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Article
| Open AccessStress-induced ordering evolution of 1D segmented heteronanostructures and their chemical post-transformations
The formation mechanisms for periodic heterostructures are still poorly understood. Here, the authors propose a versatile approach to synthesize one-dimensional segmented heterostructures and reveal a stress-induced ordering mechanism through phase-field simulations.
- Qing-Xia Chen
- , Yu-Yang Lu
- & Shu-Hong Yu
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Article
| Open AccessEnhancing photocatalytic H2O2 production with Au co-catalysts through electronic structure modification
Photocatalytic H2O2 production using Au is hindered by its inherently weak O2 adsorption. Herein, the authors modify the electronic structure of Au with MoSx to form electron deficient Au sites to promote O2 adsorption and H2O2 production.
- Xidong Zhang
- , Duoduo Gao
- & Huogen Yu
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Article
| Open AccessQuantum phase synchronization via exciton-vibrational energy dissipation sustains long-lived coherence in photosynthetic antennas
Photosynthesis in biological systems occurs in a noisy environment that reduces the lifetime of coherences in the excitation energy transfer. Here the author demonstrate that long-lasting coherences are protected by quantum phase synchronization, realized in dimers by exciton-vibrational coupling where energy dissipation occurs predominantly in resonant anti-symmetric collective modes.
- Ruidan Zhu
- , Wenjun Li
- & Yuxiang Weng
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Article
| Open AccessFrustrated Lewis pair catalyst realizes efficient green diesel production
The commercial production of green diesel suffers from the requirement for continuous sulfur replenishment to maintain catalytic activity. Here, the authors report a sulfur-free catalytic system that can efficiently produce green diesel from various feedstocks over long periods of operation.
- De-Chang Li
- , Zhengyi Pan
- & Guang-Hui Wang
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Article
| Open AccessSolvent-free selective hydrogenation of nitroaromatics to azoxy compounds over Co single atoms decorated on Nb2O5 nanomeshes
Single atom catalysts can endow exceptional activity and selectively. Here, the authors report a single atom Co catalyst and reveal the importance of geometric and electronic properties for synthesizing azoxy compounds under solvent-free conditions.
- Zhijun Li
- , Xiaowen Lu
- & Yu Wang
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Article
| Open AccessA facile one step route that introduces functionality to polymer powders for laser sintering
Polyamide-12 is the main polymer employed to produce 3D objects by laser sintering constraining the functionality of the items produced. Here, the authors report a clean and scalable approach for the functionalization of polyamide-12 particles, yielding materials that can be printed using commercial apparatus.
- Eduards Krumins
- , Liam A. Crawford
- & Steven M. Howdle
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Article
| Open AccessControlled condensation by liquid contact-induced adaptations of molecular conformations in self-assembled monolayers
Surface condensation is predetermined and is typically adjusted by chemical or topographical surface modification. Here, the authors report on a strategy to control the surface condensation behavior by adjusting molecular conformations in self-assembled monolayers.
- Guoying Bai
- , Haiyan Zhang
- & Yufeng Liu
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Article
| Open AccessSpiral packing and chiral selectivity in model membranes probed by phase-resolved sum-frequency generation microscopy
The properties of lipid membranes are intimately controlled by their complex heterogeneous structure. Here, the authors use phase-resolved sum-frequency generation microscopy to fully determine the hierarchical lipid packing from the molecular to the mesoscopic scale.
- Alexander P. Fellows
- , Ben John
- & Martin Thämer
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Article
| Open AccessPrecision ion separation via self-assembled channels
Selective nanofiltration membranes with accurate molecular sieving offer a solution to recover rare metals and other valuable elements from brines but this demands the development of membranes with precise sub-nanometer pores surpassing those available today. Here, the authors report a scalable approach for membrane fabrication in which functionalized macrocycles are seamlessly oriented via supramolecular interactions during the interfacial polycondensation on a polyacrylonitrile support layer.
- Shanshan Hong
- , Maria Di Vincenzo
- & Suzana P. Nunes
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Article
| Open AccessTwo-dimensional lead halide perovskite lateral homojunctions enabled by phase pinning
Hong et al. report 2D perovskite lateral homojunction consists of ordered and disordered phases, achieved by organic cation doping induced phase pinning, built upon which they develop tuneable optical properties under external stimuli and directional exciton diffusion in the homojunctions.
- Huilong Hong
- , Songhao Guo
- & Yongping Fu
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Article
| Open AccessBeyond nothingness in the formation and functional relevance of voids in polymer films
Voids are known to impact the properties of materials, but the nanovoids also present are less well understood than macroscopic voids. Here, the authors utilise 3D imaging and graph theory to study nanovoid formation and impact on material properties.
- Falon C. Kalutantirige
- , Jinlong He
- & Qian Chen
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Article
| Open AccessOrganocatalytic desymmetrization provides access to planar chiral [2.2]paracyclophanes
Planar chiral [2.2]paracyclophanes have a wide range of applications in asymmetric synthesis and materials science. However, they are accessed via time-consuming chiral separations or kinetic resolution approaches. Here, the authors report a simple, metal-free protocol for organocatalytic desymmetrization of prochiral diformyl[2.2]paracyclophanes.
- Vojtěch Dočekal
- , Filip Koucký
- & Jan Veselý
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Article
| Open AccessThermally stable Ni foam-supported inverse CeAlOx/Ni ensemble as an active structured catalyst for CO2 hydrogenation to methane
An inverse CeAlOx/Ni/Ni-foam structured catalyst with high thermal stability and water resistance is shown to be effective at CO2 methanation across a wide temperature range because of efficient heat/mass transport.
- Xin Tang
- , Chuqiao Song
- & Lili Lin
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Article
| Open AccessReverse water gas-shift reaction product driven dynamic activation of molybdenum nitride catalyst surface
Catalyst activation commonly occurs during reactions. This study demonstrates that the surface’s active structure in nitride catalysts during the reverse water gas-shift reaction varies with the partial pressure of reaction products, resulting in enhanced catalytic activity through positive feedback between catalytic activity and the evolution of MoNx’s active structure.
- Hui Xin
- , Rongtan Li
- & Xinhe Bao
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Article
| Open AccessLow-nuclearity CuZn ensembles on ZnZrOx catalyze methanol synthesis from CO2
The ideal metal selection and atomic-level arrangement for catalysts in CO2 hydrogenation are still uncertain. Here, copper is identified as the most effective promoter for enhancing ZnZrOx catalysts when precisely structured into CuZn ensembles, offering new insights for designing superior catalysts for CO2-based methanol synthesis.
- Thaylan Pinheiro Araújo
- , Georgios Giannakakis
- & Javier Pérez-Ramírez
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Article
| Open AccessElectrochemically coupled CH4 and CO2 consumption driven by microbial processes
The microbial valorisation of greenhouse gases could offer promising approaches climate change mitigation. Here, authors demonstrate the coupling of methane oxidation and carbon dioxide reduction by microbial consortia, facilitated by the redox cycling of iron minerals.
- Yue Zheng
- , Huan Wang
- & Feng Zhao
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Article
| Open AccessCarbon dioxide capture and functionalization by bis(N-heterocyclic carbene)-borylene complexes
Bis(N-heterocyclic carbene)-borylene complexes are capable of capturing and functionalizing CO2, but stable single-site-boron-carbon dioxide adducts are rarely reported. Here, the authors report the synthesis of a stable borylene-CO2 complex as well as the functionalization of the captured CO2.
- Jun Fan
- , An-Ping Koh
- & Cheuk-Wai So
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Article
| Open AccessHighly robust supramolecular polymer networks crosslinked by a tiny amount of metallacycles
Supramolecular polymeric materials have exhibited attractive features such as self-healing, reversibility and stimuli-responsiveness but because of the weak bonding nature of most noncovalent interactions, constructing supramolecular polymer materials with high robustness remains challenging. Here, the authors describe the construction of highly robust stimuli-responsive supramolecular polymer networks by using only a tiny amount of metallacycles as the supramolecular crosslinkers.
- Lang He
- , Yu Jiang
- & Shijun Li
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Article
| Open AccessSurface oxidation/spin state determines oxygen evolution reaction activity of cobalt-based catalysts in acidic environment
Co-based catalysts are promising candidates for oxygen evolution reaction catalysis in an acidic environment, but the structure-activity relationship is unclear. Here, the authors discover that their acidic water oxidation activity is determined by the surface oxidation/spin state.
- Jinzhen Huang
- , Camelia Nicoleta Borca
- & Emiliana Fabbri
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Article
| Open AccessA 2D chiral microcavity based on apparent circular dichroism
Here the authors induce asymmetric transmission in planar Fabry–Pérot microcavities by embedding organic thin films exhibiting apparent circular dichroism (ACD), an optical phenomenon based on 2D chirality.
- Tzu-Ling Chen
- , Andrew Salij
- & Randall H. Goldsmith
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Article
| Open AccessExpedient production of site specifically nucleobase-labelled or hypermodified RNA with engineered thermophilic DNA polymerases
A general method for enzymatic synthesis of base-modified RNA was developed using engineered thermostable DNA polymerases enabling introduction of site-specific modifications or synthesis of hypermodified RNA not accessible by in vitro transcription.
- Mária Brunderová
- , Vojtěch Havlíček
- & Michal Hocek
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Article
| Open AccessKinetically controlled metal-elastomer nanophases for environmentally resilient stretchable electronics
Metal-elastomer nanophases are critical for stretchable electronics but face mixing challenges. This study introduces a kinetic method for precise mixing, yielding gyrified nanophases with improved durability and strain-invariant conductivity, which holds promise for resilient stretchable devices.
- Soosang Chae
- , Won Jin Choi
- & Tae Il Lee
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Article
| Open AccessEnabling robust blue circularly polarized organic afterglow through self-confining isolated chiral chromophore
The preparation of systems that give blue circularly polarised organic afterglow is desirable but challenging. Here, the authors confine a chiral chromophore within a polymer matrix to limit non-radiative transitions and give blue circularly polarised organic afterglow.
- Mingjian Zeng
- , Weiguang Wang
- & Wei Huang
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Article
| Open AccessVapor-induced phase-separation-enabled versatile direct ink writing
The extrusion-based three-dimensional printing of polymers, metals, and composites requires elevated temperatures and may lead to diverse undesirable defects on printed parts. Here, the authors develop a vapor-induced phase separation printing technique to construct polymeric, metallic, and composite parts by using a polymer as a binder.
- Marc Sole-Gras
- , Bing Ren
- & Yong Huang
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Article
| Open AccessOptically induced charge-transfer in donor-acceptor-substituted p- and m- C2B10H12 carboranes
Icosahedral carboranes have long been considered to be aromatic but the extent of conjugation between these clusters and their substituents is still being debated. Here the authors demonstrate carboranes as conjugated bridges in optical functional chromophores.
- Lin Wu
- , Marco Holzapfel
- & Lei Ji
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Article
| Open AccessFine-tuning the pore environment of ultramicroporous three-dimensional covalent organic frameworks for efficient one-step ethylene purification
The construction of three-dimensional covalent organic frameworks for gas separation is challenging due to the similar physicochemical properties of the gas mixture. Here, the authors report functional three-dimensional covalent organic frameworks by fine-tunning the pore environment with pyridine units to achieve effective separation of ethane from ethylene.
- Yang Xie
- , Wenjing Wang
- & Cheng Wang
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Article
| Open AccessClosed-loop recycling of sulfur-rich polymers with tunable properties spanning thermoplastics, elastomers, and vitrimers
Sulfur-rich polymers are promising candidates for chemical recycling but lack efficient synthetic strategies for achieving diverse structures. Here, the authors report a synthesis strategy for polytrithiocarbonates which is compatible with a wide range of monomers enabling diverse structures via polycondensation of dithiols and dimethyl trithiocarbonate.
- Jin-Zhuo Zhao
- , Tian-Jun Yue
- & Wei-Min Ren
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Article
| Open AccessUpgrading CO2 to sustainable aromatics via perovskite-mediated tandem catalysis
The transformation of CO2 with renewable hydrogen into high-value products presents a sustainable route for net-zero chemical manufacture. Here the authors introduce a LaFeO3 perovskite-mediated tandem conversion of CO2, achieving remarkable performance by separating the CO2 hydrogenation and C-C coupling domains in the catalyst system.
- Guo Tian
- , Zhengwen Li
- & Fei Wei
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Article
| Open AccessUniversal inter-molecular radical transfer reactions on metal surfaces
Radicals are expected to be inactive on metal surfaces. Here the authors describe general intermolecular radical transfer reactions on Ag and Cu surfaces and confirm the reaction mechanism by extensive control experiments.
- Junbo Wang
- , Kaifeng Niu
- & Lifeng Chi
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Article
| Open AccessSlow magnetic relaxation in a europium(II) complex
This study introduces a Eu(II) single molecule magnet that exhibits slow magnetic relaxation at low temperatures. These results highlight the importance of the lanthanide ion’s crystal field in unlocking the magnet-like properties of Eu(II).
- Dylan Errulat
- , Katie L. M. Harriman
- & Muralee Murugesu
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Article
| Open AccessWater-assisted oxidative redispersion of Cu particles through formation of Cu hydroxide at room temperature
Redispersion of sintered metal species requires high temperatures in reactive atmospheres. Here, the authors report room temperature redispersion of supported Cu particles via formation of mobile hydroxylated Cu species induced by gaseous H2O and anchoring of the Cu species by surface OH groups.
- Yamei Fan
- , Rongtan Li
- & Qiang Fu
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Article
| Open AccessExciton engineering of 2D Ruddlesden–Popper perovskites by synergistically tuning the intra and interlayer structures
Guo et al. report enhanced emission and photoconductivity in 2D Ruddlesden-Popper perovskites by synergistically tuning the intra and interlayer structure via pressure. A structure descriptor considering both intra- and interlayer is then introduced for screening perovskite with desired properties.
- Songhao Guo
- , Willa Mihalyi-Koch
- & Xujie Lü
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Article
| Open AccessThermodiffusive desalination
Current desalination technologies are energy intensive and suffer from membrane degradation and fouling. Here, authors propose and explore the potential of thermodiffusion as a means of membrane-free, single-phase thermal desalination. A pathway towards a feasible thermodiffusive desalination is provided.
- Shuqi Xu
- , Alice J. Hutchinson
- & Juan F. Torres
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Article
| Open AccessLigand-modified nanoparticle surfaces influence CO electroreduction selectivity
Enhancing the kinetics and selectivity of CO2/CO electroreduction towards valuable multi-carbon products poses a scientific challenge and is imperative for practical applicability. Here the authors report that modifying copper catalysts with surface thiol ligands significantly improves acetate selectivity.
- Erfan Shirzadi
- , Qiu Jin
- & Edward H. Sargent
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Article
| Open AccessConvoluted micellar morphological transitions driven by tailorable mesogenic ordering effect from discotic mesogen-containing block copolymer
Assembly of block copolymers can be controlled to give varying morphologies and functionalities, but there are still aspects of the process that are not well understood. Here, the authors report convoluted self-assembly behaviours of block copolymers with discotic liquid crystalline moieties.
- Huanzhi Yang
- , Yunjun Luo
- & Xiaoyu Li
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Article
| Open AccessTumor-activated in situ synthesis of single-atom catalysts for O2-independent photodynamic therapy based on water-splitting
The utility of single-atom catalysts (SACs) for photodynamic therapy (PDT) has been limited by tumor hypoxia and side effects on normal tissues. Here the authors address these issues by developing an approach of tumor microenvironment-activated in situ synthesis of SACs for tumor-specific water-based PDT.
- Yiyan Yin
- , Xiyang Ge
- & Na Na
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Article
| Open AccessA silicon photoanode protected with TiO2/stainless steel bilayer stack for solar seawater splitting
Here, the authors report a Si photoanode coated with a TiO2/stainless steel bilayer to inhibit chloride adsorption and facilitate stable alkaline seawater splitting for over 50 h with an applied bias photon-to-current efficiency of 2.62%.
- Shixuan Zhao
- , Bin Liu
- & Jinlong Gong
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Article
| Open AccessArtificial kagome lattices of Shockley surface states patterned by halogen hydrogen-bonded organic frameworks
By utilizing the templating effect of a halogen hydrogen-bonded organic framework, the authors show that the Shockley surface states of coinage metals can be patterned into artificial kagome lattices with high tunability.
- Ruoting Yin
- , Xiang Zhu
- & Bing Wang
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Article
| Open AccessEmissive brightening in molecular graphene nanoribbons by twilight states
The authors demonstrate that the band structure of graphene nanoribbons is modulated by cove edges, brightening the luminescence 4-fold via emission from otherwise dark twilight states. High spectral resolution of the optical response reveals strong vibron-electron coupling
- Bernd K. Sturdza
- , Fanmiao Kong
- & Robin J. Nicholas
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Article
| Open AccessLong lifetimes white afterglow in slightly crosslinked polymer systems
It is challenging to achieve multicolor long-lived room temperature phosphorescence in intrinsic polymers, especially for white afterglow. Here, the authors report a strategy to obtain pure white afterglow micro-crosslinked polymers by covalently coupling different conjugated chromophores with precursors through a simple and rapid one-pot reaction.
- Qingao Chen
- , Lunjun Qu
- & Chaolong Yang
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Article
| Open AccessChemical unclonable functions based on operable random DNA pools
Physical unclonable functions provide algorithm-independent cryptography based on non-distributable unique tokens. Here, the authors introduce unclonable functions based on random DNA pools, enabling secure decentralized authentication.
- Anne M. Luescher
- , Andreas L. Gimpel
- & Robert N. Grass
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Article
| Open AccessEfficient bubble/precipitate traffic enables stable seawater reduction electrocatalysis at industrial-level current densities
Seawater electroreduction is a promising technique for producing hydrogen, but it is hindered by cathodic Mg2 + /Ca2+ precipitation. Here, the authors propose a microscopic bubble/precipitate traffic system that releases small-sized bubbles across the cathode to repel Mg2 + /Ca2+ precipitates from almost the entire surface area of the catalyst.
- Jie Liang
- , Zhengwei Cai
- & Bo Tang
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Article
| Open AccessLaMg6Ga6S16: a chemical stable divalent lanthanide chalcogenide
Synthesising chemically stable divalent lanthanide compounds is still faced by great challenges. Here, by using octahedra coupling tetrahedra single/double chains to construct an octahedral crystal field, authors synthesised a stable crystalline La(II)-chalcogenide, LaMg6Ga6S16.
- Yujie Zhang
- , Jiale Chen
- & Hongwei Yu
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Article
| Open AccessActivating reversible carbonate reactions in Nasicon solid electrolyte-based Na-air battery via in-situ formed catholyte
Metal-air batteries, operated in ambient air, suffer from irreversible redox reactions, limiting their energy density. Herein, the authors present a solid electrolyte-based sodium-air battery with a reversible carbonate reaction, facilitated by the in-situ formed catholyte enabled by moisture.
- Heetaek Park
- , Minseok Kang
- & Byoungwoo Kang
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Article
| Open AccessPaired electrocatalysis unlocks cross-dehydrogenative coupling of C(sp3)-H bonds using a pentacoordinated cobalt-salen catalyst
Cross-dehydrogenative coupling (CDC) of C-H bonds is an ideal approach for C-C bond construction but suffers from low selectivity of similar C-H bonds. Here, the authors describe a highly selective paired electrocatalysis strategy towards CDC combining hydrogen evolution reaction catalysis with hydride transfer catalysis.
- Ke Liu
- , Mengna Lei
- & Sheng Zhang
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Article
| Open AccessAluminum corrosion–passivation regulation prolongs aqueous batteries life
Aqueous batteries have a short lifespan due to Al current collector corrosion and Li loss from side reactions on the anode. Here, the authors propose a prototype of self-prolonging aqueous Li-ion batteries by introducing hydrolyzation-type anodic additives to regulate Al corrosion-passivation.
- Binghang Liu
- , Tianshi Lv
- & Liumin Suo
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Article
| Open AccessAggregation induced emission dynamic chiral europium(III) complexes with excellent circularly polarized luminescence and smart sensors
Chiral luminescent materials are of increasing interest in various applications, but achieving a desirable balance of properties can be challenging. Here, the authors report the development of Eu-based complexes with chiral luminescence and aggregation induced emission.
- Yun-Lan Li
- , Hai-Ling Wang
- & Hua-Hong Zou
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Article
| Open AccessNickel-catalyzed switchable arylative/endo-cyclization of 1,6-enynes
Divergent functionalizations of pi bonds allow for synthetic chemists to move from simplicity to complexity. Here, the authors report a nickel-catalyzed switchable arylation/cyclization of 1,6-enynes in which the nature of the ligand dictates the regioselectivity of alkyne arylation, while the electrophilic trapping reagents determine the selectivity of the cyclization mode.
- Wenfeng Liu
- , Wei Li
- & Wangqing Kong
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Article
| Open AccessMolecular insight into the initial hydration of tricalcium aluminate
The hydration of tricalcium aluminate is an important initial step in the structural build-up of Portland cement. Here the authors use ab initio and accelerated dynamics to describe the reactions and dynamics of this process at the molecular level.
- Xing Ming
- , Wen Si
- & Zongjin Li
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