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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 nanosheets.Based 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 catalysts.Li-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 conversion.This 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

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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 challenges.Herein,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 performance.For 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

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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 compatible.Integrated 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 transformation.Through 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

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Lineage reprogramming of fibroblasts into induced cardiac progenitor cells by CRISPR/Cas9-based transcriptional activators

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Acta Pharmaceutica Sinica B 2020年第2期10卷 313-326页

作者： Jianglin Wang Xueyan Jiang Lixin Zhao Shengjia Zuo Xiantong Chen Lingmin Zhang Zhongxiao Lin Xiaoya Zhao Yuyan Qin Xinke Zhou Xi-Yong Yu key laboratory of molecular target&clinical pharmacology and the State key laboratory of Respiratory Disease School of Pharmaceutical Sciences&the Fifth Affiliated HospitalGuangzhou Medical UniversityGuangzhou 511436China

Overexpression of exogenous lineage-determining factors succeeds in directly reprogramming fibroblasts to various cell types.Several studies have reported reprogramming of fibroblasts into induced cardiac progenitor cells(iCPCs).CRISPR/Cas9-mediated gene activation is a potential approach for cellular reprogramming due to its high precision and multiplexing capacity.Here we show lineage reprogramming to iCPCs through a dead Cas9(dCas9)-based transcription activation system.targeted and robust activation of endogenous cardiac factors,including GATA4,HAND2,MEF2 C and TBX5(G,H,M and T;GHMT),can reprogram human fibroblasts toward iCPCs.The iCPCs show potentials to differentiate into cardiomyocytes,smooth muscle cells and endothelial cells in vitro.Addition of MEIS1 to GHMT induces cell cycle arrest in G2/M and facilitates cardiac reprogramming.Lineage reprogramming of human fibroblasts into iCPCs provides a promising cellular resource for disease modeling,drug discovery and individualized cardiac cell therapy.

关键词： Lineage reprogramming Human foreskin fibroblasts Induced cardiac progenitor cells CRISPR/Cas9 SAM Cardiac transcription factors

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Direct Electrochemical Synthesis of Sulfur-Containing Triazolium Inner Salts

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Chinese Journal of Chemistry 2021年第4期39卷 942-946页

作者： Yueheng Li Zhixing Huang Guangquan Mo Wei Jiang Chengwei Zheng Pengju Feng Zhixiong Ruan key laboratory of molecular target&clinical pharmacology and the State key laboratory of Respiratory Disease School of Pharmaceutical Sciences&the Fifth Affiliated HospitalGuangzhou Medical UniversityGuangzhouGuangdong 511436China Department of Chemistry Jinan UniversityGuangzhouGuangdong 510632China

Main observation and conclusion The electrochemical thiocyanation/cyclization of aldehyde hydrazones was developed under external oxidant-free and catalyst-free conditions.In contrast to previous thiocyanation,this electrosynthetic approach enabled a cascade C-H thiocyanation/cyclization through a mild,direct electrolysis manner in an undivided cell without the additive of halogens and stoichiometric oxidants.In this protocol,commercially available and inexpensive sodium thiocyanate was used,which played a dual role as a thiocyanation reagent and electrolyte.This strategy provides expedient access to functionalized sulfur-containing triazolium inner salts with ample scope and diverse functional group tolerance.Based on the findings of mechanistic studies,a reaction mechanism was proposed.

关键词： Electrochemistry Thiocyanation Cyclization Aldehyde Hydrazone Triazolium

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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

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Enantioselective[2+2]cycloaddition of 1,2-dihydroquinolines with 3-olefinic oxindoles via Brønsted acid catalysis

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Organic Chemistry Frontiers 2022年第6期9卷 1621-1627页

作者： Biao Wang Xiao Yan Han Zhong Qin Ouyang Xu Tian key laboratory of molecular target&clinical pharmacology and the State key laboratory of Respiratory Disease School of Pharmaceutical Sciences&the Fifth Affiliated HospitalGuangzhou Medical UniversityXinzaoPanyu DistrictGuangzhou511436China College of Pharmacy Third Military Medical UniversityChongqing400038China

Mutually complementary regiodivergent Brønsted acid-catalyzed atom-economical[2+2]cycloadditionand ene reactions of 1,2-dihydroquinolines with 3-olefinic oxindoles are reported.In the presence of achiral phosphoramide catalyst,the[2+2]cycloaddition affords products with four contiguous stereocenters in good to excellent yields(up to 95%)and with high stereoselectivities(up to>99%ee,>20:1 dr).Conversely,with a stronger Brønsted acid,the trifluoromethanesulfonic acid catalyst leads to ene reactionproducts in high yields(up to 77%).Furthermore,the mechanisms of the reactions are discussed based oncontrol experiments and DFT calculations.

关键词： catalyst cycloaddition indole

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Gli1 promotes epithelial-mesenchymal transition and metastasis of non-small cell lung carcinoma by regulating snail transcriptional activity and stability

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Acta Pharmaceutica Sinica B 2022年第10期12卷 3877-3890页

作者： Xueping Lei Zhan Li Yihang Zhong Songpei Li Jiacong Chen Yuanyu Ke Sha Lv Lijuan Huang Qianrong Pan Lixin Zhao Xiangyu Yang Zisheng Chen Qiudi Deng Xiyong Yu 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 UniversityGuangzhou 511436China Department of Respiratory and Critical Care Medicine the Sixth Affiliated Hospital of Guangzhou Medical UniversityQingyuan People’s HospitalQingyuan 511518China GMU-GIBH Joint School of Life Sciences Guangzhou Medical UniversityGuangzhou 511436China

Metastasis is crucial for the mortality of non-small cell lung carcinoma(NSCLC) patients.The epithelial-mesenchymal transition(EMT) plays a critical role in regulating tumor metastasis.Glioma-associated oncogene 1(Gli1) is aberrantly active in a series of tumor tissues. However, the molecular regulatory relationships between Gli1 and NSCLC metastasis have not yet been identified. Herein,we reported Gli1 promoted NSCLC metastasis. High Gli1 expression was associated with poor survival of NSCLC patients. Ectopic expression of Gli1 in low metastatic A549 and NCI-H460 cells enhanced their migration, invasion abilities and facilitated EMT process, whereas knock-down of Gli1 in high metastatic NCI-H1299 and NCI-H1703 cells showed an opposite effect. Notably, Gli1 overexpression accelerated the lung and liver metastasis of NSCLC in the intravenously injected metastasis model. Further research showed that Gli1 positively regulated Snail expression by binding to its promoter and enhancing its protein stability, thereby facilitating the migration, invasion and EMT of NSCLC. In addition, administration of GANT-61, a Gli1 inhibitor, obviously suppressed the metastasis of NSCLC. Collectively, our study reveals that Gli1 is a critical regulator for NSCLC metastasis and suggests that targeting Gli1 is a prospective therapy strategy for metastatic NSCLC.

关键词： Non-small cell lung carcinoma Metastasis Epithelialemesenchymal transition Glioma-associated oncogene 1 Promote Snail Protein stability GANT-61

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MiR-142-3p enhances chemosensitivity of breast cancer cells and inhibits autophagy by targeting HMGB1

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Acta Pharmaceutica Sinica B 2020年第6期10卷 1036-1046页

作者： Lu Liang Jijun Fu Siran Wang Huiyu Cen Lingmin Zhang Safur Rehman Mandukhail Lingran Du Qianni Wu Peiquan Zhang Xiyong Yu key laboratory of molecular target&clinical pharmacology and the State key laboratory of Respiratory Disease School of Pharmaceutical Sciences&the Fifth Affiliated HospitalGuangzhou Medical UniversityGuangzhou 511436China Department of Prosthodontics the Second Affiliated Hospital of Harbin Medical UniversityHarbin 150001China

MiR-142-3p has been reported to act as a tumor suppressor in breast cancer.However,the regulatory effect of miR-142-3p on drug resistance of breast cancer cells and its underlying mechanism remain unknown.Here,we found that miR-142-3p was significantly downregulated in the doxorubicin(DOX)-resistant MCF-7 cell line(MCF-7/DOX).MiR-142-3p overexpression increased DOX sensitivity and enhanced DOXinduced apoptosis in breast cancer cells.High-mobility group box 1(HMGB1)is a direct functional target of miR-142-3p in breast cancer cells and miR-142-3p negatively regulated HMGB1 expression.Moreover,overexpres sion of HMGB1 dramatically reversed the promotion of apoptosis and inhibition of autophagy mediated by miR-142-3p up-regulation.In conclusion,miR-142-3p overexpression may inhibit autophagy and promote the drug sensitivity of breast cancer cells to DOX by targeting HMGB 1.The miR-142-3 p/HMGB1 axis might be a novel target to regulate the drug resistance of breast cancer patients.

关键词： Breast cancer MCF-7 cell line HMGB1 MiR-142-3p Drug resistance Chemosensitivity

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Prognostic value of the RNA editing enzyme: ADAR1, and its association with immune cells infiltration in pancreatic adenocarcinoma

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Genes & Diseases 2023年第1期10卷 41-44页

作者： Jialong Qi You Zhou Zhikai Zhu Chuanshan Xu Wenjie Chen key laboratory of molecular target&clinical pharmacology and the State&NMPA key laboratory of Respiratory Disease School of Pharmaceutical Sciences&the Fifth Affiliated HospitalGuangzhou Medical UniversityGuangzhouGuangdong 511436China Yunnan Digestive Endoscopy clinical Medical Center Department of GastroenterologyThe First People's Hospital of Yunnan ProvinceKunming 650032China Beijing Tiantan Hospital Capital Medical UniversityBeijing 100070China State key laboratory of Respiratory Disease Guangdong-Hongkong-Macao Joint Laboratory of Respiratory Infectious DiseaseGuangzhouGuangdong 510182China Sydney Vital Translational Cancer Research Centre Westbourne StNSW 2065Australia

The adenosine deaminase acting on RNA(ADAR)protein family was well characterized as RNA editing enzymes converting adenosines to inosines(A-to-l)in dsRNA structures.They share a homologous structure including the dsRNA-binding domain and the deaminase domain.ADAR1 function as the primary editing enzyme for A-to-l mutation because of its higher and ubiquitous expression compared to ADAR2 and ADAR3 in eukaryotes.

关键词： ADAR1 adenocarcinoma editing

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