Featured
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Article
| Open AccessCopper(I)-nitrene platform for chemoproteomic profiling of methionine
Methionine plays an essential role in various biological and cell regulatory processes, making its chemoproteomic profiling necessary to understand its function. Here, the authors present Copper(I)-Nitrene Platform (CuNiP) for robust and selective labelling of methionine to generate highly stable sulfonyl sulfimide conjugates under physiological conditions.
- Samrat Sahu
- , Benjamin Emenike
- & Monika Raj
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Article
| Open AccessA large-strain and ultrahigh energy density dielectric elastomer for fast moving soft robot
Dielectric elastomer actuators require high driving electric fields to achieve high performances for soft robots due to their low dielectric constant and high stiffness. Here, the authors introduce polar fluorinated groups and nanodomains aggregated by long alkyl side chains into the dielectric elastomer design to overcome these issues and develop fast soft robots.
- Wenwen Feng
- , Lin Sun
- & Chao Wang
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Article
| Open AccessActive droplets through enzyme-free, dynamic phosphorylation
Despite the importance of dynamic phosphorylation in biology, enzyme-free, synthetic systems that use dynamic phosphorylation to regulate supramolecular processes are unexplored. Here, the authors report an enzyme-free chemical reaction cycle that can dynamically phosphorylate amino acids and peptides using simple phosphorylating agents and regulate supramolecular functions.
- Simone M. Poprawa
- , Michele Stasi
- & Job Boekhoven
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Article
| Open AccessPara-selective nitrobenzene amination lead by C(sp2)-H/N-H oxidative cross-coupling through aminyl radical
Direct radical C–H amination strategies have exhibited innovation, but challenges remain with C–H amination of electron-poor nitroarenes due to the essence of the electron-deficient nitrogen radical. Herein, the authors report a transition metal-free dehydrogenative C(sp2)-H/N-H cross-coupling between electron-poor nitroarenes and amines.
- Zhen Zhang
- , Shusheng Yue
- & Hu Cai
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Article
| Open AccessA scalable Li-Al-Cl stratified structure for stable all-solid-state lithium metal batteries
Sulfide electrolytes’ incompatibility with Li metal hinders their use in all-solid-state Li metal batteries. Here, the authors propose a scalable Li-Al-Cl stratified structure, formed via strain-activated phase separation, to effectively stabilize the negative electrode/electrolyte interface.
- Han Su
- , Jingru Li
- & Jiangping Tu
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Article
| Open AccessMonosymmetric Fe-N4 sites enabling durable proton exchange membrane fuel cell cathode by chemical vapor modification
The limited durability of metal-nitrogen-carbon electrocatalysts hinders their use in proton exchange membrane fuel cells for the oxygen reduction reaction. Here the authors transform active sites from FeN4 to stable monosymmetric FeN2 + N’2 via chemical vapor modification, resulting in enhanced improving the durability of the catalyst.
- Jingsen Bai
- , Tuo Zhao
- & Wei Xing
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Article
| Open AccessLong-term relapse-free survival enabled by integrating targeted antibacteria in antitumor treatment
Tumor-resident intracellular microbiota (TRIM) could be a potential target for anticancer treatment. Here the authors report Au@Ag2Se nano-assemblies enabling bacterial killing, tumor inhibition and immune regulation in tumor microenvironment.
- Yuanlin Wang
- , Yaqian Han
- & Miao Yu
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Article
| Open AccessBioinformatics leading to conveniently accessible, helix enforcing, bicyclic ASX motif mimics (BAMMs)
Researchers mimic protein interface helices by stapling peptide side chains, or replacing hydrogen bonds with covalent ones, and synthetic helical mimics are heavily biased towards stapling. Here the authors describe bioinformatic discovery of hydrophobic triangles at helix N-termini, and rigid, bicyclic synthetic mimics of them.
- Tianxiong Mi
- , Duyen Nguyen
- & Kevin Burgess
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Article
| Open AccessPolyoxometalate-based plasmonic electron sponge membrane for nanofluidic osmotic energy conversion
Nanofluidic membranes have great potential in harvesting osmotic energy, but performance is hampered by insufficient permselectivity. Here, the authors solve this problem with a polyoxometalate-based nanofluidic plasmonic electron sponge membrane.
- Chengcheng Zhu
- , Li Xu
- & Chen Wang
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Article
| Open AccessTime-resolved THz Stark spectroscopy of molecules in solution
Stark spectroscopy of molecules in liquid solutions was once challenging due to orientation effects, solved by freezing but limiting ambient studies. Now, THz Stark spectroscopy with intense terahertz pulses enables dynamic analysis of molecules in both non-polar and polar solvents at any temperature, advancing conventional methods.
- Bong Joo Kang
- , Egmont J. Rohwer
- & Thomas Feurer
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Article
| Open AccessDisentangling the effects of structure and lone-pair electrons in the lattice dynamics of halide perovskites
By comparing CsSrBr3 and CsPbBr3 with close structural similarity but the latter lacking lone-pair electrons on the octahedral metal, the authors reveal the similar vibrational anharmonicities in the two perovskites, which disentangles the electronic properties and vibrational anharmonicities.
- Sebastián Caicedo-Dávila
- , Adi Cohen
- & David A. Egger
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Article
| Open AccessReduction of precious metal ions in aqueous solutions by contact-electro-catalysis
Currently, precious metal recovery from e-waste water is usually performed by liquid extraction or sorbent processes. Here, the authors show the untapped potential of dielectric insulators as catalysts for the 1-step selective recovery of gold in aqueous solutions by contact-electrocatalysis.
- Yusen Su
- , Andy Berbille
- & Zhong Lin Wang
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Article
| Open AccessAccelerating reliable multiscale quantum refinement of protein–drug systems enabled by machine learning
Biomacromolecule structures are vital for drug design. Here, the authors integrate one or two machine learning potentials in an ONIOM-based quantum refinement method, achieving reliable drug structures at an QM level in proteins with high efficiency.
- Zeyin Yan
- , Dacong Wei
- & Lung Wa Chung
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Article
| Open AccessIon pair sites for efficient electrochemical extraction of uranium in real nuclear wastewater
Electrochemical uranium extraction from real nuclear wastewater is appealing but challenging. Herein, Lin et al develop a strategy of ion pair site for enhanced binding of dominant uranium fluoride species in real wastewater, achieving efficient recycling of uranium as powder product.
- Tao Lin
- , Tao Chen
- & Rong He
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Article
| Open AccessSingle-zinc vacancy unlocks high-rate H2O2 electrosynthesis from mixed dioxygen beyond Le Chatelier principle
The principle of Le Chatelier is a fundamental concept in textbooks, serving as a guiding principle for controlling chemical and catalytic systems. In this study, the authors present an oxygen electroreduction system based on a single zinc vacancy catalyst, which operates in a manner that extends “beyond” Le Chatelier’s principle.
- Qi Huang
- , Baokai Xia
- & Sheng Chen
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Article
| Open AccessCrossover from gas-like to liquid-like molecular diffusion in a simple supercritical fluid
Within the phase diagram of pure substances, the supercritical state is not fully understood. Here the authors experimentally observe a gas-like to liquid-like crossover in the self-dynamics of supercritical fluid methane upon pressure increase.
- Umbertoluca Ranieri
- , Ferdinando Formisano
- & Livia E. Bove
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Article
| Open AccessIntroduction of the difluoromethyl group at the meta- or para-position of pyridines through regioselectivity switch
The direct C−H-difluoromethylation of pyridines represents a highly efficient economic way to access azines. However, the direct meta-difluoromethylation of pyridines remains elusive. Here, the authors demonstrate switchable meta- as well as para-C−H difluoromethylation of pyridines through radical processes by using oxazino pyridine intermediates.
- Pengwei Xu
- , Zhe Wang
- & Armido Studer
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Article
| Open AccessLate-stage benzenoid-to-troponoid skeletal modification of the cephalotanes exemplified by the total synthesis of harringtonolide
Many natural products exist as families of structurally similar molecules, and therefore developing skeletal modifications of common intermediates offers flexible and powerful approaches for target synthesis. Here, the authors report a single-atom insertion into the framework of the benzenoid subfamily, providing access to the troponoid congeners.
- Stefan Wiesler
- , Goh Sennari
- & Richmond Sarpong
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Article
| Open AccessSwitchable supramolecular helices for asymmetric stereodivergent catalysis
Controlling multiple stereogenic centers in a single molecular scaffold represents a challenge for current switchable asymmetric catalysts. Here, the authors achieve asymmetric stereodivergency by means of a switchable supramolecular helical catalyst allowing all stereoisomers to be obtained with high and similar enantioselectivities.
- Ran Chen
- , Ahmad Hammoud
- & Matthieu Raynal
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Article
| Open AccessRedox-induced controllable engineering of MnO2-MnxCo3-xO4 interface to boost catalytic oxidation of ethane
The exploration of heterogeneous interfaces between metal oxides has received limited attention. Here the authors demonstrated the creation of MnO2-MnxCo3-xO4 interfaces through controlled chemical reduction processes, effectively altering electron distribution and yielding a superior catalyst for ethane oxidation.
- Haiyan Wang
- , Shuang Wang
- & Xinwen Guo
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Article
| Open AccessStretchable phosphorescent polymers by multiphase engineering
Stretchable phosphorescent materials have potential in applications such as wearable electronics, but achieving a suitable balance of emission and stretchability is challenging. Here, the authors report the use of microphase separation to show stretchability with emission lifetimes maintained.
- Nan Gan
- , Xin Zou
- & Wei Huang
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Article
| Open AccessAsymmetric C–H Dehydrogenative Alkenylation via a Photo-induced Chiral α‑Imino Radical Intermediate
The direct alkenylation with simple alkenes stands out as the most ideal yet challenging strategy for obtaining high-valued desaturated alkanes. Herein, the authors present a direct asymmetric dehydrogenative α-C(sp3)-H alkenylation of carbonyls based on synergistic photoredox-cobalt-chiral primary amine catalysis under visible light.
- Zongbin Jia
- , Liang Cheng
- & Sanzhong Luo
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Comment
| Open AccessA critical discussion of the current availability of lithium and zinc for use in batteries
Aqueous zinc batteries are currently being explored as potential alternatives to non-aqueous lithium-ion batteries. In this comment, the authors highlight zinc’s global supply chain resilience and lower material costs yet caution about its higher mass requirement for comparable charge storage.
- Alessandro Innocenti
- , Dominic Bresser
- & Stefano Passerini
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Article
| Open AccessTracking nuclear motion in single-molecule magnets using femtosecond X-ray absorption spectroscopy
The authors use femtosecond K-edge X-ray absorption spectroscopy to follow nuclear motion in a manganese-based tri-nuclear single-molecule magnet, and resolve changes in bond lengths on the order of hundreds of ångströms and on sub-picosecond timescales.
- Kyle Barlow
- , Ryan Phelps
- & J. Olof Johansson
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Article
| Open AccessSustainable upcycling of mixed spent cathodes to a high-voltage polyanionic cathode material
Direct recycling of critical battery materials bring promise but a challenge for the mixed cathode chemistries. Here, the authors report a sustainable upcycling approach, transforming degraded LiFePO4 and Mn-rich cathodes into a high-voltage polyanionic material with an increased energy density and economic value.
- Guanjun Ji
- , Di Tang
- & Hui-Ming Cheng
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Article
| Open AccessAtomically dispersed asymmetric cobalt electrocatalyst for efficient hydrogen peroxide production in neutral media
The relationship between the structural configurations of M-N-C electrocatalysts and their performances in neutral environments has been insufficiently investigated. Here the authors demonstrate that an ultralow metal-loaded Co-N-C electrocatalyst, featuring the asymmetric Co-C/N/O configuration, exhibit exceptional efficiency in electrochemically producing hydrogen peroxide under neutral conditions.
- Longxiang Liu
- , Liqun Kang
- & Guanjie He
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Article
| Open AccessMechanically controlled multifaceted dynamic transformations in twisted organic crystal waveguides
Crystals with mechanical responses are of interest, but often only one or two dynamic motions can be achieved with one crystal. Here, the authors report a combination of dynamic movements in naturally twisted optical waveguiding microcrystals.
- Mehdi Rohullah
- , Vuppu Vinay Pradeep
- & Rajadurai Chandrasekar
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Article
| Open AccessRapid and scalable photocatalytic C(sp2)–C(sp3) Suzuki−Miyaura cross-coupling of aryl bromides with alkyl boranes
In recent years a growing demand for drug design approaches that incorporate a higher number of sp3-hybridized carbons fuelled the development of innovative cross-coupling strategies to reliably introduce aliphatic fragments. Here, the authors present a powerful approach for the light-mediated B-alkyl Suzuki−Miyaura crosscoupling between alkyl boranes and aryl bromides.
- Ting Wan
- , Luca Capaldo
- & Timothy Noël
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Article
| Open AccessOxidative photocatalysis on membranes triggers non-canonical pyroptosis
Oxidative damage to intracellular membrane proteins is critical to cells. Here, the authors use a water-oxidizing photocatalyst, generating ∙OH even under hypoxia, to show that membrane-specific protein oxidation triggers pyroptosis via non-canonical inflammasomes.
- Chaiheon Lee
- , Mingyu Park
- & Tae-Hyuk Kwon
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Article
| Open AccessSynergistic growth of nickel and platinum nanoparticles via exsolution and surface reaction
Utilizing “Chemistry at a point”, Ni is exsolved from a perovskite lattice under deposited Pt nanoparticles. This yields even smaller Ni Pt alloy nanoparticles on a perovskite nanofiber structure, exhibiting high catalytic activity.
- Min Xu
- , Yukwon Jeon
- & John T. S. Irvine
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Article
| Open AccessElectrochemical-repaired porous graphene membranes for precise ion-ion separation
The preparation of atom-thick lattices with Å-scale pores is desirable for achieving ion selectivity and high ion flux. Here authors present a cm-scale membrane made of atom-thick graphene film hosting zero-dimensional pores spanning only a few Å, repaired using an in situ electrochemical strategy, yielding high Li+/Mg2+ separation performance.
- Zongyao Zhou
- , Kangning Zhao
- & Kumar Varoon Agrawal
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Article
| Open AccessOperando Raman spectroscopy uncovers hydroxide and CO species enhance ethanol selectivity during pulsed CO2 electroreduction
Controlling the selectivity of the electroreduction of CO2 to value-added products is challenging. Here, authors use sub-second operando Raman spectroscopy to analyze Cu catalyst surfaces and discover the pivotal role of co-adsorbed OH and CO in enhancing ethanol selectivity.
- Antonia Herzog
- , Mauricio Lopez Luna
- & Beatriz Roldan Cuenya
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Article
| Open AccessGiant magneto-photoluminescence at ultralow field in organic microcrystal arrays for on-chip optical magnetometer
The optical detection of magnetic fields is difficult for low field strengths. Here, the authors show how strong magneto-photoluminescence can be achieved in rubrene microcrystals and demonstrate its application in a magnetometer.
- Hong Wang
- , Baipeng Yin
- & Chuang Zhang
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Article
| Open AccessDeciphering complexity in Pd–catalyzed cross-couplings
Knowledge about the full reaction signature, such as the complete profile of products and side-products is important in accelerating discovery chemistry. Here, the authors report a methodology using high-throughput experimentation and multivariate data analysis to examine Palladium- catalyzed cross-coulpling reactions.
- George E. Clarke
- , James D. Firth
- & Ian J. S. Fairlamb
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Article
| Open AccessVitrification-enabled enhancement of proton conductivity in hydrogen-bonded organic frameworks
Proton conduction is one of the interesting applications of hydrogen-bonded organic frameworks. Here, the authors report hydrogen-bonded organic framework that can be transformed into glassy state, effectively mitigating grain boundary effects, and significantly enhancing proton conduction performance.
- Feng-Fan Yang
- , Xiao-Lu Wang
- & Linfeng Liang
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Article
| Open AccessNested non-covalent interactions expand the functions of supramolecular polymer networks
Supramolecular polymer networks have unique and useful properties due to the reversible nature of their cross-links. Here, the authors show that when two distinct supramolecular interaction classes exist within a single cross-link, new functions can result.
- David J. Lundberg
- , Christopher M. Brown
- & Jeremiah A. Johnson
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Article
| Open AccessIntegrating spin-dependent emission and dielectric switching in FeII catenated metal-organic frameworks
Incorporating spin crossover motifs into mechanically interlocked molecules offers various switchable properties. Here, the authors report two FeII catenated metal-organic frameworks that exhibit spin dependent luminescence and dielectric switching.
- Xue-Ru Wu
- , Shu-Qi Wu
- & Hui-Zhong Kou
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Article
| Open AccessCorrelating activities and defects in (photo)electrocatalysts using in-situ multi-modal microscopic imaging
Physicochemical heterogeneity poses a significant constraint in photocatalyst advancement. Here the authors introduce a multimodal optical microscopy platform to assess activity and defects concurrently in photoelectrocatalysts, revealing that disorder can unexpectedly enhance local photoelectrocatalytic performance in certain instances.
- Camilo A. Mesa
- , Michael Sachs
- & Raj Pandya
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Article
| Open AccessNeutron scattering and neural-network quantum molecular dynamics investigation of the vibrations of ammonia along the solid-to-liquid transition
Through neutron scattering experiments coupled with machine learning, the authors uncover the strong role of nuclear quantum effects in the dynamics of ammonia in both its solid and technologically relevant liquid phase.
- T. M. Linker
- , A. Krishnamoorthy
- & P. D. Vashishta
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Article
| Open AccessGas adsorption and framework flexibility of CALF-20 explored via experiments and simulations
CALF-20 is a water stable structure capable of selectively separating CO2 from flue gas. Here authors use a close feedback loop between theory and experiments to understand CO2/water adsorption and framework flexibility of CALF-20.
- Rama Oktavian
- , Ruben Goeminne
- & Peyman Z. Moghadam
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Article
| Open AccessBulk transparent supramolecular glass enabled by host–guest molecular recognition
Strategies to produce supramolecular glass and the study of its intrinsic structure and mechanical properties remains largely unexplored. Here, the authors prepare a supramolecular glass via the host–guest recognition between methyl-β-cyclodextrin and para-hydroxybenzoic acid with recyclability, compatibility, and thermal processability.
- Changyong Cai
- , Shuanggen Wu
- & Shengyi Dong
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Article
| Open AccessEffect of crystal facets in plasmonic catalysis
Crystal facets are known to be important in traditional heterogeneous catalysis, yet this effect has not been studied in plasmon-assisted catalysis. Here, the authors investigate the impact facets have on CO2 reduction using plasmonic Au NPs.
- Yicui Kang
- , Simão M. João
- & Emiliano Cortés
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Article
| Open AccessBicontinuous RuO2 nanoreactors for acidic water oxidation
Developing stable water oxidation catalysts is of great importance for proton-exchange membrane water electrolyzers. Here the authors report a bicontinuous nanoreactor composed of multiscale defected RuO2 nanocrystals for robust acidic water oxidation reactivity.
- Ding Chen
- , Ruohan Yu
- & Shichun Mu
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Article
| Open AccessA locally solvent-tethered polymer electrolyte for long-life lithium metal batteries
Solid polymer electrolytes containing N,N-dimethylformamide (DMF) exhibit improved Li+ conductivity but poor cycle life due to incompatibility between the Li metal anode and DMF. Here, the authors report a polymer electrolyte composited with Hofmann-DMF complex that achieves both high Li+ conductivity and long cycle life.
- Yanfei Zhu
- , Zhoujie Lao
- & Guangmin Zhou
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Article
| Open AccessSustainable 3D printing by reversible salting-out effects with aqueous salt solutions
Here, the authors show a facile and sustainable 3D printing by utilizing a reversible salting-out effect on poly(N-isopropylacrylamide) (PNIPAM) solutions. Aqueous salt solutions lower the phase transition temperature of PNIPAM solutions below 10 °C and instantly solidify the PNIPAM solutions upon contact.
- Donghwan Ji
- , Joseph Liu
- & Jinhye Bae
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Article
| Open AccessInterplay of structural preorganization and conformational sampling in UDP-glucuronic acid 4-epimerase catalysis
Enzymes involve structural flexibility in their function, but understanding enzyme catalysis as connected to protein motions is a major challenge. Here, the authors obtain energetic description of C-H activation in nicotinamide coenzyme-dependent UDP-glucuronic acid C4 epimerase based on temperature kinetic studies and isotope effect measurements.
- Christian Rapp
- , Annika Borg
- & Bernd Nidetzky
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Article
| Open AccessN2 cleavage by silylene and formation of H2Si(μ-N)2SiH2
So far, only homoleptic N2 complexes of silicon have been reported under matrix-isolation conditions including but the activation of more inert nitrogen by silylenes remains challenging. Here the authors report on the activation of dinitrogen by silylenes under cryogenic conditions.
- Liyan Cai
- , Bing Xu
- & Xuefeng Wang
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Article
| Open AccessVisualizing the gas-sensitive structure of the CuZn surface in methanol synthesis catalysis
Industrial methanol synthesis uses materials based on Cu and ZnO. We present high-resolution imaging of active surfaces which reveals how Zn species are transported at the active Cu interface in diffusion processes controlled by the reactant gas composition.
- Sigmund Jensen
- , Mathias H. R. Mammen
- & Jeppe V. Lauritsen
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Article
| Open Access“On-Water” accelerated dearomative cycloaddition via aquaphotocatalysis
Developing water compatible synthetic methods for Sulfur(VI) fluoride exchange (SuFEx) chemistry is of paramount importance. Here the authors demonstrate a catalytic dearomative [2+2] photocycloaddition that significantly speeds up the synthesis of heterocyclic alkyl SuFEx hubs, leveraging the unique reactivity at the water-oil interface.
- Soo Bok Kim
- , Dong Hyeon Kim
- & Han Yong Bae
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