ACS Central Science最新文献

{"title":"A Conversation with Alexandra Navrotsky.","authors":"Rachel Brazil","doi":"10.1021/acscentsci.4c02126","DOIUrl":"https://doi.org/10.1021/acscentsci.4c02126","url":null,"abstract":"","PeriodicalId":10,"journal":{"name":"ACS Central Science","volume":"11 1","pages":"6-7"},"PeriodicalIF":12.7,"publicationDate":"2024-12-30","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.ncbi.nlm.nih.gov/pmc/articles/PMC11771449/pdf/","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143050972","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Lipid-Modulated, Graduated Inhibition of N-Glycosylation Pathway Priming Suggests Wide Tolerance of ER Proteostasis to Stress.","authors":"Andrew M Giltrap, Niamh Morris, Yin Yao Dong, Stephen A Cochrane, Thomas Krulle, Steven Hoekman, Martin Semmelroth, Carina Wollnik, Timea Palmai-Pallag, Elisabeth P Carpenter, Jonathan Hollick, Alastair Parkes, York Rudhard, Benjamin G Davis","doi":"10.1021/acscentsci.4c01506","DOIUrl":"10.1021/acscentsci.4c01506","url":null,"abstract":"<p><p>Protein N-glycosylation is a cotranslational modification that takes place in the endoplasmic reticulum (ER). Disruption of this process can result in accumulation of misfolded proteins, known as ER stress. In response, the unfolded protein response (UPR) restores proteostasis or responds by controlling cellular fate, including increased expression of activating transcription factor 4 (ATF4) that can lead to apoptosis. The ability to control and manipulate such a stress pathway could find use in relevant therapeutic areas, such as in treating cancerous states in which the native ER stress response is often already perturbed. The first committed step in the N-glycosylation pathway is therefore a target for potential ER stress modulation. Here, using structure-based design, the scaffold of the natural product tunicamycin allows construction of a panel capable of graduated inhibition of DPAGT1 through lipid-substituent-modulated interaction. The development of a quantitative, high-content, cellular immunofluorescence assay allowed precise determination of downstream mechanistic consequences (through the nuclear localization of key proxy transcription factor ATF4 as a readout of resulting ER stress). Only the most potent inhibition of DPAGT1 generates an ER stress response. This suggests that even low-level \"background\" biosynthetic flux toward protein glycosylation is sufficient to prevent response to ER stress. \"Tuned\" inhibitors of DPAGT1 also now seemingly successfully decouple protein glycosylation from apoptotic response to ER stress, thereby potentially allowing access to cellular states that operate at the extremes of normal ER stress.</p>","PeriodicalId":10,"journal":{"name":"ACS Central Science","volume":"11 1","pages":"107-115"},"PeriodicalIF":12.7,"publicationDate":"2024-12-26","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.ncbi.nlm.nih.gov/pmc/articles/PMC11758266/pdf/","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143044849","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"AI and Chemistry in Action: Transforming Crystallization for Scalable Water Harvesting Solutions.","authors":"Zhiling Zheng","doi":"10.1021/acscentsci.4c01838","DOIUrl":"10.1021/acscentsci.4c01838","url":null,"abstract":"","PeriodicalId":10,"journal":{"name":"ACS Central Science","volume":"10 12","pages":"2173-2174"},"PeriodicalIF":12.7,"publicationDate":"2024-12-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.ncbi.nlm.nih.gov/pmc/articles/PMC11672529/pdf/","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142902387","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"When Photoelectrons Meet Gas Molecules: Determining the Role of Inelastic Scattering in Ambient Pressure X-ray Photoelectron Spectroscopy.","authors":"Haoyi Li, Asmita Jana, Angel T Garcia-Esparza, Xiang Li, Corey J Kaminsky, Rebecca Hamlyn, Rajiv Ramanujam Prabhakar, Harry A Atwater, Joel W Ager, Dimosthenis Sokaras, Junko Yano, Ethan J Crumlin","doi":"10.1021/acscentsci.4c01841","DOIUrl":"10.1021/acscentsci.4c01841","url":null,"abstract":"<p><p>Inelastic photoelectron scattering (IPES) by gas molecules, a critical phenomenon observed in ambient pressure X-ray photoelectron spectroscopy (APXPS), complicates spectral interpretation due to kinetic energy loss in the primary spectrum and the appearance of additional features at higher binding energies. In this study, we systematically investigate IPES in various gas environments using APXPS, providing detailed insights into interactions between photoelectrons emitted from solid surfaces and surrounding gas molecules. Core-level XPS spectra of Au, Ag, Zn, and Cu metals were recorded over a wide kinetic energy range in the presence of CO₂, N₂, Ar, and H₂ gases, demonstrating the universal nature of IPES across different systems. Additionally, we analyzed spectra of scattering effects induced by gas-phase interactions without metal solids. In two reported CO₂-reduction systems (p-GaN/Au/Cu and p-Si/TaO _<i>x</i> /Cu), we elucidated that IPES is independent of the composition, structure, or size of the solid materials. Using metal foil platforms, we further developed an analytical model to extract electron excitation cross sections of gas molecules. These findings enhance our understanding of IPES mechanisms and enable the predictions of IPES structures in other solid-gas systems, providing a valuable reference for future APXPS studies and improving the accuracy of spectral analysis in gas-rich catalytic interfaces.</p>","PeriodicalId":10,"journal":{"name":"ACS Central Science","volume":"11 1","pages":"98-106"},"PeriodicalIF":12.7,"publicationDate":"2024-12-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.ncbi.nlm.nih.gov/pmc/articles/PMC11758507/pdf/","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143044864","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Stephanie Beaupark Sees Chemistry Through an Indigenous Lens.","authors":"Jonathan Feakins","doi":"10.1021/acscentsci.4c02023","DOIUrl":"https://doi.org/10.1021/acscentsci.4c02023","url":null,"abstract":"","PeriodicalId":10,"journal":{"name":"ACS Central Science","volume":"10 12","pages":"2178-2181"},"PeriodicalIF":12.7,"publicationDate":"2024-12-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.ncbi.nlm.nih.gov/pmc/articles/PMC11709082/pdf/","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142941416","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"A Pair of Fluorescent Probes Enabling Precise Diagnosis of Liver Cancer by Complementary Imaging.","authors":"Min Gao, Sun Hyeok Lee, Haw-Young Kwon, Larissa Miasiro Ciaramicoli, Eunsol Jo, Young Hyun Yu, Fengming Li, Beomsue Kim, Kyungtae Hong, Jun-Seok Lee, Namhui Kim, Yoojin Oh, Chun Young Im, Chris Soon Heng Tan, Hyung-Ho Ha, Young-Tae Chang","doi":"10.1021/acscentsci.4c01822","DOIUrl":"10.1021/acscentsci.4c01822","url":null,"abstract":"<p><p>Hepatocellular carcinoma (HCC) is by far the predominant malignant liver cancer, with both high morbidity and mortality. Early diagnosis and surgical resections are imperative for improving the survival of HCC patients. However, limited by clinical diagnosis methods, it is difficult to accurately distinguish tumor tissue and its boundaries in the early stages of cancer. Herein, we report two fluorescent probes, <b>cLG</b> and <b>hLR</b>, for the detection of cancer and healthy cells, respectively, enabling the precise diagnosis of liver cancer by providing complementary imaging. These two fluorescent probes could selectively stain the target cells in the liver tissue imaging, which is confirmed by H&E and antibody staining. Moreover, for the first time, the cancerous area and healthy area are clearly identified by the cocktail of these two probes, suggesting its potential to be used in fluorescence-guided surgery. Finally, we identify transporter SLC27A2 as the gating target of <b>cLG</b> through a systematic transporter screen using a CRISPR activation library. SMPD1 was identified as the target of <b>hLR</b> through a thermal proteome profiling. Therefore, the development of these two highly specific probes offers complementary imaging and provides a unique diagnostic tool for cancer disease, even for fluorescence-guided surgery.</p>","PeriodicalId":10,"journal":{"name":"ACS Central Science","volume":"11 1","pages":"76-83"},"PeriodicalIF":12.7,"publicationDate":"2024-12-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.ncbi.nlm.nih.gov/pmc/articles/PMC11758269/pdf/","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143044841","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Temperature-Dependent Water Oxidation Kinetics: Implications and Insights.","authors":"Tianying Liu, Pan Wang, Wei Li, David Z Wang, Damith D Lekamge, Boqiang Chen, Frances A Houle, Matthias M Waegele, Dunwei Wang","doi":"10.1021/acscentsci.4c01415","DOIUrl":"10.1021/acscentsci.4c01415","url":null,"abstract":"<p><p>As a vital process for solar fuel synthesis, water oxidation remains a challenging reaction to perform using durable and cost-effective systems. Despite decades of intense research, our understanding of the detailed processes involved is still limited, particularly under photochemical conditions. Recent research has shown that the overall kinetics of water oxidation by a molecular dyad depends on the coordination between photocharge generation and the subsequent chemical steps. This work explores similar effects of heterogeneous solar water oxidation systems. By varying a key variable, the reaction temperature, we discovered distinctly different behaviors on two model systems, TiO₂ and Fe₂O₃. TiO₂ exhibited a monotonically increasing water oxidation performance with rising temperature across the entire applied potential range, between 0.1 and 1.5 V vs the reversible hydrogen electrode (RHE). In contrast, Fe₂O₃ showed increased performance with increasing temperature at high applied potentials (>1.2 V vs RHE) but decreased performance at low applied potentials (<1.2 V vs RHE). This decrease in performance with temperature on Fe₂O₃ was attributed to an increased level of electron-hole recombination, as confirmed by intensity-modulated photocurrent spectroscopy (IMPS). The origin of the differing temperature dependences on TiO₂ and Fe₂O₃ was further ascribed to their different surface chemical kinetics. These results highlight the chemical nature of charge recombination in photoelectrochemical (PEC) systems, where surface electrons recombine with holes stored in surface chemical species. They also indicate that PEC kinetics are not constrained by a single rate-determining chemical step, highlighting the importance of an integrated approach to studying such systems. Moreover, the results suggest that for practical solar water splitting devices higher temperatures are not always beneficial for reaction rates, especially under low driving force conditions.</p>","PeriodicalId":10,"journal":{"name":"ACS Central Science","volume":"11 1","pages":"91-97"},"PeriodicalIF":12.7,"publicationDate":"2024-12-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.ncbi.nlm.nih.gov/pmc/articles/PMC11758372/pdf/","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143044861","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Computationally Assisted Noncanonical Amino Acid Incorporation.","authors":"Chengzhu Fang, Wenyuan Xu, Chao Liu, Yulin Chen, Shixian Lin, Wenlong Ding","doi":"10.1021/acscentsci.4c01544","DOIUrl":"10.1021/acscentsci.4c01544","url":null,"abstract":"<p><p>Genetic encoding of noncanonical amino acids (ncAAs) with desired functionalities is an invaluable tool for the study of biological processes and the development of therapeutic drugs. However, existing ncAA incorporation strategies are rather time-consuming and have relatively low success rates. Here, we develop a virtual ncAA screener based on the analysis and modeling of the chemical properties of all reported ncAA substrates to virtually determine the recognition potential of candidate ncAAs. Using this virtual screener, we designed and incorporated several novel Lys and Phe derivatives into proteins for various downstream applications. Among them, the genetic encoding of an electron-rich Phe analog, 3-dimethylamino-phenylalanine, was successfully applied to enhance the cation-π interaction between histone methylation and its reader proteins. Thus, our virtual screener provides a fast and powerful strategy to efficiently incorporate ncAAs with diverse functionalities.</p>","PeriodicalId":10,"journal":{"name":"ACS Central Science","volume":"11 1","pages":"84-90"},"PeriodicalIF":12.7,"publicationDate":"2024-12-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.ncbi.nlm.nih.gov/pmc/articles/PMC11758377/pdf/","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143044842","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Organic Synthesis and Catalysis Enable Facile Access to Bioactive Compounds and Drugs.","authors":"Svetlana B Tsogoeva, Kirk S Schanze","doi":"10.1021/acscentsci.4c02041","DOIUrl":"10.1021/acscentsci.4c02041","url":null,"abstract":"","PeriodicalId":10,"journal":{"name":"ACS Central Science","volume":"11 1","pages":"1-5"},"PeriodicalIF":12.7,"publicationDate":"2024-12-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.ncbi.nlm.nih.gov/pmc/articles/PMC11758363/pdf/","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143044855","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"High-Speed Sequential DNA Computing Using a Solid-State DNA Origami Register.","authors":"Qian Zhang, Mingqiang Li, Yuqing Tang, Jinyan Zhang, Chenyun Sun, Yaya Hao, Jianing Cheng, Xiaodong Xie, Sisi Jia, Hui Lv, Fei Wang, Chunhai Fan","doi":"10.1021/acscentsci.4c01557","DOIUrl":"10.1021/acscentsci.4c01557","url":null,"abstract":"<p><p>DNA computing leverages molecular reactions to achieve diverse information processing functions. Recently developed DNA origami registers, which could be integrated with DNA computing circuits, allow signal transmission between these circuits, enabling DNA circuits to perform complex tasks in a sequential manner, thereby enhancing the programming space and compatibility with various biomolecules of DNA computing. However, these registers support only single-write operations, and the signal transfer involves cumbersome and time-consuming register movements, limiting the speed of sequential computing. Here, we designed a solid-state DNA origami register that compresses output data from a 3D solution to a 2D surface, establishing a rewritable register suitable for solid-state storage. We developed a heterogeneous integration architecture of liquid-state circuits and solid-state registers, reducing the register-mediated signal transfer time between circuits to less than 1 h, thereby achieving fast sequential DNA computing. Furthermore, we designed a trace signal amplifier to read surface-stored signals back into solution. This compact approach not only enhances the speed of sequential DNA computing but also lays the foundation for the visual debugging and automated execution of DNA molecular algorithms.</p>","PeriodicalId":10,"journal":{"name":"ACS Central Science","volume":"10 12","pages":"2285-2293"},"PeriodicalIF":12.7,"publicationDate":"2024-12-11","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.ncbi.nlm.nih.gov/pmc/articles/PMC11672539/pdf/","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142902399","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}