ACS Central Science最新文献_第4页

Enhancing the Optically Detected Magnetic Resonance Signal of Organic Molecular Qubits.

IF 12.7 1区化学

ACS Central Science Pub Date : 2025-01-03 eCollection Date: 2025-01-22 DOI: 10.1021/acscentsci.4c01632

Yong Rui Poh, Joel Yuen-Zhou

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引用次数: 0

Tackling Waste Polystyrene with Sunlight

IF 12.7 1区化学

ACS Central Science Pub Date : 2025-01-02 DOI: 10.1021/acscentsci.4c0218710.1021/acscentsci.4c02187

Hyun Suk Wang, and , Athina Anastasaki*,

引用次数: 0

Enhancing the Optically Detected Magnetic Resonance Signal of Organic Molecular Qubits

IF 12.7 1区化学

ACS Central Science Pub Date : 2025-01-02 DOI: 10.1021/acscentsci.4c0163210.1021/acscentsci.4c01632

Yong Rui Poh*, and , Joel Yuen-Zhou*,

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引用次数: 0

Nickel(II)/Salox-Catalyzed Enantioselective C-H Functionalization. 镍（II）/萨洛催化的对映体选择性 C-H 功能化。

IF 12.7 1区化学

ACS Central Science Pub Date : 2025-01-02 eCollection Date: 2025-01-22 DOI: 10.1021/acscentsci.4c02049

Jia-Hao Chen, Qi-Jun Yao, Ming-Yu Zhong, Tian-Yu Jiang, Fan-Rui Huang, Xiang Li, Bing-Feng Shi

{"title":"Nickel(II)/Salox-Catalyzed Enantioselective C-H Functionalization.","authors":"Jia-Hao Chen, Qi-Jun Yao, Ming-Yu Zhong, Tian-Yu Jiang, Fan-Rui Huang, Xiang Li, Bing-Feng Shi","doi":"10.1021/acscentsci.4c02049","DOIUrl":"10.1021/acscentsci.4c02049","url":null,"abstract":"Recently, nickel catalysts have garnered considerable attention for their efficacy and versatility in asymmetric catalysis, attributed to their distinctive properties. However, the use of cost-effective and sustainable divalent nickel catalysts in C-H activation/asymmetric alkene insertion poses significant challenges due to the intricate control of stereochemistry in the transformation of the tetracoordinate C-Ni(II) intermediate. Herein, we report a Ni(II)-catalyzed enantioselective C-H/N-H annulation with oxabicyclic alkenes. This protocol offers straightforward access to chiral [2,2,1]-bridged bicyclic compounds bearing four consecutive stereocenters with high enantioselectivity (up to 96% ee). The development of a sterically hindered chiral salicyloxazoline (Salox) ligand, TMS-Salox, is key to the success of this protocol. Mechanistic investigations unveiled that a chiral Ni(III)-metalacyclic intermediate was formed through the in situ oxidation of achiral organometallic Ni(II) species and coordination of the Salox ligand. This process led to the creation of a tailored chiral pocket that guides the approach of alkenes, thereby influencing and determining the stereochemistry.","PeriodicalId":10,"journal":{"name":"ACS Central Science","volume":"11 1","pages":"127-135"},"PeriodicalIF":12.7,"publicationDate":"2025-01-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.ncbi.nlm.nih.gov/pmc/articles/PMC11758223/pdf/","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143044851","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}

引用次数: 0

Tackling Waste Polystyrene with Sunlight.

IF 12.7 1区化学

ACS Central Science Pub Date : 2025-01-02 eCollection Date: 2025-01-22 DOI: 10.1021/acscentsci.4c02187

Hyun Suk Wang, Athina Anastasaki

引用次数: 0

Nickel(II)/Salox-Catalyzed Enantioselective C–H Functionalization

IF 12.7 1区化学

ACS Central Science Pub Date : 2025-01-02 DOI: 10.1021/acscentsci.4c0204910.1021/acscentsci.4c02049

Jia-Hao Chen, Qi-Jun Yao, Ming-Yu Zhong, Tian-Yu Jiang, Fan-Rui Huang, Xiang Li and Bing-Feng Shi*,

{"title":"Nickel(II)/Salox-Catalyzed Enantioselective C–H Functionalization","authors":"Jia-Hao Chen, Qi-Jun Yao, Ming-Yu Zhong, Tian-Yu Jiang, Fan-Rui Huang, Xiang Li and Bing-Feng Shi*, ","doi":"10.1021/acscentsci.4c0204910.1021/acscentsci.4c02049","DOIUrl":"https://doi.org/10.1021/acscentsci.4c02049https://doi.org/10.1021/acscentsci.4c02049","url":null,"abstract":"Recently, nickel catalysts have garnered considerable attention for their efficacy and versatility in asymmetric catalysis, attributed to their distinctive properties. However, the use of cost-effective and sustainable divalent nickel catalysts in C–H activation/asymmetric alkene insertion poses significant challenges due to the intricate control of stereochemistry in the transformation of the tetracoordinate C–Ni(II) intermediate. Herein, we report a Ni(II)-catalyzed enantioselective C–H/N–H annulation with oxabicyclic alkenes. This protocol offers straightforward access to chiral [2,2,1]-bridged bicyclic compounds bearing four consecutive stereocenters with high enantioselectivity (up to 96% ee). The development of a sterically hindered chiral salicyloxazoline (Salox) ligand, TMS-Salox, is key to the success of this protocol. Mechanistic investigations unveiled that a chiral Ni(III)-metalacyclic intermediate was formed through the in situ oxidation of achiral organometallic Ni(II) species and coordination of the Salox ligand. This process led to the creation of a tailored chiral pocket that guides the approach of alkenes, thereby influencing and determining the stereochemistry.Ni(II)-catalyzed enantioselective C−H/N−H annulation with oxabicyclic alkenes using a sterically hindered chiral salicyloxazoline (Salox) ligand, TMS-Salox, was reported.","PeriodicalId":10,"journal":{"name":"ACS Central Science","volume":"11 1","pages":"127–135 127–135"},"PeriodicalIF":12.7,"publicationDate":"2025-01-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.acs.org/doi/epdf/10.1021/acscentsci.4c02049","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143089190","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}

引用次数: 0

A Conversation with Alexandra Navrotsky.

IF 12.7 1区化学

ACS Central Science Pub Date : 2024-12-30 eCollection Date: 2025-01-22 DOI: 10.1021/acscentsci.4c02126

Rachel Brazil

引用次数: 0

A Conversation with Alexandra Navrotsky

IF 12.7 1区化学

ACS Central Science Pub Date : 2024-12-30 DOI: 10.1021/acscentsci.4c0212610.1021/acscentsci.4c02126

Rachel Brazil,

引用次数: 0

A Conversation with Tzahi Cath

IF 12.7 1区化学

ACS Central Science Pub Date : 2024-12-30 DOI: 10.1021/acscentsci.4c0214610.1021/acscentsci.4c02146

XiaoZhi Lim,

引用次数: 0

Lipid-Modulated, Graduated Inhibition of N-Glycosylation Pathway Priming Suggests Wide Tolerance of ER Proteostasis to Stress.

IF 12.7 1区化学

ACS Central Science Pub Date : 2024-12-26 eCollection Date: 2025-01-22 DOI: 10.1021/acscentsci.4c01506

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

{"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":"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.","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}

引用次数: 0