ACS Chemical Biology最新文献_第5页

Merging Consecutive PET Processes within a Metal–Organic Cage for Abiotic–Biotic Combined Photocatalytic Biomass Reforming 在金属有机笼内合并连续 PET 过程，实现非生物-生物联合光催化生物质转化

IF 11.3 2区生物学

ACS Chemical Biology Pub Date : 2024-10-22 DOI: 10.1021/acscatal.4c0601810.1021/acscatal.4c06018

Zhefan Li, Junkai Cai*, Lingxiao Wang and Chunying Duan*,

{"title":"Merging Consecutive PET Processes within a Metal–Organic Cage for Abiotic–Biotic Combined Photocatalytic Biomass Reforming","authors":"Zhefan Li, Junkai Cai*, Lingxiao Wang and Chunying Duan*, ","doi":"10.1021/acscatal.4c0601810.1021/acscatal.4c06018","DOIUrl":"https://doi.org/10.1021/acscatal.4c06018https://doi.org/10.1021/acscatal.4c06018","url":null,"abstract":"Combining abiotic photocatalytic modules with enzymatic conversion to reform biomass represents a compelling way for sustainable energy schemes but faces marked challenges on the electron and proton transport corresponding to the cofactor regeneration and shuttling between biotic and abiotic partners. Herein, we report a consecutive photoinduced electron-transfer approach to reform biomass into fuels and active H-source for nitroarene reduction by grafting a cage-dye-NADH (nicotinamide adenine dinucleotide) clathrate with glucose dehydrogenase (GDH). Under light irradiation, the cage-dye-NADH clathrate acts as a photoactive relay to conduct two photoinduced 1e– electron-transfer reactions consecutively with a 2e– oxidation of NADH to NAD+, guaranteeing an orderly path related to cofactor regeneration. When the clathrate is positioned inside the pocket of GDH to join a biotic NAD+-mediated synthesis, the metal–organic artificial enzyme facilitates fast cofactor generation and shuttling between the artificial clathrate and the native enzyme within one working module. The grafting enzyme combines artificial photocatalysis and enzymatic dehydrogenation to endow an efficient conversion of biomass feedstocks into green H-source, innovating a unique paradigm for the sustainable energy scheme that combines energy of two photons in one turnover cycle. The superiority of the grafting enzyme allows the direct hydrogenation and reduction of fine chemicals and enables tandem nitroarene reduction with a turnover number reaching 15,000, providing a distinguished avenue for biomass utilization and solar energy conversion.","PeriodicalId":11,"journal":{"name":"ACS Chemical Biology","volume":"14 21","pages":"16374–16382 16374–16382"},"PeriodicalIF":11.3,"publicationDate":"2024-10-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142560513","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"生物学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Engineering Chemical and Catalytic Activity of Metal Surface Sites by Controlling Strain and Ligand Effects in Nonmodel Nanoparticle Catalysts 通过控制非模型纳米粒子催化剂中的应变和配体效应，实现金属表面位点的化学和催化活性工程化

IF 11.3 2区生物学

ACS Chemical Biology Pub Date : 2024-10-22 DOI: 10.1021/acscatal.4c0385710.1021/acscatal.4c03857

Bill Yan, and , Suljo Linic*,

{"title":"Engineering Chemical and Catalytic Activity of Metal Surface Sites by Controlling Strain and Ligand Effects in Nonmodel Nanoparticle Catalysts","authors":"Bill Yan,  and , Suljo Linic*, ","doi":"10.1021/acscatal.4c0385710.1021/acscatal.4c03857","DOIUrl":"https://doi.org/10.1021/acscatal.4c03857https://doi.org/10.1021/acscatal.4c03857","url":null,"abstract":"Binding energy of reactants on heterogeneous catalyst surface sites is a well-established catalytic activity descriptor for many chemical reactions. However, systematically manipulating the binding energies by engineering the catalytic surface sites has proven challenging. Herein, we propose a nanoparticle catalyst structure that contains an alloy core composed of miscible metal atoms, surrounded by layers of a different material, and covered by a layer of catalytically active metal. The alloy core controls the lattice strain of the nanoparticle and therefore the distance between the surface atoms, while the subsurface layer atoms induce a ligand effect on the surface atoms. We show that this class of materials allows us to systematically control the adsorbate binding energies with high precision. We illustrate our findings by developing nonmodel nanoparticle catalysts that employ an AuCu alloy with controlled composition as the core, Au as the surrounding layers, and Pt as the active surface metal. Electrochemical CO stripping measurements suggest that the CO binding energy on the surface Pt sites can be systematically tuned by varying the composition of the alloy core. Our analysis suggests that the change in the CO binding energy of Pt is the result of the combined ligand effect from the Au layers and strain effect from the AuCu core. The presented catalyst structure allows for precise modulation of the strain and ligand effect for tuning the local chemical environment of any catalytic materials, which may aid the development of next-generation catalysts.","PeriodicalId":11,"journal":{"name":"ACS Chemical Biology","volume":"14 21","pages":"16383–16391 16383–16391"},"PeriodicalIF":11.3,"publicationDate":"2024-10-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142560445","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"生物学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Recruitment to the Proteasome Is Necessary but Not Sufficient for Chemically Induced, Ubiquitin-Independent Degradation of Native Proteins 招募到蛋白酶体对于化学诱导的、依赖于泛素的原生蛋白降解是必要的，但并不充分

IF 3.5 2区生物学

ACS Chemical Biology Pub Date : 2024-10-22 DOI: 10.1021/acschembio.4c0042210.1021/acschembio.4c00422

Madeline Balzarini, Joel Tong, Weijun Gui, Isuru M. Jayalath, Bin-Bin Schell and Thomas Kodadek*,

{"title":"Recruitment to the Proteasome Is Necessary but Not Sufficient for Chemically Induced, Ubiquitin-Independent Degradation of Native Proteins","authors":"Madeline Balzarini, Joel Tong, Weijun Gui, Isuru M. Jayalath, Bin-Bin Schell and Thomas Kodadek*, ","doi":"10.1021/acschembio.4c0042210.1021/acschembio.4c00422","DOIUrl":"https://doi.org/10.1021/acschembio.4c00422https://doi.org/10.1021/acschembio.4c00422","url":null,"abstract":"Targeted protein degradation (TPD) is a promising strategy for drug development. Most degraders function by forcing the association of the target protein (TP) with an E3 Ubiquitin (Ub) ligase, which, in favorable cases, results in the polyubiquitylation of the TP and its subsequent degradation by the 26S proteasome. An alternative strategy would be to create chemical dimerizers that bypass the requirement for polyubiquitylation by recruiting the target protein directly to the proteasome. Direct-to-proteasome degraders (DPDs) may exhibit different characteristics than ubiquitin-dependent degraders, but few studies of this type of TPD have been published, largely due to the dearth of suitable proteasome ligands. To facilitate studies of DPDs, we report here a mammalian cell line in which the HaloTag protein is fused to the proteasome via Rpn13, one of the ubiquitin receptors. In these cells, a chloroalkane serves as a covalent proteasome ligand surrogate. We show that chimeric molecules comprised of a chloroalkane linked to a ligand for the BET family of proteins or the Cdk2/7/9 family of kinases result in ubiquitin-independent degradation of some of these target proteins. We use this system, the first that allows facile degradation of native proteins in a ubiquitin-independent fashion, to probe two issues: the effect of varying the length of the linker connecting the chloroalkane and the target ligand and the selectivity of degradation within the protein families engaged by the target ligand.","PeriodicalId":11,"journal":{"name":"ACS Chemical Biology","volume":"19 11","pages":"2323–2335 2323–2335"},"PeriodicalIF":3.5,"publicationDate":"2024-10-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142640998","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"生物学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Cu-Albumin Artificial Enzymes with Peroxidase and Oxidase Activity for Stereoselective Oxidations 具有过氧化物酶和氧化酶活性的铜-白蛋白人工酶，用于立体选择性氧化反应

IF 11.3 2区生物学

ACS Chemical Biology Pub Date : 2024-10-22 DOI: 10.1021/acscatal.4c0573210.1021/acscatal.4c05732

Maham Liaqat, Emma McDonald, Robert Jervine Valdez Ortega, Aaron Lopes, Flavia Codreanu, Hannah Carlisle, Challa V. Kumar, Xudong Yao, James F. Rusling and Jie He*,

引用次数: 0

Proteolytic Performance Is Dependent on Binding Efficiency, Processivity, and Turnover: Single Protease Insights 蛋白水解性能取决于结合效率、加工性和周转率：单一蛋白酶的启示

IF 11.3 2区生物学

ACS Chemical Biology Pub Date : 2024-10-22 DOI: 10.1021/acscatal.4c0418210.1021/acscatal.4c04182

Emily Winther Sørensen, Freya Björk Reinhold, Andreas Faber, Steen Bender, Jacob Kæstel-Hansen, Jeannette de Sparra Lundin, Errika Voutyritsa, Per Hedegaard, Sune M. Christensen and Nikos S. Hatzakis*,

{"title":"Proteolytic Performance Is Dependent on Binding Efficiency, Processivity, and Turnover: Single Protease Insights","authors":"Emily Winther Sørensen, Freya Björk Reinhold, Andreas Faber, Steen Bender, Jacob Kæstel-Hansen, Jeannette de Sparra Lundin, Errika Voutyritsa, Per Hedegaard, Sune M. Christensen and Nikos S. Hatzakis*, ","doi":"10.1021/acscatal.4c0418210.1021/acscatal.4c04182","DOIUrl":"https://doi.org/10.1021/acscatal.4c04182https://doi.org/10.1021/acscatal.4c04182","url":null,"abstract":"Proteases are essential enzymes for a plethora of biological processes and biotechnological applications, e.g., within the dairy, pharmaceutical, and detergent industries. Decoding the molecular-level mechanisms that drive protease performance is the key to designing improved biosolutions. However, the direct dynamic assessment of the fundamental partial reactions of substrate binding and activity has proven to be a challenge with conventional ensemble approaches. We developed a single-molecule (SM) assay for the direct and parallel recording of the stochastic binding interaction of Savinase, a serine-type protease broadly employed in biotechnology, with casein, while synchronously monitoring proteolytic degradation of the substrate. This assay allowed us to elucidate how the overall activity of Savinase and its variants depends on binding efficiency, turnover, and activity per binding event. We identified three distinct binding states, with mutations primarily affecting the long-lived state, indicating that it contributes to the overall activity and suggesting a level of processivity in Savinase. These insights, inaccessible through conventional methods, provide valuable perspectives for engineering proteases with improved hydrolytic performance.","PeriodicalId":11,"journal":{"name":"ACS Chemical Biology","volume":"14 21","pages":"16335–16343 16335–16343"},"PeriodicalIF":11.3,"publicationDate":"2024-10-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142560441","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"生物学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Direct Detection of Key Intermediates during the Product Release in Rhenium Bipyridine-Catalyzed CO2 Reduction Reaction 在联吡啶铼催化的二氧化碳还原反应中直接检测产物释放过程中的关键中间产物

IF 11.3 2区生物学

ACS Chemical Biology Pub Date : 2024-10-22 DOI: 10.1021/acscatal.4c0604410.1021/acscatal.4c06044

Samir Chattopadhyay, Mun Hon Cheah, Reiner Lomoth and Leif Hammarström*,

{"title":"Direct Detection of Key Intermediates during the Product Release in Rhenium Bipyridine-Catalyzed CO2 Reduction Reaction","authors":"Samir Chattopadhyay, Mun Hon Cheah, Reiner Lomoth and Leif Hammarström*, ","doi":"10.1021/acscatal.4c0604410.1021/acscatal.4c06044","DOIUrl":"https://doi.org/10.1021/acscatal.4c06044https://doi.org/10.1021/acscatal.4c06044","url":null,"abstract":"Rhenium bipyridine tricarbonyl complexes, fac-[Re(bpy)(CO)3X]n+, are highly effective in selectively converting CO2 to CO under electrochemical and photochemical conditions. Despite numerous mechanistic studies aimed at understanding its CO2 reduction reaction (CO2RR) pathway, the intermediates further into the catalytic cycle have escaped detection, and the steps leading to product release remained elusive. In this study, employing stopped-flow mixing coupled with time-resolved infrared spectroscopy, we observed, for the first time, the reduced Re-tetracarbonyl species, [Re(bpy)(CO)4]0, with a half-life of approximately 55 ms in acetonitrile solvent. This intermediate is proposed to be common in both electrochemical and photochemical CO2RR. Furthermore, we directly observed the release of the product (CO) from this intermediate. Additionally, we detected the accumulation of [Re(bpy)(CO)3(CH3CN)]+ as a byproduct following product release, a significant side reaction under conditions with a limited supply of reducing equivalents mirroring photochemical conditions. The process could be unambiguously attributed to an electron transfer-catalyzed ligand substitution reaction involving [Re(bpy)(CO)4]0 by simultaneous real-time detection of all involved species. We believe that this side reaction significantly impacts the CO2RR efficiency of this class of catalysts under photochemical conditions or during electrocatalysis at mild overpotentials.","PeriodicalId":11,"journal":{"name":"ACS Chemical Biology","volume":"14 21","pages":"16324–16334 16324–16334"},"PeriodicalIF":11.3,"publicationDate":"2024-10-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.acs.org/doi/epdf/10.1021/acscatal.4c06044","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142560442","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"生物学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Asymmetric Site-Enabled O–O Coupling in Co3O4 for Oxygen Evolution Reaction Co3O4 中用于氧进化反应的不对称位点催化 O-O 耦合

IF 11.3 2区生物学

ACS Chemical Biology Pub Date : 2024-10-22 DOI: 10.1021/acscatal.4c0416410.1021/acscatal.4c04164

Minghui Cui, Rongjing Guo, Yansong Zhou, Wenqi Zhao, Yanjing Liu, Wenbo Luo, Qiongrong Ou* and Shuyu Zhang*,

{"title":"Asymmetric Site-Enabled O–O Coupling in Co3O4 for Oxygen Evolution Reaction","authors":"Minghui Cui, Rongjing Guo, Yansong Zhou, Wenqi Zhao, Yanjing Liu, Wenbo Luo, Qiongrong Ou* and Shuyu Zhang*, ","doi":"10.1021/acscatal.4c0416410.1021/acscatal.4c04164","DOIUrl":"https://doi.org/10.1021/acscatal.4c04164https://doi.org/10.1021/acscatal.4c04164","url":null,"abstract":"The efficiency of hydrogen production from water electrolysis is mainly restricted by the sluggish oxygen evolution reaction (OER). The mainstream adsorbate evolution mechanism and lattice oxygen-mediated mechanism face a trade-off between performance and stability, while the diatomic oxygen mechanism (DOM) based on the O–O coupling provides a solution to overcome this limitation. However, the intrinsic principles that facilitate the O–O coupling remain unclear, which complicates material design. In this work, we use spinel Co3O4 as a model and identify that the asymmetric sites formed by the octahedral Co with O defects and the original octahedral Co are effective sites for O–O coupling. Based on this, we propose using the degree of asymmetry of the dual site as a descriptor to quantify the reaction free energy of rate-determining step along the DOM pathway, presenting a volcano plot relationship. Experimental validation shows that plasma-prepared Co3O4 enables O–O coupling, requiring only 287 and 420 mV overpotentials to achieve current densities of 10 and 1000 mA cm–2 in 0.5 M H2SO4, respectively. This work demonstrates efficient sites for the OER along the DOM pathway in Co3O4, providing valuable insights for designing high-performance OER catalysts.","PeriodicalId":11,"journal":{"name":"ACS Chemical Biology","volume":"14 21","pages":"16353–16362 16353–16362"},"PeriodicalIF":11.3,"publicationDate":"2024-10-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142560514","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"生物学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Water-Stable Perovskite Nanocrystals to Overcome the Photocatalysis–Stability Trade-Off in Aqueous Photo-RAFT Polymerization 在水性光-RAFT 聚合过程中克服光催化-稳定性权衡的水稳定性 Perovskite 纳米晶体

IF 11.3 2区生物学

ACS Chemical Biology Pub Date : 2024-10-22 DOI: 10.1021/acscatal.4c0340710.1021/acscatal.4c03407

Mengqiang Zhang, Jingyi Hao, Chengli Wang, Yue Zhang, Xiaomeng Zhang, Zhe Cui, Peng Fu, Minying Liu, Ge Shi, Xiaoguang Qiao, Yajing Chang, Yanjie He* and Xinchang Pang*,

{"title":"Water-Stable Perovskite Nanocrystals to Overcome the Photocatalysis–Stability Trade-Off in Aqueous Photo-RAFT Polymerization","authors":"Mengqiang Zhang, Jingyi Hao, Chengli Wang, Yue Zhang, Xiaomeng Zhang, Zhe Cui, Peng Fu, Minying Liu, Ge Shi, Xiaoguang Qiao, Yajing Chang, Yanjie He* and Xinchang Pang*, ","doi":"10.1021/acscatal.4c0340710.1021/acscatal.4c03407","DOIUrl":"https://doi.org/10.1021/acscatal.4c03407https://doi.org/10.1021/acscatal.4c03407","url":null,"abstract":"Metal halide perovskite nanocrystals (PNCs) have demonstrated remarkable photocatalytic properties in diverse photochemical reactions owing to their high absorption coefficients and long photogenerated carrier lifetimes. However, their catalytic applications have been severely hindered by their structural incompatibility with polar solvents, water in particular, due to the labile ionic nature of the perovskite. Realization of the photocatalytic performance of PNCs in an aqueous medium would significantly expand their potential in photocatalysis. Herein, judiciously designed CsPbBr3 NCs stabilized on Al2O3 nanoflowers (denoted as A-CsPbBr3 NCs) are utilized as water-stable photocatalysts for aqueous photomediated reversible addition–fragmentation chain transfer (photo-RAFT) polymerization. The A-CsPbBr3 NCs exhibited exceptional water stability and photostability owing to the stabilization effect endowed by Al2O3 nanoflowers without sacrificing their charge/carrier transport properties. Consequently, aqueous photo-RAFT polymerization was successfully performed by leveraging A-CsPbBr3 NCs as photocatalysts under visible light illumination, which was inaccessible to conventional short-ligand-capped PNCs. The effects of the excitation wavelength, catalyst loading, and architectures of PNCs on the visible-light-mediated polymerization were scrutinized to reveal the polymerization via a photoinduced electron-/energy-transfer mechanism, yielding polymers/copolymers with well-defined compositions, well-controlled molecular weights, low polydispersity, and high chain-end fidelity.","PeriodicalId":11,"journal":{"name":"ACS Chemical Biology","volume":"14 21","pages":"16313–16323 16313–16323"},"PeriodicalIF":11.3,"publicationDate":"2024-10-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142560443","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"生物学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Unveiling Intrinsic Charge Transfer Dynamics in Bone-Joint S-Scheme Heterostructures To Promote Photocatalytic Hydrogen Peroxide Generation 揭示骨接S-梯形异质结构的内在电荷转移动力学，促进光催化过氧化氢生成

IF 11.3 2区生物学

ACS Chemical Biology Pub Date : 2024-10-21 DOI: 10.1021/acscatal.4c0503110.1021/acscatal.4c05031

Yuhui Liu, Xiaoxu Deng*, Yi Wang, Qin Luo, Yunxia Liu, Shuang-Feng Yin* and Peng Chen*,

{"title":"Unveiling Intrinsic Charge Transfer Dynamics in Bone-Joint S-Scheme Heterostructures To Promote Photocatalytic Hydrogen Peroxide Generation","authors":"Yuhui Liu, Xiaoxu Deng*, Yi Wang, Qin Luo, Yunxia Liu, Shuang-Feng Yin* and Peng Chen*, ","doi":"10.1021/acscatal.4c0503110.1021/acscatal.4c05031","DOIUrl":"https://doi.org/10.1021/acscatal.4c05031https://doi.org/10.1021/acscatal.4c05031","url":null,"abstract":"Constructing compact direct Z- and S-scheme heterostructures is an efficient strategy for realizing a highly efficient charge separation and photocatalytic performance. However, the stochastic nature of interface orientation and lattice mismatch often results in a blind region for effective inner charge transfer, which hinders the logical design of compact heterojunctions. Here, experimental results and theoretical research unveiled that complicated internal charges can be directly transferred to an intermediate cocrystal plane for electron–hole recombination in compact S-scheme heterostructures, called “bone-joint” heterostructures, which facilitate the establishment of an inherent electric field to drive charge transfer. Moreover, those bone-joint structures adjust the inherent chemical and energetic interactions that manipulate the reactant adsorption mode and surface reaction energy. As a result, a synthesized catalyst displayed a remarkable hydrogen peroxide production performance and stability. This offers a paradigm for intrinsic charge transfer dynamics in heterostructures and a guiding philosophy for designing efficient heterostructures.","PeriodicalId":11,"journal":{"name":"ACS Chemical Biology","volume":"14 21","pages":"16287–16296 16287–16296"},"PeriodicalIF":11.3,"publicationDate":"2024-10-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142560477","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"生物学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Pharmacologic Induction of ERα SUMOylation Disrupts Its Chromatin Binding 药物诱导 ERα SUMOylation 会破坏其染色质结合

IF 3.5 2区生物学

ACS Chemical Biology Pub Date : 2024-10-21 DOI: 10.1021/acschembio.4c0060610.1021/acschembio.4c00606

Lizhen Wang, and , Ting Han*,

{"title":"Pharmacologic Induction of ERα SUMOylation Disrupts Its Chromatin Binding","authors":"Lizhen Wang,  and , Ting Han*, ","doi":"10.1021/acschembio.4c0060610.1021/acschembio.4c00606","DOIUrl":"https://doi.org/10.1021/acschembio.4c00606https://doi.org/10.1021/acschembio.4c00606","url":null,"abstract":"Estrogen receptor α (ERα)-positive breast cancer patients are typically treated with ERα inhibitors, including selective estrogen receptor modulators (SERMs) and selective estrogen receptor degraders (SERDs). However, the distinct pharmacological properties of various ERα inhibitors remain incompletely understood. In this study, we employed formaldehyde cross-linking followed by ERα immunoprecipitation and mass spectrometry to reveal that fulvestrant, the first FDA-approved SERD, induces the interaction between ERα and SUMO E3 ligases PIAS1 and PIAS2. Biochemical and genomic assays confirmed that fulvestrant induces SUMOylation of ERα, which inhibits ERα′s binding to chromatin DNA. In addition, raloxifene (a SERM) and elacestrant (the first FDA-approved oral SERD) were identified as compounds that similarly induce ERα SUMOylation and inhibit its chromatin interaction. Our findings reveal a mechanism by which select ERα inhibitors disrupt ERα function through SUMOylation, offering insights for the development of next-generation ERα-targeted therapies.","PeriodicalId":11,"journal":{"name":"ACS Chemical Biology","volume":"19 11","pages":"2383–2392 2383–2392"},"PeriodicalIF":3.5,"publicationDate":"2024-10-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.acs.org/doi/epdf/10.1021/acschembio.4c00606","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142640902","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"生物学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0