-
Porous Aromatic Frameworks Enabling Polyiodide Confinement toward High Capacity and Long Lifespan Zinc–Iodine Batteries Adv. Mater. (IF 29.4) Pub Date : 2024-05-07 Junfang Hu, Zhaofu Zhang, Ting Deng, Feng Chao Cui, Xiaoyuan Shi, Yuyang Tian, Guangshan Zhu
Aqueous zinc–iodine batteries (AZIBs) are attracting increasing attention because of their high safety and abundance of resources. However, the performance of AZIBs is compromised by inadequate confinement of soluble polyiodides, the undesired shuttle effect, and slow reaction kinetics. In this study, a porous aromatic framework (PAF) with abundant benzene motifs and a well-organized pore structure
-
Design of Fluorinated Elastomeric Electrolyte for Solid-State Lithium Metal Batteries Operating at Low Temperature and High Voltage Adv. Mater. (IF 29.4) Pub Date : 2024-05-07 Jinseok Park, Hyeonseok Seong, Chanho Yuk, Dongkyu Lee, Youyoung Byun, Eunji Lee, Wonho Lee, Bumjoon J. Kim
We demonstrate the low-temperature operation of solid-state lithium metal batteries (LMBs) through the development of a fluorinated and plastic-crystal-embedded elastomeric electrolyte (F-PCEE). The F-PCEE is formed via polymerization-induced phase separation between the polymer matrix and plastic crystal phase, offering a high mechanical strain (∼300%) and ionic conductivity (∼0.23 mS cm−1) at -10 °C
-
Regulation of Protein Conformation Enables Cell-Selective Targeting of Virus-Mimicking Nanoparticles for siRNA Therapy of Glioblastoma Adv. Mater. (IF 29.4) Pub Date : 2024-05-06 Han Zhu, Yi-Fan Wang, Zhi-Gang Wang, Dai-Wen Pang, Shu-Lin Liu
Orthotopic glioblastoma (GBM) has an aggressive growth pattern and complex pathogenesis, becoming one of the most common and deadly tumors of the central nervous system (CNS). The emergence of RNA therapies offers promise for the treatment of GBM. However, the efficient and precise delivery of RNA drugs to specific tumor cells in the brain with high cellular heterogeneity remains ongoing. Here, we
-
On-Command Disassembly of Microrobotic Superstructures for Transport and Delivery of Magnetic Micromachines (Adv. Mater. 18/2024) Adv. Mater. (IF 29.4) Pub Date : 2024-05-02 Fabian C. Landers, Valentin Gantenbein, Lukas Hertle, Andrea Veciana, Joaquin Llacer-Wintle, Xiang-Zhong Chen, Hao Ye, Carlos Franco, Josep Puigmartí-Luis, Minsoo Kim, Bradley J. Nelson, Salvador Pané
-
-
-
Isothiourea-Catalysed Acylative Dynamic Kinetic Resolution of Tetra-substituted Morpholinone and Benzoxazinone Lactols Angew. Chem. Int. Ed. (IF 16.6) Pub Date : 2024-05-07 Haoxiang Zhu, Alejandro Manchado, Abikani Omar Farah, Aidan McKay, David Cordes, Paul Ha-Yeon Cheong, Kevin Kasten, Andrew David Smith
The development of methods to allow the selective acylative dynamic kinetic resolution (DKR) of tetra-substituted lactols is a recognised synthetic challenge. In this manuscript, a highly enantioselective isothiourea-catalysed acylative DKR of tetra-substituted morpholinone and benzoxazinone-derived lactols is reported. The scope and limitations of this methodology have been developed, with high enantioselectivity
-
Recent Progress in Using Covalent Organic Frameworks to Stabilize Metal Anodes for Highly-Efficient Rechargeable Batteries Angew. Chem. Int. Ed. (IF 16.6) Pub Date : 2024-05-07 Jianlu Sun, Fangyuan Kang, Dongbo Yan, Tangjing Ding, Yulong Wang, Xiaosi Zhou, Qichun Zhang
Alkali metals (Li, Na, and K) and multivalent metals (Zn, Mg, Ca, and Al) have become star anodes for developing high-energy-density rechargeable batteries due to their high theoretical capacity and excellent conductivity. However, the inevitable dendrites and unstable interfaces of metal anodes pose challenges to the safety and stability of batteries. To address these issues, covalent organic frameworks
-
Enantioselective Synthesis of Tetra-substituted 3-Hydroxyphthalide Esters by Isothiourea-Catalysed Acylative Dynamic Kinetic Resolution Angew. Chem. Int. Ed. (IF 16.6) Pub Date : 2024-05-07 Shubham Agrawal, Pankaj Majhi, Alister Goodfellow, Raj Tak, David Cordes, Aidan McKay, Kevin Kasten, Michael Buehl, Andrew David Smith
A general and highly enantioselective method for the preparation of tetra-substituted 3-hydroxyphthalide esters via isothiourea-catalysed acylative dynamic kinetic resolution (DKR) is reported. Using (2S,3R)-HyperBTM (5 mol%) as the catalyst, the scope and limitations of this methodology have been extensively probed, with high enantioselectivity and good to excellent yields observed (>40 examples,
-
Synthetic Sialosides Terminated with 8-N-Substituted Sialic Acid as Selective Substrates for Sialidases from Bacteria and Influenza Viruses Angew. Chem. Int. Ed. (IF 16.6) Pub Date : 2024-05-07 Bijoyananda Mishra, Yue Yuan, Hai Yu, Hyeog Kang, Jin Gao, Robert Daniels, Xi Chen
Sialosides containing C8-modified sialic acids are challenging synthetic targets but potentially useful probes for diagnostic substrate profiling of sialidases and elucidating the binding specificity of sialic acid-interacting proteins. Here, we demonstrate efficient chemoenzymatic methods for synthesizing para-nitrophenol-tagged a2–3- and a2–6-linked sialyl galactosides containing C8-acetamido, C8-azido
-
Zwitterionic Cellulose-based Polymer Electrolyte Enabled by Aqueous Solution Casting for High-performance Solid-state Batteries Angew. Chem. Int. Ed. (IF 16.6) Pub Date : 2024-05-07 Yong Cheng, Zhichao Cai, Jinglei Xu, Zhefei Sun, Xiaoyu Wu, Jiajia Han, Huiyao Wang, Mingsheng Wang
Polyethylene oxide (PEO)-based solid-state batteries hold great promise as the next-generation batteries with high energy density and high safety. However, PEO-based electrolytes encounter certain limitations, including inferior ionic conductivity, low Li+ transference number, and poor mechanical strength. Herein, we aim to simultaneously address these issues by utilizing one-dimensional zwitterionic
-
Site-Selective Ortho/Ipso C-H Difunctionalizations of Arenes using Thianthrene as a Leaving Group Angew. Chem. Int. Ed. (IF 16.6) Pub Date : 2024-05-07 Dorian Dupommier, Martin Vuagnat, Javid Rzayev, Sourav Roy, Philippe Jubault, Tatiana Besset
Site-selective ortho/ipso C-H difunctionalizations of aromatic compounds were designed to afford polyfunctionalized arenes including challenging 1,2,3,4-tetrasubstituted ones (62 examples, up to 97% yields). To ensure the excellent regioselectivity of the process while keeping high efficiency, an original strategy based on a “C-H thianthenation/Catellani-type reaction” sequence was developed starting
-
Engineered Phenylalanine Ammonia-Lyases for the Enantioselective Synthesis of Aspartic Acid Derivatives Angew. Chem. Int. Ed. (IF 16.6) Pub Date : 2024-05-07 Ivan Buslov, Sarah Desmons, Yoan Duhoo, Xile Hu
Biocatalytic hydroamination of alkenes is an efficient and selective method to synthesize natural and unnatural amino acids. Phenylalanine ammonia-lyases (PALs) have been previously engineered to access a range of substituted phenylalanines and heteroarylalanines, but their substrate scope remains limited, typically including only arylacrylic acids. Moreover, the enantioselectivity in the hydroamination
-
Room-Temperature Near-Infrared Phosphorescence from C64 Nanographene Tetraimide by π-Stacking Complexation with Platinum Porphyrin Angew. Chem. Int. Ed. (IF 16.6) Pub Date : 2024-05-07 M. A. Niyas, Swadhin Garain, Kazutaka Shoyama, Frank Würthner
Near-Infrared (NIR) phosphorescence at room temperature is challenging to achieve for organic molecules due to negligible spin–orbit coupling and a low energy gap leading to fast non-radiative transitions. Here, we show a supramolecular host–guest strategy to harvest the energy from the low-lying triplet state of C64 nanographene tetraimide 1. 1H NMR and X-ray analysis confirmed the 1:2 stoichiometric
-
A Cages-on-Cluster Structure Constructed by Post-Clustering Covalent Modifications and Guest-Enabled Stimuli-Responsive Luminescence Angew. Chem. Int. Ed. (IF 16.6) Pub Date : 2024-05-07 Yang Yang, Shan Guo, Qian Zhang, Zong-Jie Guan, Quan-Ming Wang
A novel gold(I)-cluster-based twin-cage is constructed by post-clustering covalent modification of a hexa-aldehyde cluster precursor with triaminotriethylamines. The cages-on-cluster structure have double cavities and four binding sites, showing site discriminative binding for silver(I) and copper(I) guests. The guests in the tripodal hats affect the luminescence of the cluster: tetra-silver(I) host-guest
-
Lattice Mismatch at the Heterojunction of Perovskite Solar Cells Angew. Chem. Int. Ed. (IF 16.6) Pub Date : 2024-05-07 Yong Wang, Dexu Zheng, Kai Wang, Qi Yang, Jin Qian, Jiaju Zhou, Shengzhong (Frank) Liu, Dong Yang
Lattice mismatch significantly influences microscopic transport in semiconducting devices, affecting interfacial charge behavior and device efficacy. This atomic-level disordering, often overlooked in previous research, is crucial for device efficiency and lifetime. Recent studies have highlighted emerging challenges related to lattice mismatch in perovskite solar cells, especially at heterojunctions
-
Development of Stable Water-Soluble Supratomic Silver Clusters Utilizing A Polyoxoniobate-Protected Strategy: Giant Core-Shell-Type Ag8@Nb162 Fluorescent Nanocluster Angew. Chem. Int. Ed. (IF 16.6) Pub Date : 2024-05-07 Li-Hao Hong, Sheng-Nan Yue, Xing Huang, Cai Sun, Ping-Wei Cai, Yan-Qiong Sun, Xin-Xiong Li, Shou-Tian Zheng
Atomically precise low-nuclearity (n<10) silver nanoclusters (AgNCs) have garnered significant interest due to their size-dependent optical properties and diverse applications. However, their synthesis has remained challenging, primarily due to their inherent instability. The present study introduces a new feasible approach for clustering silver ions utilizing highly negative and redox-inert polyoxoniobates
-
A Cytochrome P450 Enzyme Catalyses Oxetane Ring Formation in Paclitaxel Biosynthesis Angew. Chem. Int. Ed. (IF 16.6) Pub Date : 2024-05-07 Changkang Li, Xinxin Yin, Shuai Wang, Songyang Sui, Jimei Liu, Xincheng Sun, Jinming Di, Ridao Chen, Dawei Chen, Yaotian Han, Kebo Xie, Jungui Dai
Oxetane synthase (TmCYP1), a novel cytochrome P450 enzyme from Taxus × media cell cultures, has been functionally characterized to efficiently catalyse the formation of the oxetane ring in tetracyclic taxoids. Transient expression of TmCYP1 in Nicotiana benthamiana using 2α,5α,7β,9α,10β,13α-hexaacetoxytaxa-4(20),11(12)-diene (1) as a substrate led to the production of a major oxetane derivative, 1β-dehydroxybaccatin
-
Molecularly Tunable Heterostructured Co-polymers Containing Electron-deficient and -rich Moieties for Visible-light and Sacrificial-agent-free H2O2 Photosynthesis Angew. Chem. Int. Ed. (IF 16.6) Pub Date : 2024-05-07 Jingzhao Cheng, Wang Wang, Jianjun Zhang, Sijie Wan, Bei Cheng, Jiaguo Yu, Shaowen Cao
As an alternative to hydrogen peroxide (H2O2) production by complex anthraquinone oxidation process, photosynthesis of H2O2 from water and oxygen without sacrificial agents is highly demanded. Herein, a covalently connected molecular heterostructure is synthesized via sequential C−H arylation and Knoevenagel polymerization reactions for visible-light and sacrificial-agent-free H2O2 synthesis. The subsequent
-
Responsive Organic Fluorescent Aggregates Based on Ion-π Interactions Away from Fluorescent Conjugated Groups Angew. Chem. Int. Ed. (IF 16.6) Pub Date : 2024-05-07 Guanqun Zhu, Zhiyang Liu, Qi Qi, Junfei Xing, Quan Li
Responsive organic luminescent aggregates have a wide range of application fields, but currently there is still a lack of reasonable molecular design strategies. Introducing ion-π interactions into molecules can effectively alter their luminescent properties. However, current research typically focuses on ion localization at luminescent conjugated groups with the strong interaction forces. In this
-
ON-OFF Control of Marangoni Self-propulsion via A Supra-amphiphile Fuel and Switch Angew. Chem. Int. Ed. (IF 16.6) Pub Date : 2024-05-07 Guiqiang Zhu, Shu Zhang, Guoxin Lu, Benwei Peng, Cuiling Lin, Liqun Zhang, Feng Shi, Qian Zhang, Mengjiao Cheng
Marangoni self-propulsion refers to motions of liquid or solids driven by a surface tension gradient, and has applications in soft robots/devices, cargo delivery, self-assembly etc. However, two problems remain to be addressed for motion control (e.g., ON-OFF) with conventional surfactants as Marangoni fuel: (1) limited motion lifetime due to saturated interfacial adsorption of surfactants; (2) in-
-
Size and Polarizability of Boron Cluster Carriers Modulate Chaotropic Membrane Transport Angew. Chem. Int. Ed. (IF 16.6) Pub Date : 2024-05-07 Giulia Salluce, Yeray Folgar-Cameán, Andrea Barba-Bon, Ivana Nikšić-Franjić, Suzan El Anwar, Bohumír Grüner, Irene Lostale-Seijo, Werner Nau, Javier Montenegro
Perhalogenated closo-borates represent a new class of membrane carriers. They owe this activity to their chaotropicity, which enables the transport of hydrophilic molecules across model membranes and into living cells. The transport efficiency of this new class of cluster carriers depends on a careful balance between their affinity to membranes and cargo, which varies with chaotropicity. However, the
-
Interface Dipole Management of D-A-Type Molecules for Efficient Perovskite Solar Cells Angew. Chem. Int. Ed. (IF 16.6) Pub Date : 2024-05-07 Hongze Wang, Junbo Wang, Qingyun He, Jingxi Chang, Shaoyu Chen, Chongyu Zhong, Mengyang Wu, Xiangru Zhao, Haoyu Chen, Qiushuang Tian, Mubai Li, Jingya Lai, Yingguo Yang, Renzhi Li, Bo Wu, Wei Huang, Tianshi Qin, Fangfang Wang
Interfacial engineering of perovskite films has been the main strategies in improving the efficiency and stability of perovskite solar cells (PSCs). In this study, three new donor-acceptor (D-A)-type interfacial dipole (DAID) molecules with hole-transporting and different anchoring units are designed and employed in PSCs. The formation of interface dipoles by the DAID molecules on the perovskite film
-
Mechanical Strain Induces and Increases Vesicular Release Monitored by Microfabricated Stretchable Electrodes Angew. Chem. Int. Ed. (IF 16.6) Pub Date : 2024-05-06 Jing Yan, Fu-Li Zhang, Kai-Qi Jin, Jia-Xin Li, Li-Jun Wang, Wen-Ting Fan, Wei-Hua Huang, Yan-Ling Liu
Exocytosis involving the fusion of intracellular vesicles with cell membrane, is thought to be modulated by the mechanical cues in the microenvironment. Single-cell electrochemistry can offer unique information about the quantification and kinetics of exocytotic events, however, the effects of mechanical force on vesicular release has been poorly explored. Herein, we developed a stretchable microelectrode
-
Unnatural Direct Interspecies Electron Transfer Enabled by Living Cell-Cell Click Chemistry Angew. Chem. Int. Ed. (IF 16.6) Pub Date : 2024-05-06 Yi-Cheng Zhao, Chong Sha, Xing-Ming Zhao, Jia-Xin Du, Long Zou, Yang-Chun Yong
Direct interspecies electron transfer (DIET) is essential for maintaining the function and stability of anaerobic microbial consortia. However, only limited natural DIET modes have been identified and DIET engineering remains highly challenging. Here, an unnatural DIET between Shewanella oneidensis MR-1 (SO, electron donating partner) and Rhodopseudomonas palustris (RP, electron accepting partner)
-
Sono-Triggered Cascade Lactate Depletion by Semiconducting Polymer Nanoreactors for Cuproptosis-Immunotherapy of Pancreatic Cancer Angew. Chem. Int. Ed. (IF 16.6) Pub Date : 2024-05-06 Ningyue Yu, Jianhui Zhou, Mengbin Ding, Meng Li, Shaojun Peng, Jingchao Li
The high level of lactate in tumor microenvironment not only promotes tumor development and metastasis, but also induces immune escape, which often leads to failures of various tumor therapy strategies. We here report a sono-triggered cascade lactate depletion strategy by using semiconducting polymer nanoreactors (SPNLCu) for cancer cuproptosis-immunotherapy. The SPNLCu mainly contain a semiconducting
-
Ultralow Catalytic Loading for Optimised Electrocatalytic Performance of AuPt Nanoparticles to Produce Hydrogen and Ammonia Angew. Chem. Int. Ed. (IF 16.6) Pub Date : 2024-05-06 Leticia S. Bezerra, Paul Brasseur, Sam Sullivan–Allsop, Rongsheng Cai, Kaline N. da Silva, Shiqi Wang, Harishchandra Singh, Ashok K. Yadav, Hugo L. S. Santos, Mykhailo Chundak, Ibrahim Abdelsalam, Vilma J. Heczko, Elton Sitta, Mikko Ritala, Wenyi Huo, Thomas J. A. Slater, Sarah J. Haigh, Pedro Camargo
The hydrogen evolution and nitrite reduction reactions are key to producing green hydrogen and ammonia. Antenna–reactor nanoparticles hold promise to improve the performances of these transformations under visible-light excitation, by combining plasmonic and catalytic materials. However, current materials involve compromising either on the catalytic activity or the plasmonic enhancement and also lack
-
Deep Red Light Driven Hydrogen Evolution by Heterojunction Polymer Dots for Diabetic Wound Healing Angew. Chem. Int. Ed. (IF 16.6) Pub Date : 2024-05-06 Feixue Mi, Zhao Liu, Xinyu Wang, Yingjie Wang, Junfeng Yang, Zhe Wang, Shengyan Yin, Xiaofeng Fang, Peng Shu, Xuanjun Zhang, Changfeng Wu
We describe small heterojunction polymer dots (Pdots) with deep-red light catalyzed H2 generation for diabetic skin wound healing. The Pdots with donor/acceptor heterojunctions showed remarkably enhanced photocatalytic activity as compared to the donor or acceptor nanoparticles alone. We encapsulate the Pdots and ascorbic acid into liposomes to form Lipo-Pdots nanoreactors, which selectively scavenge
-
Selective Photoreforming of Waste Plastics into Diesel Olefins via Single Reactive Oxygen Species Angew. Chem. Int. Ed. (IF 16.6) Pub Date : 2024-05-06 Shuai Yue, Zhiyong Zhao, Tao Zhang, Fei Li, Kewang Liu, Sihui Zhan
The accumulation of plastic waste poses a pressing environmental challenge. Catalytic conversion stands out as an ideal approach for plastics upcycling, particularly through solar-driven plastics photoreforming. However, due to the common effects of multiple reactive oxygen species (ROS), selectively generating high-value chemicals becomes challenging. In this study, we developed a universal strategy
-
Unveiling the Mechanistic Role of Chiral Palladacycles in Pd(II)-Catalyzed Enantioselective C(sp3)-H Functionalization Angew. Chem. Int. Ed. (IF 16.6) Pub Date : 2024-05-06 Chen-Hui Yuan, Xiao-Xia Wang, Keyun Huang, Lei Jiao
Palladium-catalyzed enantioselective C(sp3)-H functionalization reactions has attracted considerable attention due to its ability for the synthesis of enantiomerically enriched molecules and stimulation of novel retrosynthetic disconnections. Understanding the reaction mechanism, especially the stereochemical process of the reaction, is crucial for the rational design of more efficient catalytic systems
-
Tuning Ion Mobility in Lithium Argyrodite Solid Electrolytes via Entropy Engineering Angew. Chem. Int. Ed. (IF 16.6) Pub Date : 2024-05-06 Jing Lin, Mareen Schaller, Sylvio Indris, Volodymyr Baran, Ajay Gautam, Jürgen Janek, Aleksandr Kondrakov, Torsten Brezesinski, Florian Strauss
The development of improved solid electrolytes (SEs) plays a crucial role in the advancement of bulk-type solid-state battery (SSB) technologies. Recently, multicomponent or high-entropy SEs are gaining increased attention for their advantageous charge transport and (electro)chemical properties. However, a comprehensive understanding of how configurational entropy affects ionic conductivity is largely
-
A Luminescent Hybrid Bimetallic Halide Family with Solvent-Coordinated Rare Earth and Alkaline Earth Metals Angew. Chem. Int. Ed. (IF 16.6) Pub Date : 2024-05-06 Jiawei Lin, Pan Wang, Jiaqian Zhou, Lingling Mao
Hybrid metal halides are an extraordinary class of optoelectronic materials with extensive applications. To further diversify and study the in-depth structure-property relations, we report here a new family of 21 zero-dimensional hybrid bimetallic chlorides with the general formula A(L)n[BClm] (A = rare earth (RE), alkaline earth metals and Mn; L = solvent ligand; and B = Sb, Bi and Te). The Ln(DMSO)8[BCl6]
-
A Fluorinated Chaperone Gives X-ray Crystal Structures of Acyclic Natural Product Derivatives up to 338 Molecular Weight Angew. Chem. Int. Ed. (IF 16.6) Pub Date : 2024-05-06 Tim Berking, Jan Hartenfels, Carsten Lenczyk, Gustavo Santiso-Quinones, Wolfgang Frey, Clemens Richert
Crystallizing molecules with long flexible chains is a challenge, making it difficult to perform X-ray crystallography. Chaperones can assist in the crystallization of compounds that do not crystallize by themselves by producing solvate crystals that contain the analyte in their three-dimensional lattices. Among the most versatile chaperones for liquid analytes are tetraaryladamantanes (TAAs), but
-
Enhancing the Life Cycle of Zinc-Iodine Batteries in Ionic Liquid-Based Electrolyte Angew. Chem. Int. Ed. (IF 16.6) Pub Date : 2024-05-06 Mega Kar, Cristina Pozo-Gonzalo
Aqueous zinc-iodine (Zn-I2) batteries are gaining significant attention due to their low-cost, high safety and high theoretical capacity. Nevertheless, their long cycle and durability have been hampered due to the use of aqueous media that overtime lead to Zn dendrite formation, hydrogen evolution reaction, and polyiodide dissolution. Xiao et. al., recently reported the addition of an imidazolium-based
-
Achieving a Deeply Desodiated Stabilized Cathode Material by the High Entropy Strategy for Sodium-ion Batteries Angew. Chem. Int. Ed. (IF 16.6) Pub Date : 2024-05-06 Zhaoguo Liu, Rixin Liu, Sheng Xu, Jiaming Tian, Jingchang Li, Haoyu Li, Tao Yu, Shiyong Chu, Anita M. D'Angelo, Wei Kong Pang, Liang Zhang, Shaohua Guo, Haoshen Zhou
Manganese-based layered oxides are currently of significant interest as cathode materials for sodium-ion batteries due to their low toxicity and high specific capacity. However, the practical applications are impeded by sluggish intrinsic Na+ migration and poor structure stability as a result of Jahn-Teller distortion and complicated phase transition. In this study, a high-entropy strategy is proposed
-
Regulating Spin Density using TEMPOL Molecules for Enhanced CO2-to-Ethylene Conversion by HKUST-1 Framework Derived Electrocatalysts Angew. Chem. Int. Ed. (IF 16.6) Pub Date : 2024-05-06 Baipeng Yin, Can Wang, Shijie Xie, Jianmin Gu, Hua Sheng, De-Xian Wang, Jiannian Yao, Chuang Zhang
The selectivity of multicarbon products in the CO2 reduction reaction (CO2RR) depends on the spin alignment of neighboring active sites, which requires a spin catalyst that facilitates electron transfer with antiparallel spins for enhanced C-C coupling. Here, we design a radical-contained spin catalyst (TEMPOL@HKUST-1) to enhance CO2-to-ethylene conversion, in which spin-disordered (SDO) and spin-ordered
-
BINOL-based Chiral Macrocycles and Cages Angew. Chem. Int. Ed. (IF 16.6) Pub Date : 2024-05-06 Yabing Yu, Yaning Hu, Chengbing Ning, Wudi Shi, Ao Yang, Yibo Zhao, Zhongyan Cao, Youzhi Xu, Pingwu Du
Chirality, a fundamental principle in chemistry, biology, and medicine, is prevalent in nature and in organisms. Chiral molecules, such as DNA, RNA, and proteins, are crucial in biomolecular synthesis, as well as in the development of functional materials. Among these, 1,1´-binaphthyl-2,2´-diol (BINOL) stands out for its stable chiral configuration, versatile functionality, and commercial availability
-
Tailoring Electric Double Layer by Cation Specific Adsorption for High-voltage Quasi-solid-state Lithium Metal Batteries Angew. Chem. Int. Ed. (IF 16.6) Pub Date : 2024-05-06 Qingjie Zhou, Huaian Zhao, Chuankai Fu, Jiyuan Jian, Hua Huo, Yulin Ma, Chunyu Du, Yunzhi Gao, Geping Yin, Pengjian Zuo
The interfacial instability of high-nickel layered oxides severely plagues practical application of high-energy quasi-solid-state lithium metal batteries (LMBs). Herein, a uniform and highly oxidation-resistant polymer layer within inner Helmholtz plane is engineered by in-situ polymerizing 1-vinyl-3-ethylimidazolium (VEIM) cations preferentially adsorbed on LiNi0.83Co0.11Mn0.06O2 (NCM83) surface,
-
Multivariate Silicification-Assisted Single Enzyme Structure Augmentation for Improved Enzymatic Activity-Stability Trade-Off Angew. Chem. Int. Ed. (IF 16.6) Pub Date : 2024-05-06 Guansheng Zheng, Junxian Yang, Liang Zhou, Anna Sinelshchikova, Qi Lei, Jiangguo Lin, Stefan Wuttke, C. Jeffrey Brinker, Wei Zhu
The ability to finely tune/balance the structure and rigidity of enzymes to realize both high enzymatic activity and long-term stability is highly desired but highly challenging. In this work, we propose a new concept of silica-enzyme, referred to as “silicazyme”, where solid inorganic silica was controlled hybridization with fragile enzyme under moderate condition at single-enzyme level, realizing
-
Giant ab-Plane Birefringence in Quasi-1D Fibrous Red Phosphorus Angew. Chem. Int. Ed. (IF 16.6) Pub Date : 2024-05-06 Wujia Chen, Bowen Zhang, Kezheng Tao, Qiang Li, Jia-Lin Sun, Qingfeng Yan
Quasi-one-dimensional (quasi-1D) van der Waals crystal fibrous red phosphorus (RP) exhibits pronounced in-plane optical anisotropy, positioning it as a potential candidate for polarization-related micro-nano devices. Unfortunately, a comprehensive investigation into the complex refractive index of fibrous RP and the structure-activity relationship connecting the distinctive quasi-1D structure with
-
Nonflammable Phosphate-Based Electrolyte for Safe and Stable Potassium Batteries Enabled by Optimized Solvation Effect Angew. Chem. Int. Ed. (IF 16.6) Pub Date : 2024-05-06 Dianwei Zhang, Hongwei Hu, Xuemei Ma, Xinzhi Yu, Fuxiang Li, Jiang Zhou, Bingan Lu
Current potassium-ion batteries (PIBs) are limited in safety and lifetime owing to the lack of suitable electrolyte solutions. To address these issues, herein, we report an innovative non-flammable electrolyte design strategy that leverages an optimal moderate solvation phosphate-based solvent which strikes a balance between solvation capability and salt dissociation ability, leading to superior electrochemical
-
Revealing Hydrogen Bond Effect in Rechargeable Aqueous Zinc-Organic Batteries Angew. Chem. Int. Ed. (IF 16.6) Pub Date : 2024-05-05 Jun Guo, Jia-Yi Du, Wan-Qiang Liu, Gang Huang, Xin-bo Zhang
The surrounding hydrogen bond (H-bond) interaction around the active sites plays indispensable functions in enabling the organic electrode materials (OEMs) to fulfill their roles as ion reservoirs in aqueous zinc-organic batteries (ZOBs). Despite important, there are still no works could fully shed its real effects light on. Herein, quinone-based small molecules with a H-bond evolution model has been
-
Understanding Spin-Triplet Excited States in Carbene-Metal-Amides Angew. Chem. Int. Ed. (IF 16.6) Pub Date : 2024-05-05 Antti-Pekka M. Reponen, Giacomo Londi, Campbell S. B. Matthews, Yoann Olivier, Alexander S. Romanov, Neil C. Greenham, Alexander J Gillett
Carbene-metal-amides (CMAs) are emerging delayed fluorescence materials for organic light-emitting diode (OLED) applications. CMAs possess fast, efficient emission owing to rapid forward and reverse intersystem crossing (ISC) rates. The resulting dynamic equilibrium between singlet and triplet spin manifolds distinguishes CMAs from most purely organic thermally activated delayed fluorescence emitters
-
Programming Tetrathiafulvalene-Based Covalent Organic Frameworks for Promoted Photoinduced Molecular Oxygen Activation Angew. Chem. Int. Ed. (IF 16.6) Pub Date : 2024-05-05 Hetao Xu, Shuling Xia, Chunlei Li, Yang Li, Wandong Xing, Yi Jiang, Xiong Chen
Despite the pivotal role of molecular oxygen (O2) activation in artificial photosynthesis, the activation efficiency is often restricted by sluggish exciton dissociation and charge transfer kinetics within polymer photocatalysts. Herein, we propose two tetrathiafulvalene (TTF)-based imine-linked covalent organic frameworks (COFs) with tailored donor-acceptor (D-A) structures, TTF-PDI-COF and TTF-TFPP-COF
-
Aqueous Developable and CO2-Sourced Chemical Amplification Photoresist with High Performance Angew. Chem. Int. Ed. (IF 16.6) Pub Date : 2024-05-05 Xin-Yu Lu, Rui-Sheng Zhang, Guan-Wen Yang, Qiang Li, Bo Li, Guang-Peng Wu
Seeking high-performance photoresist is an important item for semiconductor industry due to the continuous miniaturization and intelligentization of integrated circuits. Polymer resin containing carbonate group has many desirable properties, such as high transmittance, acid sensitivity and chemical formulation, thus serving as potential photoresist material. In this work, a series of aqueous developable
-
An Engineered Nanoplatform with Tropism toward Irradiated Glioblastoma Augments Its Radioimmunotherapy Efficacy Adv. Mater. (IF 29.4) Pub Date : 2024-05-07 Zheng Wang, Fangman Chen, Yi Cao, Fan Zhang, Lina Sun, Chao Yang, Xiaochun Xie, Ziping Wu, Madi Sun, Fanshu Ma, Dan Shao, Kam W. Leong, Renjun Pei
Combining radiotherapy with immune checkpoint blockade therapy offers a promising approach to treat glioblastoma multiforme (GBM), yet challenges such as limited effectiveness and immune-related adverse events (irAEs) persist. These issues are largely due to the failure in targeting immunomodulators directly to the tumor microenvironment. To address this, we developed a biomimetic nanoplatform that
-
Oxygen-Centered Organic Radicals-Involved Unified Heterogeneous Self-Fenton Process for Stable Mineralization of Micropollutants in Water Adv. Mater. (IF 29.4) Pub Date : 2024-05-07 Liwei Zhang, Yuyan Huang, Huijie Yan, Yingyi Cheng, Yu-Xin Ye, Fang Zhu, Gangfeng Ouyang
Removing organic micropollutants from water through photocatalysis is hindered by catalyst instability and substantial residuals from incomplete mineralization. Here, we present a novel water treatment paradigm, the unified heterogeneous self-Fenton process (UHSFP), which achieved an impressive 32% photon utilization efficiency at 470 nm, and a significant 94% mineralization of organic micropollutants—all
-
Perovskite Colloidal Nanocrystal Solar Cells: Current Advances, Challenges and Future Perspectives Adv. Mater. (IF 29.4) Pub Date : 2024-05-06 Wenqiang Yang, Seung-Hyeon Jo, Tae-Woo Lee
The power conversion efficiencies (PCEs) of polycrystalline perovskite (PVK) solar cells (SCs) (PC-PeSCs) have been rapidly increased. However, PC-PeSCs are intrinsically unstable without encapsulation, and their efficiency drops during large-scale production; these problems hinder the commercial viability of PeSCs. Stability can be increased by using colloidal PVK nanocrystals (c-PeNCs), which have
-
Accelerated Engineering of ELP-based Materials through Hybrid Biomimetic-De Novo Predictive Molecular Design Adv. Mater. (IF 29.4) Pub Date : 2024-05-06 Timo Laakko, Antti Korkealaakso, Burcu Firatligil Yildirir, Piotr Batys, Ville Liljeström, Ari Hokkanen, Nonappa, Merja Penttilä, Anssi Laukkanen, Ali Miserez, Caj Södergård, Pezhman Mohammadi
Efforts to engineer high-performance protein-based materials inspired by nature have mostly focused on altering naturally occurring sequences to confer the desired functionalities, whereas de novo design lags significantly behind and calls for unconventional innovative approaches. Here, using partially disordered elastin-like polypeptides (ELPs) as initial building blocks we show that de novo engineering
-
Tandem Electric-Fields Prolong Energetic Hot Electrons Lifetime for Ultra-Fast and Stable NO2 Detection Adv. Mater. (IF 29.4) Pub Date : 2024-05-06 Yucheng Ou, Bing Wang, Nana Xu, Quzhi Song, Tao Liu, Hui Xu, Fuwen Wang, Siwei Li, Yingde Wang
Prolonging energetic hot electrons lifetimes and surface activity in the reactive site can overcome the slow kinetics and unfavorable thermodynamics of photo-activated gas sensors. However, bulk and surface recombination limit simultaneous optimization of both kinetics and thermodynamic. Here we deploy tandem electric-fields at (111)/(100)Au-CeO2 to ensure a sufficient driving force for carriers transfer
-
Scalable Customization of Crystallographic Plane Controllable Lithium Metal Anodes for Ultralong-Lasting Lithium Metal Batteries Adv. Mater. (IF 29.4) Pub Date : 2024-05-06 Jian Tan, Longli Ma, Pengshu Yi, Yuan Wang, Zhiheng Li, Zhan Fang, Xuanyang Li, Shan He, Xuefeng Wang, Mingxin Ye, Jianfeng Shen
A formidable challenge to achieve the practical applications of rechargeable lithium (Li) metal batteries (RLMBs) is to suppress the uncontrollable growth of Li dendrites. One of the most effective solutions is to fabricate Li metal anodes with specific crystal plane, but still lack of a simple and high-efficient approach. Herein, to overcome this key challenge, we report a facile and controllable
-
Atto-Scale Noise near-Infrared Organic Photodetectors Enabled by Controlling Interfacial Energetic Offset through Enhanced Anchoring Ability Adv. Mater. (IF 29.4) Pub Date : 2024-05-06 Tae Hyuk Kim, Ji Hyeon Lee, Min Ho Jang, Gyeong Min Lee, Eun Soo Shim, Seunghyun Oh, Muhammad Ahsan Saeed, Min Jong Lee, Byoung Soo Yu, Do Kyung Hwang, Chae Won Park, Sae Youn Lee, Jea Woong Jo, Jae Won Shim
The near-infrared (NIR) sensor technology is crucial for various applications such as autonomous driving and biometric tracking. Silicon photodetectors (SiPDs) are widely used in NIR applications; however, their scalability is limited by their crystalline properties. Organic photodetectors (OPDs) have attracted attention for NIR applications owing to their scalability, low-temperature processing, and
-
Gate-Tunable Positive and Negative Photoconductance in Near-Infrared Organic Heterostructures for in-Sensor Computing Adv. Mater. (IF 29.4) Pub Date : 2024-05-06 Yunqi Xu, Xiaolu Xu, Ying Huang, Ye Tian, Miao Cheng, Junyang Deng, Yifan Xie, Yanqin Zhang, Panpan Zhang, Xinhua Wang, Zhongrui Wang, Mengmeng Li, Ling Li, Ming Liu
The rapid growth of sensor data in the artificial intelligence often causes significant reductions in processing speed and power efficiency. Addressing this challenge, in-sensor computing has been introduced as an advanced sensor architecture that simultaneously senses, memorizes and processes images at the sensor level. However, this has rarely been reported for organic semiconductors that possess
-
Metal-Halogen Interactions Inducing Phase Separation for Self-Healing and Tough Ionogels with Tunable Thermoelectric Performance Adv. Mater. (IF 29.4) Pub Date : 2024-05-06 Wei Zhao, Yiwei Zheng, Aibin Huang, Meng Jiang, Lianjun Wang, Qihao Zhang, Wan Jiang
Ionic liquid-based thermoelectric gels become a compelling candidate for thermoelectric power generation and sensing due to their giant thermopower, good thermal stability, high flexibility, and low-cost production. However, the materials reported to date suffer from canonical trade-offs between self-healing ability, stretchability, strength and ionic conductivity. Herein, we develop a self-healing
-
Carbon Dioxide Capture by Emerging Innovative Polymers: Status and Perspectives Adv. Mater. (IF 29.4) Pub Date : 2024-05-06 Made Ganesh Darmayanti, Kellie L. Tuck, San H. Thang
A significant amount of research has been conducted in carbon dioxide (CO2) capture, particularly over the past decade, and continues to evolve. This review presents the most recent advancements in synthetic methodologies and CO2 capture capabilities of diverse polymer-based substances, which includes the amine-based polymers, porous organic polymers, and polymeric membranes, covering publications
-
Activating Macrophage Continual Efferocytosis via Microenvironment Biomimetic Short Fibers for Reversing Inflammation in Bone Repair Adv. Mater. (IF 29.4) Pub Date : 2024-05-05 Haoran Wang, Yu Zhang, Yipu Zhang, Chao Li, Mo Zhang, Juan Wang, Yingze Zhang, Yawei Du, Wenguo Cui, Wei Chen
Efferocytosis-mediated inflammatory reversal plays a crucial role in bone repairing process. However, in refractory bone defects, the macrophage continual efferocytosis may be suppressed due to the disrupted microenvironment homeostasis, particularly the loss of apoptotic signals and overactivation of intracellular oxidative stress. In this study, we present a polydopamine-coated short fiber matrix
-
Electron Spectroscopy and Microscopy: A Window into the Surface Electronic Properties of Polycrystalline Metal Halide Perovskites Adv. Mater. (IF 29.4) Pub Date : 2024-05-06 E. Laine Wong, Giulia Folpini, Yang Zhou, Minirah Dukhi Albaqami, Annamaria Petrozza
-
Correction to “In Situ Silver-Based Electrochemical Oncolytic Bioreactor” Adv. Mater. (IF 29.4) Pub Date : 2024-05-06 Yong Huang, Liping Zhong, Xiaotong Li, Pan Wu, Jian He, Chao Tang, Zhiping Tang, Jing Su, Zhenbo Feng, Bing Wang, Yun Ma, Hongmei Peng, Zhihao Bai, Yi Zhong, Ying Liang, Wenxi Lu, Ruiyu Luo, Jinghua Li, Haiping Li, Zhiming Deng, Xianli Lan, Ziqun Liu, Kun Zhang, Yongxiang Zhao
Adv. Mater. 2022, 34, 2109973 DOI: 10.1002/adma.202109973 Figure 2N in the published article have mistakenly used images. The 2 h image of the VitC group and the 0.5 and 2 h images of the RS-CS/rGO/Ag+-DNA group were mistakenly used. The authors have made updates. We apologize for this error. Figure 2N HepG2 cells (1 × 104) were subjected to the indicated treatments for different incubation periods
-
Correction to “Conversion of Surface Residual Alkali to Solid Electrolyte to Enable Na-Ion Full Cells with Robust Interfaces” Adv. Mater. (IF 29.4) Pub Date : 2024-05-06 Weiliang Xu, Rongbin Dang, Lin Zhou, Yang Yang, Ting Lin, Qiubo Guo, Fei Xie, Zilin Hu, Feixiang Ding, Yunpeng Liu, Yuan Liu, Huican Mao, Juan Hong, Zhanchun Zuo, Xiaoqi Wang, Rui Yang, Xu Jin, Xueyan Hou, Yaxiang Lu, Xiaohui Rong, Ning Xu, Yong-Sheng Hu
Adv. Mater. 2023, 35, 2301314 DOI: 10.1002/adma.202301314 The Acknowledgements of the “This work was supported by the National Natural Science Foundation (NSFC) of China (Grant Nos. 52202333, 52002394, and 62175254).” was incorrect. This should have read: “This work was supported by the National Key R&D Program of China (2022YFB2402500) and the National Natural Science Foundation (NSFC) of China (Grant
-
Hard single-molecule magnet behavior and strong magnetic coupling in pyrazinyl radical-bridged lanthanide metallocenes Chem (IF 23.5) Pub Date : 2024-05-06 Neha Bajaj, Niki Mavragani, Alexandros A. Kitos, Daniel Chartrand, Thierry Maris, Akseli Mansikkamäki, Muralee Murugesu