Cl ément Camp
Angew Chem Int Ed Engl. 2024 Apr 5:e202404959. doi: 10.1002/anie.202404959. Online ahead of print.ABSTRACT"The most important factor in the choice of my current research topic was the beauty of chemical structures/architectures and X-ray diffraction patterns… I recharge my batteries by scuba diving in the ocean or hiking in the mountains. Or just sleeping one more hour." Find out more about Clément Camp in his Introducing… Profile.PMID:38577832 | DOI:10.1002/anie.202404959 (Source: Angewandte Chemie)
Source: Angewandte Chemie - April 5, 2024 Category: Chemistry Source Type: research
Spontaneous α-C-H Carboxylation of Ketones by Gaseous CO2 at the Air-water Interface of Aqueous Microdroplets
We present a catalyst-free route for the reduction of carbon dioxide integrated with the formation of a carbon-carbon bond at the air/water interface of negatively charged aqueous microdroplets, at ambient temperature. The reactions proceed through carbanion generation at the α-carbon of a ketone followed by nucleophilic addition to CO2. Online mass spectrometry reveals that the product is an α-ketoacid. Several factors, such as the concentration of the reagents, pressure of CO2 gas, and distance traveled by the droplets, control the kinetics of the reaction. Theoretical calculations suggest that water in the microdrople...
Source: Angewandte Chemie - April 5, 2024 Category: Chemistry Authors: Pallab Basuri Sinchan Mukhopadhyay K S S V Prasad Reddy Keerthana Unni B K Spoorthi Jenifer Shantha Kumar Sharma S R K C Yamijala Thalappil Pradeep Source Type: research
A Light-Triggered J-Aggregation-Regulated Therapy Conversion: from Photodynamic/Photothermal Therapy to Long-Lasting Chemodynamic Therapy for Effective Tumor Ablation
Angew Chem Int Ed Engl. 2024 Apr 5:e202404395. doi: 10.1002/anie.202404395. Online ahead of print.ABSTRACTReactive oxygen species (ROS) have become an effective tool for tumor treatment. The combination of photodynamic therapy (PDT) and chemodynamic therapy (CDT) takes advantage of various ROS and enhances therapeutic effects. However, the activation of CDT usually occurs before PDT, which hinders the sustained maintenance of hydroxyl radicals (•OH) and reduces the treatment efficiency. Herein, we present a light-triggered nano-system based on molecular aggregation regulation for converting cancer therapy from PDT/photot...
Source: Angewandte Chemie - April 5, 2024 Category: Chemistry Authors: Kai Wei Yanxin Wu Xian Zheng Li Ouyang Guiping Ma Chendong Ji Meizhen Yin Source Type: research
Catalytic Access to Diastereometrically Pure Four- and Five-Membered Silyl-Heterocycles Using Transborylation
Angew Chem Int Ed Engl. 2024 Apr 5:e202401737. doi: 10.1002/anie.202401737. Online ahead of print.ABSTRACTSilyl-heterocycles offer a unique handle to expand and explore chemical space, reactivity, and functionality. The shortage of catalytic methods for the preparation of diverse and functionalized silyl-heterocycles however limits widespread exploration and exploitation. Herein the borane-catalyzed intramolecular 1,1-carboboration of silyl-alkynes has been developed for the synthesis of 2,3-dihydrosilolyl and silylcyclobut-2-enyl boronic esters. Successful, catalytic carboboration has been achieved on a variety of functio...
Source: Angewandte Chemie - April 5, 2024 Category: Chemistry Authors: Dominic R Willcox Emanuele Cocco Gary S Nichol Stephen Thomas Source Type: research
Beyond Tertiary Amines: Introducing Secondary Amines via Palladium/Norbornene-Catalyzed Ortho Amination
Angew Chem Int Ed Engl. 2024 Apr 5:e202404042. doi: 10.1002/anie.202404042. Online ahead of print.ABSTRACTSince the discovery of the palladium/norbornene (Pd/NBE)-catalyzed ortho amination in 2013, escaping the limitation of only yielding tertiary anilines has been a long-standing challenge in the past decade. Here, we describe that, by carefully choosing the phosphine ligand and NBE mediator, installation of a N-mono-alkylamino group becomes feasible. The reaction tolerates a wide range of aryl iodide substrates and various N-mono-tertiary alkylamine-derived electrophiles. Both ipso alkenylation and alkynylation can be re...
Source: Angewandte Chemie - April 5, 2024 Category: Chemistry Authors: Xin Liu Qi Zhu Guangbin Dong Source Type: research
Magnetic Silica-Coated Fluorescent Microspheres (MagSiGlow) for Simultaneous Detection of Tumor-Associated Proteins
In this study, we introduce a straightforward protocol to adapt a multiplexed single-bead assay to standard fluorescence imaging plates, enabling the simultaneous analysis of thousands of reactions per plate. Our approach focuses on the design and synthesis of bright fluorescent and magnetic microspheres (MagSiGlow) with multiple fluorescent wavelengths serving as detection markers. This imaging-based single-bead assay, combined with a scripted algorithm, allows the detection, segmentation, and co-localization on average of 7500 microspheres per field of view across five imaging channels in less than one second. We demonst...
Source: Angewandte Chemie - April 5, 2024 Category: Chemistry Authors: Elias A Halabi Isabel Gessner Katherine Yang Jae-Jun Kim Rupsa Jana Hannah M Peterson Joshua Spitzberg Ralph Weissleder Source Type: research
Layer-Controllable "2.5D" DNA Origami Crystals Synthesized by a Hierarchical Assembly Strategy
Angew Chem Int Ed Engl. 2024 Apr 5:e202402312. doi: 10.1002/anie.202402312. Online ahead of print.ABSTRACTThe finite periodic arrangement of functional nanomaterials on the two-dimensional scale enables the integration and enhancement of individual properties, making them an important research topic in the field of tuneable nanodevices. Although layer-controllable lattices such as graphene have been successfully synthesized, achieving similar control over colloidal nanoparticles remains a challenge. DNA origami technology has achieved remarkable breakthroughs in programmed nanoparticle assembly. Based on this technology, w...
Source: Angewandte Chemie - April 5, 2024 Category: Chemistry Authors: Xiaolin Xie Min Ji Xuehui Yan Yifan Yu Yong Wang Ningning Ma Hang Xing Ye Tian Source Type: research
Germaaluminocenes - Masked Heterofulvenes
Angew Chem Int Ed Engl. 2024 Apr 5:e202403652. doi: 10.1002/anie.202403652. Online ahead of print.ABSTRACTGermaaluminocenes are formed by salt metathesis reactions of dipotassium germacyclopentadienediides with cyclopentadienylaluminum dichloride. The reactivity pattern of these sandwich complexes is determined by the electrophilic central aluminum atom and by the nucleophilic dicoordinated germanium center. Surprisingly, the products formed by reactions with Lewis acids, Lewis bases, amphiphiles and compounds with polar double bonds are those expected from the reaction of a hypothetical aluminagermapentafulvene with these...
Source: Angewandte Chemie - April 5, 2024 Category: Chemistry Authors: Nadeschda Geibel Lukas B ührmann Lena Albers Marc Schmidtmann Alexander Weiz Thomas M üller Source Type: research
Light Induced Proton Coupled Charge Transfer Triggers Counterion Directional Translocation
Angew Chem Int Ed Engl. 2024 Apr 5:e202403317. doi: 10.1002/anie.202403317. Online ahead of print.ABSTRACTWe demonstrate directed translocation of ClO4- anions from cationic to neutral binding site along the synthetized BPym-OH dye molecule that exhibits coupled excited-state intramolecular proton-transfer (ESIPT) and charge-transfer (CT) reaction (PCCT). The results of steady-state and time-resolved spectroscopy together with computer simulation and modeling show that in low polar toluene the excited-state redistribution of electronic charge enhanced by ESIPT generates the driving force, which is much stronger than by CT ...
Source: Angewandte Chemie - April 5, 2024 Category: Chemistry Authors: Kai-Hsin Chang Yu-Hsuan Yang Kuan-Hsuan Su Yi Chen Ta-Chun Lin Jian-Liang Li Zong-Ying Liu Jing-Han Shi Tzu-Fang Wang Yi-Tyng Chang Alexander P Demchenko Hsiao-Ching Yang Pi-Tai Chou Source Type: research
Finding Natural, Dense, and Stable Frustrated Lewis Pairs on Wurtzite Crystal Surfaces for Small-Molecule Activation
Angew Chem Int Ed Engl. 2024 Apr 5:e202405405. doi: 10.1002/anie.202405405. Online ahead of print.ABSTRACTThe surface frustrated Lewis pairs (SFLPs) open up new opportunities for substituting noble metals in the activation and conversion of stable molecules. However, the applications of SFLPs on a larger scale are impeded by the complex construction process, low surface density, and sensitivity to the reaction environment. Herein, wurtzite-structured crystals such as GaN, ZnO, and AlP are found for developing natural, dense, and stable SFLPs. It is revealed that the SFLPs can naturally exist on the (100) and (110) surfaces...
Source: Angewandte Chemie - April 5, 2024 Category: Chemistry Authors: Xi-Yang Yu Zheng-Qing Huang Tao Ban Yun-Hua Xu Zhong-Wen Liu Chun-Ran Chang Source Type: research
An Expanded Palette of Fluorescent COS/H2S-Releasing Donors for H2S Delivery, Detection, and In Vivo Application
Angew Chem Int Ed Engl. 2024 Apr 5:e202402353. doi: 10.1002/anie.202402353. Online ahead of print.ABSTRACTHydrogen sulfide (H2S) is an important reactive sulfur species that is involved in many biological functions, and H2S imbalances have been indicated as a potential biomarker for various diseases. Different H2S donors have been developed to deliver H2S directly to biological systems, but few reports include donors with optical responses that allow for tracking of H2S release. Moreover, donor systems that use the same chemistry to deliver H2S across a palette of fluorescent responses remain lacking. Here we report five t...
Source: Angewandte Chemie - April 5, 2024 Category: Chemistry Authors: Kaylin G Fosnacht Jonathan Dorogin Payton M Jefferis Marian H Hettiaratchi Michael Dwight Pluth Source Type: research
Implanting colloidal nanoparticles into single-crystalline zeolites for Catalytic Dehydration
In this study, we demonstrate the fabrication of a core-shell structured single-crystal zeolite encompassing an Fe3O4 colloidal core via a novel confinementstepwise crystallization methodology. By engineering a confined nanocavity, anchoring nucleation sites, and executing stepwise crystallization, we have successfully encapsulated colloidal nanoparticles (CN) within single-crystal zeolites. These grafted sites, alongside the controlled crystallization process, compel the zeolite seed to nucleate and expand along the Fe3O4 colloidal nanoparticle surface, within a meticulously defined volume (1.5 × 107 ≤ V ≤ 1.3 × 108...
Source: Angewandte Chemie - April 5, 2024 Category: Chemistry Authors: Bing Ma Linlin Duan Yuzhu Ma Fanxing Bu Kun Lan Tiancong Zhao Liang Chen Lianhai Zu Liang Peng Zaiwang Zhao Jun Xu Siqing Zhong Dhaifallah M Aldhayan Abdullah M Al-Enizi Ahmed Elzatahry Wei Li Weimin Yang Dongyuan Zhao Source Type: research
Nanogels with Metal-Organic Cages as Functional Crosslinks
Angew Chem Int Ed Engl. 2024 Apr 5:e202403834. doi: 10.1002/anie.202403834. Online ahead of print.ABSTRACTA dinuclear metal-organic cage with four acrylate side chains was prepared by self-assembly. Precipitation polymerization of the cage with N‑isopropylacrylamide yielded a thermoresponsive nanogel. The host properties of the cage were retained within the gel matrix, endowing the nanogel with the capability to serve as a sorbent for chloride ions in water. Moreover, a heteroleptic cage with the drug abiraterone as co-ligand was integrated into a nanogel. The addition of chloride ions induced a structural rearrangement ...
Source: Angewandte Chemie - April 5, 2024 Category: Chemistry Authors: Chaolei Hu Kay Severin Source Type: research
Zinc-ion Anchor Induced Highly Reversible Zn Anodes for High Performance Zn-ion Batteries
Angew Chem Int Ed Engl. 2024 Apr 5:e202403050. doi: 10.1002/anie.202403050. Online ahead of print.ABSTRACTUnstable Zn interface with serious detrimental parasitic side-reactions and uncontrollable Zn dendrites severely plagues the practical application of aqueous zinc-ion batteries. The interface stability was closely related to the electrolyte configuration and Zn2+ depositional behavior. In this work, a unique Zn-ion anchoring strategy is originally proposed to manipulate the coordination structure of solvated Zn-ions and guide the Zn-ion depositional behavior. Specifically, the amphoteric charged ion additives (denoted ...
Source: Angewandte Chemie - April 5, 2024 Category: Chemistry Authors: Shuang Zhou Xinyu Meng Yining Chen Jianwen Li Shangyong Lin Chao Han Xiaobo Ji Zhi Chang Anqiang Pan Source Type: research
Bayesian Inference for Model Analyses of Supramolecular Complexes: A Case Study with Nanocarbon Hosts
Angew Chem Int Ed Engl. 2024 Apr 5:e202405388. doi: 10.1002/anie.202405388. Online ahead of print.ABSTRACTA 126π-electron nanobowl molecule, phenine tridehydrosumanene, was synthesized in 12 steps through the development of a polygon cyclization strategy that assembled the polygonal precursors via Ni-mediated macrocyclization. The bowl-shaped structure accommodated C70 as a guest at the concave site, and the ball-in-bowl structure was determined by X-ray crystallography. The host-guest equilibrium in solution was studied with titration experiments using isothermal calorimetry, which provided an interesting test case for s...
Source: Angewandte Chemie - April 5, 2024 Category: Chemistry Authors: Yuzuka Onaka Renki Sakai Toshiya M Fukunaga Koki Ikemoto Hiroyuki Isobe Source Type: research
