Featured
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Article
| Open AccessMetal free cross-dehydrogenative N-N coupling of primary amides with Lewis basic amines
While the homo N-N coupling of two NH moieties to form the hydrazide N-N bond is well developed, the crossdehydrogenative hetero N-N coupling remains unevolved. Here the authors present an efficient, PhI(OAc)2-mediated intermolecular N-N cross-coupling of primary benzamides with primary and secondary amines.
- Subban Kathiravan
- , Prakriti Dhillon
- & Ian A. Nicholls
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Article
| Open AccessKeto-anthraquinone covalent organic framework for H2O2 photosynthesis with oxygen and alkaline water
Hydrogen peroxide photosynthesis is an important reaction that suffers from poor activity due to the high energy barrier of hydrogen extraction in water. Here, we report a keto-form anthraquinone framework that shows promising performance in alkaline conditions.
- Xiangcheng Zhang
- , Silian Cheng
- & Lizhi Zhang
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Article
| Open AccessEngineering the pore environment of antiparallel stacked covalent organic frameworks for capture of iodine pollutants
Radioiodine capture from nuclear fuel waste and contaminated water sources is of environmental importance but technically challenging. Here, the authors report covalent organic frameworks with antiparallel eclipsed stacked structures with dynamic adsorption performance for iodine pollutants under various conditions.
- Yinghui Xie
- , Qiuyu Rong
- & Xiangke Wang
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Article
| Open AccessQuantifying the interfacial triboelectricity in inorganic-organic composite mechanoluminescent materials
Mechanoluminescence enables sensing applications of mechanical stimuli. Here, the authors reveal the importance of interfacial triboelectricity to this phenomenon in inorganic-organic composite materials.
- Xin Pan
- , Yixi Zhuang
- & Rong-Jun Xie
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Article
| Open AccessSolar-driven sugar production directly from CO2 via a customizable electrocatalytic–biocatalytic flow system
Solar-driven artificial food synthesis from CO2 provides an approach to overcome the limitations of natural photosynthesis, but it is very challenging. Here, the authors report a hybrid electrocatalytic-biocatalytic flow system, coupling photovoltaics-powered electrocatalysis (CO2 to formate) with a five enzyme cascade platform (formate to sugar), which achieves conversion of CO2 to C6 sugar (L-sorbose) with a solar-to-food energy conversion efficiency of 3.5%.
- Guangyu Liu
- , Yuan Zhong
- & Yujie Xiong
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Article
| Open AccessDeveloping a machine learning model for accurate nucleoside hydrogels prediction based on descriptors
Supramolecular nucleoside-based hydrogels have potential in biomedical applications, but there is no model to predict what nucleoside derivatives will form hydrogels. Here, the authors report a machine learning model to predict the ability of nucleoside derivatives to form hydrogels.
- Weiqi Li
- , Yinghui Wen
- & Hang Zhao
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Article
| Open AccessUltra-fast green hydrogen production from municipal wastewater by an integrated forward osmosis-alkaline water electrolysis system
Green hydrogen production faces increased water risks due to scarce supplies of water. Here, authors develop a modular forward osmosis-water splitting system that utilises wastewater effluent to generate high-purity hydrogen, providing a sustainable solution for water and energy security.
- Gabriela Scheibel Cassol
- , Chii Shang
- & Li Ling
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Article
| Open AccessA molecular extraction process for vanadium based on tandem selective complexation and precipitation
Amidst vanadium’s growing demand and environmental concerns in mining, the researchers, using naphthalimidedioxime, crafted a breakthrough method for eco-friendly recovery. Their acid-stable agent and non-toxic complexes offer a promising solution for large-scale vanadium recovery from diverse sources.
- Oluwatomiwa A. Osin
- , Shuo Lin
- & George K. H. Shimizu
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Article
| Open AccessThermodynamic driving forces in contact electrification between polymeric materials
Contact electrification is a widely observed phenomenon in nature and in materials. Here, the authors use molecular dynamics simulations to show the importance of thermodynamic driving forces in contact electrification in insulating materials.
- Hang Zhang
- , Sankaran Sundaresan
- & Michael A. Webb
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Article
| Open AccessStrategies for high-temperature methyl iodide capture in azolate-based metal-organic frameworks
Efficient capture of methyl iodide (CH3I) from high-temperature nuclear off-gas is quite challenging. Here, the authors present two innovative and efficient strategies to adsorb CH3I at high temperatures in an azolate-based metal-organic framework.
- Tingting Pan
- , Kaijie Yang
- & Yu Han
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Article
| Open AccessSelective sorting of hexane isomers by anion-functionalized metal-organic frameworks with optimal energy regulation
Balancing the separation selectivity and regeneration energy of alkane isomers is a daunting challenge. Here the authors utilize flexible host-guest interactions to maximize the gas-framework interactions while achieving potential energy storage to set new benchmarks for alkane isomer separation.
- Qingju Wang
- , Lifeng Yang
- & Huabin Xing
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Article
| Open AccessReduction of Li+ within a borate anion
Chemical reduction of alkali cations to their metals is extremely challenging. Here, the authors synthesized a series of redox-active borate anions stabilized by bipyridine ligands which can reduce lithium ions generating elemental lithium metal and borate radicals.
- Haokun Li
- , Jiachen Yao
- & Zhenpin Lu
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Article
| Open AccessSingle-atom platinum with asymmetric coordination environment on fully conjugated covalent organic framework for efficient electrocatalysis
In addition to maximizing atomic utilization, single-atom catalysts with defined structures can be used to investigate catalytic mechanisms and structure-activity relationships. Here, authors study a non-thermodynamically stable Pt-N2 active site for the electrochemical hydrogen evolution reaction.
- Ziqi Zhang
- , Zhe Zhang
- & Shouhua Feng
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Article
| Open AccessWater-participated mild oxidation of ethane to acetaldehyde
The direct conversion of low alkane-like ethane into high-value chemicals has posed a significant challenge. Herein, the authors successfully accomplish a one-step conversion of ethane to C2 oxygenates using a Rh single-atom catalyst under mild conditions.
- Bin Li
- , Jiali Mu
- & Yunjie Ding
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Article
| Open AccessEfficient palladium-catalyzed electrocarboxylation enables late-stage carbon isotope labelling
Carbon isotope labelling of bioactive molecules is essential for accessing the pharmacokinetic and pharmacodynamic properties of new drug entities. Here, the authors propose an electrochemical isotope-labelling protocol which enables the use of near-stoichiometric 14CO2, facilitating late-stage and single-step carbon-14 labelling of pharmaceuticals and representative precursors.
- Gabriel M. F. Batista
- , Ruth Ebenbauer
- & Troels Skrydstrup
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Article
| Open AccessUltra-photostable small-molecule dyes facilitate near-infrared biophotonics
Near-infrared small molecule dyes are attractive in biophotonics, but generally rely on expanded aromatic structures to achieve this redshift. Here the authors report the use of a ground state antiaromatic strategy for 14 aminofluorene dyes, and their use in imaging kidney injury.
- Kui Yan
- , Zhubin Hu
- & Fan Zhang
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Article
| Open AccessDeciphering the critical role of interstitial volume in glassy sulfide superionic conductors
Glass sulfide electrolytes are promising materials for solid-state Li metal batteries, yet limited understanding hinders their progress. Here, the authors decipher the dissolution process of halogen dopants in glass and introduce a synthetic strategy to increase halogen dopant’s dissolution capacity.
- Han Su
- , Yu Zhong
- & Jiangping Tu
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Article
| Open AccessNucleic-acid-base photofunctional cocrystal for information security and antimicrobial applications
Cocrystal engineering is a promising strategy for constructing multifunctional materials. Here, the authors describe nucleic-acid-base cocrystal systems with different colors of phosphorescence from their monomeric counterparts and high-temperature phosphorescence with antimicrobial effects and data encryption applications.
- Wenqing Xu
- , Guanheng Huang
- & David Lee Phillips
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Article
| Open AccessPhotoswitchable polyynes for multiplexed stimulated Raman scattering microscopy with reversible light control
Bioimaging with photocontrol and multiplexing capability is vital for studying cellular interactions and dynamics, but multiplexed stimulated Raman scattering (SRS) imaging with reversible photocontrol is elusive. Here, the authors report SRS microscopy with Carbow-switch enabling multiplexed SRS imaging and tracking in live cells with reversible photocontrol and high spatiotemporal selectivity.
- Yueli Yang
- , Xueyang Bai
- & Fanghao Hu
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Article
| Open AccessSpectroscopic visualization of reversible hydrogen spillover between palladium and metal–organic frameworks toward catalytic semihydrogenation
The authors report an in situ investigation of interfacial hydrogen spillover in Pd/ZIF-8 structures with X-ray and Raman techniques. A mechanistic picture of how Pd/ZIF-8 catalyst mediate alkyne semihydrogenation to alkynes is described.
- Qiaoxi Liu
- , Wenjie Xu
- & Yujie Xiong
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Article
| Open AccessLarge exchange-driven intrinsic circular dichroism of a chiral 2D hybrid perovskite
Li et al. report large circular dichroism in 2D chiral perovskite single crystals, arises from the inorganic sublattice, instead of chiral ligands, driven by electron-hole exchange interactions. This is evidenced by both reflective circular dichroism spectroscopy and ab initio theory.
- Shunran Li
- , Xian Xu
- & Peijun Guo
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Article
| Open AccessForward-predictive SERS-based chemical taxonomy for untargeted structural elucidation of epimeric cerebrosides
SERS-based chemical taxonomy is attractive for practical SERS applications where the identity and concentration of analytes are unknown. Here, the authors demonstrate a machine learning framework for classifying “unknown” molecules that lie outside the boundaries of the models used.
- Emily Xi Tan
- , Shi Xuan Leong
- & Xing Yi Ling
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Article
| Open AccessAtmospheric isoprene measurements reveal larger-than-expected Southern Ocean emissions
High atmospheric concentrations of isoprene have been observed in the Southern Ocean. The authors investigate their potential marine sources and show how these emissions impact the modelling of atmospheric processes and composition in remote environments.
- Valerio Ferracci
- , James Weber
- & Neil. R. P. Harris
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Article
| Open AccessA concise and scalable chemoenzymatic synthesis of prostaglandins
Prostaglandins are of interest to synthetic chemists due to their biological activities. Here, the authors present a concise chemoenzymatic synthesis method for several representative prostaglandins, achieved in 5 to 7 steps, via the common intermediate bromohydrin, a radical equivalent of Corey lactone.
- Yunpeng Yin
- , Jinxin Wang
- & Jian Li
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Article
| Open AccessStructurally diverse macrocycle co-crystals for solid-state luminescence modulation
Organic co-crystals are useful in the fabrication of functional materials, but it is challenging to achieve structural diversity of co-crystals. Here, the authors report nine sets of macrocycle cocrystals with diverse structures and stoichiometric ratios giving different luminescence properties.
- Bin Li
- , Lingling Liu
- & Chunju Li
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Article
| Open AccessDynamics of the charge transfer to solvent process in aqueous iodide
Solvated electrons can be formed through photo-induced charge-transfer-to-solvent electronic states of halide ions in water. Here, the authors use machine learning accelerated molecular dynamics simulations to follow the evolution of these states for aqueous iodide in detail.
- Jinggang Lan
- , Majed Chergui
- & Alfredo Pasquarello
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Article
| Open AccessAsymmetric synthesis of P-stereogenic phosphindane oxides via kinetic resolution and their biological activity
P-stereogenic heterocycles are privileged chiral ligands and bioactive compounds, but the catalytic asymmetric synthesis of P-stereogenic phosphindane derivatives is challenging. Here, the authors report a catalytic kinetic resolution of phosphindole oxides via rhodium-catalyzed diastereo- and enantioselective conjugate addition to access enantiopure Pstereogenic phosphindane and phosphindole derivatives.
- Long Yin
- , Jiajia Li
- & Dong Guo
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Article
| Open AccessSqueezing formaldehyde into C60 fullerene
The interconversion of the two spin isomers of formaldehyd has been studied in the gas phase but has never been observed experimentally in the condensed phase. Here the authors report the encapsulation of formaldehyde inside C60 cages and observe spin-isomer conversion of the formaldehyde guest molecules in the cryogenic solid state.
- Vijyesh K. Vyas
- , George R. Bacanu
- & Richard J. Whitby
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Article
| Open AccessTargeted sampling of natural product space to identify bioactive natural product-like polyketide macrolides
Polyketide macrolides are of interest for drug discovery but their inherent structural and stereochemical complexity hinders the exploration of related regions of chemical space more broadly. Here, the authors designed in silico and synthesized a library of tetrahydrofuran-containing polyketide macrolides, and screened them against a panel of biological assays, identifying biologically active library members.
- Darryl M. Wilson
- , Daniel J. Driedger
- & Robert A. Britton
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Article
| Open AccessLate-stage guanine C8–H alkylation of nucleosides, nucleotides, and oligonucleotides via photo-mediated Minisci reaction
Chemically modified nucleobases and oligonucleotides are essential in several fields but introducing functional groups into nucleobases requires laborious chemical synthesis. Here, the authors report site-selective alkylation at the C8-position of guanines in guanosine, GMP, GDP, and GTP, as well as late-stage alkylation of RNA/DNA oligonucleotides through photomediated Minisci reaction.
- Ruoqian Xie
- , Wanlu Li
- & Gang Chen
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Article
| Open AccessThe evolutionary origin of naturally occurring intermolecular Diels-Alderases from Morus alba
Diels-Alderases (DAs), enzymes catalyzing [4 + 2] cycloaddition reactions, are of high interest, but insights into their evolution are lacking. Here, the authors investigate the evolutionary origins of the intermolecular DAs in the biosynthesis of Moraceae plant-derived Diels-Alder-type secondary metabolites, suggesting they evolved from an ancestor functioning as a flavin adenine dinucleotide-dependent oxidocyclase.
- Qi Ding
- , Nianxin Guo
- & Xiaoguang Lei
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Review Article
| Open AccessLight-driven polymer recycling to monomers and small molecules
Chemical recycling of plastic enables renewed production of pristine materials, but generally comes at a high energy cost. This review focuses on light-driven approaches for chemically recycling and upcycling plastic waste, with emphasis on reduced energy consumption and selective transformations of challenging to recycle backbone structures.
- Laura Wimberger
- , Gervase Ng
- & Cyrille Boyer
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Article
| Open AccessLocking the lattice oxygen in RuO2 to stabilize highly active Ru sites in acidic water oxidation
RuO2 is highly active toward the acidic electrochemical oxygen evolution reaction but exhibits instability due to lattice oxygen oxidation. Here, authors prepare an interstitial Si-decorated RuO2 catalyst with improved stability for acidic water oxidation by suppressing lattice oxygen oxidation.
- Xinyu Ping
- , Yongduo Liu
- & Zidong Wei
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Article
| Open AccessSub-8 nm networked cage nanofilm with tunable nanofluidic channels for adaptive sieving
Drawing inspiration from biological cell membranes, here, the authors create sub-8 nm membranes with adaptive nanofluidic channels, mimicking the cell membrane properties, by interconnecting 0D nanoporous molecules at the oil/water interface.
- Si-Hua Liu
- , Jun-Hao Zhou
- & Jian-Ke Sun
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Article
| Open AccessExtreme Li-Mg selectivity via precise ion size differentiation of polyamide membrane
Achieving high selectivity of Li+ and Mg2+ is of paramount importance for effective lithium extraction from brines, and nanofiltration (NF) membrane plays a critical role in this process. Here the authors report the fabrication of polyamide NF membranes with ultra-high Li + /Mg2+ selectivity by modifying the interfacial polymerization process with an oil-soluble surfactant.
- Quan Peng
- , Ruoyu Wang
- & Lei Jiang
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Article
| Open AccessA restricted dynamic surface self-reconstruction toward high-performance of direct seawater oxidation
Chlorine evolution reaction and deep reconstruction of catalyst are critical issues in direct seawater electrolysis. Here, the authors propose a MoO3/CoO/carbon composite material for improved selective seawater oxidation and restricted dynamic surface self-reconstruction.
- Ling Zhou
- , Daying Guo
- & Shun Wang
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Article
| Open AccessActivation and friction in enzymatic loop opening and closing dynamics
Enzymes present loops around active sites whose closing and opening dynamics are essential for its activity. Here the authors unveil the mechanism governing loop motion, showing that it involves an activated conformational rearrangement around a couple of torsional angles taking place under the strong friction exerted by the rest of loop torsions.
- Kirill Zinovjev
- , Paul Guénon
- & Iñaki Tuñón
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Article
| Open AccessPhoto-induced intramolecular dearomative [5 + 4] cycloaddition of arenes for the construction of highly strained medium-sized-rings
Medium-sized-ring compounds are challenging synthetic targets in organic chemistry. Here the authors report an intramolecular dearomative [5 + 4] cycloaddition of naphthalene-derived vinylcyclopropanes to construct these molecules under visible-light irradiation and a proper triplet photosensitizer.
- Min Zhu
- , Yuan-Jun Gao
- & Shu-Li You
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Article
| Open Access2H-Thiopyran-2-thione sulfine, a compound for converting H2S to HSOH/H2S2 and increasing intracellular sulfane sulfur levels
Reactive sulfane sulfur species such as persulfides and H2S2 are important redox regulators and linked to H2S signaling, but their study is hindered by a lack of suitable donors to produce them. Here, the authors report 2H-thiopyran-2-thione sulfine (TTS), a compound which can specifically convert H2S to HSOH, and then to H2S2 in the presence of excess H2S.
- Qi Cui
- , Meg Shieh
- & Ming Xian
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Article
| Open AccessSynthesis of meta-carbonyl phenols and anilines
Phenols and anilines are of extreme importance for medicinal chemistry and material science but the selective preparation of meta-substituted phenols and anilines remains challenging. Here the authors report an efficient copper-catalyzed dehydrogenation strategy to exclusively synthesize meta-carbonyl phenols and anilines from carbonyl substituted cyclohexanes.
- Bao-Yin Zhao
- , Qiong Jia
- & Yong-Qiang Wang
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Article
| Open AccessPulse potential mediated selectivity for the electrocatalytic oxidation of glycerol to glyceric acid
Mitigating the deactivation of noble metal-based catalysts caused by self-oxidation and toxic adsorption poses a considerable challenge in organic electro-oxidation. This study addresses the issue by employing a pulsed potential electrolysis approach to selectively electrocatalyze the oxidation of glycerol to glyceric acid using a Pt-based catalyst.
- Wei Chen
- , Liang Zhang
- & Yuqin Zou
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Article
| Open AccessPhenol as proton shuttle and buffer for lithium-mediated ammonia electrosynthesis
The proton shuttle plays a critical role in the proton transfer process during lithium-mediated ammonia synthesis. Here, the authors establish the structure-activity relationship and design principles for effective proton shuttles.
- Xianbiao Fu
- , Aoni Xu
- & Ib Chorkendorff
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Article
| Open AccessEncoding ordered structural complexity to covalent organic frameworks
Starting from simple building blocks with specific molecular packing geometries, here, the authors synthesized structurally complex covalent organic framework COF-305 with nine different stereoisomers of its constituents showing specific sequences on topologically equivalent sites.
- Lei Wei
- , Xinyue Hai
- & Yingbo Zhao
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Article
| Open AccessWell-defined diatomic catalysis for photosynthesis of C2H4 from CO2
Principal interest lies in diatomic catalysts (DACs) for efficient CO2 to C2H4 photoconversion yet optimizing catalytic performance and exploring reaction mechanisms are impeded by heteronuclear atom random distribution. Here, a novel up-bottom ion-cutting architecture is proposed for fabricating well-defined DACs.
- Zhongkai Xie
- , Shengjie Xu
- & Shuyan Song
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Article
| Open AccessLight and matter co-confined multi-photon lithography
Mask-free multi-photon lithography allows the straightforward fabrication of nanostructures, but high precision and good resolution can be challenging to achieve. Here, the authors report a combination of photo-inhibition and chemical quenchers for improved lithography performance.
- Lingling Guan
- , Chun Cao
- & Xu Liu
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Article
| Open AccessTheoretical formulation of chemical equilibrium under vibrational strong coupling
Strong light-matter interactions in optical microcavities can be used to control molecular kinetic and thermodynamic phenomena. Here, the authors introduce a theory that describes the nonperturbative effects of infrared microcavities on chemical equilibria.
- Kaihong Sun
- & Raphael F. Ribeiro
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Article
| Open AccessControlled dissolution of a single ion from a salt interface
The strong ionic bond in salt is broken by electrostatic interactions with water, but direct observation at the level of a single ion is challenging. Here, the authors have visualized the preferential dissolution of an anion by manipulating a single water molecule.
- Huijun Han
- , Yunjae Park
- & Hyung-Joon Shin
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Article
| Open AccessN-Heterocyclic carbene-catalyzed enantioselective synthesis of planar-chiral cyclophanes via dynamic kinetic resolution
Planar-chiral cyclophanes are important for drug discovery but the enantioselective synthesis of planar-chiral cyclophanes remains challenging. Here the authors describe an N-heterocyclic carbene-catalyzed asymmetric construction of planar-chiral cyclophanes.
- Jiayan Li
- , Ziyang Dong
- & Changgui Zhao
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Article
| Open AccessBubble-water/catalyst triphase interface microenvironment accelerates photocatalytic OER via optimizing semi-hydrophobic OH radical
Temperature has demonstrated the potential to regulate the photocatalytic oxygen evolution reaction (OER). This study confirms that the temperature-induced bubble-water/catalyst triphase interface microenvironment significantly enhances OER by optimizing the formation and deprotonation of semi-hydrophobic OH radicals.
- Guanhua Ren
- , Min Zhou
- & Haifeng Wang
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