样式: 排序: IF: - GO 导出 标记为已读
-
Hierarchical Self-assembly of Multidimensional Functional Materials from Sequence-defined Peptoids Angew. Chem. Int. Ed. (IF 16.6) Pub Date : 2024-04-24 Li Shao, Dehong Hu, Shao-Liang Zheng, Thi Kim Hoang Trinh, Wenhao Zhou, Haoyu Wang, Yanxu Zong, Changning Li, Chun-Long Chen
Hierarchical self-assembly represents a powerful strategy for the fabrication of functional materials across various length scales. However, achieving precise formation of functional hierarchical assemblies remains a significant challenge and requires a profound understanding of molecular assembly interactions. In this study, we present a molecular-level understanding of the hierarchical assembly of
-
Crown Ether Electrolyte Induced Li2O2 Amorphization for Low Polarization and Long Lifespan Li-O2 batteries Angew. Chem. Int. Ed. (IF 16.6) Pub Date : 2024-04-24 Meng Li, Jiaxin Wu, Zichang You, Zhongqin Dai, Yuanfan Gu, Lei Shi, Meifen Wu, Zhaoyin Wen
Lithium-oxygen batteries possess an extremely high theoretical energy density, rendering them a prime candidate for next-generation secondary batteries. However, they still face multiple problems such as huge charge polarization and poor cycle life, which lay a significant gap between laboratory research and commercial applications. In this work, we adapt 15-crown-5 ether (C15) as solvent to regulate
-
Assembly of Glycopeptides in Living Cells Resembling Viral Infection for Cargo Delivery Angew. Chem. Int. Ed. (IF 16.6) Pub Date : 2024-04-24 Feng Tian, Ruo-Chen Guo, Chunxia Wu, Xin Liu, Zeyu Zhang, Yamei Wang, Hao Wang, Gongyu Li, Zhilin Yu
Self-assembly in living cells represents one versatile strategy for drug delivery; however, it suffers from the limited precision and efficiency. Inspired by viral traits, we here report a cascade targeting-hydrolysis-transformation (THT) assembly of glycosylated peptides in living cells holistically resembling viral infection for efficient cargo delivery and combined tumor therapy. We design a glycosylated
-
An Integrative Chemical Recycling Approach for Catalytic Oxidation of Epoxy Resin and in-situ Separation of Degraded Products Angew. Chem. Int. Ed. (IF 16.6) Pub Date : 2024-04-24 Lulu Liu, Xuehui Liu, Xiaohui Li, Shimei Xu, Yu-Zhong Wang
Although many approaches have been proposed to recycling waste epoxy resin (EP), the separation of mixed degraded products remains a challenge due to their similar structures. To address this, we present a catalytic oxidation strategy that enables mild degradation of EP and in-situ separation of degraded products through supramolecular interactions. The oxidative degradation relies on FeIV=O radicals
-
Record High Iodate Anion Capture by a Redox-Active Cationic Polymer Network Angew. Chem. Int. Ed. (IF 16.6) Pub Date : 2024-04-24 Qi Guo, Jie Li, Yuting Zhao, Lingyi Li, Linwei He, Fuqiang Zhao, Fuwan Zhai, Mingxing Zhang, Long Chen, Zhifang Chai, Shuao Wang
As a critical radioactive anionic contaminant, traditional adsorbents primarily remove iodate (IO3-) through ion exchange or hard acid-hard base interactions, but suffer from limited affinity and capacity. Herein, employing the synergistic effect of ion exchange and redox, we successfully synthesized a redox-active cationic polymer network (SCU-CPN-6, [C9H10O2N5•Cl]n) by merging guanidino groups with
-
Including the Ensemble of Unstructured Conformations in the Analysis of Protein's Native State by High-Pressure NMR Spectroscopy Angew. Chem. Int. Ed. (IF 16.6) Pub Date : 2024-04-24 Frederic Berner, Michael Kovermann
The analysis of pressure induced changes in the chemical shift of proteins allows statements on structural fluctuations proteins exhibit at ambient pressure. The inherent issue of separating general pressure effects from structural related effects on the pressure dependence of chemical shifts has so far been addressed by considering the characteristics of random coil peptides on increasing pressure
-
Paper Spray Mass Spectrometry with On-Paper Electrokinetic Manipulations: Part- Per-Trillion Detection of Per/Polyfluoroalkyl Substances in Water and Opioids in Urine Angew. Chem. Int. Ed. (IF 16.6) Pub Date : 2024-04-24 Magnus Rydberg, Merlin Bruening, Nicholas Manicke
We developed a simple, paper-based device that enables sensitive detection by mass spectrometry (MS) without solid phase extraction or other sample preparation. Using glass fiber filter papers within a 3D printed holder, the device employs electrokinetic manipulations to stack, separate, and desalt charged molecules on paper prior to spray into the MS. Due to counter-balanced electroosmotic flow and
-
On the Dendrite-Suppressing Effect of Laser-Processed Polylactic Acid-Derived Carbon Coated Zinc Anode in Aqueous Zinc Ion Batteries Angew. Chem. Int. Ed. (IF 16.6) Pub Date : 2024-04-24 Maryam Abouali, Sadaf Adhami, Somayeh Asadi Haris, Recep Yuksel
A major bottleneck limiting the commercialization of aqueous zinc ion batteries (AZIBs) is dendrite formation on the zinc anode during the plating/stripping process, which leads to rapid performance and device failure. In this regard, researchers are trying to design more stable anodes toward suppressing dendrite formation. One possible solution to tackle this problem and to extend the cycling life
-
Silylenes with a small chalcogenide substituent: Tuning frontier orbital energies from O to Te Angew. Chem. Int. Ed. (IF 16.6) Pub Date : 2024-04-24 Maximilian P. Müller, Alexander Hinz
The general synthesis of heteroleptic acyclic silylenes with a bulky carbazolyl substituent (dtbpCbz) is detailed and a series of compounds with a chalcogenide substituent of the type [(dtbpCbz)SiE16R] (E16R = OtBu, SEt, SePh, TePh) is reported. With the bulky carbazolyl substituent present, the chalcogenide moiety can be very small, as is shown by incorporating groups as small as ethyl, phenyl or
-
Repurposing Visible-Light-Excited Ene-Reductases for Diastereo- and Enantioselective Lactones Synthesis Angew. Chem. Int. Ed. (IF 16.6) Pub Date : 2024-04-24 Jinhai Yu, Qiaoyu Zhang, Beibei Zhao, Tianhang Wang, Yu Zheng, Binju Wang, Yan Zhang, Xiaoqiang Huang
Repurposing enzymes to catalyze non-natural asymmetric transformations that are difficult to achieve using traditional chemical methods is of significant importance. Although radical C-O bond formation has emerged as a powerful approach for constructing oxygen-containing compounds, controlling the stereochemistry poses a great challenge. Here we present the development of a dual bio-/photo-catalytic
-
Synthesis of 18F-labeled Aryl Trifluoromethyl Sulfones, -Sulfoxides, and -Sulfides for Positron Emission Tomography Angew. Chem. Int. Ed. (IF 16.6) Pub Date : 2024-04-24 Lukas Veth, Albert D. Windhorst, Danielle J. Vugts
Positron emission tomography (PET) is becoming increasingly important in nuclear medicine and drug discovery. To date, the development of many potential PET tracers is hampered by the lack of suitable synthetic pathways for their preparation. This is particularly true for the highly desired radiolabeling of compounds bearing [18F]CF3-groups. For instance, S(O)nCF3-groups (n = 0, 1, 2) serve as structural
-
Hyperbranched Vitrimer for Ultrahigh Energy Dissipation Angew. Chem. Int. Ed. (IF 16.6) Pub Date : 2024-04-24 Lin Cheng, Jun Zhao, Zhongqiang Xiong, Sijun Liu, Xuzhou Yan, Wei Yu
Polymers are ideally utilized as damping materials due to the high internal friction of molecular chains, enabling effective suppression of vibrations and noises in various fields. Current strategies rely on broadening the glass transition region or introducing additional relaxation components to enhance the energy dissipation capacity of polymeric damping materials. However, it remains a significant
-
C(sp3)–H (N-Phenyltetrazole)thiolation as an Enabling Tool for Molecular Diversification Angew. Chem. Int. Ed. (IF 16.6) Pub Date : 2024-04-24 Ashley Zachmann, Justine Drappeau, Shubin Liu, Erik John Alexanian
Methods enabling the broad diversification of C(sp3)–H bonds from a common intermediate are especially valuable in chemical synthesis. Herein, we report a site-selective (N-phenyltetrazole)thiolation of aliphatic and (hetero)benzylic C(sp3)–H bonds using a commercially available disulfide to access N-phenyltetrazole thioethers. The thioether products are readily elaborated in diverse fragment couplings
-
Bithiophene-Functionalized Infrared Two-Photon Absorption Metal Complexes as Single-Molecule Platforms for Synergistic Photodynamic, Photothermal, and Chemotherapy Angew. Chem. Int. Ed. (IF 16.6) Pub Date : 2024-04-24 Xue-Lian li, Meng-Fan wang, Li-Zhen Zeng, Guo-Kui Li, Run-Yu Zhao, Fu-Dan Liu, Yun Li, Yu-Fei Yan, Qishuai Liu, Zhao Li, Hongbin Zhang, Xiaoxia Ren, Feng Gao
A planar conjugated ligand functionalized with bithiophene and its Ru(II), Os(II), and Ir(III) complexes have been constructed as single-molecule platform for synergistic photodynamic, photothermal, and chemotherapy. The complexes have significant two-photon absorption at 808 nm and remarkable singlet oxygen and superoxide anion production in aqueous solution and cells when exposed to 808 nm infrared
-
Enantiopure [6]-Azairidahelicene by Dynamic Kinetic Resolution of a Configurationally Labile [4]-Helicene Angew. Chem. Int. Ed. (IF 16.6) Pub Date : 2024-04-24 Ariadna Pazos, Carlos M Cruz, Juan M. Cuerva, Ivan Rivilla, Fernando P. Cossío, Zoraida Freixa
A pair of enantiopure [6]-azairidahelicenes incorporating chirality at the metal center and on the helicenic ligand were synthesized by dynamic kinetic resolution (dkr) of a configurationally labile [4]-helicenic ligand (4-(2-pyridyl)-benzo[g]phenanthrene, L1H) using bis-cyclometalated chiral-at-metal only iridium(III) precursors as chiral inductors. The origin of the observed dkr is attributed to
-
Crystalline Porous Organic Frameworks Based on Multiple Dynamic Linkages Angew. Chem. Int. Ed. (IF 16.6) Pub Date : 2024-04-24 Bo Liu, Panyue Guo, Xinyu Guan, Xuexue Tian, Fei Du, Weiqing Xie, Hai-Long Jiang
A novel class of crystalline porous materials has been developed utilizing multilevel dynamic linkages, including covalent B-O, dative B←N and hydrogen bonds. Typically, boronic acids undergo in situ condensation to afford B3O3-based units, which further extend to molecular complexes or chains via B←N bonds. The obtained superstructures are subsequently interconnected via hydrogen bonds and π-π interactions
-
Crystalline Olefin-Linked Chiral Covalent Organic Frameworks as a Platform for Asymmetric Catalysis Angew. Chem. Int. Ed. (IF 16.6) Pub Date : 2024-04-24 Ting He, Ivan Keng Wee On, Shuai Bi, Ziyue Huang, Jingjing Guo, Zhifang Wang, Yanli Zhao
The construction of olefin-linked chiral covalent organic frameworks (COFs) with high crystallinity is highly desirable while remains great challenge due to the poor reversibility of the formation reaction for the olefin linkages during the in situ structural self-healing process. Herein, we successfully synthesized two sets of enantiomeric olefin-linked COFs. The chiral catalytic groups are uniformly
-
Building Co16-N3-based UiO-MOF to Expand Design Parameters for MOF Photosensitization Angew. Chem. Int. Ed. (IF 16.6) Pub Date : 2024-04-24 Guang-Chen Guo, Jiong-Peng Zhao, Song Guo, Wen-Xiong Shi, Fu-Chen Liu, Tong-Bu Lu, Zhi-Ming Zhang
The construction of secondary building units (SBUs) in versatile metal–organic frameworks (MOFs) represents a promising method for developing multi-functional materials, especially for improving their sensitizing ability. Herein, we developed a dual small molecules auxiliary strategy to construct a high-nuclear transition-metal-based UiO-architecture Co16-MOF-BDC with visible-light-absorbing capacity
-
The Role of Hydrogen Bonds in Thermally Responsive Crystallization-Driven Template Autocatalysis Angew. Chem. Int. Ed. (IF 16.6) Pub Date : 2024-04-23 Huimin Wu, Qing-Xuan Chen, Yang Su, Zhen Chen
Autocatalysis has been well recognized to implicate in the emergence of life and is intrinsic to the biomolecular replication. Recently, an efficient template autocatalysis driven by solvent-free crystallization has been reported. Herein, we unveil the role of intermolecular hydrogen (H) bonds formed by amides in crystallization-driven template autocatalysis (CDTA), which involves the autocatalytic
-
The Role of the Molecular Encapsulation Effect in Stabilizing Hydrogen-Bond-Rich Gel-State Lithium Metal Batteries Angew. Chem. Int. Ed. (IF 16.6) Pub Date : 2024-04-23 Hantao Xu, Wei Deng, Lei Shi, Juncai Long, Yongcai Zhang, Lin Xu, Liqiang Mai
Gel-state polymer electrolytes with superior mechanical properties, self-healing abilities and high Li+ transference numbers can be obtained by in situ polymerization of monomers with hydrogen-bonding moieties. However, it is overlooked that the active hydrogen atoms in hydrogen-bond donors experience displacement reactions with lithium metal in lithium metal batteries (LMBs), leading to corrosion
-
Nickel-Catalyzed Chemoselective Carbomagnesiation for Atroposelective Ring-Opening Difunctionalization Angew. Chem. Int. Ed. (IF 16.6) Pub Date : 2024-04-23 Tingting Sun, Linchao Guo, Qi Li, Zhi-Chao Cao
There is a pressing need for methods that can connect enantioenriched organic compounds with readily accessible building blocks via asymmetric functionalization of unreactive chemical bonds in organic synthesis and medicinal chemistry. Herein, the asymmetric chemoselective cleavage of two unactivated C(Ar)-O bonds in the same molecule is disclosed for the first time through an unusual nickel-catalyzed
-
A New Family of High Oxidation State Antiperovskite Nitrides: La3MN5 (M = Cr, Mn and Mo) Angew. Chem. Int. Ed. (IF 16.6) Pub Date : 2024-04-23 Yao Yuan, Minghui Yang, Simon D. Kloß, John Paul Attfield
Three new nitrides La3MN5 (M = Cr, Mn, and Mo) have been synthesized using a high pressure azide route. These are the first examples of ternary Cs3CoCl5-type nitrides, and show that this (MN4)NLa3 antiperovskite structure type may be used to stabilise high oxidation-state transition metals in tetrahedral molecular [MN4]n- nitridometallate anions. Magnetic measurements confirm that Cr and Mo are in
-
Formation of Supernarrow Borophene Nanoribbons Angew. Chem. Int. Ed. (IF 16.6) Pub Date : 2024-04-23 Haochen Wang, Pengcheng Ding, Guang-Jie Xia, Xiangyun Zhao, Wenlong E, Miao Yu, Zhibo Ma, Yang-Gang Wang, Lai-Sheng Wang, Jun Li, Xueming Yang
Borophenes have sparked considerable interest owing to their fascinating physical characteristics and diverse polymorphism. However, borophene nanoribbons (BNRs) with widths less than 2 nm have not been achieved. Herein, we report the experimental realization of supernarrow BNRs. Combining scanning tunneling microscopy imaging with density functional theory modeling and ab initio molecular dynamics
-
Bioorthogonal Cu Single-atom Nanozyme for Synergistic Nanocatalytic Therapy, Photothermal Therapy, Cuproptosis, and Immunotherapy Angew. Chem. Int. Ed. (IF 16.6) Pub Date : 2024-04-23 Luyan Wu, Huihui Lin, Xiang Cao, Qiang Tong, Fangqi Yang, Yinxing Miao, Deju Ye, Quli Fan
Single-atom nanozymes (SAzymes) with atomically dispersed active sites are potential substitutes for natural enzymes. A systematic study of its multiple functions can in-depth understand SAzymes’s nature, which remains elusive. Here, we develop a novel ultrafast synthesis of sputtered SAzymes by in situ bombarding-embedding technique. Using this method, sputtered copper (Cu) SAzymes (CuSA) is developed
-
Synergistic Effect of Ni/Ni(OH)2 Core-Shell Catalyst Boosts Tandem Nitrate Reduction for Ampere-Level Ammonia Production Angew. Chem. Int. Ed. (IF 16.6) Pub Date : 2024-04-23 Xinyue Shi, Minghui Xie, Kaiwen Yang, Yutao Niu, Haibin Ma, Yiming Zhu, Jiayi Li, Tingting Pan, Xiaoyan Zhou, Yujie Cui, Zhao Li, Yifu Yu, Xiaohua Yu, Jiwei Ma, Hongfei CHENG
Electrocatalytic reduction of nitrate to ammonia provides a green alternate to the Haber-Bosch method, yet it suffers from sluggish kinetics and a low yield rate. The nitrate reduction follows a tandem reaction of nitrate reduction to nitrite and subsequent nitrite hydrogenation to generate ammonia, and the ammonia Faraday efficiency (FE) is limited by the competitive hydrogen evolution reaction. Herein
-
Noncovalent Interaction Guided Precise Photoluminescence Regulation of Gold Nanoclusters in Both Isolate Species and Aggregate States Angew. Chem. Int. Ed. (IF 16.6) Pub Date : 2024-04-23 Xiaoxi Luo, Jie Kong, Hang Xiao, Dongmiao Sang, Kui He, Meng Zhou, Jinbin Liu
Designing luminophores bright in both isolate species and aggregate states is of great importance in many emerging cutting-edge applications. However, the conventional luminophores either emit in isolate species but quench in aggregate state or emit in aggregate state but darken in isolate species. Here we demonstrate that the precise regulation of noncovalent interactions can realize luminophores
-
High-Pressure-Field Induced Synthesis of Ultrafine-Sized High-Entropy Compounds with Excellent Sodium-Ion Storage Angew. Chem. Int. Ed. (IF 16.6) Pub Date : 2024-04-23 Ming Liang, Haonan Xie, biao chen, Hongye Qin, Hanwen Zhang, Jingyi Wang, Junwei Sha, Liying Ma, Enzuo Liu, Jianli Kang, Chunsheng Shi, Fang He, Xiaopeng Han, Wenbin Hu, Naiqin Zhao, Chunnian He
Emerging high entropy compounds (HECs) have attracted huge attention in electrochemical energy-related applications. The features of ultrafine size and carbon incorporation show great potential to boost the ion-storage kinetics of HECs. However, they are rarely reported because high-temperature calcination tends to result in larger crystallites, phase separation, and carbon reduction. Herein, using
-
Adhesion Peptide-Functionalized Biobased Microgels for Controlled Delivery of Pesticides Angew. Chem. Int. Ed. (IF 16.6) Pub Date : 2024-04-23 Abdulkadir Yayci, Tim Sassmann, Alexander Boes, Felix Jakob, Alexander Töpel, Anne Loreth, Carolin Rauch, Andrij Pich, Ulrich Schwaneberg
Widespread use of plant protection agents in agriculture is a major cause of pollution. Apart from active ingredients, the environmental impact of auxiliary synthetic polymers should be minimized if they are highly persistent. An alternative to synthetic polymers is the use of natural polysaccharides, which are abundant and biodegradable. In this study, we explore pectin microgels functionalized with
-
Living Self-Assembly of Monodisperse Micron-Sized Polymer Vesicles Angew. Chem. Int. Ed. (IF 16.6) Pub Date : 2024-04-23 Hui Pan, Changxu Zhang, Wenfeng Jiang, Yongfeng Zhou
Artificial vesicles are recognized as powerful platforms for a large body of research across the disciplines of chemistry, physics and biology. Despite the great progress, control of the size distribution to make uniform vesicles remains fundamentally difficult due to the highly uncontrollable growth kinetics, especially for micron-sized vesicles. Here we report a template-free living self-assembly
-
Discovery, Structure, and Engineering of a cis-Geranylfarnesyl Diphosphate Synthase Angew. Chem. Int. Ed. (IF 16.6) Pub Date : 2024-04-23 Fang-Ru Li, Qingling Wang, Xingming Pan, Hui-Min Xu, Liao-Bin Dong
cis-Prenyltransferases (cis-PTs) catalyze the sequential head-to-tail condensation of isopentenyl diphosphate (IPP) to allylic diphosphates, producing mixed E-Z prenyl diphosphates of varying lengths; yet, the specific enzymes synthesizing cis-C25 prenyl diphosphates have not been identified. In this study, we present the discovery and characterization of a cis-geranylfarnesyl diphosphate synthase
-
Acceptor-Reactivity-Controlled Stereoconvergent Synthesis and Immunological Activity of a Unique Pentasaccharide from the Cell Wall Polysaccharide of Cutibacterium acnes C7 Angew. Chem. Int. Ed. (IF 16.6) Pub Date : 2024-04-23 Tianhui Hao, Ke Feng, Hongzhen Jin, Jiawei Li, Chenkai Zhou, Xingbang Liu, Wei Zhao, Fan Yu, Tiehai Li
Bacterial cell-surface polysaccharides are involved in various biological processes and have attracted widespread attention as potential targets for developing carbohydrate-based drugs. However, the accessibility of structurally well-defined polysaccharide or related active oligosaccharide domains remains challenging. Herein, we describe an efficiently stereocontrolled approach for the first total
-
Cathodic Deposition-Assisted Synthesis of Thin Glass MOF Films for High-Performance Gas Separations Angew. Chem. Int. Ed. (IF 16.6) Pub Date : 2024-04-23 Sijie Xie, Xiaoyu Tan, Zhenhong Xue, Pieter Geysens, Hui Pan, Wei Guo, Zhenyu Zhou, Xuan Zhang, Ivo F.J. Vankelecom, Jan Fransaer
Glass metal-organic framework (MOF) films can be fabricated from their crystalline counterparts through a melt-quenching process and are prospective candidates for gas separation because of the elimination of the grain boundaries in crystalline MOF films. However, current techniques are limited to producing glass MOF films with a thickness of tens of micrometers, which leads to ultralow gas permeances
-
Polyfluorinated Organic Diammonium Induced Lead Iodide Arrangement for Efficient Two-Step-Processed Perovskite Solar Cells Angew. Chem. Int. Ed. (IF 16.6) Pub Date : 2024-04-22 Yang liu, Qiuju Liu, Lu Yusong, Jianfei Fu, Jifeng Wu, Yan Zhang, Qingyong Tian, Bin Fan, Hua Bai, Hai-Qiao Wang
The inefficient conversion of lead iodide to perovskite has become one of the major challenges in further improving the performance of perovskite solar cells fabricated by the two-step method. Herein, the discontinuous lead iodide layer realized by introduction of a polyfluorinated organic diammonium salt, octafluoro-([1,1′-biphenyl]-4,4′-diyl)-dimethanaminium (OFPP) iodide which does not form low-dimensional
-
Electrochemical Synthesis of C(sp3)-Rich Amines by Aminative Carbofunctionalization of Carbonyl Compounds Angew. Chem. Int. Ed. (IF 16.6) Pub Date : 2024-04-22 Wen-Qiang Liu, Boon Chong Lee, NingXi Song, Zhenghao He, Zi-An Shen, Yixin Lu, Ming Joo Koh
Alkylamines form the backbone of countless nitrogen-containing small molecules possessing desirable biological properties. Despite advances in amine synthesis through transition metal catalysis and photoredox chemistry, multicomponent reactions that leverage inexpensive materials to transform abundant chemical feedstocks into three-dimensional α-substituted alkylamines bearing complex substitution
-
Enrooted-type metal-support interaction boosting oxygen evolution reaction in acidic media Angew. Chem. Int. Ed. (IF 16.6) Pub Date : 2024-04-22 Wenjuan Wang, Cheng Li, Chuan Zhou, Xin Xiao, Fayan Li, Ning-yu Huang, Lei Li, Meng Danny Gu, Qiang Xu
Supported metal catalysts with appropriate metal-support interactions (MSIs) hold a great promise for heterogeneous catalysis. However, ensuring tight immobilization of metal clusters/nanoparticles on the support while maximizing the exposure of surface active sites remains a huge challenge. Herein, we report an Ir/WO3 catalyst with a new enrooted-type MSI in which Ir clusters are, unprecedentedly
-
Discovery of Alloy Catalysts Beyond Pd for Selective Hydrogenation of Reformate via First-principle Screening with Consideration of H-coverage Angew. Chem. Int. Ed. (IF 16.6) Pub Date : 2024-04-22 jiayi wang, haoxiang xu, Yihao Zhang, jianguo wu, haowen ma, xuecheng zhan, jiqin zhu, Daojian Cheng
The highly selective hydrogenation to remove olefins is a significant refining approach for the reformate. Herein, a library of transition metal for reformate hydrogenation is tested experimentally to validate the predictive level of catalytic activity from our theoretical framework, which combines ab initio calculations and microkinetic modeling, with consideration of surface H-coverage effect on
-
Boron-Catalyzed C1 Copolymerization of Arsonium and Sulfoxonium Ylides toward Unrepresented Structures and Fluorescence Properties Angew. Chem. Int. Ed. (IF 16.6) Pub Date : 2024-04-22 Mingtao Zhou, Nikos Hadjichristidis
The first synthesis of well-defined poly(methylene-co-1,1-diphenylpropenenylene) (C1-co-C1’), equivalent to poly(ethylene-co-diphenylbutadiene) copolymer was accomplished by C1 copolymerization of novel diphenylpropenyl triphenyl arsonium ylides (Ph2AY) and dimethylsulfoxonium methylide (Me2SY) using B-thexylborepane as an initiator. All polymerization conditions, including feed ratio, temperature
-
Single-Atom Iron Catalyst as an Advanced Redox Mediator for Anodic Oxidation of Organic Electrosynthesis Angew. Chem. Int. Ed. (IF 16.6) Pub Date : 2024-04-22 Xin-Yu Wang, Yong-Zhou Pan, Jiarui Yang, Wen-Hao Li, Tao Gan, Ying-Ming Pan, Hai-Tao Tang, Dingsheng Wang
Homogeneous electrocatalysts can indirect oxidate the high overpotential substrates through single-electron transfer on the electrode surface, enabling efficient operation of organic electrosynthesis catalytic cycles. However, the problems of this chemistry still exist such as high dosage, difficult recovery, and low catalytic efficiency. Single-atom catalysts (SACs) exhibit high atom utilization and
-
Dual Redox Reaction Sites for Pseudocapacitance Based on Ti and -P Functional Groups of Ti3C2PBrx MXene Angew. Chem. Int. Ed. (IF 16.6) Pub Date : 2024-04-22 Jiamin Zhu, Shengli Zhu, Zhenduo Cui, Zhaoyang Li, Shuilin Wu, Wence Xu, Zhonghui Gao, Te Ba, Chunyong Liang, Yanqin Liang, Hui Jiang
MXenes have extensive applications due to their different properties determined by intrinsic structures and various functional groups. Exploring different functional groups of MXenes leads to improved performance or potential applications. In this work, we prepared new Ti3C2PBrx (x=0.4-0.6) MXene with phosphorus functional groups (-P) through a two-step gas-phase reaction. The acquisition of -P is
-
Neuron-Like Silicone Nanofilaments@Montmorillonite Nanofillers of PEO-Based Solid-State Electrolytes for Lithium Metal Batteries with Wide Operation Temperature Angew. Chem. Int. Ed. (IF 16.6) Pub Date : 2024-04-22 Wankai Wang, Yanfei Yang, Jie Yang, Junping Zhang
Poly(ethylene oxide) (PEO)-based composite solid electrolytes (CSEs) are promising to accelerate commercialization of solid-state lithium metal batteries (SSLMBs). Nonetheless, this is hindered by the CSEs' limited ion conductivity at room temperature. Here, we propose design, synthesis, and application of the bioinspired neuron-like nanofillers for PEO-based CSEs. The neuron-like superhydrophobic
-
Electrochemically Mediated Atom Transfer Radical Polymerization Driven by Alternating Current Angew. Chem. Int. Ed. (IF 16.6) Pub Date : 2024-04-22 Francesco De Bon, Marco Fantin, Vanessa A. Pereira, Teresa J. Lourenço Bernardino, Armenio Coimbra Serra, Krzysztof Matyjaszewski, Jorge Fernando Jordao Coelho
Alternating current (AC) and pulsed electrolysis are gaining traction in electro(organic) synthesis due to their advantageous characteristics. We employed AC electrolysis in electrochemically mediated Atom Transfer Radical Polymerization (eATRP) to facilitate the regeneration of the activator CuI complex on Cu0 electrodes. Additionally, Cu0 served as a slow supplemental activator and reducing agent
-
Insights into the Distinct Behaviors between Bifunctional and Binary Organoborane Catalysts through Terpolymerization of Epoxide, CO2, and Anhydride Angew. Chem. Int. Ed. (IF 16.6) Pub Date : 2024-04-22 Rui Xie, Yuhui Wang, Shuai Li, Bo Li, Jie Xu, Jinqian Liu, Yuchen He, Guan-Wen Yang, Guang-Peng Wu
Alkyl borane compounds-mediated polymerizations have expanded to Lewis pair polymerization, free radical polymerization, ionic ring-opening polymerization, and polyhomologation. The bifunctional organoborane catalysts that contain the Lewis acid and ammonium or phosphonium salt in one molecule have demonstrated superior catalytic performance for ring-opening polymerization of epoxides and ring-opening
-
Detection of Sulfoquinovosidase Activity in Cell Lysates Using Activity-Based Probes Angew. Chem. Int. Ed. (IF 16.6) Pub Date : 2024-04-22 Zirui Li, Isabelle Pickles, Mahima Sharma, Benjamin Melling, Jeroen Codee, Luise Pallasdies, Spencer Williams, Herman Overkleeft, Gideon John Davies
The sulfolipid sulfoquinovosyl diacylglycerol (SQDG), produced by plants, algae, and cyanobacteria, constitutes a major sulfur reserve in the biosphere. Microbial breakdown of SQDG is critical for the biological utilization of its sulfur. This commences through release of the parent sugar, sulfoquinovose (SQ), catalyzed by sulfoquinovosidases (SQases). These vanguard enzymes are encoded in gene clusters
-
Controlled Synthesis of Unconventional Phase Alloy Nanobranches for Highly Selective Electrocatalytic Nitrite Reduction to Ammonia Angew. Chem. Int. Ed. (IF 16.6) Pub Date : 2024-04-22 Yunhao Wang, Yuecheng Xiong, Mingzi Sun, Jingwen Zhou, Fengkun Hao, Qinghua Zhang, Chenliang Ye, Xixi Wang, Zhihang Xu, Qingbo Wa, Fu Liu, Xiang Meng, Juan Wang, Pengyi Lu, Yangbo Ma, Jinwen Yin, Ye Zhu, Shengqi Chu, Bolong Huang, Lin Gu, Zhanxi Fan
The controlled synthesis of metal nanomaterials with unconventional phases is of significant importance to develop high-performance catalysts for various applications. However, it remains challenging to modulate the atomic arrangements of metal nanomaterials, especially the alloy nanostructures that involve different metals with distinct redox potentials. Here we report the general one-pot synthesis
-
Enhancing Built-in Electric Fields via Molecular Symmetry Modulation in Supramolecular Photocatalysts for Highly Efficient Photocatalytic Hydrogen Evolution Angew. Chem. Int. Ed. (IF 16.6) Pub Date : 2024-04-21 Xiaolin Zhu, Yihui Jia, Yuhan Liu, Jingyi Xu, Huarui He, Siyue Wang, Yang Shao, Yaxin Zhai, Yongfa Zhu
Nature-inspired supramolecular self-assemblies are attractive photocatalysts, but their quantum yields are limited by poor charge separation and transportation. A promising strategy for efficient charge transfer is to enhance the built-in electric field by symmetry breaking. Herein, an unsymmetric protonation, N-heterocyclic π-conjugated anthrazoline-based supramolecular photocatalyst SA-DADK-H+ was
-
Translocation and confinement of tetraamines in adaptable microporous cavities Angew. Chem. Int. Ed. (IF 16.6) Pub Date : 2024-04-21 Ana Rubio-Gaspar, Alechania Misturini, Reisel Millán, Neyvis Almora-Barrios, Sergio Tatay, Volodymyr Bon, Mickaele Bonneau, Vincent Guillerm, Mohamed Eddaoudi, Sergio Navalón, Stefan Kaskel, Donatella Armentano, Carlos Marti-Gastaldo
Metal-Organic Frameworks can be grafted with amines by coordination to metal vacancies to create amine-appended solid adsorbents, which are being considered as an alternative to using aqueous amine solutions for CO2 capture. In this study, we propose an alternative mechanism that does not rely on the use of neutral metal vacancies as binding sites but is enabled by the structural adaptability of heterobimetallic
-
A Carbon-Caged Rhodamine Generating Nitrosoperoxycarbonate for Photoimmunotherapy Angew. Chem. Int. Ed. (IF 16.6) Pub Date : 2024-04-21 Lei Yin, Bei Zhao, Jie Zhou, Yunxia Huang, Hao Ma, Ting Zhou, Jie Mou, Peiru Min, Jinquan Chen, Guangbo Ge, Xuhong Qian, Xiao Luo, Youjun Yang
Photoimmunotherapy is a promising cancer treatment modality. While potent 1-e- oxidative species are known to induce immunogenic cell death (ICD), they are also associated with unspecific oxidation and collateral tissue damage. This difficulty may be addressed by post-generation radical reinforcement. Namely, non-oxidative radicals are first generated and subsequently activated into powerful oxidative
-
Lithium Pre-Storage Enables High Initial Coulombic Efficiency and Stable Lithium-Enriched Silicon/Graphite Anode Angew. Chem. Int. Ed. (IF 16.6) Pub Date : 2024-04-21 Yingjie Gao, Chenghao Cui, Zhikun Huang, Guoyu Pan, Yuanfan Gu, Yanan Yang, Fan Bai, Zhuang Sun, Tao Zhang
Application of silicon-based anode is significantly challenged by low initial Coulombic efficiency (ICE) and poor cyclability. Traditional pre-lithiation reagents often pose safety concerns due to their unstable chemical nature. Achieving a balance between water-stability and high ICE in prelithiated silicon is a critical issue. Here, we present a lithium-enriched silicon/graphite material with an
-
Catalytic Asymmetric Cascade Dearomatization of Indoles via a Photoinduced Pd-Catalyzed 1,2-Bisfunctionalization of Butadienes Angew. Chem. Int. Ed. (IF 16.6) Pub Date : 2024-04-20 Xiaohang Zhan, Zhiwen Nie, Na Li, Ao Zhou, Haotian Lv, Mingrong Liang, Keqin Wu, Guijuan Cheng, Qin Yin
Photoinduced Pd-catalyzed bisfunctionalization of butadienes with a readily available organic halide and a nucleophile represents an emerging and attractive method to assemble versatile alkenes bearing various functional groups at the allylic position. However, enantiocontrol and/or diastereocontrol in the C-C or C-X bond-formation step have not been solved due to the open-shell process. Herein, we
-
Ratiometric Afterglow Luminescent Imaging of Matrix Metalloproteinase-2 Activity via an Energy Diversion Process Angew. Chem. Int. Ed. (IF 16.6) Pub Date : 2024-04-19 Weijing Huang, Wenhui Zeng, Zheng Huang, Daqing Fang, Hong Liu, Min Feng, Liang Mao, Deju Ye
Ratiometric afterglow luminescent (AGL) probes are attractive for in vivo imaging due to their high sensitivity and signal self-calibration function. However, there are currently few ratiometric AGL probes available for imaging enzymatic activity in living organisms. Here, we present an energy diversion (ED) strategy that enables the design of an enzyme-activated ratiometric AGL probe (RAG-RGD) for
-
Temporal-Focusing Multiphoton Excitation Single-Molecule Localization Microscopy Using Spontaneously Blinking Fluorophores Angew. Chem. Int. Ed. (IF 16.6) Pub Date : 2024-04-19 Jian-Zong Lai, Chun-Yu Lin, Shean-Jen Chen, Yu-Min Cheng, Manabu Abe, Tzu-Chau Lin, Fan-Ching Chien
Single-molecule localization microscopy (SMLM) based on temporal-focusing multiphoton excitation (TFMPE) and single-wavelength excitation is used to visualize the three-dimensional (3D) distribution of spontaneously blinking fluorophore-labeled subcellular structures in a thick specimen with a nanoscale-level spatial resolution. To eliminate the photobleaching effect of unlocalized molecules in out-of-focus
-
The 18F-Difluoromethyl Group: Challenges, Impact and Outlook Angew. Chem. Int. Ed. (IF 16.6) Pub Date : 2024-04-19 Joseph Ford, Sebastiano Ortalli, Veronique Gouverneur
The difluoromethyl functionality has proven useful in drug discovery, as it can modulate the properties of bioactive molecules. For PET imaging, this structural motif has been largely underexploited in (pre)clinical radiotracers due to a lack of user-friendly radiosynthetic routes. This Minireview provides an overview of the challenges facing radiochemists and summarises the efforts made to date to
-
Reaction Environment Regulation for Electrocatalytic CO2 Reduction in Acids Angew. Chem. Int. Ed. (IF 16.6) Pub Date : 2024-04-19 min Zeng, Wensheng Fang, Yiren Chen, Xinyi Zhang, Yongming Hu, Bao Yu Xia
The electrocatalytic CO2 reduction reaction (CO2RR) is a sustainable route for converting CO2 into value-added fuels and feedstocks, advancing a carbon-neutral economy. The electrolyte critically influences CO2 utilization, reaction rate and product selectivity. While typically conducted in neutral/alkaline aqueous electrolytes, the CO2RR faces challenges due to (bi)carbonate formation and its crossover
-
Chemical Control of Fluorescence Lifetime towards Multiplexing Imaging Angew. Chem. Int. Ed. (IF 16.6) Pub Date : 2024-04-19 Junbao Ma, Feng Luo, Chia-Heng Hsiung, Jianan Dai, Zizhu Tan, Songtao Ye, Lina Ding, Baoxing Shen, Xin Zhang
Fluorescence lifetime imaging has been a powerful tool for biomedical research. Recently, fluorescence lifetime-based multiplexing imaging has expanded imaging channels by using probes that harbor the same spectral channels and distinct excited state lifetime. While it is desirable to control the excited state lifetime of any given fluorescent probes, the rational control of fluorescence lifetimes
-
Delocalizing Excitation for Highly-Active Organic Photovoltaic Catalysts Angew. Chem. Int. Ed. (IF 16.6) Pub Date : 2024-04-19 Zhenzhen Zhang, Chaoying Xu, Qianlu Sun, Yufan Zhu, Wenlong Yan, Guilong Cai, Yawen Li, Wenqin Si, Xinhui Lu, Weigao Xu, Ye Yang, Yuze Lin
Localized excitation in traditional organic photocatalysts typically prevents the generation and extraction of photo-induced free charge carriers, limiting their activity enhancement under illumination. Here, we enhance delocalized photoexcitation of small molecular photovoltaic catalysts by weakening their electron-phonon coupling via rational fluoro-substitution. The optimized 2FBP-4F catalyst we
-
Machine Learning Molecular Dynamics Shows Anomalous Entropic Effect on Catalysis via Surface Pre-melting of Nanoclusters Angew. Chem. Int. Ed. (IF 16.6) Pub Date : 2024-04-19 Fu-Qiang Gong, Yun-Pei Liu, Ye Wang, Weinan E, Zhong-Qun Tian, Jun Cheng
Due to the superior catalytic activity and efficient utilization of noble metals, nanocatalysts are extensively used in the modern industrial production of chemicals. The surface structures of these materials are significantly influenced by reactive adsorbates, leading to dynamic behavior under experimental conditions. The dynamic nature poses significant challenges in studying the structure-activity
-
Cyclometallated Imides as Templates for the H-Bond Directed Iridium-Catalyzed Asymmetric Hydrogenation of N-Methyl, N-Alkyl and N-Aryl Imines Angew. Chem. Int. Ed. (IF 16.6) Pub Date : 2024-04-19 Yisong Wen, Marc Fernández-Sabaté, Agustí Lledós, Giuseppe Sciortino, James Eills, Irene Marco-Rius, Antoni Riera, Xavier Verdaguer
A combined computational and experimental approach allowed us to develop the most selective catalysts for the direct hydrogenation of N-methyl and N-alkyl imines described to date. Iridium catalysts with a cyclometallated cyclic imide group provide selectivity of up to 99% enantiomeric excess. Computational studies show that the selectivity results from the combined effect of H-bonding of the imide
-
A Photodynamic and Photochemotherapeutic Platinum-Iridium Charge-Transfer Conjugate for Anticancer Therapy Angew. Chem. Int. Ed. (IF 16.6) Pub Date : 2024-04-24 Huayun Shi, Oliver W. L. Carter, Fortuna Ponte, Cinzia Imberti, Miguel A. Gomez-Gonzalez, Fernando Cacho-Nerin, Paul D. Quinn, Julia E. Parker, Emilia Sicilia, Huaiyi Huang, Peter J. Sadler
-
An Electrocatalytic Cascade Reaction for the Synthesis of Ketones Using CO2 as a CO Surrogate Angew. Chem. Int. Ed. (IF 16.6) Pub Date : 2024-04-22 Ahmed M. Sheta, Sergio Fernández, Changwei Liu, Geyla C. Dubed-Bandomo, Julio Lloret-Fillol
-
Discovery of (±)-Penindolenes Reveals an Unusual Indole Ring Cleavage Pathway Catalyzed by P450 Monooxygenase Angew. Chem. Int. Ed. (IF 16.6) Pub Date : 2024-04-18 Ling-Hong Meng, Takayoshi Awakawa, Xiao-Ming Li, Zhiyang Quan, Sui-Qun Yang, Bin-Gui Wang, Ikuro Abe
(±)-Penindolenes A–D (1–4), the first representatives of indole terpenoids featuring a γ-lactam skeleton, were isolated from the mangrove-derived endophytic fungus Penicillium brocae MA-231. Our bioactivity tests revealed their potent antimicrobial and acetylcholinesterase inhibitory activities. The biosynthetic reactions by the five enzymes PbaABCDE leading to γ-lactam ring formation were identified