Discovery, Structure, and Engineering of a cis-Geranylfarnesyl Diphosphate Synthase
In this study, we present the discovery and characterization of a cis-geranylfarnesyl diphosphate synthase (ScGFPPS) from Streptomyces clavuligerus. This enzyme demonstrates high catalytic proficiency in generating six distinct cis-polyisoprenoids, including three C25 and three C20 variants. We further determine the crystal structure of ScGFPPS. Additionally, we unveil the crystal structure of nerylneryl diphosphate synthase (NNPS), known for synthesizing an all-cis-C20 polyisoprenoid. Comparative structural analysis of ScGFPPS and NNPS has identified key differences that influence product specificity. Through site-directe...
Source: Angewandte Chemie - April 23, 2024 Category: Chemistry Authors: Fang-Ru Li Qingling Wang Xingming Pan Hui-Min Xu Liao-Bin Dong Source Type: research
Coral -Inspired Terahertz-Infrared Bi-Stealth Electronic Skin
Angew Chem Int Ed Engl. 2024 Apr 23:e202406177. doi: 10.1002/anie.202406177. Online ahead of print.ABSTRACTThe development of electronic skin with dual stealth functionality is crucial for enabling devices to operate effectively in dynamic electromagnetic environments, thereby facilitating intelligent electromagnetic protection for autonomous perception. However, achieving compatibility between terahertz (THz) and infrared (IR) stealth technologies remains largely unexplored due to their inherent contradictions. Herein, inspired by natural corals, a novel coral-like multi-scale composite foam (CMSF) was proposed that ingen...
Source: Angewandte Chemie - April 23, 2024 Category: Chemistry Authors: Shangjing Li Kaichao Pan Jiang Du Zunfeng Liu Jun Qiu Source Type: research
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 Engl. 2024 Apr 23:e202405297. doi: 10.1002/anie.202405297. Online ahead of print.ABSTRACTBacterial 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 synthesis of a unique pentasaccharide repeating unit containing four difficult-to-construct 1,2-cis-glycosidic linkages fr...
Source: Angewandte Chemie - April 23, 2024 Category: Chemistry Authors: Tianhui Hao Ke Feng Hongzhen Jin Jiawei Li Chenkai Zhou Xingbang Liu Wei Zhao Fan Yu Tiehai Li Source Type: research
Nickel-Catalyzed Chemoselective Carbomagnesiation for Atroposelective Ring-Opening Difunctionalization
Angew Chem Int Ed Engl. 2024 Apr 23:e202401756. doi: 10.1002/anie.202401756. Online ahead of print.ABSTRACTThere 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 carbomagnesiation. This reaction facilitates the evolution of a novel atroposelective ring-opening difunctionalization...
Source: Angewandte Chemie - April 23, 2024 Category: Chemistry Authors: Tingting Sun Linchao Guo Qi Li Zhi-Chao Cao Source Type: research
A New Family of High Oxidation State Antiperovskite Nitrides: La3MN5 (M = Cr, Mn and Mo)
Angew Chem Int Ed Engl. 2024 Apr 23:e202405498. doi: 10.1002/anie.202405498. Online ahead of print.ABSTRACTThree 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 the M6+ state, but the M = Mn phase has an anomalously small paramagnetic moment and large cell volume. Neutron powder dif...
Source: Angewandte Chemie - April 23, 2024 Category: Chemistry Authors: Yao Yuan Minghui Yang Simon D Klo ß John Paul Attfield Source Type: research
Facile generation of heterotelechelic poly(2-oxazoline)s towards accelerated exploration of poly(2-oxazoline)-based nanomedicine
In this study, we present a facile end-group diversification approach for poly(2-oxazoline)s (POx), enabling quick and reliable production of hetero-telechelic polymers to facilitate POxylation. The approach relies on the careful tuning of reaction parameters to establish differential reactivity of a pentafluorobenzyl initiator fragment and the living oxazolinium chain-end, allowing the selective introduction of N-, S-, O-nucleophiles via the termination of the polymerization, and a consecutive nucleophilic para-fluoro substitution. The value of this approach for the accelerated development of nanomedicine is demonstrated ...
Source: Angewandte Chemie - April 23, 2024 Category: Chemistry Authors: Joachim F R Van Guyse Saed Abbasi Kazuko Toh Zlata Nagorna Junjie Li Anjaneyulu Dirisala Sabina Quader Satoshi Uchida Kazunori Kataoka Source Type: research
Synergistic Effect of Ni/Ni(OH)2 Core-Shell Catalyst Boosts Tandem Nitrate Reduction for Ampere-Level Ammonia Production
Angew Chem Int Ed Engl. 2024 Apr 23:e202406750. doi: 10.1002/anie.202406750. Online ahead of print.ABSTRACTElectrocatalytic 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, we design a heterostructure catalyst to remedy the above issues, which consists of Ni nanosphere core and Ni(OH)2 n...
Source: Angewandte Chemie - April 23, 2024 Category: Chemistry Authors: 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 Source Type: research
Noncovalent Interaction Guided Precise Photoluminescence Regulation of Gold Nanoclusters in Both Isolate Species and Aggregate States
Angew Chem Int Ed Engl. 2024 Apr 23:e202404129. doi: 10.1002/anie.202404129. Online ahead of print.ABSTRACTDesigning 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 bright in both isolate species and aggregate states. It is firstly discovered that the intra-cluster interaction enhances ...
Source: Angewandte Chemie - April 23, 2024 Category: Chemistry Authors: Xiaoxi Luo Jie Kong Hang Xiao Dongmiao Sang Kui He Meng Zhou Jinbin Liu Source Type: research
Adhesion Peptide-Functionalized Biobased Microgels for Controlled Delivery of Pesticides
In this study, we explore pectin microgels functionalized with anchor peptides (P-MAPs) to be used as an alternative biobased pesticide delivery system. Using complexed Cu2+ as the active ingredient, P-MAPs effectively prevented infection of grapevine plants with downy mildew under semi-field conditions on par with commercial copper pesticides. By using anchor peptides, the microgels tightly bind to the leaf surface, exhibiting excellent rain fastness and prolonged fungicidal activity. Finally, P-MAPs are shown to be easily degradable by enzymes found in nature, demonstrating their negligible long-term impact on the enviro...
Source: Angewandte Chemie - April 23, 2024 Category: Chemistry Authors: Abdulkadir Yayci Tim Sassmann Alexander Boes Felix Jakob Alexander T öpel Anne Loreth Carolin Rauch Andrij Pich Ulrich Schwaneberg Source Type: research
Cathodic Deposition-Assisted Synthesis of Thin Glass MOF Films for High-Performance Gas Separations
Angew Chem Int Ed Engl. 2024 Apr 23:e202401817. doi: 10.1002/anie.202401817. Online ahead of print.ABSTRACTGlass 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. Here, we report a novel cathodic deposition-assisted synthesis of glass ZIF-62 films with a thickness as low as ~1 μ...
Source: Angewandte Chemie - April 23, 2024 Category: Chemistry Authors: Sijie Xie Xiaoyu Tan Zhenhong Xue Pieter Geysens Hui Pan Wei Guo Zhenyu Zhou Xuan Zhang Ivo F J Vankelecom Jan Fransaer Source Type: research
Formation of Supernarrow Borophene Nanoribbons
Angew Chem Int Ed Engl. 2024 Apr 23:e202406535. doi: 10.1002/anie.202406535. Online ahead of print.ABSTRACTBorophenes 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 simulations, we demonstrate that, under the applied growth conditions, boron atoms can penetrate the outermost layer of A...
Source: Angewandte Chemie - April 23, 2024 Category: Chemistry Authors: 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 Source Type: research
The Role of the Molecular Encapsulation Effect in Stabilizing Hydrogen-Bond-Rich Gel-State Lithium Metal Batteries
Angew Chem Int Ed Engl. 2024 Apr 23:e202400032. doi: 10.1002/anie.202400032. Online ahead of print.ABSTRACTGel-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 of the lithium metal. Herein, it is discovered that the addition of hydrogen-bond acceptors to hydrogen-bond-rich gel-stat...
Source: Angewandte Chemie - April 23, 2024 Category: Chemistry Authors: Hantao Xu Wei Deng Lei Shi Juncai Long Yongcai Zhang Lin Xu Liqiang Mai Source Type: research
Enhancing Built-in Electric Fields via Molecular Symmetry Modulation in Supramolecular Photocatalysts for Highly Efficient Photocatalytic Hydrogen Evolution
Angew Chem Int Ed Engl. 2024 Apr 21:e202405962. doi: 10.1002/anie.202405962. Online ahead of print.ABSTRACTNature-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 developed. The unsymmetric protonation breaks the initial structural symmetry of DADK, resulting in ca. 50-fold increas...
Source: Angewandte Chemie - April 22, 2024 Category: Chemistry Authors: Xiaolin Zhu Yihui Jia Yuhan Liu Jingyi Xu Huarui He Siyue Wang Yang Shao Yaxin Zhai Yongfa Zhu Source Type: research
Micelles Cascade Assembly to Tandem Porous Catalyst for Waste Plastics Upcycling
Angew Chem Int Ed Engl. 2024 Apr 21:e202405252. doi: 10.1002/anie.202405252. Online ahead of print.ABSTRACTCatalytic upcycling of polyolefins into high-value chemicals represents the direction in end-of-life plastics valorization, but poses great challenges. Here, we report the synthesis of a tandem porous catalyst via a micelle cascade assembly strategy for selectively catalytic cracking of polyethylene into olefins at a low temperature. A hierarchically porous silica layer from mesopore to macropore is constructed on the surface of microporous ZSM-5 nanosheets through cascade assembly of dynamic micelles. The outer macro...
Source: Angewandte Chemie - April 22, 2024 Category: Chemistry Authors: Jiayou Feng Jindi Duan Chin-Te Hung Zhenghao Zhang Kailin Li Yan Ai Chaochao Yang Yiyue Zhao Zhengmin Yu Yahong Zhang Liang Wang Dongyuan Zhao Wei Li Source Type: research
Neuron-Like Silicone Nanofilaments@Montmorillonite Nanofillers of PEO-Based Solid-State Electrolytes for Lithium Metal Batteries with Wide Operation Temperature
Angew Chem Int Ed Engl. 2024 Apr 22:e202400091. doi: 10.1002/anie.202400091. Online ahead of print.ABSTRACTPoly(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 nanofillers are synthesized by controllably grafting silicone nanofilaments onto montmorillonite nanosheets. Compared to v...
Source: Angewandte Chemie - April 22, 2024 Category: Chemistry Authors: Wankai Wang Yanfei Yang Jie Yang Junping Zhang Source Type: research
