Featured
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Article
| Open AccessBiocatalytic stereocontrolled head-to-tail cyclizations of unbiased terpenes as a tool in chemoenzymatic synthesis
Terpene synthesis is limited by the current availability of natural cyclic building blocks. In this study, the authors employ squalene-hopene cyclases in the chemoenzymatic synthesis of head-to-tail fused terpenes and generate ten chiral scaffolds with >99% ee and de, at up to decagram scale.
- Andreas Schneider
- , Thomas B. Lystbæk
- & Bernhard Hauer
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Article
| Open AccessEvolution of the ionisation energy with the stepwise growth of chiral clusters of [4]helicene
Polycyclic aromatic hydrocarbons such as [4]helicenes are important interstellar molecules. Here, the authors show their evolution of chiral clusters upon aggregation through coincidence spectroscopy and quantum chemical calculations.
- Sérgio R. Domingos
- , Denis S. Tikhonov
- & Melanie Schnell
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Article
| Open AccessThymoquinone as an electron transfer mediator to convert Type II photosensitizers to Type I photosensitizers
Developing Type I photosensitizers (PSs) is vital for tackling hypoxic intolerance of photodynamic therapy in the hypoxic microenvironment, but elusive due to the lack of a general molecular design strategy. Here the authors report a universal and simple method to covert traditional Type II PSs to Type I PSs.
- Jiahao Zhuang
- , Guobin Qi
- & Bin Liu
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Article
| Open AccessSilver coordination-induced n-doping of PCBM for stable and efficient inverted perovskite solar cells
The bidirectional halide and silver migration cause irreversible chemical corrosion to electrodes and perovskite layer. Here, the authors employ 4,4’-dicyano-2,2’-bipyridine in the electron transport layer to coordinate silver and iodide, realizing stable solar cells with efficiency over 26%.
- Cheng Gong
- , Haiyun Li
- & Zhigang Zang
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Article
| Open AccessAssessing elevated pressure impact on photoelectrochemical water splitting via multiphysics modeling
Solar water splitting devices, though often demonstrated at atmospheric pressure, need to deliver H2 at high pressure for many applications. Here the authors use multiphysics model to evaluate the benefits and penalties of elevated pressure operation, identifying the optimum pressure range to enhance efficiency.
- Feng Liang
- , Roel van de Krol
- & Fatwa F. Abdi
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Article
| Open AccessReactive P and S co-doped porous hollow nanotube arrays for high performance chloride ion storage
P, S co-doped porous nanotube arrays on carbon felt (CoNiPS@CF) enhance chloride-ion storage for energy and water purification. This structure provides a short ion diffusion pathway, and improves activity of adsorption sites, promoting conductivity and activity for efficient chloride capture.
- Siyang Xing
- , Ningning Liu
- & Jie Ma
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Article
| Open AccessA refined picture of the native amine dehydrogenase family revealed by extensive biodiversity screening
Sustainable chemistry can benefit from biocatalysis, but a high diversity of enzymes is needed. Here, the authors screen billions of protein sequences to provide an overview of the native amine dehydrogenase family for amine synthesis.
- Eddy Elisée
- , Laurine Ducrot
- & Carine Vergne-Vaxelaire
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Article
| Open AccessChiral dinitrogen ligand enabled asymmetric Pd/norbornene cooperative catalysis toward the assembly of C–N axially chiral scaffolds
The preparation of C − N axially chiral compounds, a class of privileged scaffolds in pharmaceuticals, advanced materials and organic synthesis, has recently attracted significant interest. Herein the authors report a chiral dinitrogen ligand promoted asymmetric Catellani reaction for the synthesis of C–N axially chiral scaffolds.
- Liang Jin
- , Ya Li
- & Bing-Feng Shi
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Article
| Open AccessSub-100-fs energy transfer in coenzyme NADH is a coherent process assisted by a charge-transfer state
Excitation energy transfer is important for many photoinduced biological processes in systems with multiple chromophores. Here, the authors elucidate this process for the coenzyme NADH using ultrafast spectroscopy and quantum dynamics.
- Vishal Kumar Jaiswal
- , Daniel Aranda Ruiz
- & Artur Nenov
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Article
| Open AccessArtificial cellulosic leaf with adjustable enzymatic CO2 sequestration capability
Developing artificial leaves is crucial for advancing Net Zero Future, but most artificial leaves rely on the use of metal or semiconductors catalysts that usually have a lower catalytic activity and selectivity compared to biocatalysts. Here the AUs report Ecoleaf, a biodegradable artificial leaf that mimics the controlled expansion and contraction of stomata and enables enzymic CO2 conversion.
- Xing Zhu
- , Chenxi Du
- & Bin He
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Article
| Open AccessRapidly damping hydrogels engineered through molecular friction
Hydrogels capable of swift mechanical energy dissipation are desirable for various uses, but traditional energy absorption in hydrogels typically relies on viscoelastic mechanisms and often suffers from slow recovery. Here, the authors report a hydrogel design harnessing molecular friction to achieve efficient energy dissipation and rapid recovery.
- Zhengyu Xu
- , Jiajun Lu
- & Wei Wang
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Article
| Open AccessRule-based omics mining reveals antimicrobial macrocyclic peptides against drug-resistant clinical isolates
This study reports the genomics- and metabolomics-guided discovery of aminovinyl-(methyl-)cysteine-containing peptides (ACyP). One of these peptides, massatide A, demonstrates excellent activity against drug-resistant gram-positive pathogens.
- Zhuo Cheng
- , Bei-Bei He
- & Yong-Xin Li
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Article
| Open AccessDesign and synthesis of broadband absorption covalent organic framework for efficient artificial photocatalytic amine coupling
Creating highly active materials that effectively harness solar spectra is essential for photocatalysis, though challenging. Here the authors introduce a novel donor-acceptor covalent organic framework with a broad absorption range of 200 nm to 900 nm, achieving efficient artificial photocatalytic amine coupling.
- Yuanding Fang
- , Youxing Liu
- & Yunqi Liu
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Article
| Open AccessFully exposed Pt clusters for efficient catalysis of multi-step hydrogenation reactions
Hydrogenating di-nitroaromatics with high activity and selectivity is challenging due to the process’s complexity. Here the authors present a fully exposed Pt clusters catalyst for 2,4-dinitrotoluene hydrogenation, suggesting that the synergy between multiple active sites and moderate adsorption behavior is crucial for the high catalytic activity.
- Yang Si
- , Yueyue Jiao
- & Hongyang Liu
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Article
| Open AccessClosed-loop recycling of tough epoxy supramolecular thermosets constructed with hyperbranched topological structure
The covalent crosslinked structure of epoxy thermosets difficult their reprocessability and recyclability. Here, the authors report a method for developing closed loop recycling of strong and tough epoxy supramolecular thermosets constructed with hyperbranched topological structure in an energy-saving and easy-to-conduct way.
- Junheng Zhang
- , Can Jiang
- & Daohong Zhang
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Article
| Open AccessUltrafast light-activated polymeric nanomotors
The development of methodologies to construct fast-moving, biodegradable polymeric nanomotors remains a challenge. Here, the authors present a light-propelled nanomotor by adorning the surface of bowl-shaped stomatocytes with gold nanoparticles achieving particle translocation in mammalian cells through the temporary disruption of the cell membrane.
- Jianhong Wang
- , Hanglong Wu
- & Jan C. M. van Hest
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Article
| Open AccessAn effective and rapidly degradable disinfectant from disinfection byproducts
Here, authors highlight ecological risks of a widely used disinfectant, chloroxylenol, and identify a more efficient and safer alternative from halo-phenolic disinfection byproducts, 2,6-dichlorobenzoquinone. They leverage seawater’s slightly alkaline nature to enhance its degradability via hydrolysis.
- Jiarui Han
- , Wanxin Li
- & Xiangru Zhang
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Article
| Open AccessIdentifying critical features of iron phosphate particle for lithium preference
Olivine iron phosphate (FePO4) is widely proposed for electrochemical lithium extraction, but particles with different physical attributes demonstrate varying Li preferences. Here, the authors characterize the electrochemical lithiation and sodiation behavior of a series of FePO4 particles with different morphology to identify critical features that enhance Li selectivity.
- Gangbin Yan
- , Jialiang Wei
- & Chong Liu
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Article
| Open AccessCovalently bridging graphene edges for improving mechanical and electrical properties of fibers
The performance of macroscopic graphene fibers is hampered by lower bonding strength between individual graphene sheets. Authors mitigate this by creating covalent conjugating linkages at sheet edges, improving mechanical and electrical properties.
- Ling Ding
- , Tianqi Xu
- & Zhongfan Liu
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Article
| Open AccessMachine learning-guided realization of full-color high-quantum-yield carbon quantum dots
Optimizing the synthesis for efficient luminescent materials requires consideration of a large number of parameters. Here, the authors realize high quantum yield full-color carbon quantum dot using an iterative machine-learning experimental strategy.
- Huazhang Guo
- , Yuhao Lu
- & Liang Wang
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Article
| Open AccessCO2 electrolysis to multi-carbon products in strong acid at ampere-current levels on La-Cu spheres with channels
Efficient electroreduction of CO2 to multi-carbon products under strong acidic condition is highly challenging. Here, the authors demonstrate that combining microenvironment modulation and La doping effect could promote multicarbon products generation in acidic electrolyte.
- Jiaqi Feng
- , Limin Wu
- & Buxing Han
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Article
| Open AccessPiezoceramic membrane with built-in ultrasound for reactive oxygen species generation and synergistic vibration anti-fouling
Piezoceramic membranes in water treatment have been limited by the single vibration-based anti-fouling mechanism. The authors break this limitation using Mn/BaTiO3 membranes to generate reactive oxygen species via piezoelectric vibration, offering insights for developing piezoelectric anti-fouling and catalytic membranes.
- Yang Zhao
- , Feng Yang
- & Guandao Gao
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Article
| Open AccessCollective chiroptical activity through the interplay of excitonic and charge-transfer effects in localized plasmonic fields
Chiral interaction of molecular ensembles with confined light fields is elusive. Here, the authors report collective chiroptical effects through coupling of exciton and charge-transfer mixed molecular assemblies with plasmonic nanoparticles.
- Huacheng Li
- , Xin Xu
- & Xiang Lan
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Article
| Open AccessOxime-functionalized anti-insecticide fabric reduces insecticide exposure through dermal and nasal routes, and prevents insecticide-induced neuromuscular-dysfunction and mortality
Exposition to insecticides can be dangerous. Here, authors developed an oxime-fabric body suit and facemask that chemically deactivate insecticides and prevent insecticide-induced lethal effects, offering an affordable solution for farmer safety.
- Mahendra K. Mohan
- , Ketan Thorat
- & Praveen Kumar Vemula
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Article
| Open AccessEnantioselective synthesis of chiral amides by carbene insertion into amide N–H bond
Chiral amides are important structure in many natural products and pharmaceuticals, yet their efficient synthesis from simple amide feedstock remains challenge due to its weak Lewis basicity. Here, the authors report the enantioselective synthesis of chiral amides by N-alkylation of primary amides via Rh-catalyzed carbene N–H insertion reaction.
- Xuan-Ge Zhang
- , Zhi-Chun Yang
- & Qi-Lin Zhou
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Article
| Open AccessUltrafast electron transfer at the In2O3/Nb2O5 S-scheme interface for CO2 photoreduction
In2O3/Nb2O5 S-scheme heterojunctions fabricated via a one-step electrospinning technique facilitate contact between two phases, fostering ultrafast interfacial electron transfer to prolong lifetimes and improve CO2 photoreduction performance.
- Xianyu Deng
- , Jianjun Zhang
- & Jiaguo Yu
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Article
| Open AccessSupramolecular assembly activated single-molecule phosphorescence resonance energy transfer for near-infrared targeted cell imaging
Phosphorescence resonance energy transfer systems have potential in light-harvesting and bioimaging, but host-guest systems are rarely explored. Here, the authors report the development of a macrocyclic host-guest system for targeted cell imaging.
- Xiaolu Zhou
- , Xue Bai
- & Yu Liu
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Article
| Open AccessDifluorocarbene-induced [1,2]- and [2,3]-Stevens rearrangement of tertiary amines
The Stevens rearrangements are a fundamental and powerful tool in the synthetic organic chemistry repertoire, but these transformations are known to be limited in their tolerance for some common functional groups. Here, the authors present a methodology that uses a difluorocarbene unit to induce a Stevens rearrangement, which enables smooth inclusion of allylic and propargyl moieties in the transformation.
- Jianke Su
- , Yu Guo
- & Qiuling Song
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Perspective
| Open AccessThe role of electrocatalytic materials for developing post-lithium metal||sulfur batteries
Post-lithium metal||S batteries show promise for practical applications, but limited understanding of cell parameters and sulfur electrocatalytic conversion hampers progress. This Perspective provides critical insights on potential research directions for designing practical post-lithium metal||S batteries.
- Chao Ye
- , Huan Li
- & Shi-Zhang Qiao
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Article
| Open AccessPicosecond reactions of excited radical ion super-reductants
Classical photochemistry requires nanosecond excited-state lifetimes for diffusion-controlled reactions. Here the authors provide direct evidence for the elusive pre-association between radical ions and substrate molecules, enabling photoinduced electron transfer beyond the diffusion limit.
- Björn Pfund
- , Deyanira Gejsnæs-Schaad
- & Oliver S. Wenger
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Article
| Open AccessHeterogeneous organophotocatalytic HBr oxidation coupled with oxygen reduction for boosting bromination of arenes
Developing mild photocatalytic bromination strategies using sustainable bromo source has been attracting intense interests, but there is still much room for improvement. Here, the authors report heterogenous organophotocatalytic HBr oxidation coupled with oxygen reduction to furnish Br2 and H2O2 for effective bromination of arenes.
- Jie Wang
- , Jiahao Liang
- & Bin Liu
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Article
| Open AccessCharge redistribution of a spatially differentiated ferroelectric Bi4Ti3O12 single crystal for photocatalytic overall water splitting
Via specific acid etching, the authors report the production of spatially differentiated Bi4Ti3O12 nanosheets to accelerate photogenerated charge transfer and separation for effective water splitting in a one-step excitation system with a solar-to-hydrogen efficiency of 0.1%.
- Guangri Jia
- , Fusai Sun
- & Jimmy C. Yu
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Article
| Open AccessDirect observation of photoinduced sequential spin transition in a halogen-bonded hybrid system by complementary ultrafast optical and electron probes
Halogen bond is desired for tuning electronic properties by external stimuli. Here, authors reveal a sequential activation of spin crossover and dimer softening, unveiling a key transient state in a prototypical halogen-bonded material.
- Yifeng Jiang
- , Stuart Hayes
- & R. J. Dwayne Miller
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Article
| Open AccessA combined experimental and computational study of ligand-controlled Chan-Lam coupling of sulfenamides
Sulfenamides are a class of divalent sulfur-derived scaffolds featuring an S-N bond with many industrial applications, however, they are also challenging substrates for synthetic transformations. Here, the authors present a highly chemoselective ligand-controlled Chan–Lam coupling of sulfenamides as a straightforward route to N-arylated sulfenamides.
- Kaiming Han
- , Hong Liu
- & Tiezheng Jia
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Article
| Open AccessHighly reversible transition metal migration in superstructure-free Li-rich oxide boosting voltage stability and redox symmetry
The ordering of superstructures plays a critical role in mitigating transition metal migration, voltage decay, and maintaining redox symmetry in Li-rich layered oxides. Here, this study reveals that even in the absence of such superstructure ordering, cathodes can still attain these crucial characteristics.
- Tianwei Cui
- , Jialiang Xu
- & Yongzhu Fu
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Article
| Open AccessBicarbonate-binding catalysis for the enantioselective desymmetrization of keto sulfonium salts
Although anion-binding processes are well-known for their crucial role in molecular recognition, this type of phenomenon has only recently been utilized for catalysis. Here, the authors present an enantioselective desymmetrization of cyclic keto sulfonium salts through enantioselective deprotonation/ring opening process by anion-binding catalysis.
- José Alemán
- , Jorge Humbrías-Martín
- & Jose A. Fernández-Salas
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Article
| Open AccessMolecular ferroelectric with low-magnetic-field magnetoelectricity at room temperature
The authors report a molecular ferroelectric (TMCM)[FeCl4], which shows strong magnetostrictive and magnetoelectric effects at room temperature. The spin-lattice coupling of FeCl4 and flexible structure of organic cations are responsible for these effects.
- Zhao-Bo Hu
- , Xinyu Yang
- & You Song
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Article
| Open AccessSelf-protecting CoFeAl-layered double hydroxides enable stable and efficient brine oxidation at 2 A cm−2
Developing high-performance electrodes for catalyzing brine oxidation is essential for cost effective hydrogen production. Here, this study reveals the self-protective mechanism of CoFeAl layered double hydroxides, enabling stable operation in the presence of concentrated seawater at 2 A cm−2.
- Wei Liu
- , Jiage Yu
- & Xiaoming Sun
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Article
| Open AccessRecovery of europium from E-waste using redox active tetrathiotungstate ligands
Rare-earth elements (REEs) are vital to the modern economy, yet their mining poses both geopolitical and environmental challenges. Here, authors present a highly selective method for the recovery of europium from spent fluorescent lamps using redox active tetrathiotungstate ligands.
- Marie A. Perrin
- , Paul Dutheil
- & Victor Mougel
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Article
| Open AccessChatMOF: an artificial intelligence system for predicting and generating metal-organic frameworks using large language models
LLMs can be augmented with tools to increase their capabilities. Here, authors have developed an artificial intelligence system called ChatMOF combining LLMs and specialised libraries and utilities to predict and generate metal-organic frameworks.
- Yeonghun Kang
- & Jihan Kim
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Article
| Open AccessQuantitative prediction of rate constants and its application to organic emitters
The quantitative prediction of rate constants and quantum yields is crucial to understand various phenomena and their mechanisms in nature. Here, the authors apply quantum chemical calculation to reproduce experimental data of multiple-resonance thermally activated delayed fluorescence emitters.
- Katsuyuki Shizu
- & Hironori Kaji
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Article
| Open AccessCircumventing bottlenecks in H2O2 photosynthesis over carbon nitride with iodine redox chemistry and electric field effects
H2O2 photosynthesis using g-C3N4 is considered an alternative to anthraquinone processes. Inspired by the optical instability of potassium iodide, the I− /I3− internal redox mediator and external electric field are integrated into the g-C3N4, achieving satisfactory H2O2 production.
- Chang-Wei Bai
- , Lian-Lian Liu
- & Han-Qing Yu
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Article
| Open AccessRedox dynamics and surface structures of an active palladium catalyst during methane oxidation
Palladium-based catalysts are highly effective for the complete oxidation of methane. Here, the authors employ operando transmission electron microscopy, near-ambient pressure X-ray photoelectron spectroscopy, and density functional theory calculations to investigate the active state and catalytic function of Pd nanoparticles in methane oxidation.
- Shengnan Yue
- , C. S. Praveen
- & Xing Huang
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Article
| Open AccessEfficient intersystem crossing and tunable ultralong organic room-temperature phosphorescence via doping polyvinylpyrrolidone with polyaromatic hydrocarbons
Room temperature phosphorescent polymers have potential in a range of applications, but achieving the desired properties can be challenging. Here, the authors report the development of such polymer materials by doping with polyaromatic hydrocarbons.
- Guangxin Yang
- , Subin Hao
- & Li Dang
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Article
| Open AccessConcentrated solar CO2 reduction in H2O vapour with >1% energy conversion efficiency
This work reports a single-atom Ni incorporated CeO2 catalyst that boosts the efficiency of solar CO2 reduction under concentrated light irradiation.
- Yuqi Ren
- , Yiwei Fu
- & Maochang Liu
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Article
| Open AccessInsight into selectivity of photocatalytic methane oxidation to formaldehyde on tungsten trioxide
Tungsten trioxide (WO3) is considered the most promising photocatalyst for the highly selective oxidation of methane to formaldehyde, though the origins of its catalytic activity and reaction mechanism are still debated. Here, the authors use WO3 with {001} and {110} facets as model photocatalysts, demonstrating that the photocatalytic oxidation of methane to formaldehyde in WO3 depends on the surface structure, leading to different formaldehyde selectivity.
- Yingying Fan
- , Yuheng Jiang
- & Zhiyong Tang
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Article
| Open AccessRevealing the structural evolution of CuAg composites during electrochemical carbon monoxide reduction
Revealing catalyst structural evolution during catalysis is critical. Here, authors reveal that a Cu-Ag oxide precursor undergoes a transformation during CO electroreduction to a composite consisting of Ag nanoparticles enveloped by thin layers of amorphous Cu, which is likely the real active phase.
- Di Wang
- , Hyun Dong Jung
- & Lei Wang
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Article
| Open AccessA dual spin-controlled chiral two-/three-dimensional perovskite artificial leaf for efficient overall photoelectrochemical water splitting
Enhancing the efficiency of solar-driven water splitting is challenging but highly interesting. Here the authors report a dual spin-controlled 2D/3D perovskite photoelectrode that achieves 12.55% efficiency by utilizing the chiral-induced spin selectivity phenomenon.
- Hyungsoo Lee
- , Chan Uk Lee
- & Jooho Moon
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Article
| Open AccessPhotochemically responsive polymer films enable tunable gliding flights
Miniature passive fliers are of interest, but there are challenges in controlling their motion. Here, the authors report the use of light-responsive thin films for optical control of the gliding of passive fliers.
- Jianfeng Yang
- , M. Ravi Shankar
- & Hao Zeng
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