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| Open AccessPd/NiMoO4/NF electrocatalysts for the efficient and ultra-stable synthesis and electrolyte-assisted extraction of glycolate
Here, the authors report a path for electrocatalytic conversions of alcohols through in-situ acid-base reaction and the design of electrocatalysts. In this work, the electrocatalyst had reduced Pd content, improved efficiency, and lowered costs.
- Kai Shi
- , Di Si
- & Jianlin Shi
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Article
| Open AccessA Janus carbaporphyrin pseudo-dimer
Carbaporphyrin dimers, known for their interesting photophysical properties and application in metal-organic chemistry, generally contain two identical subunits. Here, the authors highlight the benefits that can accrue from breaking the inherent symmetry of carbaporphyrin dimers and details a new approach to creating heterobimetallic complexes.
- Haodan He
- , Jiyeon Lee
- & Xian-Sheng Ke
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Article
| Open AccessCrosslinking-induced patterning of MOFs by direct photo- and electron-beam lithography
Precise and scalable patterning is essential for the use of metal-organic frameworks (MOFs) in solid-state electronics and photonics. Here, the authors report on resistance-free, direct photo- and electron-beam lithography of MOF films using crosslinking chemistry.
- Xiaoli Tian
- , Fu Li
- & Jinghong Li
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Article
| Open AccessFlash healing of laser-induced graphene
Laser-induced graphene (LIG) can be obtained via a practically convenient approach, but its amorphous characteristics limit its applications. Here, the authors report a flash Joule heating strategy to improve the crystalline quality and conductivity of LIG, leading to strain sensors with enhanced sensitivity.
- Le Cheng
- , Chi Shun Yeung
- & Ruquan Ye
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Article
| Open AccessThe formation of unsaturated IrOx in SrIrO3 by cobalt-doping for acidic oxygen evolution reaction
SrIrO3-based catalyst is a promising candidate for acidic oxygen evolution reaction (OER), but the active sites and factors responsible for its effectiveness remain ambiguous. Here, the authors reveal that dynamic dissolution of Co in Co-SrIrO3 leads to the formation of unsaturated IrOx, enabling high-efficiency OER.
- Jia-Wei Zhao
- , Kaihang Yue
- & Gao-Ren Li
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Article
| Open AccessIsotope engineering achieved by local coordination design in Ti-Pd co-doped ZrCo-based alloys
Hydrogen isotope effect in metal-hydrogen systems disturbs precise Deuterium/Tritium (D/T) ratio control. Here, the authors demonstrate a local coordination strategy that comprises thermodynamic destabilization with vibration enhancement of interstitial isotopes for isotope engineering.
- Jiacheng Qi
- , Xu Huang
- & Lixin Chen
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Article
| Open AccessEnhancement of electrocatalysis through magnetic field effects on mass transport
Magnetic fields can enhance electrocatalysis, yet its effect on mass transport has been overlooked. Here, the authors track the motion induced on the electrolyte ions, demonstrating that mass transport effects can double the catalyst activity with low reactant availability, as in oxygen reduction.
- Priscila Vensaus
- , Yunchang Liang
- & Magalí Lingenfelder
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Article
| Open AccessUmpolung reactivity of strained C–C σ-bonds without transition-metal catalysis
Umpolung reactions typically focus on carbonyls or imine derivatives. Here, the authors report the umpolung reaction of C–C σ-bonds in bicyclo[1.1.0]butanes (BCBs) with electrophilic alkenes, yielding various cyclobutenes or conjugated dienes.
- Dachang Bai
- , Xiuli Guo
- & Junbiao Chang
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Article
| Open AccessUltrafast photoinduced C-H bond formation from two small inorganic molecules
The formation of C–H bonds via reaction of small inorganic molecules is of great interest for understanding the transition from inorganic to organic matter, but the detailed mechanisms remain elusive. Here, the authors demonstrate real-time visualization and coherent control of the ultrafast C–H bond formation dynamics in a light-induced bimolecular reaction from inorganic species.
- Zhejun Jiang
- , Hao Huang
- & Jian Wu
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Article
| Open AccessTrialkoxysilane-Induced Iridium-Catalyzed para-Selective C–H Bond Borylation of Arenes
Controlling regioselectivity is one of the most challenging aspects for the construction of aryl boron compounds, and there are few practical and general strategies for such transformations. Here, the authors report an iridium-catalyzed trialkoxysilane protecting group-assisted regioselective C–H borylation with various aromatic compounds.
- Guodong Ju
- , Zhibin Huang
- & Yingsheng Zhao
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Article
| Open AccessExtending carbon chemistry at high-pressure by synthesis of CaC2 and Ca3C7 with deprotonated polyacene- and para-poly(indenoindene)-like nanoribbons
The authors demonstrate that carbides with infinite chains of fused [C6] and [C5] rings are synthesized at deep planetary pressures and temperatures. Hydrolysis of these carbides may lead to polycyclic aromatic hydrocarbons in the Universe.
- Saiana Khandarkhaeva
- , Timofey Fedotenko
- & Leonid Dubrovinsky
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Article
| Open AccessJanus electronic state of supported iridium nanoclusters for sustainable alkaline water electrolysis
The hydrogen spillover effect improves the efficiency of the H2 evolution reaction but is incompatible with the O2 evolution reaction in alkaline water electrolysis. Here, the authors show that the Janus electronic state of supported Ir nanoclusters can couple hydrogen spillover and O2 evolution.
- Yaoda Liu
- , Lei Li
- & Zhengfei Dai
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Article
| Open AccessUltraviolet light blocking optically clear adhesives for foldable displays via highly efficient visible-light curing
The slow curing speed of UV-based methods to produce UV-blocking optically clear adhesive (OCA) for display panels poses a barrier to commercialization. Here, authors introduce a visible-light driven photo-initiating system for rapid production of OCAs, demonstrating efficient UV-blocking ability.
- Yonghwan Kwon
- , Seokju Lee
- & Min Sang Kwon
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Article
| Open AccessHighly efficient multi-resonance thermally activated delayed fluorescence material toward a BT.2020 deep-blue emitter
The realization of a BT.2020 blue emitter is challenging due to the spectral redshift associated with π-extension. Here, the authors report a multi-resonance thermally activated delayed fluorescence emitter, exhibiting ultrapure deep-blue narrow emission and CIEy ≤ 0.05 exceeding 20% efficiency.
- Junki Ochi
- , Yuki Yamasaki
- & Takuji Hatakeyama
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Article
| Open AccessAn all-in-one tetrazine reagent for cysteine-selective labeling and bioorthogonal activable prodrug construction
Prodrugs have the potential for improving therapeutic index and expanding drug targets, but current prodrug activation strategies that are responsive to endogenous stimuli can result in unintended drug release and systemic toxicity. Here, the authors report 3-vinyl−6-oxymethyltetrazine (voTz) as an all-in-one reagent for modular preparation of tetrazine-caged prodrugs and chemoselective labeling of peptides to produce bioorthogonal activable peptide-prodrug conjugates.
- Xinyu He
- , Jie Li
- & Haoxing Wu
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Article
| Open AccessBiomimetic NIR-II fluorescent proteins created from chemogenic protein-seeking dyes for multicolor deep-tissue bioimaging
Near-infrared-I/II fluorescent proteins (NIR-I/II FPs) are crucial for in vivo imaging, but their availability is still scarce. Here, the authors make use of protein-seeking NIR-II dyes as chromophores, which covalently bind to tag proteins and thus creating biomimetic NIR-II FPs.
- Jiajun Xu
- , Ningning Zhu
- & Shoujun Zhu
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Article
| Open AccessCarbon redirection via tunable Fenton-like reactions under nanoconfinement toward sustainable water treatment
Regulating the carbon evolution pathway during chemical oxidation is critical, but challenging, for sustainable water treatment. Here, the authors report an adaptive approach to drive carbon redirection from molecular fragmentation to polymerization under tunable nanoconfinement.
- Xiang Gao
- , Zhichao Yang
- & Bingcai Pan
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Article
| Open AccessDefect-induced triple synergistic modulation in copper for superior electrochemical ammonia production across broad nitrate concentrations
Converting nitrate to ammonia in wastewater with a wide range of nitrate concentrations remains a challenging task. Here the authors report defect-rich Cu nanowire electrocatalyst which can achieve 50 to 1100 mA cm−2 and over 90% Faradaic efficiency using 1–100 mM nitrate wastewater.
- Bocheng Zhang
- , Zechuan Dai
- & Genqiang Zhang
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Article
| Open AccessStereoselective assembly of C-oligosaccharides via modular difunctionalization of glycals
C-oligosaccharides are found in natural products and drug molecules, but their synthesis is challenging. Here, the authors report a strategy for the stereoselective and efficient synthesis of Coligosaccharides via palladium-catalyzed nondirected C1–H glycosylation/C2-alkenylation, cyanation, and alkynylation of 2-iodoglycals with glycosyl chloride donors.
- Ya-Nan Ding
- , Mei-Ze Xu
- & Yong-Min Liang
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Article
| Open AccessElectroreduction of unactivated alkenes using water as hydrogen source
The reduction of unactivated alkyl alkenes is a difficult challenge in organic chemistry. Here, the authors present a silicon-mediated electroreduction of alkyl alkenes, using water as a hydrogen source, enabled by [Fe]-H.
- Yanwei Wang
- , Qian Wang
- & Youai Qiu
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Article
| Open AccessPhoto-modulated activation of organic bases enabling microencapsulation and on-demand reactivity
Oil-water emulsion techniques can be used for encapsulation of chemicals and control of reactivity, but is challenging for highly reactive materials such as acids and bases. Here, the authors report the encapsulation of bases by masking of reactivity with photo-removable protecting groups.
- Wenle Li
- , Xiaocun Lu
- & Nancy R. Sottos
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Article
| Open AccessAutonomous closed-loop mechanistic investigation of molecular electrochemistry via automation
Electrochemical research often requires stringent combinations of experimental parameters that are demanding to manually locate. Here the authors report an autonomous electrochemical platform that implements an adaptive, closed-loop workflow for mechanistic investigation of molecular electrochemistry.
- Hongyuan Sheng
- , Jingwen Sun
- & Chong Liu
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Article
| Open AccessSupramolecular polynuclear clusters sustained cubic hydrogen bonded frameworks with octahedral cages for reversible photochromism
The development of supramolecular porous crystalline frameworks with architectures from secondary building units remains challenging. Here, the authors report ammonium node-assembled clusters as supramolecular secondary building units to sustain a body centered cubic hydrogenbonded framework with octahedral cages for haloform encapsulation and reversible photochromism.
- Xiaojun Ding
- , Jing Chen
- & Gang Ye
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Article
| Open AccessChiral BINOL-phosphate assembled single hexagonal nanotube in aqueous solution for confined rearrangement acceleration
Supramolecular confined catalysis aims to mimic the active pocket of an enzyme to enhance the efficiency and selectivity of catalytic reactions. Here, the authors describe the formation of chiral nanotubes stable in aqueous solution employing a chiral BINOL-phosphate which can accelerate the 3-aza-Cope rearrangement by a nanotubular interior confinement effect.
- Kang Li
- , Wei-Min Qin
- & Yue-Peng Cai
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Article
| Open AccessUltrathin organosiloxane membrane for precision organic solvent nanofiltration
The use of membranes under harsh conditions, particularly involving the separation of complex organic solvents, remains challenging. Here the authors demonstrate an ultrathin organosiloxane polymer membrane using initiated chemical vapor deposition to effectively separate solutes within the molecular weight range of 150–300 g mol−1.
- Jihoon Choi
- , Keonwoo Choi
- & Dong-Yeun Koh
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Article
| Open AccessTailoring coordination environments of single-atom electrocatalysts for hydrogen evolution by topological heteroatom transfer
The rational design of carbon-supported transition metal single atom catalysts with precise coordination tailoring remains challenging. Here, the authors develop a topological heteroatom-transfer strategy to precisely control the P coordination in Co single atoms for hydrogen evolution.
- Sheng Qian
- , Feng Xu
- & Jingqi Tian
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Article
| Open AccessConstructing regulable supports via non-stoichiometric engineering to stabilize ruthenium nanoparticles for enhanced pH-universal water splitting
Establishing optimal metal-support interactions is crucial for creating efficient catalysts for water splitting. Here, stable Ti–O–Ru interface formation and minimal work function difference between Ru nanoparticles and non-stoichiometric Ti4O7 lead to exceptional bifunctional activity of Ru/Ti4O7 for both HER and OER across pH-universal environments, maintaining stable operation for 500 h.
- Sheng Zhao
- , Sung-Fu Hung
- & Shengjie Peng
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Article
| Open AccessHairpin trimer transition state of amyloid fibril
Amyloid fibrils are ordered protein assemblies implicated in neurodegenerative disease. Here the authors show that hairpin trimers can be transition states of fibril nucleation, explaining how different fibril isoforms may arise from alternative nucleation sites.
- Levent Sari
- , Sofia Bali
- & Milo M. Lin
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Article
| Open AccessThe initial stages of cement hydration at the molecular level
Despite being crucial for elucidating the cement hydration mechanism, the initial hydration stage is poorly understood. Here, authors uncover the unbiased Ca dissolution pathway during the initial hydration of calcium silicates via atomistic simulations and reveal a key Ca ligand structure.
- Xinhang Xu
- , Chongchong Qi
- & Hegoi Manzano
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Article
| Open AccessRoom temperature 3D carbon microprinting
Three-dimensional carbon microstructures with ultra-high aspect ratios are grown with a facile process using a metal-free catalyst and low-power visible light at room temperature, unlocking applications in flexible sensors and beyond.
- Fernand E. Torres-Davila
- , Katerina L. Chagoya
- & Laurene Tetard
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Article
| Open AccessAn integrated high-throughput robotic platform and active learning approach for accelerated discovery of optimal electrolyte formulations
Solubility determines energy density in redox flow batteries. Here, authors combine automated experiments with machine learning to efficiently identify solvents that significantly enhance solubility, testing less than 10% of over 2000 candidates.
- Juran Noh
- , Hieu A. Doan
- & Yangang Liang
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Article
| Open AccessIdentifying a key spot for electron mediator-interaction to tailor CO dehydrogenase’s affinity
Carbon monoxide dehydrogenases (CODH) employ artificial electron mediators like viologens for biocatalysis, but little is known about the interaction between the mediators and the enzyme. Here, the authors discover the critical site for viologen interactions at the D-cluster of Carboxydothermus hydrogenoformans CODH2 via alanine mutations and crystallography, and report variants with increased ethyl viologen affinity.
- Suk Min Kim
- , Sung Heuck Kang
- & Yong Hwan Kim
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Article
| Open AccessNi-catalyzed enantioconvergent deoxygenative reductive cross-coupling of unactivated alkyl alcohols and aryl bromides
The direct reductive coupling of alkyl alcohol and aryl halide enables efficient access to valuable compounds, but the asymmetric pattern remains unknown. Here the authors describe the enantioconvergent deoxygenative reductive cross-coupling of unactivated alkyl alcohol and aryl bromide in the presence of an NHC activating agent.
- Li-Li Zhang
- , Yu-Zhong Gao
- & Ze-Peng Yang
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Article
| Open AccessBioorthogonal photocatalytic proximity labeling in primary living samples
Studying subcellular proteomes in primary living cells is crucial for understanding health and disease. Here, the authors introduce CAT-S, a non-genetic method based on photocatalysis, enabling in situ deciphering of mitochondrial proteomes in primary cells from mouse tissues and human blood.
- Ziqi Liu
- , Fuhu Guo
- & Xinyuan Fan
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Article
| Open AccessUnderstanding the effect of spatially separated Cu and acid sites in zeolite catalysts on oxidation of methane
Methane is a potent greenhouse gas, and its removal is critical. Here, the authors demonstrate that spatially separated Cu and acid sites in Cu/zeolites influence product distribution and efficiency for methane oxidation.
- Peipei Xiao
- , Yong Wang
- & Toshiyuki Yokoi
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Article
| Open AccessCatalytic polymer self-cleavage for CO2 generation before combustion empowers materials with fire safety
Overcoming this challenge of fire hazards by carbon, hydrogen, and oxygen rich materials remains challenging. Here, the authors demonstarte that catalytic polymer auto-pyrolysis before combustion releases CO2, equipping the material with fire retardant properties.
- Wei Luo
- , Ming-Jun Chen
- & Hai-Bo Zhao
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Article
| Open AccessSingle [0001]-oriented zinc metal anode enables sustainable zinc batteries
The authors present a single [0001]-oriented Zn metal anode with high reversibility and demonstrate the significance of the Zn(0002) metal anode, characterized by a single crystalline orientation, for promoting ultra-sustainable homoepitaxial growth.
- Xiaotan Zhang
- , Jiangxu Li
- & Jiang Zhou
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Article
| Open AccessAnomalous anti-Kasha excited-state luminescence from symmetry-breaking heterogeneous carbon bisnanohoops
It is a long-standing scientific controversy to achieve anti-Kasha emissions by tuning structures at a molecular level. Herein, the authors constructed two symmetry-breaking heterogeneous carbon bisnanohoops with unusual anti-Kasha characteristics.
- Xinyu Zhang
- , Cheng Chen
- & Pingwu Du
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Article
| Open AccessEnantioselective total synthesis of (‒)-lucidumone enabled by tandem prins cyclization/cycloetherification sequence
The Ganoderma meroterpenoids are a growing class of natural products with a wide range of biological activities. Here, the authors report the enantioselective total synthesis of the Ganoderma meroterpenoid (‒)-lucidumone, featuring a copper-catalyzed enantioselective silicon-tethered intramolecular Diels-Alder cycloaddition to assemble the bicyclo[2.2.2]octane framework and a domino deprotection/Prins reaction/cycloetherification/oxidation sequence to generate concurrenly the tetrahydrofuran and the fused indanone skeleton.
- Xian-Zhang Liao
- , Ran Wang
- & Guang Li
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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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