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| Open AccessA molecular T-pentomino for separating BTEX hydrocarbons
Globally important BTEX hydrocarbons are separated using a T-shaped host with the shape and crystal tiling characteristics of a pentomino. A strategy based on designing and applying crystalline molecular ominos to perform separations of hydrocarbons and other environmentally-relevant compounds is outlined.
- Christopher J. Hartwick
- , Eric W. Reinheimer
- & Leonard R. MacGillivray
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Article
| Open AccessRetinal photoisomerization versus counterion protonation in light and dark-adapted bacteriorhodopsin and its primary photoproduct
Malakar et al. investigate the photochemical dynamics in the isomerization of bacteriorhodopsin light and dark-adapted forms and in the first photocycle intermediate, K. The results prompt a reevaluation of the counter ion model, revealing that a different protonation then that shown in the classic quadrupole so far considered must be employed to account for the experimental data.
- Partha Malakar
- , Samira Gholami
- & Sanford Ruhman
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Article
| Open AccessRegulating ion affinity and dehydration of metal-organic framework sub-nanochannels for high-precision ion separation
Understanding ion transport mechanisms in confined environments is key to achieving efficient membrane-based ion separation. Here, the authors regulate the ion affinity and dehydration in metal-organic framework sub-nanochannels and achieve a high-precise mono-/di-valent cation separation.
- Ri-Jian Mo
- , Shuang Chen
- & Zhong-Qiu Li
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Article
| Open AccessEffect of inorganic material surface chemistry on structures and fracture behaviours of epoxy resin
The mechanisms of adhesion between polymers and inorganic materials are not fully understood. Here, authors demonstrate the clear evidence that the surface chemistry impacts the crosslinked structures of resins near the interfaces, resulting in different fracture behaviours and adhesive strengths.
- Tomohiro Miyata
- , Yohei K. Sato
- & Hiroshi Jinnai
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Article
| Open AccessUltrafast underwater self-healing piezo-ionic elastomer via dynamic hydrophobic-hydrolytic domains
Elastomers capable of autonomous self-healing and mechanical stimulus sensing in aquatic environments are interesting for applications in underwater soft electronics. Here, the authors present a hydrophobic-hydrolytic molecularly engineered self-healing piezo-ionic elastomer with underwater self-healing properties and mechanosensitive ion channels.
- Zhengyang Kong
- , Elvis K. Boahen
- & Do Hwan Kim
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Article
| Open AccessAbnormal thermally-stimulated dynamic organic phosphorescence
In thermally stimulated phosphorescent materials a thermal stimulus inevitably quenches the emission due to intensive non radiative transition. Here, the authors report an abnormal thermally stimulated phosphorescence behavior in organic phosphors and show enhancement of phosphorescence and change of the emission color upon temperature increase.
- He Wang
- , Huili Ma
- & Zhongfu An
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Article
| Open AccessDesymmetric homologating annulation to access chiral pentafulvenes and their application in bioimaging
Polycyclic/multisubstituted pentafulvenes are of interest as they frequently occur in biologically relevant motifs, electrochromic dyes, and solar cells. Here, the authors report an enantioselective homologating annulation of cyclopent-4-ene-dione with 3-cyano-4-methylcoumarins through L-tert-leucine derived thiourea catalysis, affording a wide range of enantioenriched polycyclic multi-substituted embedded aminopentafulvenes.
- Sanjay Singh
- , Ravi Saini
- & Ravi P. Singh
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Article
| Open AccessSurface hydrophobization of zeolite enables mass transfer matching in gas-liquid-solid three-phase hydrogenation under ambient pressure
A modified zeolite nanoreactor with organosilanes boosts hydrogenation of aldehydes/ketones in water at ambient pressure. This method, promoting H2 and substrate mass transfer, achieves a 4.3-fold increase in reaction rate, offering a sustainable approach for organic synthesis under mild conditions.
- Shuai Wang
- , Riming Hu
- & Guozhu Chen
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Article
| Open AccessInterrogating site dependent kinetics over SiO2-supported Pt nanoparticles
Kim and co-workers introduce a new ‘kinetic site deconvolution’ method to identify active sites on heterogeneous catalysts by linking reaction rates to specific adsorption environments.
- Taek-Seung Kim
- , Christopher R. O’Connor
- & Christian Reece
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Article
| Open AccessSelenium substitution for dielectric constant improvement and hole-transfer acceleration in non-fullerene organic solar cells
Dielectric constant of non-fullerene acceptors plays a critical role in organic solar cells in terms of exciton dissociation and charge recombination. Here, authors report selenium substitution on central core of acceptors to improve dielectric constant, realizing devices with efficiency of 19.0%.
- Xinjun He
- , Feng Qi
- & Wallace C. H. Choy
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Article
| Open AccessBioengineered amyloid peptide for rapid screening of inhibitors against main protease of SARS-CoV-2
The main protease (Mpro) plays a crucial role in the replication of SARS-CoV-2, thereby making it an attractive target for COVID-19 treatment. Here, the authors develop a colorimetric screening platform for discovering Mpro inhibitors using engineered amyloid peptide-based nanocomplexes.
- Dongtak Lee
- , Hyo Gi Jung
- & Dae Sung Yoon
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Article
| Open AccessInter-site structural heterogeneity induction of single atom Fe catalysts for robust oxygen reduction
Here, authors report an inter-site structural heterogeneity induced effect of hierarchical single atom Fe catalysts for robust oxygen reduction. Dynamic evolutions and insights into structure-activity relationship are presented.
- Peng Zhang
- , Hsiao-Chien Chen
- & Yuan Pan
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Article
| Open AccessWater-dispersible X-ray scintillators enabling coating and blending with polymer materials for multiple applications
Water dispersible X-ray scintillators are highly desirable for multiple application scenarios. Zhang et al report the synthesis of new X-ray scintillator nanocrystals anchored on the surface of water dispersible halloysite nanotubes, enabling radiation exposure monitoring, flexible scintillator screens, and information encryption.
- Hailei Zhang
- , Bo Zhang
- & Richard Hoogenboom
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Article
| Open AccessRectifying artificial nanochannels with multiple interconvertible permeability states
Transmembrane channels have inspired the development of biomimetic channels. Here, the authors present a class of artificial nanochannels based on DNAzyme-functionalized glass nanopipettes to allow for the control of channel permeability.
- Ruocan Qian
- , Mansha Wu
- & Yi Lu
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Article
| Open AccessCopper nanoparticles encapsulated in zeolitic imidazolate framework-8 as a stable and selective CO2 hydrogenation catalyst
Here, authors report an inter-site structural heterogeneity induced effect of hierarchical single atom Fe catalysts for robust oxygen reduction. Dynamic evolutions and insights into structure-activity relationship are presented.
- Vijay K. Velisoju
- , Jose L. Cerrillo
- & Pedro Castaño
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Article
| Open AccessReversible chirality inversion of an AuAgx-cysteine coordination polymer by pH change
Reactive chiral systems have attracted much attention in biology, optoelectronics, and photonics; however, a comprehensive understanding of these systems remains incomplete. Here the authors show the reversible chirality of AuAgx-cys coordination polymers induced by pH changes.
- Bing Ni
- , Dustin Vivod
- & Helmut Cölfen
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Article
| Open AccessWood-inspired metamaterial catalyst for robust and high-throughput water purification
Continuous industrialization and human activities have led to severe water quality deterioration. Here, a structure-function integrated system is developed by Douglas fir wood inspired metamaterial catalysts with robust and high throughput water purification performances.
- Lei Zhang
- , Hanwen Liu
- & Jian Lu
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Article
| Open AccessMolecular anchoring of free solvents for high-voltage and high-safety lithium metal batteries
Advanced electrolyte is essential for high-energy-density lithium metal batteries. Here, the authors design a molecular anchoring dilute electrolyte via intermolecular hydrogen bonding with free solvents to improve the battery electrochemical and thermal stabilities.
- Zhuangzhuang Cui
- , Zhuangzhuang Jia
- & Xiaodi Ren
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Article
| Open AccessEndogenous stimuli-responsive separating microneedles to inhibit hypertrophic scar through remodeling the pathological microenvironment
The treatment of hypertrophic scar (HS) is hindered by the low bioavailability of drugs and the pathological microenvironment. Here the authors report a separating microneedle drug delivery system responsive to high reactive oxygen species levels and overexpression of matrix metalloproteinases to remodel the pathological microenvironment for HS treatment.
- Zhuo-Ran Yang
- , Huinan Suo
- & Jintao Zhu
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Article
| Open AccessMelt-quenched glass formation of a family of metal-carboxylate frameworks
How to melt and quench the largest subclass of MOFs, metal carboxylate frameworks, into glasses is a major challenge. Here, the authors develop a strategy by grafting the zwitterions onto the carboxylate ligands and incorporating organic acids into the framework channels to realize the glass formation.
- Wen-Long Xue
- , Guo-Qiang Li
- & Chong-Qing Wan
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Article
| Open AccessIdentification of a potent palladium-aryldiphosphine catalytic system for high-performance carbonylation of alkenes
The development of stable and efficient ligands is of vital significance to enhance the catalytic performance of carbonylation reactions of alkenes. Here, the authors develop an aryldiphosphine ligand, used in palladium-catalyzed regioselective carbonylation of alkenes, exhibiting high catalytic performance and strong oxygen-resistance stability.
- Kang Zhao
- , Hongli Wang
- & Feng Shi
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Article
| Open AccessStatic charge is an ionic molecular fragment
What is static charge? Analysis of molecularly well-defined surfaces shows that static charge is an ionic molecular fragment. Contact electrification causes the heterolytic cleavage of covalent bonds, generating these fragments.
- Yan Fang
- , Chi Kit Ao
- & Siowling Soh
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Article
| Open AccessNanopore analysis of salvianolic acids in herbal medicines
Natural herbs, which contain pharmacologically active compounds, have been historically used as medicines but the analysis of their chemical components is time-consuming and complex. Here, the authors report a phenylboronic acid appended Mycobacterium smegmatis porin A (MspA) nanopore for sensing a variety of bioactive compounds based on salvianolic acid, without the need for sample separation or purification.
- Pingping Fan
- , Shanyu Zhang
- & Shuo Huang
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Article
| Open AccessHomo-BacPROTAC-induced degradation of ClpC1 as a strategy against drug-resistant mycobacteria
Antimicrobial resistance is a global health threat and the development of alternative strategies to overcome it is of high interest. Here, the authors report proteolysis targeting chimeras active in bacteria (BacPROTACs) that bind to ClpC1, a component of the mycobacterial protein degradation machinery, and apply them for targeting a range of mycobacterial strains, including antibiotic-resistant ones.
- Lukas Junk
- , Volker M. Schmiedel
- & Guido Boehmelt
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Article
| Open AccessNanopore analysis of cis-diols in fruits
Fruits contain a large variety of cis-diols but their rapid and direct analysis without complex sample pretreatment was not achieved. Here, the authors report a Mycobacterium smegmatis porin A nanopore modified with a phenylboronic acid adapter for recognition of 1,2-diphenols, alditols, α-hydroxy acids and saccharides in fruits.
- Pingping Fan
- , Zhenyuan Cao
- & Shuo Huang
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Article
| Open AccessCrystallization of molecular layers produced under confinement onto a surface
Molecules arranged in close proximity to a surface form molecular layers, exhibiting distinct properties. However, the creation of these layers is challenging. Here, the authors present a technique for generating molecular layers through crystallization induced by gas blowing onto a surface.
- Jincheng Tong
- , Nathan de Bruyn
- & Cinzia Casiraghi
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Article
| Open AccessIn-cell NMR suggests that DNA i-motif levels are strongly depleted in living human cells
I-Motifs (iM) are non-canonical DNA structures potentially forming in the accessible, single stranded, cytosine-rich genomic region, but the specific contributions of several factors involved in their formation are unknown. Using in-cell NMR, the authors examined DNA i-motif formation in human cells at body temperature, suggesting i-M occur in a small portion (<1%) of genomic sites predisposed to its formation.
- Pavlína Víšková
- , Eva Ištvánková
- & Lukáš Trantírek
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Article
| Open AccessJanus microparticles-based targeted and spatially-controlled piezoelectric neural stimulation via low-intensity focused ultrasound
Wireless and localized stimulation of neural cells remains challenging. Here, the authors propose piezoelectric magnetic Janus microparticles that can target and stimulate neurons under low-intensity ultrasound through voltage-gated ion channels.
- Mertcan Han
- , Erdost Yildiz
- & Metin Sitti
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Article
| Open AccessA programmable hybrid digital chemical information processor based on the Belousov-Zhabotinsky reaction
Computing platforms based on chemical processes can be an alternative to digital computers in some scenarios but have limited programmability. Here the authors demonstrate a hybrid computing platform combining digital electronics and an oscillatory chemical reaction and demonstrate its computational capabilities.
- Abhishek Sharma
- , Marcus Tze-Kiat Ng
- & Leroy Cronin
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Article
| Open AccessA non-canonical nucleophile unlocks a new mechanistic pathway in a designed enzyme
The authors previously showed that a histidine nucleophile and a flexible arginine can work in synergy to accelerate the Morita Baylis-Hillman (MBH) reaction. Here, they report another efficient MBHase that employs a non-canonical Nδ-methylhistidine nucleophile paired with a catalytic glutamate, providing an alternative mechanistic solution for MBH catalysis.
- Amy E. Hutton
- , Jake Foster
- & Anthony P. Green
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Article
| Open AccessAqueous pyruvate partly dissociates under deep ultraviolet irradiation but is resilient to near ultraviolet excitation
The photochemistry of the pyruvate anion plays an important role in the Earth’s atmosphere and aqueous environments. Here, the authors show that excitation of aqueous pyruvate by 200 nm light leads to decarboxylation with a quantum efficiency of 20%, while excitation by 340 nm light does not cause a reaction.
- Jan Thøgersen
- , Fani Madzharova
- & Frank Jensen
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Article
| Open AccessPrediction of highly stable 2D carbon allotropes based on azulenoid kekulene
Discovery of 2D materials with useful electronic properties is challenging. Here, the authors use DFT to design a stable semiconducting 2D carbon allotrope for optoelectronic applications that has light charge carriers and unusual secondary bandgap.
- Zhenzhe Zhang
- , Hanh D. M. Pham
- & Rustam Z. Khaliullin
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Article
| Open AccessDynamic chloride ion adsorption on single iridium atom boosts seawater oxidation catalysis
The seawater oxidation reaction faces challenges from competitive chloride oxidation reaction. Herein, the authors have utilized chlorine adsorption to modulate the single-atom Ir coordination state and promote seawater oxidation and catalyst stability.
- Xinxuan Duan
- , Qihao Sha
- & Xiaoming Sun
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Article
| Open AccessColor construction of multi-colored carbon fibers using glucose
Color construction of black carbon fibers is a challenge due to their stable physicochemical properties. Here, the authors demonstrate the tunable structural color of carbon fibers endowed by the dynamic growth of carbon spheres using glucose.
- Sijie Zhou
- , Chunhua Zhang
- & Weilin Xu
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Article
| Open AccessDynamic mechanostereochemical switching of a co-conformationally flexible [2]catenane controlled by specific ionic guests
By virtue of the rotational motions of interlocked macrocycles, the authors describe a chameleon-like catenane host that can adjust its co-conformation for selective binding to copper(I) or sulfate ion. While the cationic copper(I) complex is achiral, the interlocked rings in the catenane host rotate and re-orient into a chiral co-conformation upon forming the anionic sulfate complex.
- Yueliang Yao
- , Yuen Cheong Tse
- & Ho Yu Au-Yeung
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Article
| Open AccessSilver-catalyzed direct conversion of epoxides into cyclopropanes using N-triftosylhydrazones
Epoxides are prominent small-ring O-heterocycles found in a variety of bioactive natural products and pharmaceuticals. Here, the authors report a silver carbene strategy to achieve O-to-C atom exchange of epoxides in a single step, affording diverse fluoroalkylcyclopropanes.
- Linxuan Li
- , Paramasivam Sivaguru
- & Xihe Bi
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Article
| Open AccessInfluence of electric double layer rigidity on CO adsorption and electroreduction rate
High-pressure infrared spectroscopy shows concentrated cations suppress CO adsorption. Here the authors report two electrochemical interfaces forming distinct double layer structures and reaction rates at elevating pressure and various potentials.
- Jiajie Hou
- , Bingjun Xu
- & Qi Lu
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Article
| Open AccessEfficient all-small-molecule organic solar cells processed with non-halogen solvent
The development of non-halogen solvent processed all-small-molecule organic solar cells was challenging. Here, the authors employ a small molecule donor with strong aggregation property to improve molecular pre-aggregation in tetrahydrofuran, realizing ternary device with efficiency of 16.1%.
- Wei Gao
- , Ruijie Ma
- & Gang Li
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Article
| Open AccessA structural and dynamic visualization of the interaction between MAP7 and microtubules
Integrated structural data show that the MAP7 microtubule binding domain stabilizes the microtubule lattice through binding along protofilaments. Both strong and weak interactions between MAP7 and the lattice extend beyond a single tubulin dimer and include the tubulin C-terminal tails.
- Agnes Adler
- , Mamata Bangera
- & Marc Baldus
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Article
| Open AccessCation desolvation-induced capacitance enhancement in reduced graphene oxide (rGO)
Understanding local electrochemical processes can help improve electrochemical energy storage. Here, the authors report a charge storage mechanism in aqueous electrolyte for reduced graphene oxide using an electrochemical quartz crystal microbalance.
- Kangkang Ge
- , Hui Shao
- & Patrice Simon
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Article
| Open AccessExtensive photochemical restructuring of molecule-metal surfaces under room light
The nature of the molecule-metal interface is crucial for many technological applications. Here, the authors show that the photostability of the material can be sensitive to room light when coated with a single molecular layer, with implications for devices and processes.
- Chenyang Guo
- , Philip Benzie
- & Jeremy J. Baumberg
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Article
| Open AccessOn-surface cyclization of vinyl groups on poly-para-phenylene involving an unusual pentagon to hexagon transformation
On-surface synthesis relies on carefully designed molecular precursors that are thermally activated to afford desired, covalently coupled architectures. Here, the authors study the intramolecular reactions of vinyl groups in a poly-para-phenylene-based model system and provide a comprehensive description of the reaction steps taking place on the Au(111) surface under ultrahigh vacuum conditions.
- Marco Di Giovannantonio
- , Zijie Qiu
- & Roman Fasel
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Article
| Open AccessDynamic control of DNA condensation
Artificial biomolecular condensates are valuable tools to study the design principles of phase separation. Here, the authors demonstrate and characterize a model system of artificial DNA condensates whose kinetic formation and dissolution depends on DNA inputs that activate or deactivate the phase separating DNA subunits.
- Siddharth Agarwal
- , Dino Osmanovic
- & Elisa Franco
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Article
| Open AccessDioxygen compatible electron donor-acceptor catalytic system and its enabled aerobic oxygenation
The photochemical properties of Electron Donor-Acceptor (EDA) complexes present exciting opportunities, but often require an inert atmosphere to maintain high efficiency. Here, the authors develop a photocatalytic system through rational design, which overcomes the oxygen-sensitive limitation of traditional EDA photocatalytic systems.
- Jialiang Wei
- , Junhong Meng
- & Ning Jiao
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Article
| Open AccessDimethyl sulfate and diisopropyl sulfate as practical and versatile O-sulfation reagents
O-Sulfation is a vital post-translational modification in bioactive molecules, yet there are significant challenges for the synthesis. Here, the authors report a general and robust approach to O-sulfation by harnessing the tunable reactivity of dimethyl sulfate or diisopropyl sulfate under tetrabutylammonium bisulfate activation.
- Shuaishuai Yue
- , Guoping Ding
- & Jiakun Li
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Article
| Open AccessGeneral alkyl fluoride functionalization via short-lived carbocation-organozincate ion pairs
Many alkyl fluorides are readily available, but the synthetic applications trail behind the widely accepted utility of other halides. Here, the authors report a practical Csp3-F bond functionalization method that expands the currently restricted synthetic space of unactivated C(sp3)-F bonds, but also uses benzylic, propargylic and acyl fluorides.
- D. Lucas Kane
- , Bryan C. Figula
- & Christian Wolf
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Article
| Open AccessCharging modulation of the pyridine nitrogen of covalent organic frameworks for promoting oxygen reduction reaction
The catalytic efficacy of covalent organic frameworks (COFs) is constrained by their restricted electro-transfer capability and weak binding affinities for reaction intermediates. Here the authors report COFs with various pyridinic-based units for tuning their catalytic activity towards oxygen reduction reaction.
- Xiubei Yang
- , Qizheng An
- & Gaofeng Zeng
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Article
| Open AccessOrthoID: profiling dynamic proteomes through time and space using mutually orthogonal chemical tools
Proteomics at the organelle contact site remains challenging due to the spatial and temporal dynamics of proteins. Here, the authors developed OrthoID, a mutually orthogonal dual enzymatic proteomics approach to explore the proteome at the contact site of the endoplasmic reticulum and mitochondria.
- Ara Lee
- , Gihyun Sung
- & Kimoon Kim
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Article
| Open AccessScalable production of structurally colored composite films by shearing supramolecular composites of polymers and colloids
Structurally coloured composite films are flexible optical materials with potential in a range of applications, but their production is impacted by long time-frames and limited materials. Here, the authors report a method for the production of large scale films by shearing supramolecular composites.
- Miaomiao Li
- , Bolun Peng
- & Jintao Zhu
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