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Article
| Open AccessConverting inorganic sulfur into degradable thermoplastics and adhesives by copolymerization with cyclic disulfides
The inherent instability of poly(sulfur) renders the conversion of elementary sulfur into sulfur-rich polymers challenging which limits the use of this industrial by-product. Here, the authors demonstrate that inorganic sulfur can be utilized by copolymerizing with cyclic disulfides, producing high-performance thermoplastic elastomers with self-healing ability and degradability.
- Yuanxin Deng
- , Zhengtie Huang
- & Da-Hui Qu
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Article
| Open AccessHigh yield electrosynthesis of oxygenates from CO using a relay Cu-Ag co-catalyst system
Using CO and H2O to electrosynthesize oxygenates is a possible low-carbon synthetic route. Here, the authors study the CO adsorption behavior on Ag catalysts and design a Cu-Ag nanostructure catalyst with a relay mechanism that enhances the electrosynthesis of oxygenates.
- Nannan Meng
- , Zhitan Wu
- & Kian Ping Loh
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Article
| Open AccessCellulose nanofiber-mediated manifold dynamic synergy enabling adhesive and photo-detachable hydrogel for self-powered E-skin
Certain devices require rapid adhesion and detachment, but achieving both can be challenging. Here, the authors report the development of a supramolecular hydrogel with reversible tough adhesion and triggered photodetachment.
- Lei Zhang
- , Lu Chen
- & Chaoji Chen
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Article
| Open AccessCapture of single Ag atoms through high-temperature-induced crystal plane reconstruction
Terminal hydroxyl groups on γ-Al2O3 surfaces serve as anchoring sites for Ag. Based on the surface energy of different crystal planes of γ-Al2O3 at various temperatures, the authors propose a high-temperature-induced crystal plane transformation method to construct terminal hydroxyl anchoring sites.
- Jiaxin Li
- , Kai Li
- & Hong He
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Article
| Open AccessProbing the activated complex of the F + NH3 reaction via a dipole-bound state
Experimental characterization of the transition state in chemical reactions is challenging due to its transient nature. Here, Zhang et al. observe quantum states near the activated complex region of the F + NH3 → HF + NH2 reaction via a dipole-bound state of the FNH3- anion formed upon photodetachment, which allows probing regions of reactive potential energy surfaces out of the Franck-Condon-active areas.
- Rui Zhang
- , Shuaiting Yan
- & Chuangang Ning
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Article
| Open AccessConstructing ordered and tunable extrinsic porosity in covalent organic frameworks via water-mediated soft-template strategy
The synthesis of covalent organic frameworks (COFs) by a soft-template methodology is challenging. Here, the authors attach the soft templates to the COFs backbone via ion bonds, avoiding crystallization incompatibilities and allowing subsequent removal of the template by ion exchange for enhanced U(VI)/Th(IV) adsorption performance.
- Ningning He
- , Yingdi Zou
- & Lijian Ma
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Article
| Open AccessEfficient recovery and recycling/upcycling of precious metals using hydrazide-functionalized star-shaped polymers
Despite the use of amine-functionalized polymers as metal adsorbents, they are generally ineffective at recovering precious metals. Here the authors prepare a star-shaped, hydrazide-functionalized polymer as a recoverable standalone adsorbent with high precious metal adsorption capability/selectivity and practical feasibility.
- Seung Su Shin
- , Youngkyun Jung
- & Jung-Hyun Lee
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Article
| Open AccessMulti-color dual wavelength vat photopolymerization 3D printing via spatially controlled acidity
Dual wavelength vat photopolymerization has emerged as a powerful approach to create multimaterial objects but require changing the resin during the printing process. Here, the authors develop a method of dual-wavelength 3D printing that can directly access multicolor parts without requiring changing of resin feedstocks or introduction of new materials during the printing process.
- Kyle C. H. Chin
- , Grant Ovsepyan
- & Andrew J. Boydston
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Article
| Open AccessOne pot conversion of phenols and anilines to aldehydes and ketones exploiting α gem boryl carbanions
For the carbonylation reactions to synthesize aldehyde, ester, amide, and other carbonyl derivatives, a transition metal-free and CO- free reaction was challenging but highly demanded. Here, the authors report a transition metal-free and CO- free method for deoxygenetive/denitrogenetive conversion of phenols and anilines to aldehydes and ketones.
- Kanak Kanti Das
- , Debasis Aich
- & Santanu Panda
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Article
| Open AccessElectrochemical C−H deuteration of pyridine derivatives with D2O
Despite the established C − H deuteration of pyridine derivatives synthetic methods with good D-incorporation, under milder conditions with easy operation procedures is still on the way. Here, the authors develop a straightforward, metal-free, and acid-/base-free electrochemical C4-selective C − H deuteration of pyridine derivatives with high selectivity and excellent D-incorporation at room temperature, which use D2O as economic and convenient D-source.
- Zhiwei Zhao
- , Ranran Zhang
- & Youai Qiu
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Article
| Open AccessIn-silico-assisted derivatization of triarylboranes for the catalytic reductive functionalization of aniline-derived amino acids and peptides with H2
Machine learning has not been strategically applied to design main-group catalysts. Here, the authors built an in-silico library of triarylboranes, which was used to identify reactive catalysts for functionalizing amino acids and peptides with H2.
- Yusei Hisata
- , Takashi Washio
- & Yoichi Hoshimoto
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Article
| Open AccessIntegrated optimization modelling framework for low-carbon and green regional transitions through resource-based industrial symbiosis
This study reports a quantitative tool for resource-based industries aimed at supporting sustainable, low-carbon regional transitions. The results provide optimal transition paths over traditional methods, highlighting the need for cleaner technology and industrial symbiosis.
- Xin Xie
- , Hang Fu
- & Shanying Hu
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Article
| Open AccessStarch-mediated colloidal chemistry for highly reversible zinc-based polyiodide redox flow batteries
The development of porous membranes that could work under high power density brings promise but a challenge with polyiodide cross-over for aqueous Zn-I flow batteries. Here, the authors develop a colloidal starch-based catholyte to inhibit cross-over that endows reversible flow cell performance.
- Zhiquan Wei
- , Zhaodong Huang
- & Chunyi Zhi
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Article
| Open AccessEnantioselective synthesis of chiral α,α-dialkyl indoles and related azoles by cobalt-catalyzed hydroalkylation and regioselectivity switch
Catalytic and enantioselective construction of chiral α,α-dialkyl indoles represents an important yet challenging objective to be developed. Herein the authors describe a cobalt catalyzed enantioselective anti-Markovnikov alkene hydroalkylation via the remote stereocontrol for the synthesis of α,α-dialkyl indoles and other N-heterocycles.
- Jiangtao Ren
- , Zheng Sun
- & Zhihui Shao
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Article
| Open AccessDecarboxylative stereoretentive C–N coupling by harnessing aminating reagent
Accessing chiral alkylamines is highly important due to their ubiquity in bioactive molecules. Here, the authors present the development of stereoretentive decarboxylative amidation of carboxylic acids using dioxazolone under ambient conditions.
- Jeonguk Kweon
- , Bumsu Park
- & Sukbok Chang
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Article
| Open AccessLow-index mesoscopic surface reconstructions of Au surfaces using Bayesian force fields
Metal surfaces have long been known to reconstruct, but key mechanistic aspects are poorly understood. Here, the authors use Bayesian force fields to gain insights into gold surface reconstructions that are crucial for material science and catalysis.
- Cameron J. Owen
- , Yu Xie
- & Boris Kozinsky
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Article
| Open AccessCarbon–nitrogen transmutation in polycyclic arenol skeletons to access N-heteroarenes
Developing skeletal editing tools, especially to realize the single-atom transmutation in a ring system without altering the ring size is challenging. Here, the authors introduce a skeletal editing strategy that enables polycyclic arenols to be readily converted into N-heteroarenes through carbon–nitrogen transmutation.
- Hong Lu
- , Yu Zhang
- & Hao Wei
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Article
| Open AccessCoordination cages integrated into swelling poly(ionic liquid)s for guest encapsulation and separation
The efficient encapsulation of guests by coordination cages in the solid state is prevented by their flexibility, dynamicity, and metal-ligand bond reversibility. Here, the authors report coordination cages integrated into poly(ionic liquid)s to control swelling and mechanical properties of the gels and develop efficient and regenerable supramolecular separation materials.
- Xiang Zhang
- , Dawei Zhang
- & Mingyuan He
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Article
| Open AccessThe role of memory-dependent friction and solvent viscosity in isomerization kinetics in viscogenic media
Molecular isomerization in solution is dependent on coupling of solute and solvent via memory-dependent friction. Here, by applying memory kernel extraction to molecular dynamics simulations, the authors demonstrate the role of friction in determining isomerization kinetics.
- Benjamin A. Dalton
- , Henrik Kiefer
- & Roland R. Netz
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Article
| Open AccessFacilitating the dry reforming of methane with interfacial synergistic catalysis in an Ir@CeO2−x catalyst
Dry reforming of methane is an attractive route to convert greenhouse gases into valuable syngas. Here, the authors demonstrate design strategy to prepare efficient catalysts towards activation of both C–H and C = O bonds and provide atomic-level insights into interfacial synergistic catalysis.
- Hui Wang
- , Guoqing Cui
- & Min Wei
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Article
| Open AccessGiant dielectric tunability in ferroelectric ceramics with ultralow loss by ion substitution design
The authors realize composite optimization in dielectric tunable materials by simultaneously achieving low electric field, large tunability, and low loss through ion substitution design in ferroelectric tunable materials.
- Ruitao Li
- , Diming Xu
- & Di Zhou
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Article
| Open AccessOzone as an environmental driver of influenza
Temperature and absolute humidity are associated with influenza activity, and recent data from Hong Kong have suggested ozone as an additional environmental driver. Here, the authors investigate the relationship between ozone and influenza transmission using surveillance data from the USA and find evidence for an inhibitory effect.
- Fang Guo
- , Pei Zhang
- & Linwei Tian
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Article
| Open AccessColor morphing surfaces with effective chemical shielding
Photochromic materials suffer from degradation when exposed to harsh chemical environments, but this can be overcome by providing chemical shielding via superomniphobicity. Here, the authors show the design rationale and careful materials selection for fabrication of color morphing surfaces that can simultaneously display excellent chemical resistance.
- Adil Majeed Rather
- , Sravanthi Vallabhuneni
- & Arun Kumar Kota
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Article
| Open AccessCell-penetrating protein-recognizing polymeric nanoparticles through dynamic covalent chemistry and double imprinting
Molecular recognition of proteins is essential for achieving their biological functions but it is challenging to prepare selective protein-binding materials. Here the authors report a method that combines dynamic covalent chemistry and double molecular imprinting to construct protein-recognizing nanoparticles capable of specific inhibition of protein–protein interactions.
- Avijit Ghosh
- , Mansi Sharma
- & Yan Zhao
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Article
| Open AccessPolymer hetero-electrolyte enabled solid-state 2.4-V Zn/Li hybrid batteries
Zn batteries suffer from low voltage due to the high redox potential of the Zn anode and the low potential of traditional cathodes. Here, the authors develop a polymer hetero-electrolyte, which allows separated Zn and Li reversibility and achieves a 2.4 V-Zn battery based on the LiNi0.5Mn1.5O4 cathode.
- Ze Chen
- , Tairan Wang
- & Chunyi Zhi
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Article
| Open AccessDinuclear gold-catalyzed divergent dechlorinative radical borylation of gem-dichloroalkanes
The widespread use of organoboronic acids has prompted the development of synthetic methodologies to meet the demands on structural diversity and functional group tolerance. Herein, the authors disclose a divergent radical dechloroborylation reaction enabled by dinuclear gold catalysis with visible light irradiation.
- Cheng-Long Ji
- , Hongliang Chen
- & Jin Xie
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Article
| Open AccessStereospecific syn-dihalogenations and regiodivergent syn-interhalogenation of alkenes via vicinal double electrophilic activation strategy
Restricted reaction mechanism of anti-dihalogenation of alkenes makes it challenging to alter the diastereochemical course into the complementary syn-dihalogenation process. Here, the authors report a conceptually distinctive strategy for the simultaneous double electrophilic activation of the two alkene carbons from the same side to realize syn-dihalogenation.
- Hyeon Moon
- , Jungi Jung
- & Won-jin Chung
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Article
| Open AccessSelective production of methylindan and tetralin with xylose or hemicellulose
Indan and tetralin are used as fuel additives and intermediates in the manufacture of many products, including thermal-stable jet fuel. Here the authors report a route for the synthesis of methylindan and tetralin by the hydrogenolysis of xylose or hemicellulose over a non-noble metal catalyst, followed by further reaction over zeolite H-ZSM-5. Reviewer recognition:
- Zhufan Zou
- , Zhenjie Yu
- & Ning Li
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Article
| Open AccessCreep-type all-solid-state cathode achieving long life
Electrochemical-mechanical issues bring challenges but create new opportunities to design innovative all-solid-state batteries. Here, the authors propose to use the (de)lithiation-stress-creep synergistic time-dependent evolution to boost the electrochemical performance of all-solid-state batteries.
- Xiaolin Xiong
- , Ting Lin
- & Liumin Suo
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Article
| Open AccessDelayed room temperature phosphorescence enabled by phosphines
Room-temperature phosphorescence usually occurs immediately after the removal of excitation. Here the authors achieve combined instant and delayed phosphorescence through introduction of phosphines into carbazole emitters.
- Guang Lu
- , Jing Tan
- & Hui Xu
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Article
| Open AccessDiastereo-divergent synthesis of chiral hindered ethers via a synergistic calcium(II)/gold(I) catalyzed cascade hydration/1,4-addition reaction
Developing an efficient method for the stereocontrolled synthesis of all stereoisomers of chiral hindered ethers is highly desirable but challenging. Here, the authors report an asymmetric cascade reaction catalyzed by a bimetallic catalytic system with control over the configuration of the stereocenters of tetra-aryl substituted ethers.
- Xiangfeng Lin
- , Xia Mu
- & Can Li
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Article
| Open AccessA human-machine interface for automatic exploration of chemical reaction networks
Automated reaction exploration is the key to systematic elucidation of chemical mechanisms. Here, the authors introduce a generally applicable algorithm to steer an automated exploration towards region of interest in chemical reaction space.
- Miguel Steiner
- & Markus Reiher
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Article
| Open AccessThe role of charge in microdroplet redox chemistry
Redox reactions exhibit different thermodynamics and kinetics in water microdroplets compared to the bulk. Here, the authors use reactive molecular dynamics to show the importance of charged reactive species in explaining reactivity under confinement.
- Joseph P. Heindel
- , R. Allen LaCour
- & Teresa Head-Gordon
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Article
| Open AccessBoosting organic phosphorescence in adaptive host-guest materials by hyperconjugation
Room-temperature phosphorescence is usually inefficient in purely organic material. Here, the authors achieve near-unity phosphorescence efficiency with color tunability in adaptive host-guest materials through use of hyperconjugation.
- Huili Ma
- , Lishun Fu
- & Wei Huang
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Article
| Open AccessSwitchable chemoselective aryne reactions between nucleophiles and pericyclic reaction partners using either 3-methoxybenzyne or 3-silylbenzyne
Due to the electrophilic nature of arynes, it is very challenging to control chemoselectivity, when substrates possess multiple competing reaction sites. Here, the authors demonstrate that chemoselective control between two major types of benzyne transformation is accomplished by varying the 3-substituent on aryne intermediate.
- Hongcheng Tan
- , Shuxin Yu
- & Yang Li
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Article
| Open AccessIsostructural doping for organic persistent mechanoluminescence
Organic mechanoluminescent materials have potential in a range of applications, but it can be challenging to achieve long-lived emission. Here, the authors report isostructural doping as a strategy to achieve multicolour and high efficiency organic mechanoluminescence, applied in stress sensing.
- Zongliang Xie
- , Yufeng Xue
- & Bin Liu
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Article
| Open AccessNoncovalent synthesis of homo and hetero-architectures of supramolecular polymers via secondary nucleation
Synthesis of supramolecular polymers with controlled architecture is desirable but challenging. Here, the authors use a secondary nucleation event to prepare a range of supramolecular polymer architectures.
- Srinu Kotha
- , Rahul Sahu
- & Kotagiri Venkata Rao
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Article
| Open AccessIn situ enzymatic control of colloidal phoresis and catalysis through hydrolysis of ATP
The design of synthetic systems that can sense chemical gradients and respond with directional motility and chemical activity is of interest. Here, the authors realize and control such behaviors in a synthetic system by tailoring multivalent interactions of adenosine nucleotides with catalytic microbeads.
- Ekta Shandilya
- , Bhargav Rallabandi
- & Subhabrata Maiti
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Article
| Open AccessCatalytic 1,1-diazidation of alkenes
Compared to well-developed catalytic 1,2-diazidation of alkenes, the corresponding catalytic 1,1-diazidation of alkenes has not been realized. Here, the authors report an efficient approach for catalytic 1,1-diazidation of alkenes by redox-active selenium catalysis.
- Wangzhen Qiu
- , Lihao Liao
- & Xiaodan Zhao
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Article
| Open AccessNucleoside Phosphorylases make N7-xanthosine
Nucleoside-processing enzymes exhibit strict regioselectivity for glycosylation of purine nucleobases at N9. Here, the authors report an exception and show that wild type nucleoside phosphorylases also furnish N7-xanthosine, a non-native ribosylation regioisomer of xanthosine.
- Sarah Westarp
- , Felix Brandt
- & Felix Kaspar
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Article
| Open AccessAllotrope-dependent activity-stability relationships of molybdenum sulfide hydrogen evolution electrocatalysts
The stability of non-noble catalysts is key for their use in proton exchange membrane water electrolysers. Here, authors study activity-stability relationships of MoSx allotropes for H2 production, reporting allotrope-dependent stabilities and dissolution pathways, and propose operation guidelines.
- Daniel Escalera-López
- , Christian Iffelsberger
- & Serhiy Cherevko
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Article
| Open AccessSpatial decoupling of bromide-mediated process boosts propylene oxide electrosynthesis
The practical application of electrosynthesis of propylene oxide is hindered by limited performance. Here, the authors report a spatial decoupling strategy by utilizing the bromide mediator to link propylene and anode within separated reactors, realizing high-performance electrosynthesis of propylene oxide.
- Mingfang Chi
- , Jingwen Ke
- & Jie Zeng
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Article
| Open AccessHighly efficient in crystallo energy transduction of light to work
Crystals are known to have a range of responses to light, but multiple responses in the same material are rare. Here, the authors report different mechanical effects in response to light across three polymorphs as a result of a dimerization reaction.
- Jiawei Lin
- , Jianmin Zhou
- & Junbo Gong
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Article
| Open AccessAll-natural 2D nanofluidics as highly-efficient osmotic energy generators
Researchers report a sustainable nanofluidic osmotic energy harvester made from natural montmorillonite clay nanosheets and recycled cellulose. Scaled-up films of 700 cm2 show power output of 8 W m−2 with stability over 30 days
- Jiadong Tang
- , Yun Wang
- & Tieyong Zuo
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Article
| Open AccessMolecular tuning boosts asymmetric C-C coupling for CO conversion to acetate
This work presents a general surface molecular tuning strategy to promote the electrochemical reduction of CO.
- Jie Ding
- , Fuhua Li
- & Bin Liu
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Article
| Open AccessSelf-condensation-assisted chemical vapour deposition growth of atomically two-dimensional MOF single-crystals
2D MOFs have a variety of applications, including molecular separation and atomically thin electronics. Here authors demonstrate the preparation of monolayer and few-layer MOF single-crystals using a self-condensation-assisted CVD method.
- Lingxin Luo
- , Lingxiang Hou
- & Jian Zheng
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Article
| Open AccessEfficient tandem electroreduction of nitrate into ammonia through coupling Cu single atoms with adjacent Co3O4
An optimal catalyst for nitrate electroreduction should satisfy the simultaneously optimized adsorption of intermediates. Here, the authors report a tandem electrocatalyst by combining Cu single atoms with Co3O4 nanosheets, enhancing the binding with NO2−, thus promoting nitrate electroreduction to NH3.
- Yan Liu
- , Jie Wei
- & Jie Zeng
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Article
| Open AccessTimescale correlation of shallow trap states increases electrochemiluminescence efficiency in carbon nitrides
Differences in timescales of electron transfer reactions limit the efficiency of electrochemiluminescence. Here, the authors coordinate the timescales using shallow trap states in carbon nitride to achieve high efficiencies applied in nitrite sensing.
- Yanfeng Fang
- , Hong Yang
- & Yuanjian Zhang
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Article
| Open AccessPlasma-assisted manipulation of vanadia nanoclusters for efficient selective catalytic reduction of NOx
Achieving supported nanoclusters with unique geometric and electronic structures continues to pose a challenge. Here, the authors introduce a plasma-assisted treatment approach for generating supported metal oxide nanoclusters, facilitated by the rapid transformation of monomeric dispersed metal oxides.
- Yong Yin
- , Bingcheng Luo
- & Xiang Li
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