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Article
| Open AccessComparative quantum-classical dynamics of natural and synthetic molecular rotors show how vibrational synchronization modulates the photoisomerization quantum efficiency
The control of reaction quantum efficiencies is a fundamental photochemical problem. Here the authors use comparative quantum-classical dynamics to reveal that the synchronization of specific vibrations with the reaction coordinate is a key promoting factor.
- Alejandro Blanco-Gonzalez
- , Madushanka Manathunga
- & Massimo Olivucci
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Article
| Open AccessIron-catalyzed stereoselective C–H alkylation for simultaneous construction of C–N axial and C-central chirality
A highly efficient stereoselective C−H alkylation of indoles with aryl alkenes is achieved by sustainable iron catalysis, leading to atropoenriched and enantioenriched substituted indoles with high structural diversity. Detailed mechanistic studies by experiment, Mössbauer spectroscopy and computation reveal the origin of the catalytic efficacy and stereoselectivity.
- Zi-Jing Zhang
- , Nicolas Jacob
- & Lutz Ackermann
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Article
| Open AccessConfining single Er3+ ions in sub-3 nm NaYF4 nanoparticles to induce slow relaxation of the magnetisation
Many of the most industrially important magnets require the addition of rare-earths to improve their coercivity and magnetic performance. Here, the authors place a single paramagnetic rare-earth ion, Er3+, in a diamagnetic nanoparticle, and study the slow relaxation of the resulting nanoparticles, providing vital information for the further development of rare-earth magnetic materials.
- Diogo A. Gálico
- , Emille M. Rodrigues
- & Muralee Murugesu
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Article
| Open AccessMultiple hydrogen-bonding induced nonconventional red fluorescence emission in hydrogels
The development of fluorescent polymer hydrogels without the use of extended pi-conjugation is challenging. Here, the authors report the use of clustering-trigger emission to give red fluorescence on boiling polymer hydrogels, with tuneable emission properties.
- Jiayu Wu
- , Yuhuan Wang
- & Feng Zhou
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Article
| Open AccessConsummating ion desolvation in hard carbon anodes for reversible sodium storage
Hard carbon is regarded as a promising negative electrode for Na-ion batteries but suffers from low initial Coulombic efficiency (ICE). Here, the authors identify the time-dependent ion pre-desolvation on the nanopore of hard carbons, which remarkably improves the ICE by simply extending the aging time.
- Ziyang Lu
- , Huijun Yang
- & Haoshen Zhou
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Article
| Open AccessEstablishing superfine nanofibrils for robust polyelectrolyte artificial spider silk and powerful artificial muscles
Spider silk has desirable properties, but these are hard to replicate with artificial materials. Here, the authors report a polyelectrolyte artificial spider silk, with control over dissociation of the polymer chains by introduction of ions, and thermally driven supercontraction.
- Wenqian He
- , Meilin Wang
- & Zunfeng Liu
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Article
| Open AccessA comprehensive synthetic library of poly-N-acetyl glucosamines enabled vaccine against lethal challenges of Staphylococcus aureus
Poly-β-(1–6)-N-acetylglucosamine (PNAG) is an important vaccine target, but the impact of the number and position of free amine vs N-acetylation on its antigenicity is not well understood. Here, the authors report a divergent strategy to synthesize a comprehensive library of PNAG pentasaccharides, enabling the identification of enhanced epitopes for vaccines against Staphylococcus aureus including drug resistant strains.
- Zibin Tan
- , Weizhun Yang
- & Xuefei Huang
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Article
| Open AccessScalable computation of anisotropic vibrations for large macromolecular assemblies
Normal mode analysis is a crucial step in structural biology, but is based on an expensive diagonalisation of the system’s Hessian. Here the authors present INCHING, a GPU-based approach to accelerate this task up to >250 times over current methods for macromolecular assemblies.
- Jordy Homing Lam
- , Aiichiro Nakano
- & Vsevolod Katritch
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Article
| Open AccessAn isolable, chelating bis[cyclic (alkyl)(amino)carbene] stabilizes a strongly bent, dicoordinate Ni(0) complex
Notwithstanding their success as strongly σ-donating and π-accepting ligands, to date no chelating bis[cyclic (alkyl)(amino)carbenes] have been reported. Here the authors describe a chelating, C2-symmetric bis[cyclic (alkyl)(amino)carbene] ligand, as well as its pseudotetrahedral complexes with iron, cobalt, nickel, and zinc dihalides.
- Braulio M. Puerta Lombardi
- , Morgan R. Faas
- & Roland Roesler
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Article
| Open AccessHighly defective ultra-small tetravalent MOF nanocrystals
Crystalline materials’ properties are highly dependent on their size. Here authors report a general synthesis of ultrasmall (4–6 nm) and highly defective Zr/Hf-Metal Organic Frameworks nanoparticles that present enhanced peptide hydrolysis performance.
- Shan Dai
- , Charlotte Simms
- & Christian Serre
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Article
| Open AccessPathway-divergent coupling of 1,3-enynes with acrylates through cascade cobalt catalysis
The development of divergent reaction pathways controlled by different ligands is a critical goal. Here the authors describe a cobalt-catalyzed strategy for cascade coupling of 1,3-enynes with two molecules of acrylates through three reaction modes.
- Heng Wang
- , Xiaofeng Jie
- & Fanke Meng
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Article
| Open AccessIn situ captured antibacterial action of membrane-incising peptide lamellae
Inspired by the alternating chirality backbone pattern of some effective peptide antimicrobials, here authors design lysine-rich heterochiral peptides that show antimicrobial activity.
- Kamal el Battioui
- , Sohini Chakraborty
- & Tamás Beke-Somfai
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Article
| Open AccessDehydroxylative radical N-glycosylation of heterocycles with 1-hydroxycarbohydrates enabled by copper metallaphotoredox catalysis
N-Glycosylated heterocycles play important roles in biological systems and drug development, but the synthesis heavily relies on ionic N-glycosylation. Herein, the authors report a dehydroxylative radical method for synthesizing N-glycosides by leveraging copper metallaphotoredox catalysis.
- Da-Peng Liu
- , Xiao-Sen Zhang
- & Xiang-Guo Hu
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Article
| Open AccessPolarizability matters in enantio-selection
Polarizability, a property that is closely related to softness in the classic theory of Hard and Soft Acids and Bases (HSAB), has been largely overlooked in connecting with enantio-selection in the past. Here, the authors show local polarizability-based electronic effects can rationalize a wide range of stereochemical outcomes in widely-known asymmetric catalytic reactions.
- Fumin Chen
- , Yu Chen
- & Xiangyou Xing
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Article
| Open AccessAn organic proton cage that is ultra-resistant to hydroxide-promoted degradation
Organic cations are typically unstable under low-humidity, alkaline conditions. Here, the authors report an organic cation featuring a proton protected within a cage that can withstand vapor-phase alkaline conditions.
- Chase L. Radford
- , Torben Saatkamp
- & Steven Holdcroft
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Article
| Open AccessHighly efficient anion exchange membrane water electrolyzers via chromium-doped amorphous electrocatalysts
Modulating the electronic structure of active metal sites is crucial to enhance the activity of anion-exchange membrane water electrolyzers. Here, the authors elaborate Cr-doped amorphous metal oxide catalysts with excellent activity and stability.
- Sicheng Li
- , Tong Liu
- & Tao Yao
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Article
| Open AccessLocal CO2 reservoir layer promotes rapid and selective electrochemical CO2 reduction
Converting CO2 to valuable chemicals is of high interest. Here the authors address the challenge of low CO2 solubility in water by incorporating a metal-organic framework layer to enhance CO2 pre-concentration and activation before its electroreduction by the underlying solid electrocatalyst.
- Subhabrata Mukhopadhyay
- , Muhammad Saad Naeem
- & Idan Hod
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Article
| Open AccessCatalytic role of in-situ formed C-N species for enhanced Li2CO3 decomposition
Sluggish kinetics of the CO2 reactions lead to the accumulation of Li2CO3 residuals, which hinders the cycling stability of Li-CO2 batteries. Here, the authors reveal the catalytic role of in-situ formed C-N species in enhancing the reversibility of Li2CO3 and cycle life of Li-CO2 batteries.
- Fangli Zhang
- , Wenchao Zhang
- & Zaiping Guo
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Article
| Open AccessDouble cross-linked 3D layered PBI proton exchange membranes for stable fuel cell performance above 200 °C
Phosphoric acid (PA) doped proton exchange membranes (PEMs) often degrade above 200 °C due to membrane creeping, PA dehydration, and condensation. Here, the authors introduce gel-state polybenzimidazole PEMs with double cross-linked 3D layered structures, enabling efficient and stable fuel cell operation above 200 °C.
- Liang Zhang
- , Mengjiao Liu
- & Lixin Xue
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Article
| Open AccessIterative SuFEx approach for sequence-regulated oligosulfates and its extension to periodic copolymers
The synthesis of sequence-regulated oligosulfates has not yet been established due to the difficulties in precise reactivity control. Here, the authors report a multi-directional divergent iterative method to furnish oligosulfates based on a chain homologation approach, in which the fluorosulfate unit is regenerated.
- Min Pyeong Kim
- , Swatilekha Kayal
- & Sung You Hong
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Article
| Open AccessPalladium-catalyzed asymmetric carbene coupling en route to inherently chiral heptagon-containing polyarenes
Developing facile and direct synthesis routes for enantioselective construction of cyclic π-conjugated molecules is crucial but the chirality orginiating from the distorted structure around heptagon-containing polyarenes is largely overlooked. Herein the authors present a highly enantioselective synthesis for fabrication of all carbon heptagon-containing polyarenes via palladium-catalyzed carbene-based cross–coupling of benzyl bromides and N-arylsulfonylhydrazones.
- Huan Zhang
- , Chuan-Jun Lu
- & Ren-Rong Liu
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Article
| Open AccessRedefined ion association constants have consequences for calcium phosphate nucleation and biomineralization
While clusters in calcium orthophosphate nucleation have long been known, their speciation and mechanistic pathways to hydroxyapatite remain debated. Here the authors report a revision of ion association in the calcium phosphate system and explore the consequences thereof on the early stages of phase separation.
- David P. McDonogh
- , Julian D. Gale
- & Denis Gebauer
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Article
| Open AccessIn-situ low-temperature sulfur CVD on metal sulfides with SO2 to realize self-sustained adsorption of mercury
Efficient removal of gaseous mercury (Hg0) from industrial flue gas is commonly constrained by SO2. Here, authors propose an in-situ sulfur CVD method on metal sulfides that reverses the harmful effects of SO2, achieving self-sustained adsorption of Hg0 and breaking the capacity limitations.
- Qinyuan Hong
- , Haomiao Xu
- & Naiqiang Yan
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Article
| Open AccessLate-stage meta-C–H alkylation of pharmaceuticals to modulate biological properties and expedite molecular optimisation in a single step
Installation of small aliphatic motifs within pharmaceuticals provides a medicinally relevant tool in drug discovery programmes. Here, the authors report a late-stage meta-C–H alkylation method facilitating the biological properties modulation of therapeutic agents.
- Lucas Guillemard
- , Lutz Ackermann
- & Magnus J. Johansson
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Article
| Open AccessElectric-field-assisted proton coupling enhanced oxygen evolution reaction
Manganese complexes have long been utilized by nature to catalyze the oxygen evolution reaction (OER) but mirroring their efficiency in artificial electrochemical systems has proven difficult. This study centers on alpha-manganese dioxide (α-MnO2), which closely mimics natural MnIV-O-MnIII-HxO motifs, presenting a novel method for manipulating proton coupling within the OER process using an external electric field.
- Xuelei Pan
- , Mengyu Yan
- & Liqiang Mai
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Article
| Open AccessRapid evolutionary change in trait correlations of single proteins
Trait correlations impact evolvability as selection on one trait can influence others. Here, the authors examine trait correlation in two proteins, a fluorescent protein & an antibiotic resistance enzyme, observing rapid evolution of trait correlations through changes in the biophysical properties of these proteins.
- Pouria Dasmeh
- , Jia Zheng
- & Andreas Wagner
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Article
| Open AccessExtrinsic hydrophobicity-controlled silver nanoparticles as efficient and stable catalysts for CO2 electrolysis
A key factor for the electrochemical reduction of CO2 to CO is limiting the competing H2 evolution reaction. Here, authors use real-time synchrotron X-ray computed tomography to show that a silver nanoparticle-ligand catalyst structure improves water management, thereby maintaining CO production.
- Young-Jin Ko
- , Chulwan Lim
- & Hyung-Suk Oh
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Article
| Open AccessNoncovalent interaction with a spirobipyridine ligand enables efficient iridium-catalyzed C–H activation
Exploitation of noncovalent interactions has received much attention for the design of metal catalysts. However, because of the weak nature, CH-π interactions have been less utilized for the control of organic reactions. Here, the authors report that the CH-π interaction can be used to kinetically accelerate catalytic C-H activation of arenes.
- Yushu Jin
- , Boobalan Ramadoss
- & Laurean Ilies
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Article
| Open AccessRapid room-temperature phosphorescence chiral recognition of natural amino acids
Chiral recognition of amino acids with luminescence, despite its advantages, is usually slow and lacks generality. Here, the authors demonstrate that L-phenylalanine derived benzamide can manifest the structural difference between the natural, left-handed amino acid and its right-handed counterpart via the difference in room-temperature phosphorescence, irrespective of the specific chemical structure.
- Xiaoyu Chen
- , Renlong Zhu
- & Guoqing Zhang
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Article
| Open AccessSelenium catalysis enables negative feedback organic oscillators
Multiple autocatalytic reactions producing thiols are known, but negative feedback loop motifs are unavailable for thiol chemistry. Here, the authors develop a negative feedback loop based on the selenocarbonates, in which thiols induce the release of aromatic selenols that catalyze the oxidation of thiols by organic peroxides.
- Xiuxiu Li
- , Polina Fomitskaya
- & Sergey N. Semenov
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Article
| Open AccessAn enzymatic continuous-flow reactor based on a pore-size matching nano- and isoporous block copolymer membrane
Continuous-flow biocatalysis with immobilized enzymes is a sustainable route for chemical synthesis, but inadequate biocatalytic efficiency caused by non-productive enzyme immobilization or enzyme-carrier mismatches presents a challenge for its application. Here, the authors report an approach for the fabrication of a high-performance enzymatic continuous-flow reactor via integrating scalable isoporous block copolymer membranes as carriers with an oriented one-step enzyme immobilization via a genetically fused material binding peptide.
- Zhenzhen Zhang
- , Liang Gao
- & Volker Abetz
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Article
| Open AccessIntelligent perceptual textiles based on ionic-conductive and strong silk fibers
Perception plays a pivotal role in advancing future intelligent textiles. Here, the authors develop smart perceptual textiles using natural-derived ionic-conductive silk fibers. These textiles can electrically detect external hazards and precisely pinpointing human touch, making them suitable for smart protective clothing and soft human-machine interfaces.
- Haojie Lu
- , Yong Zhang
- & Yingying Zhang
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Article
| Open AccessPhotocatalytic Z/E isomerization unlocking the stereodivergent construction of axially chiral alkene frameworks
The stereospecific Z/E isomerization of tetrasubstituted alkenes remains underdeveloped, thus lacking in a stereodivergent synthesis of axially chiral alkenes. Here, authors report the atroposelective synthesis of tetrasubstituted alkene analogues by asymmetric allylic substitution-isomerization, followed by the photocatalyzed Z/E isomerization.
- Jie Wang
- , Jun Gu
- & Ying He
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Article
| Open AccessNanoparticles as an antidote for poisoned gold single-atom catalysts in sustainable propylene epoxidation
The poisoning of single-atom catalysts hampers their performance. Here, the authors propose Au nanoparticles as an antidote for poisoned Au single-atom catalysts, with trace addition shown to reinforce and sustain propylene epoxidation.
- Qianhong Wang
- , Keng Sang
- & Xuezhi Duan
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Article
| Open AccessOrbital hybridization of donor and acceptor to enhance the conductivity of mixed-stack complexes
Mixed-stack complexes consisting of alternating donors and acceptors typically show low electrical conductivity. Here, the authors improved the conductivity by hybridizing the frontier orbitals of the donor and acceptor at the neutral–ionic boundary.
- Tomoko Fujino
- , Ryohei Kameyama
- & Hatsumi Mori
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Article
| Open AccessBioadhesive interface for marine sensors on diverse soft fragile species
It is useful to be able to equip marine animals with sensors, but it can be challenging to attach these to soft marine organisms. Here, the authors use an adhesive hydrogel to achieve rapid attachment of sensors to marine life including jellyfish, squid and lobster.
- Camilo Duque Londono
- , Seth F. Cones
- & Xuanhe Zhao
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Article
| Open AccessAssembly of short amphiphilic peptoids into nanohelices with controllable supramolecular chirality
Helical protein assemblies are an important biological structure, but are challenging to mimic with synthetic materials. Here, the authors report the use of peptoids to form nanohelix structures with controllable supramolecular chirality.
- Renyu Zheng
- , Mingfei Zhao
- & Chun-Long Chen
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Article
| Open AccessUnconventional mechanical and thermal behaviours of MOF CALF-20
CALF-20 MOF is considered a benchmark sorbent for industrial scale CO2 capture. Here authors use machine-learning potential simulations to show that CALF-20 exhibits anomalous structural responses to temperature and strain stimuli, with potential applications in mechanical/thermal sensing.
- Dong Fan
- , Supriyo Naskar
- & Guillaume Maurin
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Article
| Open AccessOn the role of asymmetric molecular geometry in high-performance organic solar cells
The correlation between asymmetric molecular geometry of non-fullerene acceptors and their optoelectronic properties was unclear. Here, the authors found asymmetric ones exhibit increased open-circuit voltage compared to their symmetric counterparts due to reduced non-radiative charge recombination.
- Jinfeng Huang
- , Tianyi Chen
- & Lijian Zuo
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Article
| Open AccessHybridizing carbonate and ether at molecular scales for high-energy and high-safety lithium metal batteries
Here, authors report a linear functionalized solvent through molecular hybridization. Complementary ethers and carbonates are integrated into a single molecule, exhibiting properties suited for high-energy and high safety lithium metal batteries.
- Jiawei Chen
- , Daoming Zhang
- & Yongyao Xia
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Article
| Open AccessElectrocatalytic hydrogenation of acetonitrile to ethylamine in acid
Proton exchange membrane electrolyzers hold promise for ethylamine synthesis from acetonitrile, yet local acidity fosters proton reduction. Here, authors systematically screen metal catalysts, verifying their effectiveness in such electrolyzers.
- Chongyang Tang
- , Cong Wei
- & Xiangfeng Duan
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Article
| Open AccessX-ray-activated polymerization expanding the frontiers of deep-tissue hydrogel formation
Photo-crosslinking polymerization facilitates precise control of hydrogel formation for various applications including tissue engineering, but most existing photo-crosslinking methods fail to achieve deep-tissue penetration, especially within bone structures. Here the authors report a strategy of low-dose X-ray-activated polymerization that enables deep-tissue hydrogel formation.
- Hailei Zhang
- , Boyan Tang
- & Gang Han
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Article
| Open Access3D printable strong and tough composite organo-hydrogels inspired by natural hierarchical composite design principles
The preparation of composite hydrogels can allow for mechanical properties to be enhanced, and hierarchical structures can be effective. Here, the authors report improved mechanical properties by the addition of ceramic platelets to an organohydrogel in direct ink writing.
- Quyang Liu
- , Xinyu Dong
- & Wei Zhai
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Article
| Open AccessTopology selectivity of a conformationally flexible precursor through selenium doping
Research into the control of conformational arrangements is of great importance for achieving bespoke nanoarchitectures. Here, the authors achieve topology selectivity of a conformationally flexible precursor by Se doping.
- Liangliang Cai
- , Tianhao Gao
- & Andrew T. S. Wee
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Article
| Open AccessAlkyne-tagged SERS nanoprobe for understanding Cu+ and Cu2+ conversion in cuproptosis processes
Simultaneously quantifying mitochondrial Cu+ and Cu2+ levels is vital for understanding the molecular mechanism of mitochondria-related biological events. Here the authors report an alkynyl-labeled SERS probe to simultaneously monitor free Cu+ and Cu2+ in mitochondria, and unveil their roles during ischemia and cuproptosis processes.
- Sihan Zhang
- , Yuxiao Mei
- & Yang Tian
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Article
| Open AccessDouble-walled Al-based MOF with large microporous specific surface area for trace benzene adsorption
Trace benzene poses a risk to the health and safety of humans, resulting in a challenging task. Here authors synthesise double-walled Al-based MOF ZJU-520(Al) with trace benzene adsorption (5.98 mmol g–1) and excellent benzene/cyclohexane separation ability.
- Laigang Hu
- , Wenhao Wu
- & Kun Yang
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Article
| Open AccessEmbedding biocatalysts in a redox polymer enhances the performance of dye-sensitized photocathodes in bias-free photoelectrochemical water splitting
A robust and efficient dye-sensitized NiO bio-hybrid photocathode based on a redox polymer and [FeFe]- hydrogenase has been developed to couple with a BiVO4 photoanode for water splitting without applied bias.
- Fangwen Cheng
- , Olha Pavliuk
- & Haining Tian
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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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