Chem最新文献_第10页

Design of light- and chemically responsive protein assemblies through host-guest interactions

IF 23.5 1区化学

Chem Pub Date : 2025-02-10 DOI: 10.1016/j.chempr.2024.102407

Zhiyin Zhang, Huat T. Chiang, Ying Xia, Nicole Avakyan, Ravi R. Sonani, Fengbin Wang, Edward H. Egelman, James J. De Yoreo, Lilo D. Pozzo, F. Akif Tezcan

{"title":"Design of light- and chemically responsive protein assemblies through host-guest interactions","authors":"Zhiyin Zhang, Huat T. Chiang, Ying Xia, Nicole Avakyan, Ravi R. Sonani, Fengbin Wang, Edward H. Egelman, James J. De Yoreo, Lilo D. Pozzo, F. Akif Tezcan","doi":"10.1016/j.chempr.2024.102407","DOIUrl":"https://doi.org/10.1016/j.chempr.2024.102407","url":null,"abstract":"Host-guest (HG) interactions have been widely used to build responsive materials and molecular machines owing to their inherently dynamic nature, interaction specificity, and responsiveness to diverse stimuli. Here, we have set out to exploit these advantages of HG chemistry in the design of dynamic protein assemblies, using a C4 symmetric protein, C98RhuA, as a building block. We show that a C98RhuA variant individually modified with β-cyclodextrin (βCD) (host) or azobenzene (guest) functionalities can specifically pair with each other to form highly ordered 1D and 2D assemblies. Association and dissociation of βCDRhuA-azoRhuA assemblies can be controlled by UV and visible light as well as by small-molecule modulators of βCD-azobenzene interactions. Kinetics analyses reveal that βCDRhuA-azoRhuA nanotubes assemble without a nucleation barrier, a highly unusual occurrence for helical supramolecular systems. Taken together, our findings provide a compelling example for achieving complex structural and dynamic outcomes in protein assembly through simple chemical design.","PeriodicalId":268,"journal":{"name":"Chem","volume":"41 1","pages":""},"PeriodicalIF":23.5,"publicationDate":"2025-02-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143375293","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Homeostatic artificial cells enable self-protection in prototissue spheroids

IF 23.5 1区化学

Chem Pub Date : 2025-02-07 DOI: 10.1016/j.chempr.2024.102409

Joshua Krehan, Chuen-Ru Li, Marcos Masukawa, Esther Amstad, Andreas Walther

{"title":"Homeostatic artificial cells enable self-protection in prototissue spheroids","authors":"Joshua Krehan, Chuen-Ru Li, Marcos Masukawa, Esther Amstad, Andreas Walther","doi":"10.1016/j.chempr.2024.102409","DOIUrl":"https://doi.org/10.1016/j.chempr.2024.102409","url":null,"abstract":"Prototissues made from artificial cells (ACs) aim to replicate the behaviors of living tissues, such as communication, collective behavior, and homeostasis. Despite progress in developing diverse AC types, building prototissues and achieving effective communication as well as collective behavior in such prototissues remain challenging. We introduce ACs with an intrinsic homeostatic pH control mechanism that can be organized into prototissues to collectively maintain a stable microenvironment and protect cargo from environmental pH fluctuations. These ACs contain pH-modulating enzymes within a pH-sensitive membrane, allowing for self-regulation through chemo-structural feedback. They adjust pH by importing substrates within a specific pH range and self-regulate to control substrate influx. This enables them to modulate local pH, manage cargo release, and facilitate interactive communication in organized spheroids. Our findings demonstrate the potential of homeostatic ACs to create advanced synthetic tissue mimics, replicating protective and communicative functions of living tissues for biomedical and tissue engineering applications.","PeriodicalId":268,"journal":{"name":"Chem","volume":"13 1","pages":""},"PeriodicalIF":23.5,"publicationDate":"2025-02-07","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143258282","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Zwitterionic polymer intertwined metal-organic framework-based quasi-solid-state electrolyte for long cycle life dual-ion batteries

IF 23.5 1区化学

Chem Pub Date : 2025-02-07 DOI: 10.1016/j.chempr.2024.102402

Yeji Lee, Hyerin Woo, Jieun Kang, Soomin Hwang, Soojin Park, Sarah S. Park

引用次数: 0

Coordination-templated construction of single-crystal covalent organic frameworks

IF 23.5 1区化学

Chem Pub Date : 2025-02-06 DOI: 10.1016/j.chempr.2024.102398

Wenqiang Zhang, Yuting Zhang, Weili Ma, Xing Han, Wei Gong, Yan Liu, Yong Cui

引用次数: 0

Enhanced X-ray luminescence in one-dimensional Cu–I coordination polymers via ligand halogen engineering

IF 23.5 1区化学

Chem Pub Date : 2025-02-05 DOI: 10.1016/j.chempr.2024.102401

Wentao Wu, Shuyi Lin, Jian-Xin Wang, Yafeng Xu, Tengyue He, Yang Zhou, Peng Yuan, Partha Maity, Issatay Nadinov, Simil Thomas, Renwu Huang, Catherine S.P. De Castro, Jun Yin, Husam N. Alshareef, Osman M. Bakr, Omar F. Mohammed

{"title":"Enhanced X-ray luminescence in one-dimensional Cu–I coordination polymers via ligand halogen engineering","authors":"Wentao Wu, Shuyi Lin, Jian-Xin Wang, Yafeng Xu, Tengyue He, Yang Zhou, Peng Yuan, Partha Maity, Issatay Nadinov, Simil Thomas, Renwu Huang, Catherine S.P. De Castro, Jun Yin, Husam N. Alshareef, Osman M. Bakr, Omar F. Mohammed","doi":"10.1016/j.chempr.2024.102401","DOIUrl":"https://doi.org/10.1016/j.chempr.2024.102401","url":null,"abstract":"Cu(I) halide-based scintillators are emerging as eco-friendly alternatives to traditional X-ray imaging scintillators because of their high luminescence efficiency and solution processability. Although much progress has been made in zero-dimensional (0D) Cu–I cluster scintillators, there has been limited focus on one-dimensional (1D) Cu–I coordination polymers because of their lower luminescence efficiencies. This study presents a ligand halogen engineering strategy for significantly enhancing the photoluminescence efficiency of 1D Cu–I coordination polymers by utilizing halogen-based chemical modifications. The chlorine-modified ligands increase structural rigidity, reducing electronic repulsion between copper and iodine atoms and minimizing photon loss through non-radiative recombination pathways, resulting in an impressive photoluminescence quantum yield of nearly 100%. The designed scintillators demonstrate improved radioluminescence intensity, low detection limits, and exceptional spatial resolution (16 lp/mm). This research offers an approach for creating highly emissive 1D Cu–I coordination polymers and highlights their potential in X-ray imaging applications in medical diagnosis and security checks.","PeriodicalId":268,"journal":{"name":"Chem","volume":"28 1","pages":""},"PeriodicalIF":23.5,"publicationDate":"2025-02-05","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143124916","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Systematic evolution of functional oligonucleotides for targeted protein degradation

IF 23.5 1区化学

Chem Pub Date : 2025-02-04 DOI: 10.1016/j.chempr.2024.102408

Huang Su, Yifan Chen, Xuyang Zhao, Zengyi Lu, Tongxuan Wei, Qinguo Liu, Xiyang Liu, Qinhao Zhang, Siqi Bian, Qianwei Qiu, Panzhu Yao, Wenlang Liu, Zheng Zheng, Da Xu, Liqin Zhang

{"title":"Systematic evolution of functional oligonucleotides for targeted protein degradation","authors":"Huang Su, Yifan Chen, Xuyang Zhao, Zengyi Lu, Tongxuan Wei, Qinguo Liu, Xiyang Liu, Qinhao Zhang, Siqi Bian, Qianwei Qiu, Panzhu Yao, Wenlang Liu, Zheng Zheng, Da Xu, Liqin Zhang","doi":"10.1016/j.chempr.2024.102408","DOIUrl":"https://doi.org/10.1016/j.chempr.2024.102408","url":null,"abstract":"Targeted protein degradation (TPD) technologies leveraging the ubiquitin-proteasome system address “undruggable” proteins but struggle with optimizing targeting warheads and linkers. This study introduces a systematic platform for creating aptamer-based TPD molecules on demand. We developed a microbead-displayed oligonucleotide-E3 ligand chimera library and applied in vitro ubiquitination systems by using a fluorescent assay with bead sorting to identify high-affinity aptamer-chimera degraders that bind to target proteins and recruit E3 ligase for ubiquitination. This approach, tested with CRBN and VHL E3 ligases, successfully degraded BRD4 and IRAK4 proteins. Additionally, we evolved a bispecific RNA aptamer degrader, demonstrating the versatility of our platform. The selected aptamer chimeras achieved degradation rates of up to 87% for BRD4. Functional assays showed effective inhibition of cancer cell proliferation, induction of apoptosis, and significant tumor growth suppression in a subcutaneous tumor model. These findings highlight the potential of aptamer-based TPD technologies as powerful tools for cancer treatment.","PeriodicalId":268,"journal":{"name":"Chem","volume":"40 1","pages":""},"PeriodicalIF":23.5,"publicationDate":"2025-02-04","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143083605","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Engineered material-binding peptide empowers biocatalysis in stainless steel flow reactors for phosphate recovery

IF 23.5 1区化学

Chem Pub Date : 2025-01-30 DOI: 10.1016/j.chempr.2024.102395

Yi Lu, Florian Bourdeaux, Binbin Nian, Pirathiha Manimaran, Bhupesh Verma, Max Rommerskirchen, Sebastian Bold, Leilei Zhu, Yu Ji, Johannes Henrich Schleifenbaum, Ulrich Schwaneberg

{"title":"Engineered material-binding peptide empowers biocatalysis in stainless steel flow reactors for phosphate recovery","authors":"Yi Lu, Florian Bourdeaux, Binbin Nian, Pirathiha Manimaran, Bhupesh Verma, Max Rommerskirchen, Sebastian Bold, Leilei Zhu, Yu Ji, Johannes Henrich Schleifenbaum, Ulrich Schwaneberg","doi":"10.1016/j.chempr.2024.102395","DOIUrl":"https://doi.org/10.1016/j.chempr.2024.102395","url":null,"abstract":"Biocatalysis in stainless steel flow reactors is limited by inefficient enzyme immobilization on stainless steel surfaces. Herein, we report a universal and generally applicable strategy to achieve efficient enzyme immobilization in stainless steel flow reactors by utilizing an engineered material-binding peptide (MBP) with improved binding toward stainless steel. Through this method, phytase from Yersinia mollaretii (YmPh) was immobilized and showed high activity in hydrolyzing phytic acid to produce phosphate over multiple cycles. The MBP liquid chromatography peak I (LCI) was selected and engineered for improved stainless steel binding. The variant LCISS4 (LCI A14K/Y30R/D45R) showed an 8.2-fold improved binding to stainless steel compared with the LCI wild type. YmPh-LCISS4 immobilized in additively manufactured stainless steel flow reactors exhibited strong washing resistance and high reusability. The immobilization strategy presented here, based on LCISS4, enables robust and oriented enzyme immobilization on stainless steel, making it an appealing tool for industrial biocatalysis.","PeriodicalId":268,"journal":{"name":"Chem","volume":"23 1","pages":""},"PeriodicalIF":23.5,"publicationDate":"2025-01-30","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143057302","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Synthesis and magnetic property of a telluryl radical

IF 23.5 1区化学

Chem Pub Date : 2025-01-29 DOI: 10.1016/j.chempr.2024.102392

Dongmin Wang, Wang Chen, Rong Sun, Jun-Liang Liu, Bingwu Wang, Shengfa Ye, Gengwen Tan, Song Gao

引用次数: 0

Osmium atomic sites on CuS nanoplates for efficient two-electron oxygen reduction into H2O2

IF 23.5 1区化学

Chem Pub Date : 2025-01-29 DOI: 10.1016/j.chempr.2024.102393

Yingjun Sun, Zhengyi Qian, Mingzi Sun, Yingjie Li, Qinghua Zhang, Yan Nie, Lin Gu, Mingchuan Luo, Jianguo Liu, Bolong Huang, Shaojun Guo

{"title":"Osmium atomic sites on CuS nanoplates for efficient two-electron oxygen reduction into H2O2","authors":"Yingjun Sun, Zhengyi Qian, Mingzi Sun, Yingjie Li, Qinghua Zhang, Yan Nie, Lin Gu, Mingchuan Luo, Jianguo Liu, Bolong Huang, Shaojun Guo","doi":"10.1016/j.chempr.2024.102393","DOIUrl":"https://doi.org/10.1016/j.chempr.2024.102393","url":null,"abstract":"Electrocatalytic hydrogen peroxide (H2O2) production from O2 reduction is attractive because of its wide applications; however, the lack of efficient and selective electrocatalysts hinders its further development. Herein, we have created a class of electrocatalysts by anchoring osmium (Os) single atomic sites on ultrathin copper sulfide nanoplates (Os1-CuS NPs) to greatly boost the electroreduction of O2 into H2O2 via a two-electron pathway. The Os single-atomic-site catalyst with sulfur coordination achieved a record-high Os loading (25.9 wt %) and an exceptional H2O2 production rate (8.2 mol gcat−1 h−1) with near-perfect selectivity (∼98%), making it a top performer among metal-based electrocatalysts. In situ attenuated total reflectance surface-enhanced infrared absorption spectroscopy (ATR-SEIRAS) and density functional theory (DFT) calculations revealed that the introduced Os sites promote a selective 2e− oxygen reduction pathway by strengthening OOH binding and thus suppressing the undesired 4e− pathway. This study advances the design of high-performance single-atomic-site electrocatalysts for selective H2O2 generation.","PeriodicalId":268,"journal":{"name":"Chem","volume":"59 1","pages":""},"PeriodicalIF":23.5,"publicationDate":"2025-01-29","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143055272","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Enantioselective synthesis of amino acids by photocatalytic reduction of CO2 on chiral mesostructured ZnS

IF 23.5 1区化学

Chem Pub Date : 2025-01-27 DOI: 10.1016/j.chempr.2024.102390

Yongping Cui, Jing Ai, Yingying Duan, Menghui Jia, Tianwei Ouyang, Aokun Liu, Lu Yu, Junhong Liu, Xi Liu, Chaoyang Chu, Yuanbo Li, Yanhang Ma, Liwei Chen, Lu Han, Jinquan Chen, Changlin Tian, Shunai Che, Yuxi Fang

{"title":"Enantioselective synthesis of amino acids by photocatalytic reduction of CO2 on chiral mesostructured ZnS","authors":"Yongping Cui, Jing Ai, Yingying Duan, Menghui Jia, Tianwei Ouyang, Aokun Liu, Lu Yu, Junhong Liu, Xi Liu, Chaoyang Chu, Yuanbo Li, Yanhang Ma, Liwei Chen, Lu Han, Jinquan Chen, Changlin Tian, Shunai Che, Yuxi Fang","doi":"10.1016/j.chempr.2024.102390","DOIUrl":"https://doi.org/10.1016/j.chempr.2024.102390","url":null,"abstract":"Reduction and fixation of CO2 in natural systems via solar energy generate diverse products, ranging from small molecules to biomolecules. To date, only a few multicarbon species have been obtained by artificial CO2 photoreduction, especially abiotic photosynthesis of biomolecules with various functional groups, which is a challenging issue. Herein, we report the photocatalytic synthesis of amino acids from CO2 and NH3 on a chiral mesostructured ZnS (CMZ). Serine is the main component of various amino acids, with an enantiomeric excess (ee) greater than 96% and a total yield of over 30 μmol gcat−1. We propose that the chirality-induced spin polarization of CMZ boosts the creation of triplet OCCO by aligning its parallel electron spins, and the helical lattice distortion reduces the free energy of ∗OCCO. Enantiospecific activation energies of reactions driven by the spin-polarized electrons in CMZ lead to the formation of enantiomeric amino acids.","PeriodicalId":268,"journal":{"name":"Chem","volume":"5 1","pages":""},"PeriodicalIF":23.5,"publicationDate":"2025-01-27","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143044240","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0