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Article
| Open AccessWhy •CF2H is nucleophilic but •CF3 is electrophilic in reactions with heterocycles
Empirically observed regiochemistries indicate that the CF2H radical has a nucleophilic character similar to alkyl radicals, but the CF3 radical is electrophilic in reactions with heterocycles. Here, the authors report DFT calculations, reproducing experimental selectivities and leading to an explanation of this difference.
- Meng Duan
- , Qianzhen Shao
- & K. N. Houk
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Article
| Open AccessMultiple photofluorochromic luminogens via catalyst-free alkene oxidative cleavage photoreaction for dynamic 4D codes encryption
Photochromic systems with high contrast and multiple colours are useful for responsive materials, but it is challenging to achieve multiple colours with one molecule. Here, the authors report a photochromic system controlled by oxidative cleavage on light irradiation.
- Lin Lu
- , Bo Wu
- & Ben Zhong Tang
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Article
| Open AccessAtomically dispersed MoNi alloy catalyst for partial oxidation of methane
The catalytic partial oxidation of methane (POM) is a promising technology for synthesizing syngas but suffers from severe over-oxidation on the catalyst surface. Here the authors demonstrate that regulating O* occupation in an atomically dispersed MoNi alloy can achieve high catalytic performance for POM.
- Zheyuan Ding
- , Sai Chen
- & Jinlong Gong
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Article
| Open AccessPhotocatalytic toluene oxidation with nickel-mediated cascaded active units over Ni/Bi2WO6 monolayers
By introducing Ni dopants into monolayer Bi2WO6, Bi/O frustrated Lewis pairs, unsaturated W atoms, and Ni active units are formed. The authors show that these units facilitate oxygen species transfer and enhance photocatalytic toluene oxidation.
- Yingzhang Shi
- , Peng Li
- & Xianzhi Fu
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Article
| Open AccessHigh-performance near-infrared OLEDs maximized at 925 nm and 1022 nm through interfacial energy transfer
The low photoluminescence quantum yield of near-infrared (NIR) emitters has limited their application in organic light-emitting diodes (OLEDs). Here, authors realize NIR OLEDs through interfacial energy transfer from platinum(II) complexes to a non-fullerene acceptor based on a sandwiched structure.
- Chieh-Ming Hung
- , Sheng-Fu Wang
- & Pi-Tai Chou
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Article
| Open AccessAtroposelective synthesis of biaxial bridged eight-membered terphenyls via a Co/SPDO-catalyzed aerobic oxidative coupling/desymmetrization of phenols
Biaryl compounds with an axial chirality are valuable architectures but few methods have been developed for the construction of bridged biaryls, a subclass of these compounds that bear a tether to connect the two arenes and form a medium-sized ring. Here, the authors design a Co/SPDO-catalyzed aerobic oxidative coupling/desymmetrization sequence of prochiral phenols for the enantioselective synthesis of biaxial bridged m-terphenyls embedded in an azocane.
- Shuang-Hu Wang
- , Shi-Qiang Wei
- & Tong-Mei Ding
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Article
| Open AccessCO electrolysis to multicarbon products over grain boundary-rich Cu nanoparticles in membrane electrode assembly electrolyzers
Producing valuable chemicals like ethylene via catalytic CO conversion is an important nonpetroleum route. Here, authors demonstrate high-rate electrosynthesis of multicarbon chemicals via CO electrolysis, with a multicarbon product partial current density of 4.35 A cm−2 at a cell voltage of 2.78 V.
- Hefei Li
- , Pengfei Wei
- & Xinhe Bao
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Article
| Open AccessX-ray radiation damage cycle of solvated inorganic ions
A radiation damage cycle in X-ray-ionized solvated Mg ions is reported by the authors leading to production of water radicals and low-energy electrons. The Mg ion ends in its initial state quickly and can restart the cycle, multiplying the local damage.
- Dana Bloß
- , Florian Trinter
- & Andreas Hans
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Article
| Open AccessCatalytic asymmetric synthesis of planar-chiral dianthranilides via (Dynamic) kinetic resolution
Chirality has long fascinated chemists, but asymmetric synthesis has largely focused on central, axial, and helical chirality to date. Here, the authors synthesize dianthranilides with planar chirality, via cinchona alkaloid-catalyzed (dynamic) kinetic resolution.
- Chun-Yan Guan
- , Shuai Zou
- & Guang-Jian Mei
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Article
| Open AccessMolecular-strain induced phosphinidene reactivity of a phosphanorcaradiene
Phosphanorcaradienes can serve as synthons for transient phosphinidene but the synthesis remains challenging. Here, the authors report a synthesis protocol for a phosphanorcaradiene, in which one of the benzene rings is intramolecularly dearomatized through attachment to the phosphorus atom.
- Yizhen Chen
- , Peifeng Su
- & Gengwen Tan
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Article
| Open AccessPhoto-cycloaddition reactions of vinyldiazo compounds
Heterocycles, highly prized by the pharmaceutical industry, are often constructed from diazo compounds. Here, the authors report that direct photolysis of vinyldiazo compounds followed by [3+2]-cycloaddition gives access to these motifs.
- Ming Bao
- , Klaudia Łuczak
- & Michael P. Doyle
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Article
| Open AccessCatalytic asymmetric [4 + 2] dearomative photocycloadditions of anthracene and its derivatives with alkenylazaarenes
While significant progress has been made in classical Diels-Alder reactions, the use of simple and inert feedstock chemicals under mild reaction conditions still remains challenging. Here the authors present the development of catalytic asymmetric [4 + 2] dearomative photocycloaddition involving anthracene and its derivatives with alkenylazaarenes.
- Dong Tian
- , Wenshuo Shi
- & Zhiyong Jiang
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Article
| Open AccessOrganic and inorganic sublattice coupling in two-dimensional lead halide perovskites
By resonant pumping the organic cation in 2D perovskite, Fu et al. report the electronic and mechanical couplings between the organic and inorganic sublattices, evidenced by the reduced bandgap and modified lattice degree of freedom within the inorganic sublattice, and slow heat transfer process.
- Jianhui Fu
- , Tieyuan Bian
- & Tze Chien Sum
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Article
| Open AccessA spatially localized DNA linear classifier for cancer diagnosis
Molecular computing is an emerging paradigm with a crucial role in clinical diagnosis. Here, authors develop a spatially localized, DNA-integrated circuits-based classifier, DNA IC-CLA, which enables accurate cancer diagnosis for clinical samples in a faster and more effective manner.
- Linlin Yang
- , Qian Tang
- & Da Han
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Article
| Open AccessSupramolecular metallic foams with ultrahigh specific strength and sustainable recyclability
Porous materials with high strength are desirable for many applications. Here, the authors present a supramolecular metallic foam enabled by nanostructured liquid metals connected with high-density metal-ligand coordination to exhibit ultrahigh specific strength and recyclability.
- Xin Yang
- , Xin Huang
- & Xinxing Zhang
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Article
| Open AccessEmergence of a short peptide based reductase via activation of the model hydride rich cofactor
Biological cofactors such as dihydronicotinamides are exploited by extant enzymes as hydride transfer agents and electron carriers but are generally inefficient to facilitate any reactions on their own. Here, the authors report short peptide-based amyloid nanotubes featuring exposed arrays of cationic and hydrophobic residues that can bind small hydride transfer agents (NaBH4) to facilitate efficient reduction of ester substrates in water.
- Ayan Chatterjee
- , Surashree Goswami
- & Dibyendu Das
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Article
| Open AccessPretreatment-free SERS sensing of microplastics using a self-attention-based neural network on hierarchically porous Ag foams
Detection and identification of microplastics (MPs) in environmental samples is hampered by the need for isolation and pretreatment methods. Here, the authors combine porous Ag substrates with self-attention neural networks to directly identify six types of MPs in environmental samples.
- Olga Guselnikova
- , Andrii Trelin
- & Yusuke Yamauchi
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Article
| Open AccessDynamics underlie the drug recognition mechanism by the efflux transporter EmrE
Here, the authors reveal the protonation of a single membrane embedded glutamate residue within the homodimer of the efflux transporter EmrE modulates the structure and dynamics in an allosteric manner using NMR spectroscopy.
- Jianping Li
- , Ampon Sae Her
- & Nathaniel J. Traaseth
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Article
| Open AccessCobalt-catalyzed cross-electrophile coupling of alkynyl sulfides with unactivated chlorosilanes
Transition-metal catalyzed cross-electrophile coupling (XEC) is a powerful tool for the construction of molecules but XEC between carbon electrophile and chlorosilanes to access organosilicon compounds remains underdeveloped. Here the authors disclose a highly efficient cobalt-catalyzed cross-electrophile alkynylation of a broad range of unactivated chlorosilanes with alkynyl sulfides as a stable and practical alkynyl electrophiles.
- Donghui Xing
- , Jinlin Liu
- & Liangbin Huang
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Article
| Open AccessInternal water circulation mediated synergistic co-hydrolysis of PET/cotton textile blends in gamma-valerolactone
Recycling strategies for mixed plastics and textile blends currently aim for recycling only one of the components. Here the authors demonstrate a water coupling strategy to co-hydrolyze polyester/cotton textile blends into polymer monomers and platform chemicals.
- Shun Zhang
- , Wenhao Xu
- & Yu-Zhong Wang
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Article
| Open AccessZero-field J-spectroscopy of quadrupolar nuclei
Zero to ultralow-field NMR provides chemical information in the absence of a high magnetic field but it is difficult to measure molecules with quadrupolar nuclei due to their fast relaxation. This study examines zero-field J-spectra from isotopologues of ammonium cations, with quadrupolar nuclei, revealing the presence of a primary isotope effect of −58 mHz.
- Román Picazo-Frutos
- , Kirill F. Sheberstov
- & Danila A. Barskiy
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Article
| Open AccessProton-coupled transport mechanism of the efflux pump NorA
Efflux pumps confer antibiotic resistance by coupling proton import with drug export. In this work, the authors uncover the proton-coupled transport mechanism for the clinically relevant efflux pump NorA from the pathogenic bacterium S. aureus.
- Jianping Li
- , Yan Li
- & Nathaniel J. Traaseth
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Article
| Open AccessThe impact of magnesium content on lithium-magnesium alloy electrode performance with argyrodite solid electrolyte
All-solid-state lithium-based batteries require high stack pressure during operation. Here, we investigate the mechanical, transport, and interfacial properties of Li-rich magnesium alloy and show enhanced performance at low pressure and ambient temperature for alloy-based electrodes with less than 5 at% Mg content.
- Jack Aspinall
- , Krishnakanth Sada
- & Mauro Pasta
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Article
| Open AccessEnantioselective nickel-catalyzed anodic oxidative dienylation and allylation reactions
Precision control of stereochemistry in radical reactions remains a formidable challenge. Here the authors demonstrate an electricity driven asymmetric Lewis acid catalysis to facilitate asymmetric dienylation and allylation reactions, resulting in the formation of all-carbon quaternary stereocenters.
- Qinglin Zhang
- , Jiayin Zhang
- & Chang Guo
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Article
| Open AccessEnhancement of phase transition temperature through hydrogen bond modification in molecular ferroelectrics
The authors propose a hydrogen bond modification method to achieve introduction of polarization and enhancement of phase transition temperature in molecular ferroelectrics, exploring the piezoelectric prototype devices of the molecular ferroelectric.
- Yu-An Xiong
- , Sheng-Shun Duan
- & Yu-Meng You
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Article
| Open AccessSynergetic regulation of SEI mechanics and crystallographic orientation for stable lithium metal pouch cells
The application of Li-metal batteries (LMBs) is impeded by unstable solid electrolyte interphase (SEI) and uncontrollable Li dendrites growth. Here, the authors present an YF3/PMMA composite layer to achieve high-performance LMBs via the synergetic regulation of SEI mechanics and Li crystallography.
- Yanhua Zhang
- , Rui Qiao
- & Jiangxuan Song
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Article
| Open AccessIn-situ noncovalent interaction of ammonium ion enabled C–H bond functionalization of polyethylene glycols
The noncovalent interaction of ammonium ion with multidentate oxygen-based host serving as a key reacting center in catalytic reactions is rare. In this work, the authors report a noncovalent interaction of ammonium ion enabled reactivity enhancement process, achieving the C–H functionalization of polyethylene glycols with acrylates.
- Zongnan Zhang
- , Xueli Lv
- & Rong Zeng
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Article
| Open AccessUrea-formaldehyde resin room temperature phosphorescent material with ultra-long afterglow and adjustable phosphorescence performance
Organic room temperature phosphorescent materials have useful properties, but development can be limited by processing and stability challenges. Here, the authors report a derivatisation strategy for the preparation of room temperature phosphorescent materials responsive to an electrostatic field.
- Wensheng Xu
- , Bowei Wang
- & Ligong Chen
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Article
| Open AccessMolecular orbital breaking in photo-mediated organosilicon Schiff base ferroelectric crystals
Switchable structural and physical bistability in ferroelectric materials can be achieved as result of molecular orbital breaking. Here, the authors describe the photo-mediated bistability in organosilicon Schiff base ferroelectric crystals for the modulation of dielectric, second-harmonic generation, and ferroelectric polarization and showing good in vitro biocompatibility.
- Zhu-Xiao Gu
- , Nan Zhang
- & Han-Yue Zhang
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Article
| Open AccessSpider-silk-inspired strong and tough hydrogel fibers with anti-freezing and water retention properties
Hydrogel fibres have potential in a range of applications such as flexible electronics, but achieving the desired mechanical properties can be challenging. Here, the authors report spider silk-inspired hydrogel fibres with tuneable mechanical properties suitable for flexible electronics.
- Shaoji Wu
- , Zhao Liu
- & Yurong Yan
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Article
| Open AccessUnusual facet and co-catalyst effects in TiO2-based photocatalytic coupling of methane
Designing photocatalysts to enhance the efficiency of non-oxidative coupling of methane is a challenging task. Here, the authors report that the anatase TiO2 with exposed {101} facets and Pd co-catalyst enables efficient and selective methane coupling to ethane via a heterogeneous-homogeneous hybrid reaction pathway.
- Huizhen Zhang
- , Pengfei Sun
- & Ye Wang
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Article
| Open AccessHighly porous metal-organic framework liquids and glasses via a solvent-assisted linker exchange strategy of ZIF-8
The canonical metal-organic framework ZIF-8 does not melt and form a glass. Here, authors incorporated two additional organic linkers into ZIF-8 to generate meltable derivatives which can be transformed into highly porous glasses by melt-quenching.
- Wen-Long Xue
- , Pascal Kolodzeiski
- & Sebastian Henke
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Article
| Open AccessDirect observation of electron transfer in solids through X-ray crystallography
Electron transfer in solids is a fundamental process in many functional nanomaterials. Here, the authors directly observe this process via x-ray crystallography for incorporating of electron-donor guest molecules in macrocyclic nanotube crystals.
- Daiji Ogata
- , Shota Koide
- & Junpei Yuasa
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Article
| Open AccessHeat-activated growth of metastable and length-defined DNA fibers expands traditional polymer assembly
The combination of dynamic, energy driven folding and growth with structural stiffness and length control is difficult to achieve in synthetic polymer self-assembly. Here the authors show that highly charged, monodisperse DNA oligomers assemble via seeded growth into length-controlled supramolecular fibers during heating.
- Michael D. Dore
- , Muhammad Ghufran Rafique
- & Hanadi F. Sleiman
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Article
| Open AccessSyntheses and reactivities of strained fused-ring metallaaromatics containing planar eleven-carbon chains
7C-10C and 12C-carbolong complexes with planar ligand skeletons containing 7-10 and 12 carbon atoms have been previously reported but 11C-carbolong complexes with a planar carbon-chain ligand are elusive. Here, the authors prepare metallabenzyne-fused metallapentalenes and metallabenzene-fused metallapentalynes, both representing 11C-carbolong complexes with a planar carbon-chain ligand
- Binbin Xu
- , Wei Mao
- & Haiping Xia
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Article
| Open AccessTitanium catalyzed [2σ + 2π] cycloaddition of bicyclo[1.1.0]-butanes with 1,3-dienes for efficient synthesis of stilbene bioisosteres
Natural stilbenes show significant potential in the prevention and treatment of diseases due to their diverse pharmacological activities. Here the authors present a mild and effective Ti-catalyzed intermolecular radical-relay cycloaddition reaction with good regio- and trans-selectivity offering rapid access to structurally diverse stilbene bioisosteres.
- Yonghong Liu
- , Zhixian Wu
- & Lei Shi
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Article
| Open AccessReal-time observation of two distinctive non-thermalized hot electron dynamics at MXene/molecule interfaces
Photoexcited MXenes could transfer charge carriers to or heat molecules at their interfaces. Here, the authors show using time-resolved spectroscopy that the non-thermalized carriers can directly transfer to molecules or heat them within 125 fs.
- Qi Zhang
- , Wei Li
- & Xueming Yang
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Article
| Open AccessNylons with Highly-Bright and Ultralong Organic Room-Temperature Phosphorescence
It may be useful to obtain nylon with room temperature phosphorescence, but identifying a suitable luminophore is challenging. Here, the authors report the doping of nylon with cyano-substituted benzimidazole derivatives for room temperature phosphorescent nylons.
- Dian-Xue Ma
- , Zhong-Qiu Li
- & Yu-Wu Zhong
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Article
| Open AccessA rationally designed miniature of soluble methane monooxygenase enables rapid and high-yield methanol production in Escherichia coli
Soluble methane monooxygenase (sMMO) is a potentially value biocatalyst, but production of active recombinant sMMO is very challenging. Here the authors report the rational design and construction of a catalytically active miniature sMMO which enables high-yield production of methanol in E. coli.
- Yeonhwa Yu
- , Yongfan Shi
- & Jeewon Lee
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Article
| Open AccessAbiotic formation of alkylsulfonic acids in interstellar analog ices and implications for their detection on Ryugu
Alkylsulfonic acids represent an alternative source of sulfur for the origins of life. Here the authors demonstrate, via laboratory simulation experiments, the formation of these compounds in interstellar analog ices with implications for their incorporation into asteroids such as Ryugu.
- Mason McAnally
- , Jana Bocková
- & Ralf I. Kaiser
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Article
| Open AccessOrganocatalytic skeletal reorganization for enantioselective synthesis of S-stereogenic sulfinamides
The enantioselective synthesis of S-stereogenic sulfinamides has garnered considerable attention due to their unique structural and physicochemical properties but catalytic asymmetric synthesis of sulfinamides still remains challenging. Here, the authors present the synthesis of S-stereogenic sulfinamides through the peptide-mimic phosphonium salt-catalyzed asymmetric skeletal reorganization of simple prochiral and racemic sulfoximines.
- Zanjiao Liu
- , Siqiang Fang
- & Tianli Wang
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Article
| Open AccessDiastereoselective dearomatization of indoles via photocatalytic hydroboration on hydramine-functionalized carbon nitride
Dearomative hydroboration of predominantly existing indole derivatives provides a straightforward strategy to synthesize boryl indolines, but developing eco-friendly methods for remains challenging. Here, the authors develop a method for heterogeneous photocatalytic trans-hydroboration of indole derivatives with NHC-borane.
- Qiao Zhang
- , Wengang Xu
- & Mingbo Wu
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Article
| Open AccessIntermolecular interactions probed by rotational dynamics in gas-phase clusters
The authors demonstrate, using coincident Coulomb explosion imaging, that the rotational dynamics of single nitrogen molecules can be used as a probe to sense the interactions with surrounding Ar atoms in gas-phase clusters.
- Chenxu Lu
- , Long Xu
- & Jian Wu
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Article
| Open AccessDual-mode harvest solar energy for photothermal Cu2-xSe biomineralization and seawater desalination by biotic-abiotic hybrid
Biotic-abiotic photosynthetic systems hold great promise to innovate solar-driven chemical transformation. Here, the authors construct a biotic-abiotic hybrid system composed of Shewanella oneidensis MR-1 and biogenic Se0 nanoparticles for photothermal Cu2-xSe biomineralization and then for seawater desalination.
- Sheng-Lan Gong
- , YangChao Tian
- & Li-Jiao Tian
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Article
| Open AccessObservation of unusual outer-sphere mechanism using simple alkenes as nucleophiles in allylation chemistry
Allylic substitution reaction of alkenes has been well-developed, but it has limitations, partly due to the intrinsic predilection for an inner-sphere mechanism. Herein, the authors present an outer-sphere mechanism in Rh-catalyzed allylic substitution reaction of simple alkenes using gem-difluorinated cyclopropanes as allyl surrogates.
- Yaxin Zeng
- , Han Gao
- & Ying Xia
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Article
| Open AccessHeavy-atom tunnelling in singlet oxygen deactivation predicted by instanton theory with branch-point singularities
Singlet oxygen relaxes in water to its triplet ground state. Here, the authors show that heavy-atom tunnelling speeds up this reaction from time scales longer than the age of the universe to microseconds.
- Imaad M. Ansari
- , Eric R. Heller
- & Jeremy O. Richardson
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Article
| Open AccessCell-free biosynthesis and engineering of ribosomally synthesized lanthipeptides
Ribosomally synthesized and post-translationally modified peptides (RiPPs) are a major class of natural products with potent biological activities but a vast majority of RiPP gene clusters remain unexplored in microbial genomes. Here, the authors report a unified biocatalysis (UniBioCat) system based on cell-free gene expression for rapid biosynthesis and engineering of RiPPs.
- Wan-Qiu Liu
- , Xiangyang Ji
- & Jian Li
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Article
| Open AccessA facile synthesis of α,β-unsaturated imines via palladium-catalyzed dehydrogenation
α,β-unsaturated compounds serve as versatile synthons in organic chemistry, but the α,β-desaturation of aliphatic imines is challenging due to easy hydrolysis and preferential dimerization. Herein, the authors report the synthesis of α,β-unsaturated imines by employing a pre-fluorination and palladium-catalyzed dehydrogenation reaction sequence.
- Chunyang Zhao
- , Rongwan Gao
- & Junkai Fu
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Article
| Open AccessElectrostatic-induced ion-confined partitioning in graphene nanolaminate membrane for breaking anion–cation co-transport to enhance desalination
Two-dimensional graphene-based membranes have gained much interest, but they suffer from poor rejection for monovalent salts. Here, the authors develop an electrostatic-induced ion partitioning strategy to suppress anion-cation transmembrane co-transport, improving the desalination performance.
- Haiguang Zhang
- , Jiajian Xing
- & Xie Quan
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