Bottom-up Growth of Convex Sphere with Adjustable Cu(0)/Cu(I) Interfaces for Effective C2 Production from CO2 Electroreduction
In this study, we for the first time introduce a bottom-up growth of convex sphere with adjustable Cu(0)/Cu(I) interfaces (Cux@Cu2O convex spheres). Interestingly, the interfaces are dynamically modulated by varying hydrothermal time, thus regulating the conversion of C1 and C2 products. In particular, the 4 h hydrothermal treatment applied to Cu0.25@Cu2O convex sphere with the favorable Cu(0)/Cu(I) interface results in the highest selectivity for C2 products (90.5%). In situ Fourier-transform infrared spectroscopy measurements and density functional theory calculations reveal that the Cu(0)/Cu(I) interface lowers the ener...
Source: Angewandte Chemie - May 4, 2024 Category: Chemistry Authors: Huan Liu Chenghan Yang Tong Bian Huijun Yu Yuming Zhou Yiwei Zhang Source Type: research
Gas-Phase Formation of Sulfurous Acid (H2SO3) in the Atmosphere
Angew Chem Int Ed Engl. 2024 May 4:e202405572. doi: 10.1002/anie.202405572. Online ahead of print.ABSTRACTSulfurous acid (H2SO3) is known to be thermodynamically instable decomposing into SO2 and H2O. All attempts to detect this elusive acid in solution failed up to now. Reported H2SO3 formation from an experiment carried out in a mass spectrometer as well as results from theoretical calculations, however, indicated a possible kinetic stability in the gas phase. Here, it is shown experimentally that H2SO3 is formed in the OH radical-initiated gas-phase oxidation of methanesulfinic acid (CH3S(O)OH) at 295 ± 0.5 K and 1 bar...
Source: Angewandte Chemie - May 4, 2024 Category: Chemistry Authors: Torsten Berndt Erik H Hoffmann Andreas Tilgner Hartmut Herrmann Source Type: research
Reconstructing Solvation Structure by Steric Hindrance-Coordination Push-Pull of Dipolymer-H2O-Zn2+ toward Long-life Aqueous Zinc-Metal Batteries
Angew Chem Int Ed Engl. 2024 May 4:e202401163. doi: 10.1002/anie.202401163. Online ahead of print.ABSTRACTAqueous zinc-metal batteries are prospective energy storge devices due to their intrinsically high safety and cost effectiveness. Yet, uneven deposition of zinc ions in electrochemical reduction and side reactions at the anode interface significantly hinder their development and application. Here, we propose a solvation-interface attenuation strategy enabled by a frustrated tertiary amine amphiphilic dipolymer electrolyte additive. The configuration of superhydrophilic segments with covalently bonded lipophilic spacers...
Source: Angewandte Chemie - May 4, 2024 Category: Chemistry Authors: Die Luo Xinyu Ma Pan Du Zuo Chen Qiurui Lin Yuhan Liu Ben Niu Xianru He Xin Wang Source Type: research
Intrarenal pH-Responsive Self-Assembly of Luminescent Gold Nanoparticles for Diagnosis of Early Kidney Injury
Angew Chem Int Ed Engl. 2024 May 4:e202406016. doi: 10.1002/anie.202406016. Online ahead of print.ABSTRACTMetabolic acidosis-induced kidney injury (MAKI) is asymptomatic and lack of clinical biomarkers in early stage, but rapidly progresses to severe renal fibrosis and ultimately results in end-stage kidney failure. Therefore, developing rapid and noninvasive strategies direct responsive to renal tubular acidic microenvironment rather than delayed biomarkers are essential for timely renoprotective interventions. Herein, we develop pH-responsive luminescent gold nanoparticles (p-AuNPs) in the second near-infrared emission c...
Source: Angewandte Chemie - May 4, 2024 Category: Chemistry Authors: Zhipeng Zhao Kui He Ben Liu Wenyan Nie Xiaoxi Luo Jinbin Liu Source Type: research
Organocatalytic Enantioselective 1,12-Addition of Alkynyl Biphenyl Quinone Methides Formed In Situ
Angew Chem Int Ed Engl. 2024 May 2:e202400143. doi: 10.1002/anie.202400143. Online ahead of print.ABSTRACTThe chemistry of quinone methides formed in situ has been flourishing in recent years. In sharp contrast, the development and utilization of biphenyl quinone methides are rare. Herein, we achieved a remote stereocontrolled 1,12-conjugate addition of biphenyl quinone methides formed in situ for the first time. In the presence of a suitable chiral phosphoric acid, alkynyl biphenyl quinone methides were generated from α-[4-(4-hydroxyphenyl)phenyl]propargyl alcohols, followed by enantioselective 1,12-conjugate addition wi...
Source: Angewandte Chemie - May 3, 2024 Category: Chemistry Authors: Xing Wang Boming Shen Meiwen Liu Ziyang Wang Chang Liu Pengfei Li Peiyuan Yu Wenjun Li Source Type: research
Switchable Dual Circularly Polarized Luminescence in Through-Space Conjugated Chiral Foldamers
Angew Chem Int Ed Engl. 2024 May 2:e202407605. doi: 10.1002/anie.202407605. Online ahead of print.ABSTRACTOrganic materials with switchable dual circularly polarized luminescence (CPL) are highly desired because they can not only directly radiate tunable circularly polarized light themselves but also induce CPL for guests by providing chiral environment in self-assembled structures or serving as the hosts for energy transfer systems. However, most organic molecules only exhibit single CPL and it remains challenging to develop organic molecules with dual CPL. Herein, novel through-space conjugated chiral foldamers are const...
Source: Angewandte Chemie - May 3, 2024 Category: Chemistry Authors: Pingchuan Shen Shaoshao Jiao Zeyan Zhuang Xiaobing Dong Shaoxin Song Jinshi Li Ben Zhong Tang Zujin Zhao Source Type: research
Formation of a Porous Crystalline Mg1 ‒ x Al2O y Overlayer on Metal Catalysts via Controlled Solid-State Reactions for High-temperature Stable Catalysis
Angew Chem Int Ed Engl. 2024 May 3:e202404398. doi: 10.1002/anie.202404398. Online ahead of print.ABSTRACTCatalyst deactivation by sintering and coking is a long-standing issue in metal-catalyzed harsh high-temperature hydrocarbon reactions. Ultrathin oxide coatings of metal nanocatalysts have recently appeared attractive to address this issue, while the porosity of the overlayer is difficult to control to preserve the accessibility of embedded metal nanoparticles, thus often leading to a large decrease in activity. Here, we report that a nanometer-thick alumina coating of MgAl2O4-supported metal catalysts followed by high...
Source: Angewandte Chemie - May 3, 2024 Category: Chemistry Authors: Lihua Cai Shanlei Han Wenlong Xu Si Chen Xianxian Shi Junling Lu Source Type: research
ß-Phenethylamine Synthesis via Latent Dual Electrophilicity of N-Pyridinium Aziridines
Angew Chem Int Ed Engl. 2024 May 3:e202406335. doi: 10.1002/anie.202406335. Online ahead of print.ABSTRACTß-Phenethylamines are widely represented in biologically and pharmacologically active organic small molecules. Here, we introduce N-pyridinium aziridines as latent dual electrophiles for the synthesis of ß-phenethylamines. Bromide-promoted ring opening generates ß-halopyridinium amines. Selective Ni-catalyzed C-C cross-coupling between organozinc nucleophiles and the benzylic C-Br electrophile affords a diverse family of ß-functionalized phenethylaminopyridinium salts, and coupling is stereoconvergent in the presen...
Source: Angewandte Chemie - May 3, 2024 Category: Chemistry Authors: Samya Samanta Promita Biswas Braeden O'Bannon David C Powers Source Type: research
A Stretchable and Tough Graphene Film Enabled by Mechanical Bond
Angew Chem Int Ed Engl. 2024 May 3:e202404481. doi: 10.1002/anie.202404481. Online ahead of print.ABSTRACTThe pursuit of fabricating high-performance graphene films has aroused considerable attention due to their potential for practical applications. However, developing both stretchable and tough graphene films remains a formidable challenge. To address this issue, we herein introduce mechanical bond to comprehensively improve the mechanical properties of graphene films, utilizing [2]rotaxane as the bridging unit. Under external force, the [2]rotaxane cross-link undergoes intramolecular motion, releasing hidden chain and i...
Source: Angewandte Chemie - May 3, 2024 Category: Chemistry Authors: Chunyu Wang Boyue Gao Fuyi Fang Wenhao Qi Ge Yan Jun Zhao Wenbin Wang Ruixue Bai Zhaoming Zhang Zhitao Zhang Wenming Zhang Xuzhou Yan Source Type: research
A Gold(I)-Acetylene Complex Synthesised using Single-Crystal Reactivity
Angew Chem Int Ed Engl. 2024 May 3:e202404264. doi: 10.1002/anie.202404264. Online ahead of print.ABSTRACTUsing single-crystal to single-crystal solid/gas reactivity the gold(I) acetylene complex [Au(L1)(η2-HC≡CH)][BArF4] is cleanly synthesized by addition of acetylene gas to single crystals of [Au(L1)(CO)][BArF4] [L1 = tris-2-(4,4'-di-tert-butylbiphenyl)phosphine, ArF = 3,5-(CF3)2C6H3]. This simplest gold-alkyne complex has been characterized by single crystal X-ray diffraction, solution and solid-state NMR spectroscopy and periodic DFT. Bonding of HC≡CH with [Au(L1)]+ comprises both σ-donation and π-backdonation w...
Source: Angewandte Chemie - May 3, 2024 Category: Chemistry Authors: Chloe L Johnson Daniel J Storm Muhammad Arif Sajjad Matthew R Gyton Simon B Duckett Stuart A Macgregor Andrew S Weller Miquel Navarro Jesus Campos Source Type: research
Controlling On-Surface Photoactivity: The Impact of π-Conjugation in Anhydride-Functionalized Molecules on a Semiconductor Surface
Angew Chem Int Ed Engl. 2024 May 3:e202405983. doi: 10.1002/anie.202405983. Online ahead of print.ABSTRACTOn-surface synthesis has become a prominent method for growing low-dimensional carbon-based nanomaterials on metal surfaces. However, the necessity of decoupling organic nanostructures from metal substrates to exploit their properties requires either transfer methods or new strategies to perform reactions directly on inert surfaces. The use of on-surface light-induced reactions directly on semiconductor/insulating surfaces represents an alternative approach to address these challenges. Here, exploring the photochemical...
Source: Angewandte Chemie - May 3, 2024 Category: Chemistry Authors: Federico Frezza Ana S ánchez-Grande Sofia Canola Anna Lamancov á Pingo Mutombo Qifan Chen Christian W äckerlin Karl-Heinz Ernst Matthias Muntwiler Nicola Zema Marco Di Giovannantonio Dana Nachtigallov á Pavel Jel ínek Source Type: research
Active Oxygenated Structure-Intensified CO2 Capture Enables Efficient Electrochemical Ethylene Production Over Carbon Nanofibers
Angew Chem Int Ed Engl. 2024 May 3:e202401707. doi: 10.1002/anie.202401707. Online ahead of print.ABSTRACTThe pursuit of high efficacy C-C coupling during the electrochemical CO2 reduction reaction remains a tremendous challenge owing to the high energy barrier of CO2 activation and insufficient coverage of the desired intermediates on catalytic sites. Inspired by the concept of capture-coupled CO2 activation, we fabricated quinone-grafted carbon nanofibers via an in situ oxidative carbonylation strategy. The quinone functionality of carbon nanofibers promotes the capture of CO2 followed by activation. At a current density...
Source: Angewandte Chemie - May 3, 2024 Category: Chemistry Authors: Tingting Zhang Jun Wang Huishan Shang Bing Zhang Yanqiang Huang Jing He Xu Xiang Source Type: research
Eosinophil-activating Semiconducting Polymer Nanoparticles for Cancer Photo-immunotherapy
Angew Chem Int Ed Engl. 2024 May 3:e202405358. doi: 10.1002/anie.202405358. Online ahead of print.ABSTRACTEosinophils are important immune effector cells that affect T cell-mediated antitumor immunity. However, the low frequency and restrained activity of eosinophils restricted the development of cancer immunotherapies. We herein report an eosinophil-activating semiconducting polymer nanoparticle (SPNe) to improve photodynamic tumor immunogenicity, modulate eosinophil chemotaxis, and reinvigorate T-cell immunity for activated cancer photo-immunotherapy. SPNe is composed of an amphiphilic semiconducting polymer and a dipept...
Source: Angewandte Chemie - May 3, 2024 Category: Chemistry Authors: Chi Zhang Jingsheng Huang Mengke Xu Jie Yu Wei Xin Shasha He Kanyi Pu Source Type: research
Fluorinated Surface Engineering towards High-rate and Durable Potassium-ion Battery
We report an ultra-thin and KF-enriched SEI triggered by tuned fluorinated surface design in electrode. Our results reveal that fluorination engineering alters the interfacial chemical environment to facilitate inherited electronic conductivity, enhance adsorption ability of potassium, induce localized surface polarization to guide electrolyte decomposition behavior for SEI formation, and especially, enrich the KF crystals in SEI by self-sacrifice from C-F bond cleavage. Hence, the regulated fluorinated electrode with generated ultra-thin, uniform, and KF-enriched SEI shows improved capacity of 439.3 mAh g-1 (3.82 mAh cm--...
Source: Angewandte Chemie - May 3, 2024 Category: Chemistry Authors: Xixue Zhang Feng Wu Difan Fang Renjie Chen Li Li Source Type: research
Spin-State Control in Dysprosium(III) Metallacrown Magnets via Thioacetal Modification
Angew Chem Int Ed Engl. 2024 May 3:e202404271. doi: 10.1002/anie.202404271. Online ahead of print.ABSTRACTIntegrating controllable spin states into single-molecule magnets (SMMs) enables precise manipulation of magnetic interactions at a molecular level, but remains a synthetic challenge. Herein, we developed a 3d-4f metallacrown (MC) magnet [DyNi5(quinha)5(Clsal)2(py)8](ClO4)∙4H2O (H2quinha = quinaldichydroxamic acid, HClsal = 5-chlorosalicylaldehyde) wherein a square planar NiII is stabilized by chemical stacking. Thioacetal modification was employed via post-synthetic ligand substitutions and yielded [DyNi5(quinha)5(C...
Source: Angewandte Chemie - May 3, 2024 Category: Chemistry Authors: Wei Deng Si-Guo Wu Ze-Yu Ruan Ya-Ping Gong Shan-Nan Du Hai-Ling Wang Yan-Cong Chen Wei-Xiong Zhang Jun-Liang Liu Ming-Liang Tong Source Type: research
