Chemical Science最新文献_第8页

Correction: An innovative chalcogenide transfer agent for improved aqueous quantum dot synthesis

IF 8.4 1区化学

Chemical Science Pub Date : 2024-12-06 DOI: 10.1039/d4sc90237h

Guillaume Petit, Cedric Malherbe, Pauline Bianchi, Jean-Christophe M. Monbaliu

引用次数: 0

Tetrapodal iron complexes invoke observable intermediates in nitrate and nitrite reduction

IF 8.4 1区化学

Chemical Science Pub Date : 2024-12-06 DOI: 10.1039/d4sc06570k

Jewelianna M. Moore, Alison R. Fout

{"title":"Tetrapodal iron complexes invoke observable intermediates in nitrate and nitrite reduction","authors":"Jewelianna M. Moore, Alison R. Fout","doi":"10.1039/d4sc06570k","DOIUrl":"https://doi.org/10.1039/d4sc06570k","url":null,"abstract":"This study investigates the mechanistic pathways of nitrate and nitrite reduction by the tetrapodal iron complex [Py2Py(afamcyp)2Fe]OTf2, revealing key intermediates to elucidate the reaction process. Using UV-Vis, IR, mass and NMR spectroscopies, stable binding of oxyanions to the iron centre was observed, supporting the formation of the iron(III)–hydroxide intermediate [Py2Py(afamcyp)2Fe(OH)]OTf2. This intermediate is less stable than in previous systems, providing insights into the behaviour of metalloenzymes. A bimetallic mechanism is proposed for nitrogen oxyanion reduction where additional iron is required to drive the complete reaction, resulting in the formation of the final nitrosyl complex, Py2Py(pimcyp)2Fe(NO), and water. Our findings enhance the understanding of iron-based reduction processes and contribute to the broader knowledge of oxyanion reduction mechanisms.","PeriodicalId":9909,"journal":{"name":"Chemical Science","volume":"8 1","pages":""},"PeriodicalIF":8.4,"publicationDate":"2024-12-06","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142782948","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

Reacon: a template- and cluster-based framework for reaction condition prediction

IF 8.4 1区化学

Chemical Science Pub Date : 2024-12-06 DOI: 10.1039/d4sc05946h

Zihan Wang, Kangjie Lin, Jianfeng Pei, Luhua Lai

引用次数: 0

Reversing Selectivity of Bambusuril Macrocycles toward Inorganic Anions by Installing Spacious Substituents on Their Portals

IF 8.4 1区化学

Chemical Science Pub Date : 2024-12-06 DOI: 10.1039/d4sc07150f

Carola Rando, Surbhi Grewal, Jan Sokolov, Petr Kulhanek, Vladimir Sindelar

引用次数: 0

Efficient Encapsulation of Insulin by Giant Macrocycle as a Powerful Approach to the Inhibition of Its Fibrillation

IF 8.4 1区化学

Chemical Science Pub Date : 2024-12-06 DOI: 10.1039/d4sc06859a

Ruotong Wang, Zihan Fang, Shenghui Li, Ziliang Zhang, Ming Dong, JunYi Chen, Qingbin Meng, Chunju Li

{"title":"Efficient Encapsulation of Insulin by Giant Macrocycle as a Powerful Approach to the Inhibition of Its Fibrillation","authors":"Ruotong Wang, Zihan Fang, Shenghui Li, Ziliang Zhang, Ming Dong, JunYi Chen, Qingbin Meng, Chunju Li","doi":"10.1039/d4sc06859a","DOIUrl":"https://doi.org/10.1039/d4sc06859a","url":null,"abstract":"Diabetes is a lifelong metabolic disease that requires frequent subcutaneous injections of insulin. However, free insulin is prone to the formation of immunogenic fibrillar aggregates in physiologic conditions which puzzles its biomedical applications. Here an inhibition approach for insulin fibrils was developed through entire encapsulation by a giant macrocyclic inhibitor agent. Negatively charged water-soluble Pentaphen[3]arene sulfate (PP[3]AS), bearing 15 benzenes on its skeleton, was designed and synthesized. In vitro and in vivo safety tests preliminary demonstrated that PP[3]AS had excellent biocompatibility. PP[3]AS could not only effectively inhibit the formation of amyloid, but also disaggregate intractable mature insulin fibrils. This macrocyclic inhibitor exhibited effective host-guest complexation toward insulin at C-terminal 11-mer peptide sequence of B chain with association constants of (5.69 ± 0.50) × 106 M-1. Such complexation behavior was distinctive to traditional macrocycles, which could only recognize the amino acid residues from the side due to their limited cavity sizes. Control experiments also proved that smaller cucurbit[7]uril and carboxylatopillar[5]arene could not prevent insulin from fibrillation under the same test conditions. Notably, co-administrated with equimolar PP[3]AS could keep normoglycemic for at least 300 min in streptozotocin-induced diabetic model mice, whereas mice received free insulin became hyperglycemic again within ~150 min","PeriodicalId":9909,"journal":{"name":"Chemical Science","volume":"199 1","pages":""},"PeriodicalIF":8.4,"publicationDate":"2024-12-06","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142783021","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

Electronic regulation of single-atomic Ti sites on metal hydroxide for boosting photocatalytic CO₂ reduction. 金属氢氧化物上单原子 Ti 位点的电子调控，促进光催化二氧化碳还原。

IF 7.6 1区化学

Chemical Science Pub Date : 2024-12-05 DOI: 10.1039/d4sc07257j

Ning-Yu Huang, Bai Li, Duojie Wu, Di Chen, Yu-Tao Zheng, Bing Shao, Wenjuan Wang, Meng Gu, Lei Li, Qiang Xu

{"title":"Electronic regulation of single-atomic Ti sites on metal hydroxide for boosting photocatalytic CO2 reduction.","authors":"Ning-Yu Huang, Bai Li, Duojie Wu, Di Chen, Yu-Tao Zheng, Bing Shao, Wenjuan Wang, Meng Gu, Lei Li, Qiang Xu","doi":"10.1039/d4sc07257j","DOIUrl":"https://doi.org/10.1039/d4sc07257j","url":null,"abstract":"Photocatalytic CO2 reduction is considered a sustainable method to address energy and environmental issues by converting CO2 into fuels and chemicals, yet the performance is still unsatisfactory. Single atom catalysts hold promising potential in photocatalysis, but the selection of metal species is still limited, especially in early transition metals. Herein, inspired by the structure of anatase TiO2, single Ti sites were successfully incorporated into a metal hydroxide support for the first time via cationic defects, significantly enhancing the photocatalytic performance by more than 30 times (from 0.26 to 8.09 mmol g-1 h-1). Based on the theoretical calculation and in situ characterization, the enhancement of photocatalytic performance can be attributed to the regulation of the electronic structure by the introduction of atomically dispersed Ti sites, leading to stronger binding with intermediates and enhanced charge transfer.","PeriodicalId":9909,"journal":{"name":"Chemical Science","volume":" ","pages":""},"PeriodicalIF":7.6,"publicationDate":"2024-12-05","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.ncbi.nlm.nih.gov/pmc/articles/PMC11638847/pdf/","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142827395","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 fluorobenzene-bound dysprosium half-sandwich dication single-molecule magnet.

IF 7.6 1区化学

Chemical Science Pub Date : 2024-12-04 DOI: 10.1039/d4sc06661h

Sophie C Corner, William J A Blackmore, Gemma K Gransbury, Andrea Mattioni, George F S Whitehead, Nicholas F Chilton, David P Mills

{"title":"A fluorobenzene-bound dysprosium half-sandwich dication single-molecule magnet.","authors":"Sophie C Corner, William J A Blackmore, Gemma K Gransbury, Andrea Mattioni, George F S Whitehead, Nicholas F Chilton, David P Mills","doi":"10.1039/d4sc06661h","DOIUrl":"10.1039/d4sc06661h","url":null,"abstract":"Dysprosium single-molecule magnets (SMMs) with two mutually trans-anionic ligands have shown large crystal field (CF) splitting, giving record effective energy barriers to magnetic reversal (U eff) and hysteresis temperatures (T H). However, these complexes tend to be bent, imposing a transverse field that reduces the purity of the m J projections of the CF states and promotes magnetic relaxation. A complex with only one charge-dense anionic ligand could have more pure CF states, and thus high U eff and T H. Here we report an SMM with this topology, a half-sandwich Dy(iii) complex [Dy(Cp*)(FPh)6][{Al[OC(CF3)3]3}2(μ-F)]2 (1-Dy; Cp* = C5Me5), and its Y(iii) analogue 1-Y; 1-Dy exhibits U eff = 545(30) cm-1 and T H = 14 K at sweep rates of 22 Oe s-1. The Cp* ligand imposes a strong axial CF, which is assisted by one axial fluorobenzene; the five equatorially-bound neutral fluorobenzenes present only weak transverse interactions to give a pseudo-pentagonal bipyramidal geometry. The salt metathesis reaction of 1-Y with KCp''' (Cp''' = {C5H2(SiMe3)3-1,2,4}) gave the sandwich complex [Y(Cp''')(Cp*)(FPh)2][{Al[OC(CF3)3]3}2(μ-F)] (4-Y), showing that the fluorobenzenes of 1-Y are easily displaced. We envisage that these methodologies could be adapted in future to prepare high-performance axial Dy SMMs with ligands that are more sterically demanding than Cp*.","PeriodicalId":9909,"journal":{"name":"Chemical Science","volume":" ","pages":""},"PeriodicalIF":7.6,"publicationDate":"2024-12-04","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.ncbi.nlm.nih.gov/pmc/articles/PMC11616726/pdf/","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142784230","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

Correction: Perylene-derivative singlet exciton fission in water solution

IF 7.6 1区化学

Chemical Science Pub Date : 2024-12-04 DOI: 10.1039/D4SC90232G

Chloe Magne, Simona Streckaite, Roberto A. Boto, Eduardo Domínguez-Ojeda, Marina Gromova, Andrea Echeverri, Flavio Siro Brigiano, Minh-Huong Ha-Thi, Marius Franckevičius, Vidmantas Jašinskas, Annamaria Quaranta, Andrew A. Pascal, Matthieu Koepf, David Casanova, Thomas Pino, Bruno Robert, Julia Contreras-García, Daniel Finkelstein-Shapiro, Vidmantas Gulbinas and Manuel J. Llansola-Portoles

引用次数: 0

Design of an abiotic unimolecular three-helix bundle

IF 8.4 1区化学

Chemical Science Pub Date : 2024-12-04 DOI: 10.1039/d4sc07336c

Shuhe Wang, Johannes Sigl, Lars Allmendinger, Victor Maurizot, Ivan Huc

引用次数: 0

Acid-responsive singlet oxygen nanodepots.

IF 7.6 1区化学

Chemical Science Pub Date : 2024-12-04 DOI: 10.1039/d4sc06553k

Zengwei Ran, Maolin Wang, Zhu Yuan, Yan Zhang, Guhuan Liu, Ronghua Yang

{"title":"Acid-responsive singlet oxygen nanodepots.","authors":"Zengwei Ran, Maolin Wang, Zhu Yuan, Yan Zhang, Guhuan Liu, Ronghua Yang","doi":"10.1039/d4sc06553k","DOIUrl":"10.1039/d4sc06553k","url":null,"abstract":"The singlet oxygen carrier addresses the challenges of traditional photodynamic therapy (PDT), which relies on the presence of oxygen within solid tumors and struggles with light penetration issues. However, the inability to control the release of singlet oxygen has hindered precise treatment applications. Here, we introduce an acid-responsive singlet oxygen nanodepot (aSOND) designed to overcome this limitation. The aSOND is synthesized using a responsive diblock copolymer system that includes a hydrophilic PEG block and a pH-responsive block with singlet oxygen loading sites. In neutral or alkaline environments, the aSOND releases singlet oxygen slowly, ensuring stability in blood circulation. In contrast, in acidic environments such as the tumor microenvironment or intracellular lysosomes, protonation of the tertiary amine group within the pH responsive block increases the hydration of the polymer, triggering a rapid release of singlet oxygen. This feature enables controlled, tumor-specific release of reactive oxygen species (ROS). The aSOND system effectively implements an \"OFF-ON\" singlet oxygen therapy, demonstrating high spatiotemporal selectivity and independence from both oxygen supply and external light, offering a promising approach for targeted cancer therapy.","PeriodicalId":9909,"journal":{"name":"Chemical Science","volume":" ","pages":""},"PeriodicalIF":7.6,"publicationDate":"2024-12-04","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.ncbi.nlm.nih.gov/pmc/articles/PMC11633660/pdf/","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142817416","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