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| Open AccessStereospecific syn-dihalogenations and regiodivergent syn-interhalogenation of alkenes via vicinal double electrophilic activation strategy
Restricted reaction mechanism of anti-dihalogenation of alkenes makes it challenging to alter the diastereochemical course into the complementary syn-dihalogenation process. Here, the authors report a conceptually distinctive strategy for the simultaneous double electrophilic activation of the two alkene carbons from the same side to realize syn-dihalogenation.
- Hyeon Moon
- , Jungi Jung
- & Won-jin Chung
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Article
| Open AccessSelective production of methylindan and tetralin with xylose or hemicellulose
Indan and tetralin are used as fuel additives and intermediates in the manufacture of many products, including thermal-stable jet fuel. Here the authors report a route for the synthesis of methylindan and tetralin by the hydrogenolysis of xylose or hemicellulose over a non-noble metal catalyst, followed by further reaction over zeolite H-ZSM-5. Reviewer recognition:
- Zhufan Zou
- , Zhenjie Yu
- & Ning Li
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Article
| Open AccessCreep-type all-solid-state cathode achieving long life
Electrochemical-mechanical issues bring challenges but create new opportunities to design innovative all-solid-state batteries. Here, the authors propose to use the (de)lithiation-stress-creep synergistic time-dependent evolution to boost the electrochemical performance of all-solid-state batteries.
- Xiaolin Xiong
- , Ting Lin
- & Liumin Suo
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Article
| Open AccessDelayed room temperature phosphorescence enabled by phosphines
Room-temperature phosphorescence usually occurs immediately after the removal of excitation. Here the authors achieve combined instant and delayed phosphorescence through introduction of phosphines into carbazole emitters.
- Guang Lu
- , Jing Tan
- & Hui Xu
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Article
| Open AccessDiastereo-divergent synthesis of chiral hindered ethers via a synergistic calcium(II)/gold(I) catalyzed cascade hydration/1,4-addition reaction
Developing an efficient method for the stereocontrolled synthesis of all stereoisomers of chiral hindered ethers is highly desirable but challenging. Here, the authors report an asymmetric cascade reaction catalyzed by a bimetallic catalytic system with control over the configuration of the stereocenters of tetra-aryl substituted ethers.
- Xiangfeng Lin
- , Xia Mu
- & Can Li
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Article
| Open AccessA human-machine interface for automatic exploration of chemical reaction networks
Automated reaction exploration is the key to systematic elucidation of chemical mechanisms. Here, the authors introduce a generally applicable algorithm to steer an automated exploration towards region of interest in chemical reaction space.
- Miguel Steiner
- & Markus Reiher
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Article
| Open AccessThe role of charge in microdroplet redox chemistry
Redox reactions exhibit different thermodynamics and kinetics in water microdroplets compared to the bulk. Here, the authors use reactive molecular dynamics to show the importance of charged reactive species in explaining reactivity under confinement.
- Joseph P. Heindel
- , R. Allen LaCour
- & Teresa Head-Gordon
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Article
| Open AccessBoosting organic phosphorescence in adaptive host-guest materials by hyperconjugation
Room-temperature phosphorescence is usually inefficient in purely organic material. Here, the authors achieve near-unity phosphorescence efficiency with color tunability in adaptive host-guest materials through use of hyperconjugation.
- Huili Ma
- , Lishun Fu
- & Wei Huang
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Article
| Open AccessSwitchable chemoselective aryne reactions between nucleophiles and pericyclic reaction partners using either 3-methoxybenzyne or 3-silylbenzyne
Due to the electrophilic nature of arynes, it is very challenging to control chemoselectivity, when substrates possess multiple competing reaction sites. Here, the authors demonstrate that chemoselective control between two major types of benzyne transformation is accomplished by varying the 3-substituent on aryne intermediate.
- Hongcheng Tan
- , Shuxin Yu
- & Yang Li
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Article
| Open AccessIsostructural doping for organic persistent mechanoluminescence
Organic mechanoluminescent materials have potential in a range of applications, but it can be challenging to achieve long-lived emission. Here, the authors report isostructural doping as a strategy to achieve multicolour and high efficiency organic mechanoluminescence, applied in stress sensing.
- Zongliang Xie
- , Yufeng Xue
- & Bin Liu
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Article
| Open AccessNoncovalent synthesis of homo and hetero-architectures of supramolecular polymers via secondary nucleation
Synthesis of supramolecular polymers with controlled architecture is desirable but challenging. Here, the authors use a secondary nucleation event to prepare a range of supramolecular polymer architectures.
- Srinu Kotha
- , Rahul Sahu
- & Kotagiri Venkata Rao
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Article
| Open AccessIn situ enzymatic control of colloidal phoresis and catalysis through hydrolysis of ATP
The design of synthetic systems that can sense chemical gradients and respond with directional motility and chemical activity is of interest. Here, the authors realize and control such behaviors in a synthetic system by tailoring multivalent interactions of adenosine nucleotides with catalytic microbeads.
- Ekta Shandilya
- , Bhargav Rallabandi
- & Subhabrata Maiti
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Article
| Open AccessCatalytic 1,1-diazidation of alkenes
Compared to well-developed catalytic 1,2-diazidation of alkenes, the corresponding catalytic 1,1-diazidation of alkenes has not been realized. Here, the authors report an efficient approach for catalytic 1,1-diazidation of alkenes by redox-active selenium catalysis.
- Wangzhen Qiu
- , Lihao Liao
- & Xiaodan Zhao
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Article
| Open AccessNucleoside Phosphorylases make N7-xanthosine
Nucleoside-processing enzymes exhibit strict regioselectivity for glycosylation of purine nucleobases at N9. Here, the authors report an exception and show that wild type nucleoside phosphorylases also furnish N7-xanthosine, a non-native ribosylation regioisomer of xanthosine.
- Sarah Westarp
- , Felix Brandt
- & Felix Kaspar
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Article
| Open AccessAllotrope-dependent activity-stability relationships of molybdenum sulfide hydrogen evolution electrocatalysts
The stability of non-noble catalysts is key for their use in proton exchange membrane water electrolysers. Here, authors study activity-stability relationships of MoSx allotropes for H2 production, reporting allotrope-dependent stabilities and dissolution pathways, and propose operation guidelines.
- Daniel Escalera-López
- , Christian Iffelsberger
- & Serhiy Cherevko
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Article
| Open AccessSpatial decoupling of bromide-mediated process boosts propylene oxide electrosynthesis
The practical application of electrosynthesis of propylene oxide is hindered by limited performance. Here, the authors report a spatial decoupling strategy by utilizing the bromide mediator to link propylene and anode within separated reactors, realizing high-performance electrosynthesis of propylene oxide.
- Mingfang Chi
- , Jingwen Ke
- & Jie Zeng
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Article
| Open AccessHighly efficient in crystallo energy transduction of light to work
Crystals are known to have a range of responses to light, but multiple responses in the same material are rare. Here, the authors report different mechanical effects in response to light across three polymorphs as a result of a dimerization reaction.
- Jiawei Lin
- , Jianmin Zhou
- & Junbo Gong
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Article
| Open AccessAll-natural 2D nanofluidics as highly-efficient osmotic energy generators
Researchers report a sustainable nanofluidic osmotic energy harvester made from natural montmorillonite clay nanosheets and recycled cellulose. Scaled-up films of 700 cm2 show power output of 8 W m−2 with stability over 30 days
- Jiadong Tang
- , Yun Wang
- & Tieyong Zuo
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Article
| Open AccessMolecular tuning boosts asymmetric C-C coupling for CO conversion to acetate
This work presents a general surface molecular tuning strategy to promote the electrochemical reduction of CO.
- Jie Ding
- , Fuhua Li
- & Bin Liu
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Article
| Open AccessSelf-condensation-assisted chemical vapour deposition growth of atomically two-dimensional MOF single-crystals
2D MOFs have a variety of applications, including molecular separation and atomically thin electronics. Here authors demonstrate the preparation of monolayer and few-layer MOF single-crystals using a self-condensation-assisted CVD method.
- Lingxin Luo
- , Lingxiang Hou
- & Jian Zheng
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Article
| Open AccessEfficient tandem electroreduction of nitrate into ammonia through coupling Cu single atoms with adjacent Co3O4
An optimal catalyst for nitrate electroreduction should satisfy the simultaneously optimized adsorption of intermediates. Here, the authors report a tandem electrocatalyst by combining Cu single atoms with Co3O4 nanosheets, enhancing the binding with NO2−, thus promoting nitrate electroreduction to NH3.
- Yan Liu
- , Jie Wei
- & Jie Zeng
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Article
| Open AccessTimescale correlation of shallow trap states increases electrochemiluminescence efficiency in carbon nitrides
Differences in timescales of electron transfer reactions limit the efficiency of electrochemiluminescence. Here, the authors coordinate the timescales using shallow trap states in carbon nitride to achieve high efficiencies applied in nitrite sensing.
- Yanfeng Fang
- , Hong Yang
- & Yuanjian Zhang
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Article
| Open AccessPlasma-assisted manipulation of vanadia nanoclusters for efficient selective catalytic reduction of NOx
Achieving supported nanoclusters with unique geometric and electronic structures continues to pose a challenge. Here, the authors introduce a plasma-assisted treatment approach for generating supported metal oxide nanoclusters, facilitated by the rapid transformation of monomeric dispersed metal oxides.
- Yong Yin
- , Bingcheng Luo
- & Xiang Li
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Article
| Open AccessCyclodipeptide oxidase is an enzyme filament
Many cyclic dipeptide natural products can be modified by cyclodipeptide oxidase enzymes. Here, the authors report the structural characterization of the cyclodipeptide oxidase AlbAB and show that it assembles into heterooligomeric enzyme filaments.
- Michael P. Andreas
- & Tobias W. Giessen
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Article
| Open AccessVisible-light-excited robust room-temperature phosphorescence of dimeric single-component luminophores in the amorphous state
Organic room temperature phosphorescence (RTP) is limited to rigid environments. Here, the authors report a single-component system with robust persistent RTP emissions in various aggregation states, such as crystalline, fine powder, and amorphous.
- Danman Guo
- , Wen Wang
- & Zhiyong Yang
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Article
| Open AccessStaggered structural dynamic-mediated selective adsorption of H2O/D2O on flexible graphene oxide nanosheets
Graphene oxide is a promising material for molecular separation technologies. Here, the authors propose a realistic staggered stacking structure that plays a crucial role in H/D recognition in water adsorption, as well as high mobilities of water.
- Ryusuke Futamura
- , Taku Iiyama
- & Katsumi Kaneko
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Article
| Open AccessUnderstanding X-ray absorption in liquid water using triple excitations in multilevel coupled cluster theory
Accurate modeling of X-ray absorption (XA) is necessary to interpret experimental spectra. Here, the authors use coupled cluster models and path-integral ab initio molecular dynamics to provide insights into the XA spectrum of liquid water.
- Sarai Dery Folkestad
- , Alexander C. Paul
- & Henrik Koch
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Article
| Open AccessProgramming viscoelastic properties in a complexation gel composite by utilizing entropy-driven topologically frustrated dynamical state
Tuning the physical interactions and structures to govern the viscoelastic properties in hydrogels without altering the chemistry is challenging. Here the authors design a complexation gel composite and utilize the physical principle of topologically frustrated dynamical state to tune the correlated structures between the guest polycation chains and negatively charged host gels.
- Gui Kang Wang
- , Yi Ming Yang
- & Di Jia
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Article
| Open AccessProbing the surface charge of condensates using microelectrophoresis
The surface charge and ζ-potential of biomolecular condensates is key to their interactions with membranes and proteins. Here, the authors developed a method to determine the ζ-potential of condensates using microelectrophoresis and single-droplet tracking.
- Merlijn H. I. van Haren
- , Brent S. Visser
- & Evan Spruijt
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Article
| Open AccessUnravelling and reconstructing the biosynthetic pathway of bergenin
Bergenin is a rare C-glycoside of 4-O-methyl gallic acid with multiple pharmacological properties. Here, the authors report the elucidation of the biosynthetic pathway of bergenin in Ardisia japonica and its bioproduction by engineered E. coli.
- Ruiqi Yan
- , Binghan Xie
- & Lin Yang
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Article
| Open AccessBiocompatible aggregation-induced emission active polyphosphate-manganese nanosheets with glutamine synthetase-like activity in excitotoxic nerve cells
Glutamine synthetase (GS) relies on Adenosine triphosphate (ATP) to activate glutamate (Glu) and are vital for maintaining ammonia and Glu homeostasis, but GS function is impaired during ATP-deficient neurotoxic events. Here the authors report polyphosphate-manganese nanosheets having GS-like activity independent of ATP to promote the conversion of Glu to glutamine in excitatory neurotoxic cells.
- Jing Wang
- , Xinyang Zhao
- & Wei Wei
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Perspective
| Open AccessEmerging trends in chiral inorganic nanomaterials for enantioselective catalysis
Considerable attention has been directed towards chiral nanocatalysts due to their significant role in facilitating asymmetric organic transformations. Here the authors highlight the recent advancements and notable examples in the field of chiral inorganic nanocatalysts.
- Si Li
- , Xinxin Xu
- & Chuanlai Xu
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Article
| Open AccessComparative quantum-classical dynamics of natural and synthetic molecular rotors show how vibrational synchronization modulates the photoisomerization quantum efficiency
The control of reaction quantum efficiencies is a fundamental photochemical problem. Here the authors use comparative quantum-classical dynamics to reveal that the synchronization of specific vibrations with the reaction coordinate is a key promoting factor.
- Alejandro Blanco-Gonzalez
- , Madushanka Manathunga
- & Massimo Olivucci
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Article
| Open AccessEfficient ammonia synthesis from the air using tandem non-thermal plasma and electrocatalysis at ambient conditions
The conversion of atmospheric N2 into NH3 under ambient pressure is highly interesting but very challenging. In this study, the authors present a tandem air-NOx and NOx-NH3 system that combines non-thermal plasma-enabled N2 oxidation with Ni(OH)x/Cu-catalyzed electrochemical NOx−reduction, resulting in a high NH3 yield from N2 under ambient pressure conditions.
- Wei Liu
- , Mengyang Xia
- & Guidong Yang
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Article
| Open AccessIron-catalyzed stereoselective C–H alkylation for simultaneous construction of C–N axial and C-central chirality
A highly efficient stereoselective C−H alkylation of indoles with aryl alkenes is achieved by sustainable iron catalysis, leading to atropoenriched and enantioenriched substituted indoles with high structural diversity. Detailed mechanistic studies by experiment, Mössbauer spectroscopy and computation reveal the origin of the catalytic efficacy and stereoselectivity.
- Zi-Jing Zhang
- , Nicolas Jacob
- & Lutz Ackermann
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Article
| Open AccessControl of polymers’ amorphous-crystalline transition enables miniaturization and multifunctional integration for hydrogel bioelectronics
Soft elastic materials could be useful in the fabrication of brain-machine interfaces, but achieving the desirable material properties can be challenging. Here, the authors report control of the amorphous-crystalline transition of polymers to alter hydrogel properties and monitor mouse behaviour.
- Sizhe Huang
- , Xinyue Liu
- & Siyuan Rao
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Article
| Open AccessConfining single Er3+ ions in sub-3 nm NaYF4 nanoparticles to induce slow relaxation of the magnetisation
Many of the most industrially important magnets require the addition of rare-earths to improve their coercivity and magnetic performance. Here, the authors place a single paramagnetic rare-earth ion, Er3+, in a diamagnetic nanoparticle, and study the slow relaxation of the resulting nanoparticles, providing vital information for the further development of rare-earth magnetic materials.
- Diogo A. Gálico
- , Emille M. Rodrigues
- & Muralee Murugesu
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Article
| Open AccessMultiple hydrogen-bonding induced nonconventional red fluorescence emission in hydrogels
The development of fluorescent polymer hydrogels without the use of extended pi-conjugation is challenging. Here, the authors report the use of clustering-trigger emission to give red fluorescence on boiling polymer hydrogels, with tuneable emission properties.
- Jiayu Wu
- , Yuhuan Wang
- & Feng Zhou
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Article
| Open AccessConsummating ion desolvation in hard carbon anodes for reversible sodium storage
Hard carbon is regarded as a promising negative electrode for Na-ion batteries but suffers from low initial Coulombic efficiency (ICE). Here, the authors identify the time-dependent ion pre-desolvation on the nanopore of hard carbons, which remarkably improves the ICE by simply extending the aging time.
- Ziyang Lu
- , Huijun Yang
- & Haoshen Zhou
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Article
| Open AccessEstablishing superfine nanofibrils for robust polyelectrolyte artificial spider silk and powerful artificial muscles
Spider silk has desirable properties, but these are hard to replicate with artificial materials. Here, the authors report a polyelectrolyte artificial spider silk, with control over dissociation of the polymer chains by introduction of ions, and thermally driven supercontraction.
- Wenqian He
- , Meilin Wang
- & Zunfeng Liu
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Article
| Open AccessSweat permeable and ultrahigh strength 3D PVDF piezoelectric nanoyarn fabric strain sensor
Electronic packaging causes piezoelectric sensors to be airtight, resulting in poor wearing comfort. To address this issue, the authors develop a 3D all-fiber piezoelectric sensor with sweat permeable using the advanced 3D textile technology.
- Wei Fan
- , Ruixin Lei
- & Shengbo Ge
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Article
| Open AccessA comprehensive synthetic library of poly-N-acetyl glucosamines enabled vaccine against lethal challenges of Staphylococcus aureus
Poly-β-(1–6)-N-acetylglucosamine (PNAG) is an important vaccine target, but the impact of the number and position of free amine vs N-acetylation on its antigenicity is not well understood. Here, the authors report a divergent strategy to synthesize a comprehensive library of PNAG pentasaccharides, enabling the identification of enhanced epitopes for vaccines against Staphylococcus aureus including drug resistant strains.
- Zibin Tan
- , Weizhun Yang
- & Xuefei Huang
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Article
| Open AccessScalable computation of anisotropic vibrations for large macromolecular assemblies
Normal mode analysis is a crucial step in structural biology, but is based on an expensive diagonalisation of the system’s Hessian. Here the authors present INCHING, a GPU-based approach to accelerate this task up to >250 times over current methods for macromolecular assemblies.
- Jordy Homing Lam
- , Aiichiro Nakano
- & Vsevolod Katritch
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Article
| Open AccessAn isolable, chelating bis[cyclic (alkyl)(amino)carbene] stabilizes a strongly bent, dicoordinate Ni(0) complex
Notwithstanding their success as strongly σ-donating and π-accepting ligands, to date no chelating bis[cyclic (alkyl)(amino)carbenes] have been reported. Here the authors describe a chelating, C2-symmetric bis[cyclic (alkyl)(amino)carbene] ligand, as well as its pseudotetrahedral complexes with iron, cobalt, nickel, and zinc dihalides.
- Braulio M. Puerta Lombardi
- , Morgan R. Faas
- & Roland Roesler
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Article
| Open AccessHighly defective ultra-small tetravalent MOF nanocrystals
Crystalline materials’ properties are highly dependent on their size. Here authors report a general synthesis of ultrasmall (4–6 nm) and highly defective Zr/Hf-Metal Organic Frameworks nanoparticles that present enhanced peptide hydrolysis performance.
- Shan Dai
- , Charlotte Simms
- & Christian Serre
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Article
| Open AccessPathway-divergent coupling of 1,3-enynes with acrylates through cascade cobalt catalysis
The development of divergent reaction pathways controlled by different ligands is a critical goal. Here the authors describe a cobalt-catalyzed strategy for cascade coupling of 1,3-enynes with two molecules of acrylates through three reaction modes.
- Heng Wang
- , Xiaofeng Jie
- & Fanke Meng
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Article
| Open AccessIn situ captured antibacterial action of membrane-incising peptide lamellae
Inspired by the alternating chirality backbone pattern of some effective peptide antimicrobials, here authors design lysine-rich heterochiral peptides that show antimicrobial activity.
- Kamal el Battioui
- , Sohini Chakraborty
- & Tamás Beke-Somfai
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Article
| Open AccessDehydroxylative radical N-glycosylation of heterocycles with 1-hydroxycarbohydrates enabled by copper metallaphotoredox catalysis
N-Glycosylated heterocycles play important roles in biological systems and drug development, but the synthesis heavily relies on ionic N-glycosylation. Herein, the authors report a dehydroxylative radical method for synthesizing N-glycosides by leveraging copper metallaphotoredox catalysis.
- Da-Peng Liu
- , Xiao-Sen Zhang
- & Xiang-Guo Hu
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Article
| Open AccessPolarizability matters in enantio-selection
Polarizability, a property that is closely related to softness in the classic theory of Hard and Soft Acids and Bases (HSAB), has been largely overlooked in connecting with enantio-selection in the past. Here, the authors show local polarizability-based electronic effects can rationalize a wide range of stereochemical outcomes in widely-known asymmetric catalytic reactions.
- Fumin Chen
- , Yu Chen
- & Xiangyou Xing
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