress amplifier(designated as Cu PA) is fabricated to suppress tumor growth through elevating the cellular level of reactive oxygen species(ROS) and eliminating M2 macrophages. Among which,cooper ion(Cu2+) is capable of coordinating with thioredoxin(Trx) inhibitor of PX-12 and signal transducer and activator of transcription 6(STAT6) inhibitor of AS1517499 with the assistance of distearoyl phosphoethanolamine-PEG2000(DSPE-PEG2000), which can extensively increase the stability to enhance drug delivery in vitro and in vivo. Furthermore, CuPA can upregulate intracellular ROS to cause tumor cell death through restraining Trx and degrading GSH. Also, Cu PA-mediated STAT6 inhibition results in the elimination of M2 macrophage to reverse the immunosuppressive tumor microenvironment. Finally,the elevated oxidative stress and increased immune activation amplify the synergistic antitumor effect without causing obvious side effect. This work provides a new sight for synergistic tumor suppression through chemo-immunotherapy in consideration of the complex resistant tumor microenvironment.

关键词： Oxidative stress M2 macrophage Metal coordination Chemotherapy GSH degradation