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Article
| Open AccessDynamic control of DNA condensation
Artificial biomolecular condensates are valuable tools to study the design principles of phase separation. Here, the authors demonstrate and characterize a model system of artificial DNA condensates whose kinetic formation and dissolution depends on DNA inputs that activate or deactivate the phase separating DNA subunits.
- Siddharth Agarwal
- , Dino Osmanovic
- & Elisa Franco
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Article
| Open AccessDioxygen compatible electron donor-acceptor catalytic system and its enabled aerobic oxygenation
The photochemical properties of Electron Donor-Acceptor (EDA) complexes present exciting opportunities, but often require an inert atmosphere to maintain high efficiency. Here, the authors develop a photocatalytic system through rational design, which overcomes the oxygen-sensitive limitation of traditional EDA photocatalytic systems.
- Jialiang Wei
- , Junhong Meng
- & Ning Jiao
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Article
| Open AccessDimethyl sulfate and diisopropyl sulfate as practical and versatile O-sulfation reagents
O-Sulfation is a vital post-translational modification in bioactive molecules, yet there are significant challenges for the synthesis. Here, the authors report a general and robust approach to O-sulfation by harnessing the tunable reactivity of dimethyl sulfate or diisopropyl sulfate under tetrabutylammonium bisulfate activation.
- Shuaishuai Yue
- , Guoping Ding
- & Jiakun Li
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Article
| Open AccessGeneral alkyl fluoride functionalization via short-lived carbocation-organozincate ion pairs
Many alkyl fluorides are readily available, but the synthetic applications trail behind the widely accepted utility of other halides. Here, the authors report a practical Csp3-F bond functionalization method that expands the currently restricted synthetic space of unactivated C(sp3)-F bonds, but also uses benzylic, propargylic and acyl fluorides.
- D. Lucas Kane
- , Bryan C. Figula
- & Christian Wolf
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Article
| Open AccessCharging modulation of the pyridine nitrogen of covalent organic frameworks for promoting oxygen reduction reaction
The catalytic efficacy of covalent organic frameworks (COFs) is constrained by their restricted electro-transfer capability and weak binding affinities for reaction intermediates. Here the authors report COFs with various pyridinic-based units for tuning their catalytic activity towards oxygen reduction reaction.
- Xiubei Yang
- , Qizheng An
- & Gaofeng Zeng
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Article
| Open AccessOrthoID: profiling dynamic proteomes through time and space using mutually orthogonal chemical tools
Proteomics at the organelle contact site remains challenging due to the spatial and temporal dynamics of proteins. Here, the authors developed OrthoID, a mutually orthogonal dual enzymatic proteomics approach to explore the proteome at the contact site of the endoplasmic reticulum and mitochondria.
- Ara Lee
- , Gihyun Sung
- & Kimoon Kim
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Article
| Open AccessScalable production of structurally colored composite films by shearing supramolecular composites of polymers and colloids
Structurally coloured composite films are flexible optical materials with potential in a range of applications, but their production is impacted by long time-frames and limited materials. Here, the authors report a method for the production of large scale films by shearing supramolecular composites.
- Miaomiao Li
- , Bolun Peng
- & Jintao Zhu
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Article
| Open AccessElectrofreezing of liquid water at ambient conditions
By performing long ab initio molecular dynamics simulations of water under external electric fields, for up to 500 picoseconds, the authors identify a transition to a ferroelectric amorphous phase at ambient conditions.
- Giuseppe Cassone
- & Fausto Martelli
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Article
| Open AccessZirconium and hafnium catalyzed C–C single bond hydroboration
Selective cleavage and subsequent functionalization of C−C single bonds present a fundamental challenge, and the use of inexpensive and Earth-abundant group IV metals for catalytic C−C single-bond cleavage is largely underdeveloped. Here, the authors report zirconium-catalyzed C−C single-bond cleavage and subsequent hydroboration reactions.
- Sida Li
- , Haijun Jiao
- & Lipeng Wu
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Article
| Open AccessTuning light-driven oxidation of styrene inside water-soluble nanocages
Selective functionalization of C(sp2)–H bonds under ambient conditions is a persistent synthetic challenge in organic chemistry. Here the authors combine host-guest charge-transfer-based photoredox chemistry with supramolecular nano-confinement to achieve selective carbonylation of styrene by tuning the dioxygen concentration.
- Souvik Ghosal
- , Ankita Das
- & Jyotishman Dasgupta
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Article
| Open AccessMirror-image ligand discovery enabled by single-shot fast-flow synthesis of D-proteins
Mirror-image phage display has the potential for high-throughput generation of biologically stable macrocyclic D-peptide binders but is hindered by the optimization required for D-protein chemical synthesis. Here, the authors report a general mirror-image phage display pipeline based on automated flow peptide synthesis and use it to prepare and characterize 12 L/D-protein pairs.
- Alex J. Callahan
- , Satish Gandhesiri
- & Bradley L. Pentelute
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Article
| Open AccessSingle-atom tailored atomically-precise nanoclusters for enhanced electrochemical reduction of CO2-to-CO activity
Tailoring catalytic performance of atomically-precise metal nanoclusters catalysts is of great interest but remains challenging. Here, the authors report a co-eletropolymerization strategy to modify well-defined Au8 nanoclusters by single-atom sites to enhance its electrocatalytic activity for the reduction of CO2 towards CO.
- Yi-Man Wang
- , Fang-Qin Yan
- & Shuang-Quan Zang
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Article
| Open AccessContinuous strain tuning of oxygen evolution catalysts with anisotropic thermal expansion
Tuning compressive strain is an effective way to accelerate the oxygen evolution reaction kinetics. Here the authors show that anisotropic thermal expansion induces compressive strains on IrO6 octahedron in Sr2IrO4, shifting its d-band center downward and accelerating water oxidation kinetics beyond traditional thermal diffusion effects.
- Yu Du
- , Fakang Xie
- & Zhigang Zou
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Article
| Open AccessUnderstanding activity-stability tradeoffs in biocatalysts by enzyme proximity sequencing
Understanding the complex relationships between enzyme sequence, folding stability and catalytic activity is essential for applications, but current technologies cannot simultaneously resolve both stability and activity phenotypes and couple these to gene sequences at large scale. Here, the authors report Enzyme Proximity Sequencing (EP-Seq), a deep mutational scanning method to assay both expression level and catalytic activity of thousands of oxidoreductase variants from a cellular pool in a single experiment.
- Rosario Vanella
- , Christoph Küng
- & Michael A. Nash
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Article
| Open AccessDisentangling the multiorbital contributions of excitons by photoemission exciton tomography
Understanding excitonic optical excitations is integral to improving optoelectronic and photovoltaic semiconductor devices. Here, Bennecke et al. use photoemission exciton tomography to unravel the multiorbital electron and hole contributions of entangled excitonic states in the prototypical organic semiconductor C60.
- Wiebke Bennecke
- , Andreas Windischbacher
- & Stefan Mathias
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Article
| Open AccessNickel-catalyzed electrophiles-controlled enantioselective reductive arylative cyclization and enantiospecific reductive alkylative cyclization of 1,6-enynes
Transition metal-catalyzed asymmetric cyclization of 1,6-enynes is a powerful tool for the construction of chiral nitrogen-containing heterocycles, but limiting to the use of aryl or alkenyl metal reagents. Here, the authors report Ni-catalyzed enantioselective anti-arylative cyclization and enantiospecific cis-alkylative cyclization of 1,6-enynes.
- Wenfeng Liu
- , Yunxin Xing
- & Kun Shen
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Article
| Open AccessChemoenzymatic indican for light-driven denim dyeing
Conventional blue denim dyeing has both environmental and health-related consequences. Here, Bidart et al. use enzyme engineering to develop a viable method for the bulk production of indican and demonstrate dying processes which could significantly reduce the negative consequences of this billion-dollar industry.
- Gonzalo Nahuel Bidart
- , David Teze
- & Ditte Hededam Welner
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Article
| Open AccessRemote-carbonyl-directed sequential Heck/isomerization/C(sp2)–H arylation of alkenes for modular synthesis of stereodefined tetrasubstituted olefins
The synthesis of highly substituted olefins has been pursued for decades. Here, the authors show a carbonyl-directed sequential Heck/isomerization/C–H arylation of alkenes for modular synthesis of stereodefined all-carbon tetrasubstituted olefins.
- Runze Luan
- , Ping Lin
- & Weiping Su
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Article
| Open AccessDual-site segmentally synergistic catalysis mechanism: boosting CoFeSx nanocluster for sustainable water oxidation
Efficient oxygen evolution reaction electrocatalysts are essential for sustainable clean energy conversion. Here, the authors propose a Co-Fe dual-site to facilitate the ferromagnetic O-O bond coupling to achieve a great balance between activity and stability.
- Siran Xu
- , Sihua Feng
- & Jia-Nan Zhang
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Article
| Open AccessNanocurvature-induced field effects enable control over the activity of single-atom electrocatalysts
Modulating interfacial electric fields provides a means to control electrocatalyst activity for a broad range of reactions. Here the authors show that this can be achieved by tuning the nanocurvature of carbon supported single-atom catalysts.
- Bingqing Wang
- , Meng Wang
- & Yanwei Lum
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Article
| Open AccessDistance effect of single atoms on stability of cobalt oxide catalysts for acidic oxygen evolution
Dissolution of Co atoms in acidic media impedes the application of cobalt oxides in proton exchange membrane water electrolyzers. Here, the authors reveal a stabilizing effect induced by Ir single atoms on cobalt oxides that suppress Co dissolution.
- Zhirong Zhang
- , Chuanyi Jia
- & Jie Zeng
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Article
| Open AccessIn situ copper faceting enables efficient CO2/CO electrolysis
Copper electrocatalysts enable carbon dioxide/carbon monoxide reduction but suffer from low production rates. Here, the authors promote in situ growth of Cu(100) during electrolysis, enabling efficient and stable electrosynthesis of multicarbon products at industrially-relevant current densities
- Kaili Yao
- , Jun Li
- & Hongyan Liang
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Article
| Open AccessObservation of geometric phase effect through backward angular oscillations in the H + HD → H2 + D reaction
In a combined experimental and theoretical study of the H + HD → H2 + D reaction at low collision energy (1.72 eV), the authors obtain detailed information on the quantum reaction dynamics surrounding a conical intersection.
- Shihao Li
- , Jiayu Huang
- & Xueming Yang
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Article
| Open AccessTransient chemical and structural changes in graphene oxide during ripening
Graphene oxide is in demand for various applications - however, this is complicated by changing physicochemical properties over time. Here, the authors show the intrinsic, metastable, and transient states of graphene oxide colloids upon ripening.
- Hayato Otsuka
- , Koki Urita
- & Katsumi Kaneko
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Article
| Open AccessMechanically interlocked [c2]daisy chain backbone enabling advanced shape-memory polymeric materials
Mechanically interlocked structures in polymer backbones can give interesting functionality, but can be challenging to prepare and control. Here, the authors report the development of polymers with a daisy chain unit in the backbone that are capable of shape memory behaviour.
- Shang-Wu Zhou
- , Danlei Zhou
- & Da-Hui Qu
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Article
| Open AccessSelf-regulated reversal deformation and locomotion of structurally homogenous hydrogels subjected to constant light illumination
Environmentally adaptive hydrogels have great potential as soft robotics but achieving self-regulated reversal shape deformation in homogenous hydrogels under a constant stimulus is challenging. Here, the authors report responsive hydrogels functionalized with two photoswitchable spiropyrans that exhibit self-regulated transient deformation reversal when subjected to constant illumination.
- Kexin Guo
- , Xuehan Yang
- & Chuang Li
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Article
| Open AccessCreation of a point-of-care therapeutics sensor using protein engineering, electrochemical sensing and electronic integration
Low-cost point-of-care sensors are vital for precision medicine. Here, the authors have repurposed a glucometer for breast cancer therapeutic detection capable of sensing tamoxifen in human blood, utilizing blood glucose to power and amplify the therapeutic signals
- Rong Cai
- , Chiagoziem Ngwadom
- & Caroline M. Ajo-Franklin
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Article
| Open AccessCoverage enhancement accelerates acidic CO2 electrolysis at ampere-level current with high energy and carbon efficiencies
The increased surface coverage of CO2 electroreduction (CO2R) intermediates promotes CO2R at high operating current densities under strongly acidic conditions. Here the authors report a 77.4% single-pass carbon efficiency for conversion of acidic CO2R to pure formic acid.
- Xiaohan Yu
- , Yuting Xu
- & Miao Zhong
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Article
| Open AccessMechanistic exploration of polytetrafluoroethylene thermal plasma gasification through multiscale simulation coupled with experimental validation
PTFE waste, a growing ecological concern, urges the exploration of disposal methods. This study investigates PTFE’s plasma gasification, revealing POCD (oxygen) and FHD (steam) pathways. Experiments validate the above mechanism, showing an 80.12% fluorine recovery in 5 min under optimal conditions.
- Chu Chu
- , Long Long Ma
- & Guanyi Chen
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Article
| Open AccessAnomalously bright single-molecule upconversion electroluminescence
The efficiency of upconversion electroluminescence remains very low for single-molecule emitters. Here, the authors report over one order of magnitude improvement in the emission efficiency via engineering energy-level alignments for triplet relayed upconversion involving only carrier injection.
- Yang Luo
- , Fan-Fang Kong
- & Zhen-Chao Dong
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Article
| Open AccessEfficient direct repairing of lithium- and manganese-rich cathodes by concentrated solar radiation
Rapid capacity decay and voltage drop hinder lithium- and manganese-rich cathode material (LMRO) development. Here, the authors apply concentrated solar radiation arrays on cycled LMRO electrodes, inducing inverse spinel phase to boost redox activity and reversibility, yielding enhanced electrochemical performance.
- Hailong Wang
- , Xin Geng
- & Xin He
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Article
| Open AccessIn situ modulating coordination fields of single-atom cobalt catalyst for enhanced oxygen reduction reaction
The electrochemical oxygen reduction reaction plays an important role in new energy technologies such as fuel cells and metal-air batteries. Here the authors present a cobalt catalyst with a symmetry-broken Cl−Co−N4 moiety capable of dynamically modulating electron occupancy at active sites during practical reaction conditions to optimize oxygen reduction performance.
- Meihuan Liu
- , Jing Zhang
- & Qinghua Liu
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Article
| Open AccessDirect in-situ insights into the asymmetric surface reconstruction of rutile TiO2 (110)
The reconstruction of rutile TiO2 (110) impacts its surface chemistry and catalytic properties. Here, the authors offer a detailed understanding of the asymmetric surface reconstruction of TiO2 (110)-(1×2) through a combination of STEM and DFT calculations.
- Wentao Yuan
- , Bingwei Chen
- & Yong Wang
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Article
| Open AccessUnveiling the nature of Pt-induced anti-deactivation of Ru for alkaline hydrogen oxidation reaction
Despite the high intrinsic activity of Ru for hydrogen oxidation reaction, the surface oxidation-induced deactivation limits the application. Here, the authors report the introduction of Pt atoms could prevent the surface oxidation-related interfacial water network damage, preventing the deactivation of Ru.
- Yanyan Fang
- , Cong Wei
- & Gongming Wang
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Article
| Open AccessIterative design of training data to control intricate enzymatic reaction networks
Kinetic modeling of in vitro enzymatic reaction networks (ERNs) is severely hampered by the lack of training data. Here, authors introduce a methodology that combines an active learning-like approach and flow chemistry to create optimized datasets for an intricate ERN.
- Bob van Sluijs
- , Tao Zhou
- & Wilhelm T. S. Huck
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Article
| Open AccessPhotocured room temperature phosphorescent materials from lignosulfonate
It is elusive to manufacture room temperature phosphorescent (RTP) materials through effective and ambient processing approaches. Here the authors report the production of photocured RTP materials using lignosulfonate to act as RTP chromophore and photoinitiator, achieving easy preparation, low cost and good performance.
- Hongda Guo
- , Mengnan Cao
- & Zhijun Chen
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Article
| Open AccessTunable afterglow for mechanical self-monitoring 3D printing structures
Organic afterglow materials have potential in self-monitoring applications but it is challenging to design materials with desired properties. Here, the authors report the development of a lifetime tunable organic afterglow system for use in mechanical self-monitoring 3D printed structures.
- Rongjuan Huang
- , Yunfei He
- & Wei Huang
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Article
| Open AccessLarge dynamics of a phase separating arginine-glycine-rich domain revealed via nuclear and electron spins
The authors show the RNA-induced droplet formation by a component of Cajal bodies and reveal the large nanoseconds mobility of glycine residues inside droplets as a molecular factor potentially contributing to the large dynamics of Cajal bodies.
- Giuseppe Sicoli
- , Daniel Sieme
- & Nasrollah Rezaei-Ghaleh
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Article
| Open AccessSmart touchless human–machine interaction based on crystalline porous cages
Smart sensors are important components in the development of touchless human-machine interaction systems. Here, the authors describe a smart 3D porous crystalline organic cage-based system that exhibits remarkable responsiveness to fingertip humidity, contributing to the advancement of touchless human-machine interaction technology.
- Jinrong Wang
- , Weibin Lin
- & Niveen M. Khashab
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Article
| Open AccessIntegrating single-cell and spatially resolved transcriptomic strategies to survey the astrocyte response to stroke in male mice
Astrocytes adopt diverse states in response to brain injuries. Here, the authors develop a platform for spatially resolved, single-cell transcriptomics and proteomics, called tDISCO (tissue-digital microfluidic isolation of single cells for -Omics) to uncover the spatial boundaries of molecularly distinct reactive astrocyte populations in stroke.
- Erica Y. Scott
- , Nickie Safarian
- & Maryam Faiz
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Article
| Open AccessUltrathin, ultralight dual-scale fibrous networks with high-infrared transmittance for high-performance, comfortable and sustainable PM0.3 filter
Development of high-performance, comfortable and sustainable air filters is challenging. Here, authors design an ultrathin, ultralight dual scale fiber mat composed of true nanofibers and submicron-fibers to integrate the high protection, thermal wet comfort and save raw materials.
- Yuchen Yang
- , Xiangshun Li
- & Yuekun Lai
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Article
| Open Access4D printed hydrogel scaffold with swelling-stiffening properties and programmable deformation for minimally invasive implantation
3D printing has potential in designing personalised scaffolds, but minimally invasive implantation is still challenging. Here, the authors report the development of a polyurethane material with temperature triggered shape memory and water triggered deformation that allows for transcatheter delivery.
- Bo Liu
- , Hui Li
- & Xiaoli Zhao
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Article
| Open AccessSpontaneous crystallization of strongly confined CsSnxPb1-xI3 perovskite colloidal quantum dots at room temperature
Photoactive pure-iodine all-inorganic colloidal perovskite quantum dots (QDs) are attractive for optoelectronic applications, however their synthesis at room temperature is challenging. Here the authors report a room temperature strongly confined strategy to synthesize CsSnxPb1-xI3 QDs.
- Louwen Zhang
- , Hai Zhou
- & Guojia Fang
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Article
| Open AccessSuperexchange-stabilized long-distance Cu sites in rock-salt-ordered double perovskite oxides for CO2 electromethanation
Cu-oxide-based catalysts are promising for CO2 electromethanation but suffer from inevitable reduction and structural collapse. Here the authors report a Cu-based rock-salt-ordered double perovskite oxide with superexchange-stabilized long-distance Cu sites for efficient and stable CO2 methanation.
- Jiawei Zhu
- , Yu Zhang
- & Heqing Jiang
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Article
| Open AccessRationally designed nanotrap structures for efficient separation of rare earth elements over a single step
Extracting rare earth elements (REEs) from wastewater is essential for the growth of an eco-friendly sustainable economy but separating individual rare earth elements remains challenging. Here, the authors report a REE nanotrap that features dense uncoordinated carboxyl groups and triazole N atoms in a two-fold interpenetrated metalorganic framework which is highly responsive to the size variation of rareearth ions.
- Qing-Hua Hu
- , An-Min Song
- & Jian-Ding Qiu
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Article
| Open AccessHarmonic amide bond density as a game-changer for deciphering the crosslinking puzzle of polyamide
Relating the degree of network crosslinking as a descriptor to the desalination performance of crosslinked polymer membranes remains challenging. Here, the authors introduce a parameter based on distinct amide bonds per unit mass of polyamide, to unravel the relationship between the crosslinked networks of polyamide membranes and their desalination performance.
- Yu-Ren Xue
- , Chang Liu
- & Zhi-Kang Xu
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Article
| Open AccessEfficient catalyst-free N2 fixation by water radical cations under ambient conditions
The growth and sustainable development of humanity is heavily dependent upon N2 fixation. Herein, authors developed an ambient catalyst-free disproportionation of N2 by water plasma to yield economically valuable nitroxyl and hydroxylamine products.
- Xiaoping Zhang
- , Rui Su
- & Huanwen Chen
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Article
| Open AccessCooperative Cu/azodiformate system-catalyzed allylic C–H amination of unactivated internal alkenes directed by aminoquinoline
The oxidative intermolecular amination of C-H bonds represents a straightforward method to construct aliphatic allylic amines. However, the utilization of widely available internal alkenes remains a synthetic challenge. Here, the authors present a regioselective Cu-catalyzed oxidative allylic C-H amination of internal olefins with azodiformates.
- Le Wang
- , Cheng-Long Wang
- & Shu-Yu Zhang
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Article
| Open AccessMetal-free photocatalytic cross-electrophile coupling enables C1 homologation and alkylation of carboxylic acids with aldehydes
Enhancing the sp3-hybridized character of molecular structures in drug discovery is paramount. Here, the authors introduce a deoxygenative cross-electrophile coupling technique that pairs easily accessible carboxylic acid-derived redox-active esters with aldehyde sulfonyl hydrazones, employing Eosin Y as an organophotocatalyst under visible light irradiation.
- Stefano Bonciolini
- , Antonio Pulcinella
- & Timothy Noël
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