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| Open AccessEffect of current density on the solid electrolyte interphase formation at the lithium∣Li6PS5Cl interface
The interface between the Li metal electrode and inorganic solid electrolyte is crucial for developing reliable all-solid-state Li batteries. Here, the authors show that the Li plating current density distinctly affects the chemistry and morphology of interphase components formed at the interface.
- Sudarshan Narayanan
- , Ulderico Ulissi
- & Mauro Pasta
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Article
| Open AccessBreaking through water-splitting bottlenecks over carbon nitride with fluorination
Graphitic carbon nitride has long been considered a poor oxygen evolution catalyst. Here, the authors report a simple fluorination strategy to prevent the accumulation of inert C=O on carbon nitride to break through this bottleneck.
- Ji Wu
- , Zhonghuan Liu
- & Yongsheng Yan
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Article
| Open AccessJanus regulation of ice growth by hyperbranched polyglycerols generating dynamic hydrogen bonding
Regulation of ice growth and ice growth inhibition are critical and different materials mimicking anti freeze proteins or ice binding surfaces have been developed. Here, the authors combine both concepts in a hyperbranched polyglycerols to change the ice growth activity.
- Sang Yup Lee
- , Minseong Kim
- & Dong June Ahn
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| Open AccessPhotodimerization induced hierarchical and asymmetric iontronic micropatterns
Hierarchical surface micro/nanopatterns enable iontronic materials to show performance enhancement in piezoionic mechanoreception and skin-interfaced coupling electrode adhesion. Here, the author proposes a facile and robust method to fabricate hierarchical and asymmetrical iontronic micropatterns through programmed regulation of the internal stress distribution and local ionic migration.
- Zehong Wang
- , Tiantian Li
- & Xuesong Jiang
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Article
| Open AccessSelective activation of four quasi-equivalent C–H bonds yields N-doped graphene nanoribbons with partial corannulene motifs
Selective activation of C–H bonds is a key challenge in organic reactions. Here, the authors achieve the selective activation of four quasi-equivalent C–H bonds, leading to the formation of N-doped graphene nanoribbons with partial corannulene motifs.
- Yixuan Gao
- , Li Huang
- & Hong-Jun Gao
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| Open AccessRevealing solid electrolyte interphase formation through interface-sensitive Operando X-ray absorption spectroscopy
Solid electrolyte interphase (SEI) formation on Li-ion battery anodes is critical for long-term performance. Here, the authors use operando soft X-ray absorption spectroscopy in total electron yield mode to resolve the chemical evolution of the SEI during electrochemical formation on silicon anodes.
- Jack E. N. Swallow
- , Michael W. Fraser
- & Robert S. Weatherup
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Article
| Open AccessThe Donnan potential revealed
Donnan electrical potential is widely adopted to describe ion distribution between two solutions separated by a permeable membrane with implications for many chemical and biological systems. Aydogan Gokturk et al. directly measures this potential for the first time and compare the data with theoretical models.
- Pinar Aydogan Gokturk
- , Rahul Sujanani
- & Ethan J. Crumlin
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| Open AccessEvolution of Br⋯Br contacts in enantioselective molecular recognition during chiral 2D crystallization
Halogen-mediated interactions control molecular recognition in many chemical and biological systems. Here, the authors demonstrate two types of Br⋯Br contacts and their importance in chiral on-surface crystallization.
- Zhen-Yu Yi
- , Xue-Qing Yang
- & Li-Jun Wan
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Article
| Open AccessAdsorbate chemical environment-based machine learning framework for heterogeneous catalysis
A combination of electronic structure calculations and machine learning strategies is developed to predict structures of complex heterogeneous catalysts in realistic environments, yielding new opportunities for optimization for energy applications.
- Pushkar G. Ghanekar
- , Siddharth Deshpande
- & Jeffrey Greeley
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| Open AccessRole of chemisorbing species in growth at liquid metal-electrolyte interfaces revealed by in situ X-ray scattering
Growth at liquid-liquid interfaces differ inherently from that on solids, making it attractive for nanomaterial formation. Here, the authors use X-ray scattering to derive a detailed microscopic picture of lead-halide growth on liquid mercury that reveals the key importance of anion adsorption.
- Andrea Sartori
- , Rajendra P. Giri
- & Olaf M. Magnussen
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| Open AccessUnconventional interfacial water structure of highly concentrated aqueous electrolytes at negative electrode polarizations
Water-in-salt electrolytes can be useful for future electrochemical energy storage systems. Here, the authors investigate the potential-dependent double-layer structures at the interface between a gold electrode and a highly concentrated aqueous electrolyte solution via in situ Raman measurements.
- Chao-Yu Li
- , Ming Chen
- & Tianquan Lian
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Article
| Open AccessSelf-sorting in macroscopic supramolecular self-assembly via additive effects of capillary and magnetic forces
The selective assembly of μm-to-mm sized components is challenging because of the short-ranged molecular recognition. Here, the authors demonstrate a self-sorting mechanism to automatically identify the surface chemistry via additivity and competence between long-ranged magnetic/capillary forces.
- Minghui Tan
- , Pan Tian
- & Feng Shi
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Article
| Open AccessElectron-mediated control of nanoporosity for targeted molecular separation in carbon membranes
Controlled molecular separation by membranes requires 2D materials with precise structures to achieve the desired selectivity. Here authors demonstrate precise selectivity tuning in carbon membranes using electron irradiation.
- Banseok Oh
- , Hyeokjun Seo
- & Dong-Yeun Koh
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Article
| Open AccessThree-dimensional nanoframes with dual rims as nanoprobes for biosensing
Most SERS-active nanostructures suffer from low robustness against misalignment to field polarization. Here, the authors demonstrate three-dimensional nanoframes of octahedral geometry, with two rims engraved on each facet, as polarization-independent SERS nanoprobes.
- Hajir Hilal
- , Qiang Zhao
- & Sungho Park
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| Open AccessElectrically switched underwater capillary adhesion
Wang et al. report an underwater capillary adhesive that is strengthened by the conjunction of inner water bridge and outer air shell, and switched timely by a small direct current voltage. The design can also be constructed on flexible tapes, which can be applied to non-conductive substrates.
- Huanxi Zheng
- , Jing Li
- & Zuankai Wang
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Article
| Open AccessCompeting electronic states emerging on polar surfaces
Defect-free surfaces with excess charge are typically described as a homogeneous 2D electron gas. Here, in contrast, the authors find that the KTaO3(001) surface hosts a charge density wave coexisting with a pattern of electron polarons, highly localized states of excess electrons bound to a lattice distortion.
- Michele Reticcioli
- , Zhichang Wang
- & Cesare Franchini
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| Open AccessNanoparticle elasticity affects systemic circulation lifetime by modulating adsorption of apolipoprotein A-I in corona formation
Nanoparticle elasticity is known to affect physiological fate but how this occurs is largely unknown. Here, the authors report on a study using nanoparticles differing in elasticity alone to show a difference in the protein corona, in particular apolipoprotein A-1 absorption, corresponds to differences in circulation time.
- Mingyang Li
- , Xinyang Jin
- & Lihua Yang
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Article
| Open AccessMagnetic molecules as local sensors of topological hysteresis of superconductors
Magnetic molecules have long been seen to hold promise in magnetic sensing applications. In this paper, Serrano et al show that a single layer of a magnetic molecule, a terbium based complex, is sensitive to the local magnetic field variation of a superconducting surface on which it is deposited.
- Giulia Serrano
- , Lorenzo Poggini
- & Roberta Sessoli
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| Open AccessEnhancement of electrocatalytic oxygen evolution by chiral molecular functionalization of hybrid 2D electrodes
While solar-to-fuel catalysis requires the careful transfer of electrons, there are still challenges understanding how electron spin contributes to reactivity. Here, authors employ chiral fused thiadiazole-helicenes to control spin polarization in oxygen evolution electrocatalysts.
- Yunchang Liang
- , Karla Banjac
- & Magalí Lingenfelder
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| Open AccessSpontaneous water-on-water spreading of polyelectrolyte membranes inspired by skin formation
Stable interfaces between immiscible solvents are crucial for chemical synthesis and assembly, but interfaces between miscible solvents have been less explored. Here the authors report the spontaneous water-on-water spreading and self-assembly of polyelectrolytes.
- Sihan Tang
- , Jiang Gong
- & Qiang Zhao
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| Open AccessA confined-etching strategy for intrinsic anisotropic surface wetting patterning
Anisotropic functional patterned surfaces have shown significant applications in microfluidics, biomedicine, and optoelectronics. Here, authors demonstrate a fast and mask-free etching method for accurate surface patterning by confined decomposition, enabling the efficient fabrication of complex patterns.
- Rui Feng
- , Fei Song
- & Yu-Zhong Wang
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Article
| Open AccessPeriodic corner holes on the Si(111)-7×7 surface can trap silver atoms
Positioning and trapping single atoms at specific sites of surfaces is a challenging goal that can advance the development of single atom devices. Here the authors demonstrate that single Ag atoms are trapped inside corner holes of the Si(111)-7×7 surface for more than 4 days at room temperature, and suggest that this behavior may be shared by other elements.
- Jacek R. Osiecki
- , Shozo Suto
- & Arunabhiram Chutia
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| Open AccessUnderstanding the complementarities of surface-enhanced infrared and Raman spectroscopies in CO adsorption and electrochemical reduction
Infrared and Raman spectroscopies are often assumed to provide similar insights into heterogeneous reaction mechanisms. This study shows that these techniques provide similar data when CO is strongly bound to a surface, yet distinct subpopulations of CO are probed when binding is weaker.
- Xiaoxia Chang
- , Sudarshan Vijay
- & Bingjun Xu
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| Open AccessAtomic overlayer of permeable microporous cuprous oxide on palladium promotes hydrogenation catalysis
It remains a challenge to fabricate metal catalysts with interfacial active sites distributed on the whole two-dimensional (2D) surface of metal nanoparticles. Here the authors demonstrate that the overgrowth of atomic-thick porous Cu2O on Pd readily creates an unprecedented 2D catalytically active metal-support interface with significantly enhanced catalysis toward the semi-hydrogenation of alkynes.
- Kunlong Liu
- , Lizhi Jiang
- & Nanfeng Zheng
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| Open AccessStopping molecular rotation using coherent ultra-low-energy magnetic manipulations
Manipulating the rotational motions of molecules may provide a tool for controlling chemical processes. Here the authors demonstrate that the rotation of a D2 molecule can be stopped, upon collision with a metal surface, by a magnetic field that affects the rotational levels to a much smaller extent than the energy difference upon de-excitation.
- Helen Chadwick
- , Mark F. Somers
- & Gil Alexandrowicz
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| Open Access3D nanoprinting via spatially controlled assembly and polymerization
Additive manufacturing methods at the macroscale have seen significant advances in recent times, but advances for the bottom-up formation of nanoscale polymeric features are yet to be realized. Here, the authors demonstrate that rapid crosslinking of an AFM delivered norbornene crosslinker in presence of a surface-tethered metathesis catalysts facilitates the curing of delivered material in an extremely rapid fashion
- Thomas G. Pattison
- , Shuo Wang
- & Greg G. Qiao
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Article
| Open AccessHost-guest liquid gating mechanism with specific recognition interface behavior for universal quantitative chemical detection
In field, visual, chemical detection is of use for a wide range of possible applications. Here, the authors report on the creation of a host-guest liquid gating mechanism where detection of the target host triggers gate opening allowing for gas through the liquid gate, which can be used for visual detection.
- Huimeng Wang
- , Yi Fan
- & Xu Hou
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| Open AccessChemically identifying single adatoms with single-bond sensitivity during oxidation reactions of borophene
Here, the authors report the use of ultrahigh vacuum tip-enhanced Raman spectroscopy to characterize the oxidation processes of monolayer borophene with atomic-scale resolution and single-bond sensitivity, demonstrating the potential of the technique for probing the local chemistry of surface adsorbates on low-dimensional materials.
- Linfei Li
- , Jeremy F. Schultz
- & Nan Jiang
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| Open AccessOn-surface synthesis of triangulene trimers via dehydration reaction
Preparing triangulene-based high spin structures is of interest for molecular spintronics. Here, the authors generate high spin triangulene trimers on Au(111) via a surface-assisted dehydration reaction.
- Suqin Cheng
- , Zhijie Xue
- & Ping Yu
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Article
| Open AccessCatalyst-controlled functionalization of carboxylic acids by electrooxidation of self-assembled carboxyl monolayers
This work leverages substrate self-assembly at an electrode to promote selective substrate electrooxidation in the presence of oxidatively sensitive catalysts. This strategy is applied to decarboxylative coupling of carboxylic acids with olefins.
- Heather A. Hintz
- & Christo S. Sevov
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Article
| Open AccessProtruding Pt single-sites on hexagonal ZnIn2S4 to accelerate photocatalytic hydrogen evolution
An alternative approach to defect-trapped Pt single-sites on a semiconductor is reported. Here, protruding Pt sites inhibit charge recombination and cause a tip effect which enhances H2 evolution yield rates with minimal co-catalyst loading.
- Xiaowei Shi
- , Chao Dai
- & Mingshan Zhu
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| Open AccessIdentification of CO2 adsorption sites on MgO nanosheets by solid-state nuclear magnetic resonance spectroscopy
The characterization of the surface structure and binding sites of materials is crucial for designing advanced materials for adsorption processes. Here, the authors use 17O solid-state nuclear magnetic resonance spectroscopy to identify specific CO2 adsorption sites on MgO nanosheets.
- Jia-Huan Du
- , Lu Chen
- & Luming Peng
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Article
| Open AccessOn-surface synthesis and characterization of nitrogen-substituted undecacenes
Heteroatom substitution in larger acenes represents a fundamental step towards precise engineering of the remarkable electronic properties of the acene family. Here, the authors present an on-surface synthesis strategy and detailed characterization for three undecacene analogs substituted with four nitrogen atoms.
- Kristjan Eimre
- , José I. Urgel
- & Carlo A. Pignedoli
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Article
| Open AccessNanobubbles explain the large slip observed on lubricant-infused surfaces
Why are lubricant-infused surfaces so effective at reducing drag in microfluidic flow? Here, authors reveal that infused nanostructured Teflon wrinkles induce large interfacial slip due to the spontaneous nucleation of surface nanobubbles, a mechanism likely to occur on most rough infused surfaces.
- Christopher Vega-Sánchez
- , Sam Peppou-Chapman
- & Chiara Neto
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| Open AccessCan electric fields drive chemistry for an aqueous microdroplet?
Theoretical studies of the air-water interface of a water droplet show a wide distribution of strong electric fields at the surface that can make or break chemical bonds to accelerate chemical reactions over the bulk water phase.
- Hongxia Hao
- , Itai Leven
- & Teresa Head-Gordon
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| Open AccessResolving sub-angstrom ambient motion through reconstruction from vibrational spectra
Tracking single molecule movements is a challenging task, but highly desired for applications and fundamental studies. Here the authors reconstruct the sub-angstrom relative movements of a molecule interacting with a metal adatom, by measuring its vibrational spectrum in a self-assembled monolayer, continuously modified by the adatom in a nanoparticle-on-mirror construct.
- Jack Griffiths
- , Tamás Földes
- & Jeremy J. Baumberg
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| Open AccessCoexisting multi-states in catalytic hydrogen oxidation on rhodium
Catalytic reactions may exhibit oscillations in the reaction rate even at constant external parameters. Here, the authors observe and explain the coexistence of such oscillations and the steady states of catalytic activity in H2 oxidation on differently structured grains of a polycrystalline Rh foil.
- P. Winkler
- , J. Zeininger
- & G. Rupprechter
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| Open AccessRapid oxygen exchange between hematite and water vapor
Knowing how individual water molecules interact with surfaces is crucial for understanding surface and interface phenomena. Here, the authors show how local water-water interactions enable an unforeseen and surprisingly rapid mechanism of atom exchange between a common mineral and its surroundings.
- Zdenek Jakub
- , Matthias Meier
- & Gareth S. Parkinson
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Article
| Open AccessUltra-thin self-healing vitrimer coatings for durable hydrophobicity
By now a plethora of ultrathin hydrophobic coatings are available but their durability are not well developed. Here, the authors present a thin, durable and fluorine-free PDMS-based vitrimer coating that implements many desirable aspects like energy efficiency, durability and sustainability.
- Jingcheng Ma
- , Laura E. Porath
- & Christopher M. Evans
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Article
| Open AccessFlat epitaxial quasi-1D phosphorene chains
Similarly to graphene, attempts to fabricate phosphorene by epitaxy or starting from a few layers of bulk black phosphorus have failed so far. Here, the authors present a controllable bottom-up approach to grow atomically thin, crystalline 1D flat phosphorus chains on a Ag(111) substrate.
- Wei Zhang
- , Hanna Enriquez
- & Hamid Oughaddou
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Article
| Open AccessNanoscale cooperative adsorption for materials control
Adsorption is a fundamentally important process but challenging to quantify, especially at the nanoscale. Here, the authors map the adsorption affinity and cooperativity of various ligands on single gold nanoparticles and discover adsorption crossover behaviors between different facets, leading to a strategy to control particle shape.
- Rong Ye
- , Ming Zhao
- & Peng Chen
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Article
| Open AccessLiquid flow reversibly creates a macroscopic surface charge gradient
Reactions at the interface between mineral surfaces and flowing liquids are ubiquitous in nature. Here the authors explore, using surface-specific sum frequency generation spectroscopy and numeric calculations, how the liquid flow affects the charging and dissolution rates leading to flow-dependent charge gradients along the surface.
- Patrick Ober
- , Willem Q. Boon
- & Mischa Bonn
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Article
| Open AccessSelf-assembly of N-heterocyclic carbenes on Au(111)
Although N-heterocyclic carbenes (NHCs) are a promising class of ligands for forming robust self-assembled monolayers on metals, many questions remain about their behavior on surfaces. Here, the authors address these fundamental questions—such as the factors controlling NHC orientation, mobility, and ability to self-assemble—through an in-depth examination of NHC overlayers on Au(111).
- Alex Inayeh
- , Ryan R. K. Groome
- & Alastair B. McLean
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Article
| Open AccessMotion of water monomers reveals a kinetic barrier to ice nucleation on graphene
The dynamics of water molecules at interfaces controls natural and artificial processes, but experimental investigations have been challenging. Here the authors investigate water molecules on a graphene surface using helium spin-echo spectroscopy, and reveal a regime where freely mobile molecules undergo strong repulsive mutual interactions which inhibit ice nucleation.
- Anton Tamtögl
- , Emanuel Bahn
- & William Allison
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Article
| Open AccessOn-surface preparation of coordinated lanthanide-transition-metal clusters
The preparation of lanthanide-transition metal clusters containing multiple lanthanide atoms remains challenging. Here, the authors present the controlled on-surface formation of ligand-stabilized heterometallic Ce/Au clusters containing two, three and four Ce atoms bridged by Au adatoms.
- Jing Liu
- , Jie Li
- & Yongfeng Wang
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Article
| Open AccessIn situ identification of the metallic state of Ag nanoclusters in oxidative dispersion
Designing ultra small metal nanoclusters or single atoms with metallic state is a challenge. Here, the authors demonstrate the stabilization of ultra small silver clusters in the nearly-metallic state by oxygen adsorption at high temperature, using in situ spectroscopy and microscope technologies.
- Rongtan Li
- , Xiaoyan Xu
- & Xinhe Bao
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Article
| Open AccessProbing intramolecular vibronic coupling through vibronic-state imaging
Vibronic coupling is a key feature of molecular electronic transitions, but its visualization in real space is an experimental challenge. Here the authors, using scanning tunneling microscopy induced luminescence, resolve the effect of vibronic coupling with different modes on the electron distributions in real space in a single pentacene molecule.
- Fan-Fang Kong
- , Xiao-Jun Tian
- & J. G. Hou
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Article
| Open AccessIce-nucleating proteins are activated by low temperatures to control the structure of interfacial water
Ice-nucleating proteins promote ice formation at high sub-zero temperatures, but the mechanism is still unclear. The authors investigate a model ice-nucleating protein at the air-water interface using vibrational sum frequency generation spectroscopy and simulations, revealing its reorientation at low temperatures, which increases contact with water molecules and promotes their ordering.
- Steven J. Roeters
- , Thaddeus W. Golbek
- & Tobias Weidner
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Article
| Open AccessBulk tungsten-substituted vanadium oxide for low-temperature NOx removal in the presence of water
NH3 selective catalytic reduction is an important technique for NOx removal but water vapor critically inhibits the reaction at a low temperature. Here the authors show bulk W-substituted VOx exhibits higher NOx removal ability than the TiO2 supported vanadia catalyst in the presence of water.
- Yusuke Inomata
- , Hiroe Kubota
- & Toru Murayama