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| Open AccessA cost-effective and humidity-tolerant chloride solid electrolyte for lithium batteries
Stable inorganic solid electrolytes are instrumental in developing high-voltage Li metal batteries. Here, the authors present the synthesis and electrochemical energy storage properties of a cost-effective and humidity-tolerant chloride solid electrolyte.
- Kai Wang
- , Qingyong Ren
- & Cheng Ma
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Article
| Open AccessEvanescent waves modulate energy efficiency of photocatalysis within TiO2 coated optical fibers illuminated using LEDs
Coupling photocatalyst-coated optical fibers (P-OFs) with LEDs shows potential in environmental applications. Here the authors report a strategy to maximize P-OF light usage and simultaneously establish a new platform to quantify photocatalytic performance.
- Yinghao Song
- , Li Ling
- & Chii Shang
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Article
| Open AccessTransforming biorefinery designs with ‘Plug-In Processes of Lignin’ to enable economic waste valorization
The current biorefineries yield lignin with inadequate fractionation for bioconversion, yet substantial changes of these biorefinery designs could jeopardize carbohydrate efficiency and increase capital costs. Here the authors resolve the dilemma by designing ‘plug-in processes of lignin’ to enable economic waste valorization.
- Zhi-Hua Liu
- , Naijia Hao
- & Joshua S. Yuan
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Article
| Open AccessA robotic prebiotic chemist probes long term reactions of complexifying mixtures
The transition of prebiotic chemistry to present-day chemistry lasted a very long period of time, but the current laboratory investigations of this process are mostly limited to a couple of days. Here, the authors develop a fully automated robotic prebiotic chemist designed for long-term chemical experiments exploring unconstrained multicomponent reactions, which can run autonomously and uses simple chemical inputs.
- Silke Asche
- , Geoffrey J. T. Cooper
- & Leroy Cronin
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| Open AccessNon-associative phase separation in an evaporating droplet as a model for prebiotic compartmentalization
Prebiotic compartmentalization could prove essential for the evolution of life. Guo et al. show that liquid-liquid separation in an aqueous two-phase system driven by evaporation may already suffice to facilitate chemical processes required for the RNA world hypothesis.
- Wei Guo
- , Andrew B. Kinghorn
- & Ho Cheung Shum
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Article
| Open AccessRegulating coordination number in atomically dispersed Pt species on defect-rich graphene for n-butane dehydrogenation reaction
Direct dehydrogenation has been a thematic research area resulting from the energy shortage and petroleum gas upgrading scenario. Here, the authors fabricate fully exposed Pt3 clusters and correlate dehydrogenation activity with average coordination number of Pt-Pt bond.
- Xiaowen Chen
- , Mi Peng
- & Ding Ma
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Article
| Open AccessUltra-strong polymeric hollow fiber membranes for saline dewatering and desalination
Osmotically assisted reverse osmosis can overcome limitations of the reverse osmosis process but a strong membrane which can withstand a high hydraulic pressure is crucial. Here, the authors develop strong polymer thin film composite hollow fiber membranes with exceptionally high hydraulic burst pressures of up to 110 bar, while maintaining high water permeance and salt rejection.
- Can Zeng Liang
- , Mohammad Askari
- & Tai-Shung Chung
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Article
| Open AccessOlefin oligomerization by main group Ga3+ and Zn2+ single site catalysts on SiO2
Silica-supported, single site, main group Zn(II) and Ga(III) ions catalyze ethylene and propylene oligomerization. Here, experimental and theoretical evidence suggests a Cossee-Arlman reaction mechanism similar to that for transition metal catalysts.
- Nicole J. LiBretto
- , Yinan Xu
- & Jeffrey T. Miller
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Article
| Open AccessGallium nitride catalyzed the direct hydrogenation of carbon dioxide to dimethyl ether as primary product
The conversion of CO2 to valuable chemicals is still challenged by catalyst developments. Herein, the authors found that GaN is an efficient catalyst for selective CO2 hydrogenation to dimethyl ether as the primary product, in contrast to the traditional methanol-intermediate route over hybrid catalysts.
- Chang Liu
- , Jincan Kang
- & Zhong-Wen Liu
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Article
| Open AccessRaw biomass electroreforming coupled to green hydrogen generation
The scale-up of the coupling of water electroreduction (HER) with organic electrooxidation remains challenging. Here the authors address this challenge by coupling HER with electrooxidation of raw biomass chitin, cogenerating acetate and green hydrogen safely at high current density.
- Hu Zhao
- , Dan Lu
- & Hong Li
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Article
| Open AccessNanostructure of nickel-promoted indium oxide catalysts drives selectivity in CO2 hydrogenation
Palladium-promoted indium oxide is a catalyst with potential to realize the large-scale conversion of CO2 into the commodity methanol. This work focuses on the low-cost nickel as an alternative appealing promoter, revealing the atomic-level catalyst design unlocking maximal selectivity and activity.
- Matthias S. Frei
- , Cecilia Mondelli
- & Javier Pérez-Ramírez
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Article
| Open AccessElectrochemical reduction of acetonitrile to ethylamine
Industrial synthesis of primary amine often features poor selectivity because of the formation of secondary and tertiary amine byproducts. Here, the authors report an electrocatalytic route to ethylamine through selective electroreduction of acetonitrile at ambient temperature and pressure.
- Rong Xia
- , Dong Tian
- & Feng Jiao
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Article
| Open AccessEnhancing stability by trapping palladium inside N-heterocyclic carbene-functionalized hypercrosslinked polymers for heterogeneous C-C bond formations
Catalyst deactivation caused by the aggregation of active metal species poses great challenges for supported metal catalyzed solid-liquid reactions. Here, the authors develop a hypercrosslinked polymer integrated with N-heterocyclic carbene (NHC) as bifunctional support to stabilize palladium in heterogeneous C-C bond formations.
- Chengtao Yue
- , Qi Xing
- & Fuwei Li
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Article
| Open AccessDirecting reaction pathways via in situ control of active site geometries in PdAu single-atom alloy catalysts
Single-atom alloys are promising catalysts for a number of different reactions. Here, the authors demonstrate that carbon monoxide can be used to transition a PdAu catalyst between a single atom and a cluster phase which exhibit distinct selectivities for ethanol dehydrogenation.
- Mengyao Ouyang
- , Konstantinos G. Papanikolaou
- & E. Charles H. Sykes
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Article
| Open AccessExploring the roles of roughness, friction and adhesion in discontinuous shear thickening by means of thermo-responsive particles
Understanding shear thickening in colloidal suspensions is of great practical importance. Hsu et al. create responsive polymer-coated silica particles whose rheology can be tuned in situ, following modifications of their tribology, which is separately characterized at the single-colloid level.
- Chiao-Peng Hsu
- , Joydeb Mandal
- & Lucio Isa
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Article
| Open AccessA tailored multi-functional catalyst for ultra-efficient styrene production under a cyclic redox scheme
Styrene is an important commodity chemical that is highly energy and CO2 intensive to produce. Here, authors report a redox-oxidative dehydrogenation scheme and a tailored core-shell redox catalyst to convert ethylbenzene to styrene with up to 91.4% single-pass yield and 82% energy savings.
- Xing Zhu
- , Yunfei Gao
- & Fanxing Li
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Article
| Open AccessDynamic structure of active sites in ceria-supported Pt catalysts for the water gas shift reaction
Revealing the structure and dynamics of active sites is essential to understand catalytic mechanisms. Here the authors demonstrate the dynamic nature of perimeter Pt0−O vacancy−Ce3+ sites in Pt/CeO2 and the key effects of their dynamics on the mechanism of the water gas shift reaction.
- Yuanyuan Li
- , Matthew Kottwitz
- & Anatoly I. Frenkel
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Comment
| Open AccessSingle atom catalysis poised to transition from an academic curiosity to an industrially relevant technology
During the past decade, initial skepticism rapidly changed into widespread recognition of the role of single atoms in heterogeneous catalysts. The next decade could usher in the era of industrial applications as manufacturing of durable single atom catalysts is perfected.
- Abhaya K. Datye
- & Hua Guo
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Article
| Open AccessInsights on forming N,O-coordinated Cu single-atom catalysts for electrochemical reduction CO2 to methane
Single-atom catalysts (SACs) are promising candidates to catalyze CO2 reduction for the formation of high value hydrocarbons but most of the reactions yield CO. Here, the authors show a low-temperature calcining process to fabricate a carbon-dots-based SAC to efficiently convert CO2 to methane.
- Yanming Cai
- , Jiaju Fu
- & Wenlei Zhu
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Article
| Open AccessIonic liquid enables highly efficient low temperature desalination by directional solvent extraction
Directional Solvent Extraction is an emerging non-membrane desalination technology for sea water desalination but is limited by throughput and energy efficiency. Here, the authors demonstrate that the production rate and energy efficiency can be increased by using ionic liquids as directional solvent.
- Jiaji Guo
- , Zachary D. Tucker
- & Tengfei Luo
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Article
| Open AccessWaveguide photoreactor enhances solar fuels photon utilization towards maximal optoelectronic – photocatalytic synergy
Concentrating photo-intensities on photocatalyst has diminishing returns. Here the authors show the catalyst on glass rod waveguide at optimal low intensity results in high efficiency in the gas phase reverse water gas shift reaction in an annular glass cylindrical rod photoreactor.
- Joel Y. Y. Loh
- , Abhinav Mohan
- & Nazir P. Kherani
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Article
| Open AccessCarbon hollow fiber membranes for a molecular sieve with precise-cutoff ultramicropores for superior hydrogen separation
Energy-efficient hydrogen purification technologies are needed for the hydrogen economy. Here the authors report facile and scalable fabrication of asymmetric carbon molecular sieve membranes for the separation of hydrogen and carbon dioxide.
- Linfeng Lei
- , Fengjiao Pan
- & Michael D. Guiver
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Article
| Open AccessDirected transforming of coke to active intermediates in methanol-to-olefins catalyst to boost light olefins selectivity
Methanol-to-olefins is hindered by rapid catalyst deactivation due to coke deposition. Here the authors demonstrate an approach of directly transforming coke to active intermediates to simultaneously recover catalyst activity and boost light olefins selectivity.
- Jibin Zhou
- , Mingbin Gao
- & Zhongmin Liu
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Article
| Open AccessShielded goethite catalyst that enables fast water dissociation in bipolar membranes
Bipolar membranes integrated water dissociation and acid-base generations have great potential in emerging sustainable technologies but remains inefficient. Here, the authors circumvent this inefficiency and instability of the membranes by developing polyaniline shielded catalytic bipolar membranes.
- Muhammad A. Shehzad
- , Aqsa Yasmin
- & Tongwen Xu
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Article
| Open AccessSimultaneous interlayer and intralayer space control in two-dimensional metal−organic frameworks for acetylene/ethylene separation
Designing efficient adsorbents for trace gas removal remains a serious challenge. Here, the authors show promise in layered 2D metal−organic frameworks, often overlooked in favor of 3D frameworks, for separating trace acetylene from ethylene with enhanced performance and high stability.
- Jin Shen
- , Xin He
- & Qilong Ren
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Article
| Open AccessStabilization of ε-iron carbide as high-temperature catalyst under realistic Fischer–Tropsch synthesis conditions
ε-Fe2C has been identified as the highly active phase for Fischer-Tropsch synthesis (FTS), but is stable only at low-temperature. Here, the authors show that ε-Fe2C phase can be stabilized even at ~ 573 K by being encapsulated inside graphene layers, and retains high activity in FTS.
- Shuai Lyu
- , Li Wang
- & Ye Wang
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Article
| Open AccessJanus electrocatalytic flow-through membrane enables highly selective singlet oxygen production
Electrocatalytic processes are promising for automated and scalable synthesis of singlet oxygen, but they are energy- and chemical-intensive. Here the authors present a Janus electrocatalytic membrane that selectively produces singlet oxygen with low energy consumption and free of chemical precursors.
- Yumeng Zhao
- , Meng Sun
- & Menachem Elimelech
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Article
| Open AccessNanorods with multidimensional optical information beyond the diffraction limit
Development of functional nanostructures can enable a range of applications in imaging and nanoscale science. Here, the authors fabricate and characterize complex heterogeneous nanorods with diverse, tunable sub-wavelength structures.
- Shihui Wen
- , Yongtao Liu
- & Dayong Jin
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Article
| Open AccessFeedback regulation of crystal growth by buffering monomer concentration
Gaining control over crystallization processes is challenging. Herein, the authors describe a protocol for the controlled growth of DNA nanotubes by feedback regulation: the coupling of a reversible bimolecular monomer buffering reaction delivers the optimal monomer concentration and leads to reliable crystal growth in a simple manner.
- Samuel W. Schaffter
- , Dominic Scalise
- & Rebecca Schulman
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Article
| Open AccessThe impact of nitrogen oxides on electrochemical carbon dioxide reduction
Understanding the impact of nitrogen oxides, common contaminants in CO2 emission from industries is a key to commercializing CO2 electrolysis technologies. Here, the authors conduct an investigation of CO2 electroreduction on copper, silver, and tin catalysts in the presence of nitric oxide, nitrogen dioxide, or nitrous oxide.
- Byung Hee Ko
- , Bjorn Hasa
- & Feng Jiao
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Article
| Open AccessInverse ZrO2/Cu as a highly efficient methanol synthesis catalyst from CO2 hydrogenation
Enhancing the intrinsic activity and space time yield of Cu based heterogeneous methanol synthesis catalysts is one of the major topics in CO2 hydrogenation. Here the authors develop a highly active inverse catalyst composed of fine ZrO2 islands dispersed on metallic Cu nanoparticles.
- Congyi Wu
- , Lili Lin
- & Ding Ma
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Article
| Open AccessDirect conversion of methane to formaldehyde and CO on B2O3 catalysts
Partial oxidation of methane to value-added C1 products remains challenging due to the favorable formation of fully-oxidized CO2. Here, the authors show supported B2O3 catalysts with tri-coordinated BO3 units as the active site are highly selective in oxidizing methane to HCHO and CO.
- Jinshu Tian
- , Jiangqiao Tan
- & Yong Wang
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Article
| Open AccessElectropolymerization of robust conjugated microporous polymer membranes for rapid solvent transport and narrow molecular sieving
Conjugated microporous polymers (CMPs) have great potential in membrane applications but are often brittle. Here, the authors develop an electropolymerization process to form a skin-core architecture which allows them to overcome mechanical limitations while keeping the excellent separation performance of CMP membranes.
- Zongyao Zhou
- , Xiang Li
- & Zhiping Lai
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Article
| Open AccessExploiting two-dimensional morphology of molybdenum oxycarbide to enable efficient catalytic dry reforming of methane
The two-dimensional morphology of molybdenum oxycarbide (2D-Mo2COx) nanosheets dispersed on silica is found vital for the dry reforming of methane. Here the authors show that the specific activity of 2D-Mo2COx/SiO2 exceeds that of other Mo2C-based catalysts by ca. 3 orders of magnitude.
- Alexey Kurlov
- , Evgeniya B. Deeva
- & Christoph R. Müller
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Article
| Open AccessVisible-light-driven amino acids production from biomass-based feedstocks over ultrathin CdS nanosheets
Chemical production of amino acids from renewable carbon sources in an energy-saving manner is highly desirable. Here, the authors report visible-light-driven, CdS nanosheets-promoted synthesis of amino acids from biomass-based feedstock and NH3 under mild reaction conditions.
- Song Song
- , Jiafu Qu
- & Ning Yan
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Article
| Open AccessCopper catalysis at operando conditions—bridging the gap between single nanoparticle probing and catalyst-bed-averaging
Characterizing individual catalyst nanoparticles at operando conditions is a cornerstone of catalysis research. Here the authors utilize plasmonic optical nanoimaging in a nanofluidic reactor to map the impact of reactor geometry on single Cu particle oxidation state dynamics and active phase during CO oxidation.
- David Albinsson
- , Astrid Boje
- & Christoph Langhammer
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Article
| Open AccessGold catalysts containing interstitial carbon atoms boost hydrogenation activity
Gold is among the least active metals toward molecules at a solid-liquid or solid-gas interface. Here the authors demonstrate that the gold nanocatalysts with d electron gain due to C occupying interstitial sites in its lattice boost catalytic hydrogenation.
- Yafei Sun
- , Yueqiang Cao
- & Ying Wan
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Matters Arising
| Open AccessPitfalls in identifying active catalyst species
- Jiazheng Ren
- & Yongsheng Chen
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Matters Arising
| Open AccessReply to: “Pitfalls in identifying active catalyst species”
- Xavier Isidro Pereira-Hernández
- , Andrew DeLaRiva
- & Abhaya K. Datye
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Comment
| Open AccessSingle atom catalysis: a decade of stunning progress and the promise for a bright future
Controlling the hybridization of single atoms in suitable host materials opens unique opportunities for catalyst design, but equally faces many challenges. Here, we highlight emerging directions from the last, highly productive, decade in single-atom catalysis and identify frontiers for future research.
- Sharon Mitchell
- & Javier Pérez-Ramírez
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Article
| Open AccessMetal 3D printing technology for functional integration of catalytic system
Metal 3D printing is a very promising technology to revolutionize catalytic systems. Here the authors show that metal 3D printing products themselves can simultaneously serve as chemical reactors and catalysts for conversion of C1 molecules into high value-added chemicals.
- Qinhong Wei
- , Hangjie Li
- & Noritatsu Tsubaki
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Article
| Open AccessTransition metal-like carbocatalyst
Metal-free catalysts can offer uniquely different activity and selectivity from transition metal-based counterparts. Here, the authors report metal-free nitrogen-assembly carbon with closely-placed nitrogen as active sites, achieving catalytic cleavage of strong bonds including H-H, C-O and C-H.
- Zhicheng Luo
- , Renfeng Nie
- & Long Qi
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Article
| Open AccessEntropy-stabilized single-atom Pd catalysts via high-entropy fluorite oxide supports
Fabricating intrinsically stable single-atom catalysts (SACs) on traditional supports remains a formidable challenge in catalysis. Here, the authors propose a new strategy to construct a sintering-resistant Pd SAC on a novel equimolar high-entropy fluorite oxide.
- Haidi Xu
- , Zihao Zhang
- & Sheng Dai
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Article
| Open AccessHigh-throughput gas separation by flexible metal–organic frameworks with fast gating and thermal management capabilities
Separation processes in industry use substantial energy and energy-efficient purification systems should be developed for sustainability. Here the authors report a flexible metal–organic framework for high-throughput separation of CO2 from a CO2/CH4 gas mixture in a pressure vacuum swing adsorption system.
- Shotaro Hiraide
- , Yuta Sakanaka
- & Hideki Tanaka
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Article
| Open AccessCatalytic nanosponges of acidic aluminosilicates for plastic degradation and CO2 to fuel conversion
The synthesis of solid acids with strong zeolite-like acidity and textural properties like amorphous aluminosilicates (ASAs) is still a challenge. Here the authors synthesized “acidic amorphous aluminosilicates”, with Brønsted acidic sites like in zeolites and textural properties like ASAs for catalyzing various reactions.
- Ayan Maity
- , Sachin Chaudhari
- & Vivek Polshettiwar
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Article
| Open AccessAlkaline thermal treatment of seaweed for high-purity hydrogen production with carbon capture and storage potential
While biomass may serve as a renewable source of carbon-neutral hydrogen, it is challenging both to utilize as-found bio-resources and to suppress CO2 formation. Here, authors convert wet, salty seaweed using alkaline thermal treatment to produce high-purity hydrogen and suppress carbon emission.
- Kang Zhang
- , Woo-Jae Kim
- & Ah-Hyung Alissa Park
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Article
| Open AccessA scalable method for preparing Cu electrocatalysts that convert CO2 into C2+ products
Selective reduction of carbon dioxide to high-value products is key for advancing carbon capture and utilization technologies. Here the authors prepare a copper catalyst for electrocatalytic conversion of carbon dioxide to C2+ products with enhanced selectivity that is attributed to a high density of surface defects.
- Taehee Kim
- & G. Tayhas R. Palmore
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Comment
| Open AccessTowards brain-tissue-like biomaterials
Many biomaterials have been developed which aim to match the elastic modulus of the brain for improved interfacing. However, other properties such as ultimate toughness, tensile strength, poroviscoelastic responses, energy dissipation, conductivity, and mass diffusivity also need to be considered.
- Eneko Axpe
- , Gorka Orive
- & Eric A. Appel
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Article
| Open AccessThe dynamics of overlayer formation on catalyst nanoparticles and strong metal-support interaction
Tuning the catalytic activity of metal nanoparticles by encapsulation is a long known process, but mechanistically poorly understood. Here, Beck and colleagues reveal the encapsulation mechanism by support material and the outstanding role of oxygen in the encapsulation mechanism by extensive in situ characterization.
- Arik Beck
- , Xing Huang
- & Jeroen A. van Bokhoven