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Rational design of platinum(Ⅱ)complexes with orthogonally oriented triazolyl ligand with emission enhancement characteristics for cancer chemotherapy in vivo

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Science China Chemistry 2023年第10期66卷 2878-2884页

作者： Yeye Ai Zherui Zhang Yuexuan Fei Ruirong Ye Angela Sin-Yee Law zong-wan mao Junqiu Liu Yongguang Li Vivian Wing-Wah Yam Key Laboratory of Organosilicon Chemistry and Material Technology of Ministry of Education College of Material Chemistry and Chemical EngineeringHangzhou Normal UniversityHangzhou 311121China Institute of Molecular Functional Materials State Key Laboratory of Synthetic Chemistry and Department of ChemistryThe University of Hong KongHong KongChina School of Chemistry Sun Yat-Sen UniversityGuangzhou 510275China State Key Laboratory of Supramolecular Structure and Materials Jilin UniversityChangchun 130012China

The mitochondria are essential for tumorigenesis and have been regarded as important targets in cancer chemotherapy.Herein,the mitochondria-targeted platinum(Ⅱ)complexes have been prepared.The introduction of the triazole group with larger steric hindrance through post-click reaction converts the hybridization of carbon from sp to sp^(2),endowing the complexes with an orthogonally oriented ligand with restricted rotation and emission enhancement characteristics.Methylation of the triazolyl ligand has led to platinum(Ⅱ)complexes that can efficiently enter cancer cells and selectively accumulate in mitochondria,leading to significant enhancement in phosphorescence.In vivo anti-cancer investigations have demonstrated their distinct antitumor efficacy in substantial inhibition of tumor growth in breast cancer mice through dissipation of mitochondrial membrane potential,inducing apoptosis of tumor cell with negligibly systemic cytotoxicity.

关键词： platinum(Ⅱ)complexes post-click reaction emission enhancement mitochondria-targeting antitumor

A Rhein-Based Rh(Ⅲ) Arene Complex with Anti-tumor Cell Proliferative Activity Inhibits RNA Demethylase FTO

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Chinese Journal of Chemistry 2022年第10期40卷 1156-1164页

作者： Lu Liu Yaqiong Kong Liang He Xiuxiu wang Meng-Meng wang Hongjiao Xu Cai-Guang Yang Zhi Su Jing Zhao zong-wan mao Yue Huang Hong-Ke Liu School of Chemistry and Materials Science Nanjing Normal UniversityNanjingJiangsu 210023China State Key Laboratory of Drug Research Shanghai Institute of Materia MedicaChinese Academy of SciencesShanghai 201203China Schoolof Chemistry Sun Yat-Sen UniversityGuangzhouGuangdong 510275China School of Chemistry and Chemial Enginering Nanjing UniversityNanjingJingsu 210023China School of Pharmaceutical Science and Technology Hangzhou Institute for Advanced StudyUniversity of Chinese Academy of SciencesHangzhouZhejiang 310024China

Metallodrugs with fine-tuned coordination between metals and bioactive ligands can achieve cytotoxic effects in cancer therapy and have been considered as a new approach for drug design.However,it has yet to be elucidated whether these metallodrugs target epitranscriptomic proteins for gene expression regulation.This report describes a rhein-based Rh(l)-arene complex,Rh1,that exhibited promising antiproliferative ffects in several tumor cellines.Rh1 induced cell death through the autophagy,cell cycle arrest,and accumulation of intracllular reactive oxygen species(ROs),In addition,Rh1 upregulated the global N^(6)-methyladenosine(m^(6)A)levels in A549 cells in the fat mass-and obesity-associated protein(FTO)-dependent manner.Collectively,the metal-based FTO inhibitor Rh1 effectively suppressed tumor cell proliferation and modulated the abundance of cellular m^(6)A,highlighting the potential of metal-based agents to target and regulate epitranscriptomics for tumor suppression.

关键词： Rhodium mRNA Antiproliferation FTO m^(6)A

Anion-Responsive Manganese Porphyrin Facilitates Chloride Transport and Induces Immunogenic Cell Death

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CCS Chemistry 2022年第7期4卷 2409-2419页

作者： Fang-Xin wang Jie-Wei Liu Xiao-Qiao Hong Cai-Ping Tan Li Zhang Wen-Hua Chen Peter J.Sadler zong-wan mao MOE Key Laboratory of Bioinorganic and Synthetic Chemistry Department of ChemistrySun Yat-Sen UniversityGuangzhou 510275 Department of Chemistry University of WarwickCoventry CV47AL School of Biotechnology and Health Sciences Wuyi UniversityJiangmen 529020

Chloride is the most abundant anion in living systems.Most natural or synthetic chloride anionophores function via hydrogen-bonding interactions.However,dynamic metal-anion coordination can also be an efficient way of transporting chloride across membranes.Here,we investigate anion transport by manganese(Ⅲ)meso-tetraphenylporphyrin chloride{[Mn(TPP)Cl],TPP=meso-tetraphenylporphyrin}complex that exhibits labile axial coordination.[Mn(TPP)Cl]showed high chloride transport activity in a bilayer vesicle model with an EC_(50) value of 4.42×10^(−3) mol%.In living cells,[Mn(TPP)Cl]induced rapid chloride influx and autophagy.The release of Ca^(2+)and adenosine 5′-triphosphate(ATP),as well as the relocation of calreticulin,revealed that[Mn(TPP)Cl]caused immunogenic cell death.Proteomic analysis indicated that[Mn(TPP)Cl]impaired several physiological processes,including DNA synthesis,transcription,mitochondrial respiration,RNA translation,and immune response.Our study suggests that dynamic metal-anion interactions across membranes might provide a practical strategy for the interference of chloride homeostasis.

关键词： manganese porphyrin anionophore chloride transport autophagy immunogenic cell death

Super-resolution quantification of nanoscale damage to mitochondria in live cells

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Nano Research 2020年第8期13卷 2149-2155页

作者： Xintian Shao Qixin Chen Lianting Hu Zhiqi Tian Liuyi Liu Fei Liu Fengshan wang Peixue Ling zong-wan mao Jiajie Diao Shandong Academy of Pharmaceutical Sciences Key Laboratory of BiopharmaceuticalsEngineering Laboratory of Polysaccharide DrugsNational-Local Joint Engineering Laboratory of Polysaccharide DrugsJinan250101China Department of Cancer Biology University of Cincinnati College of MedicineCincinnatiOH45267USA School of Pharmaceutical Sciences Cheeloo College of MedicineShandong UniversityJinan250012China Xintian Shao Qixin Chenand Lianting Hu contributed equally to this work.Shandong First Medical University&Shandong Academy of Medical SciencesJinan250062China Xintian Shao Qixin Chenand Lianting Hu contributed equally to this work.School of Information ManagementWuhan UniversityWuhan430072China MOE Key Laboratory of Bioinorganic and Synthetic Chemistry School of ChemistrySun Yat-Sen UniversityGuangzhou510275China

Mitochondrial damage,characterized by altered morphological distribution and the damage of cristae,is closely associated with mitochondrial disease.However,imaging methods for capturing mitochondrial morphology at the nanoscale level in live samples remain unavailable,which seriously hinders the accurate evaluation and diagnosis of mitochondrial-related diseases.In response,we propose a super-resolution quantification strategy based on structured illumination microscopy(SIM)for the rapid,accurate evaluation of mitochondrial morphology.Using the strategy,we accurately captured the morphological distribution of mitochondria at the nanoscale level in a way generally applicable to checking various cell processes and identifying patients with mitochondrial disease who exhibit the SLC25A46 mutation.We also used algorithm-assisted super-resolution imaging to quantitatively analyze damage to mitochondrial cristae,which supports a novel drug screening strategy—high-resolution drug screening—for investigating drugs’pharmacodynamics on organelles in living cells.In short,our strategy improves the accurate examination of changes in mitochondrial morphology in living cells and indicates new ways in which SIM-imaging can assist in diagnosing mitochondrial disease at the single-cell level.

关键词： mitochondria structured illumination microscopy quantification analyze morphology cristae

Structural Insight into the Substrate Gating Mechanism by Staphylococcus aureus Aldehyde Dehydrogenase

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CCS Chemistry 2020年第5期2卷 946-954页

作者： Xuan Tao Zhemin Zhang Xiao Zhang Hongyan Li Hongzhe Sun zong-wan mao Wei Xia MOE Key Laboratory of Bioinorganic and Synthetic Chemistry School of ChemistrySun Yat-sen UniversityGuangzhou510275 Department of Chemistry The University of Hong KongPokfulam RoadHong Kong

Staphylococcus aureus produces staphyloxanthin,a C30 carotenoid with golden color,as an antioxidant to promote bacterial resistance to reactive oxygen species.The biosynthesis pathway of staphyloxanthin involves a series of catalytic enzymes.Aldehyde dehydrogenase(AldH)is a dehydrogenase recently identified to convert 4,4’-diaponeurosporenaldehyde into 4,4’-diaponeurosporenoic acid during staphyloxanthin biosynthesis.Here,we present the crystallographic structures of apo-and holo-forms of S.aureus AldH.The dimeric enzyme contains a unique C-terminal helix,which resembles a“gatekeeper”helix found in human membrane-bound fatty aldehyde dehydrogenase(FALDH).Particularly,the helix adopts“open”and“closed”conformations in apo-and holo-AldH,respectively,to control the access of the substrate tunnel.Mutagenesis in combination with in vitro and in vivo activity assays identifies several residues essential for S.aureus AldH substrate recognition and enzyme catalytic turnover.Our results provide insights into substrate recognition of S.aureus AldH toward polyunsaturated long-chain aldehydes at atomic resolution.

关键词： Staphylococcus aureus virulence factor substrate recognition aldehyde dehydrogenase protein structure

Engineering Functional Inorganic-Organic Hybrid System Advances in siRNA Therapeutics

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Engineering Functional Inorganic-Organic Hybrid System Advan...

2018年中西部地区无机化学化工学术研讨会

作者： Yuna Qian zong-wan mao Jianliang Shen State Key Laboratory of Ophthalmology Optometry and Vision Science Wenzhou Medical University MOE Key Laboratory of Bioinorganic and Synthetic Chemistry School of Chemistry Sun Yat-sen University Wenzhou Institute of Biomaterials and Engineering Chinese Academy of Science

Cancer treatment still faces a lot of obstacles such as tumor heterogeneity, drug resistance and systemic toxicities. Beyond the traditional treatment modalities, exploitation of RNA interference（RNAi） as an emerging approach has immense potential for treatment various gene-caused diseases including cancer. The last decade has witnessed enormous research and achievements focused on RNAi biotechnology. However, delivery of small interference RNA（siRNA） remains a key challenge in the development of clinical RNAi therapeutics. Indeed, nanomaterials-formulated siRNA systems have potential applications for protection of siRNA from degradation, improving the accumulation in the target tissues, enhancing the siRNA therapy and reducing the side effects. Here, we explore and summarize the role of functional inorganic-organic hybrid systems involved in the siRNA therapeutics advancements. Inorganic-organic hybrid platforms as the vectors for siRNA delivery are promising to give credit to the interdisciplinary cooperation between inorganic, organic, biology and medicine.

关键词： Cancer RNA interference small interfering RNA delivery inorganic-organic hybrid nanoparticles

Halogen Ion-Selective Phosphorescence Turn-on Probe Based on Induction of Pt-Pt Interactions

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Halogen Ion-Selective Phosphorescence Turn-on Probe Based on...

第十一届全国化学生物学学术会议

作者： Jing Yang Qian Cao zong-wan mao School of Chemistry Sun Yat-Sen University

We have found the halogen ion（I-, Br-, Cl-） induced aggregation and self-assembly of the square-planar cytometalated platinum（II） complexes in aqueous media for the first time, which open a new use of square-planar platinum（II） complexes for detecting halogen ions in biological systems1 with large Stoke shifts and p H independence. The aggregation is driven by the coordination and electrostatic interactions between the halogen ion and the complex, and by the Pt-Pt interactions and ligand stacking, thus exhibiting the MMLCT transition features and phosphorescence turn-on behavior. Herein, square-planar geometry of platinum complexes is indispensable2. Once the bidentate rigid ligand is replaced by two monodentate ligands, a resulting non-square flexible structure will fail to the halogen ion response.

关键词： Pt-Pt interaction Halogen ion-selective Phosphorescent Turn-on probe

Functional Inorganic-Organic Hybrid Nanomaterials for Theranostic Applications

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中国化学会第十四届全国生物无机化学学术会议

作者： Yuna Qian zong-wan mao 沈建良 Wenzhou Institute of Biomaterials and Engineering Chinese Academy of Science MOE Key Laboratory of Bioinorganic and Synthetic Chemistry School of Chemistry Sun Yat-sen University State Key Laboratory of Ophthalmology Optometry and Vision Science Wenzhou Medical University

Patients with cancer have limited treatment options, since some the diseases do not respond to endocrine or targeted therapies. Approximately 15% of breast cancers are classified as triple negative, which is a highly aggressive form of breast cancer that lacks expression of the estrogen receptor（ER）, progesterone receptor（PR）, and Her2/neu. Therefore, therapeutic options are limited for the TNBC patients as hormonal and targeted therapies cannot be exploited. Accordingly, there is an urgent need to develop new therapeutic agents against TNBC. Here, we explore and summarize the role of functional inorganic-organic hybrid systems involved in the siRNA, combination, theranostic therapeutics advancements. Inorganic-organic hybrid platforms as the vectors for drug delivery are promising to give credit to the interdisciplinary cooperation between inorganic, organic, biology and medicine.

关键词： Cancer RNA interference Theranostic applications hybrid nanoparticles

Functional Inorganic-Organic Hybrid Nanomaterials for Theranostic Applications

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Functional Inorganic-Organic Hybrid Nanomaterials for Theran...

第十一届全国化学生物学学术会议

作者： Yuna Qian zong-wan mao 沈建良 Wenzhou Institute University of Chinese Academy of Sciences MOE Key Laboratory of Bioinorganic and Synthetic Chemistry School of ChemistrySun Yatsen University 中科院温州生物材料与工程研究所

Patients with cancer have limited treatment options,since some the diseases do not respond to endocrine or targeted therapies.Approximately 15% of breast cancers are classified as triple negative,which is a highly aggressive form of breast cancer that lacks expression of the estrogen receptor（ER）,progesterone receptor（PR）,and Her2/neu.Therefore,therapeutic options are limited for the TNBC patients as hormonal and targeted therapies cannot be exploited.Accordingly,there is an urgent need to develop new therapeutic agents against TNBC.Here,we explore and summarize the role of functional inorganic-organic hybrid systems involved in the siRNA,combination,theranostic therapeutics advancements.Inorganic-organic hybrid platforms as the vectors for drug delivery are promising to give credit to the interdisciplinary cooperation between inorganic,organic,biology and medicine.

关键词： Cancer RNA interference Theranostic applications hybrid nanoparticles