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.
Inorganic, Nanoscale and Physical Chemistry
Jacilynn Brant: materials chemistry and functional materials.
Long Chen: photo- and heterogeneous catalysis.
Margherita Citroni: physical and analytical chemistry.
Ariane Vartanian: nanoscale and supramolecular chemistry.
Welcome to the Nature Communications Editors’ Highlights webpage on inorganic, nanoscale and physical chemistry. Each month our editors select a small number of Articles recently published in Nature Communications that they believe are particularly interesting or important.
The aim is to provide a snapshot of some of the most exciting work published in the area of inorganic, nanoscale and physical chemistry at Nature Communications.
Make sure to check the Editors' Highlights page each month for new featured articles.
Ligand engineering to achieve enhanced ratiometric oxygen sensing in a silver cluster-based metal-organic framework
Incorporating dual fluorescence and phosphorescence into a single matrix is attractive for oxygen sensing, but material design is challenging. Here the authors achieve dual fluorescence-phosphorescence from a single linker chromophore in a silver chalcogenolate-cluster-based metal-organic framework.
Low temperature synthesis of plasmonic molybdenum nitride nanosheets for surface enhanced Raman scattering
Molybdenum nitride is promising for catalysis, energy storage and Raman scattering, but it is synthesized under harsh conditions. Here the authors synthesize highly crystalline molybdenum nitride nanosheets using a relatively mild, non-aqueous solvothermal approach that can be extended to other nitrides.
Highly compressible and anisotropic lamellar ceramic sponges with superior thermal insulation and acoustic absorption performances
Temperature-invariant highly compressible ceramic sponges are attractive for thermal insulators and energy absorbers, but development is limited by complex preparation processes. Here the authors report large-scale fabrication of silica-alumina composite ceramic sponges via blow spinning and calcination.
Two dimensional lamellar membranes are attractive for anomalous water and ion transfer, but performance is hindered by swelling. Here, the authors stabilize a MXene membrane laminar architecture with fixed nanochannels, achieving highly selective acid recovery from iron-based wastewater.
3D-3D topotactic transformation in aluminophosphate molecular sieves and its implication in new zeolite structure generation
Zeolites have pore structures that are attractive for shape-selective catalysis and separation, but targeted synthesis is challenging. Here, the authors propose using a 3D-3D topotactic transformation to synthesize targeted zeolites, including some that may be not feasible with conventional methods.
High-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.
Efficient radiation monitoring ensures safety in nuclear power, but beta-ray scintillators should be developed for use near a highly radioactive and hot reactor. Here, the authors report a two-dimensional halide perovskite-based beta-ray scintillator with high irradiation hardness and thermotolerance.
Molybdenum disulfide membranes are attractive for filtration of nanoscale species but should be optimized for application. Here, the authors report composite membranes with tunable surface charge, pore size and interlayer spacing, achieving efficient filtration of small-molecule dyes and osmosis.
Large-scale production of fibers from two dimensional materials opens a pathway to promising applications. Here the authors report meter-long MXene fibers with high electrical conductivity that are fabricated via continuous wet spinning and demonstrated in electrical wires.
Unique hole-accepting carbon-dots promoting selective carbon dioxide reduction nearly 100% to methanol by pure water
Solar-driven CO2 reduction by abundant water to alcohols is hindered by the sluggish water oxidation reaction. Here, the authors demonstrate that the microwave-synthesized carbon-dots possess unique hole-accepting nature, allowing stoichiometric oxygen and methanol production from water and CO2 with nearly 100% selectivity to methanol.
The unique interplay between copper and zinc during catalytic carbon dioxide hydrogenation to methanol
In spite of numerous works, the nature of high activity of Cu/ZnO catalyst in methanol synthesis remains the subject of intensive debate. Here, the authors study the carbon dioxide hydrogenation mechanism using high-pressure operando techniques which allow them to unify different, seemingly contradicting, models.
Elucidation of the chemical structure of natural products constitutes one of the main challenges in Natural Sciences. Here, the authors show that an amino acid-based metal–organic framework exhibits hydrolase-like catalytic activity and crystallographic determination of the resulting products.
The design of oxide-metal interface for heterogeneous catalysis has been hampered by the limited fundamental understanding. Here, the authors demonstrate that the activities of cuprous oxide nanostructures for CO oxidation can be tuned via the oxide-metal (Cu2O/M, M = Pt, Ag, Au) interaction.
Structural changes in noble metal nanoparticles during CO oxidation and their impact on catalyst activity
How nanoparticle (NP) catalysts re-structure under reaction conditions and how these changes associate with catalytic activity remains poorly understood. Here, the authors present operando TEM studies of Pd NPs during CO oxidation, which show reversible changes in both structure and activity with temperature.
Platinum nanocatalysts play critical roles in CO oxidation. Herein, the authors discover that under-coordinated Pt atoms at the edges of the first cluster layer are rendered cationic by direct contact with the Al2O3 support, which affects the overall CO oxidation activity.
Reacting CO2 and ethane to achieve value-added C3 oxygenates offers opportunities to simultaneously reduce CO2 emissions and upgrade underutilized ethane in shale gas. Here, the authors report a successful oxygenate production strategy enabled by inserting CO2-derived CO into ethane-derived ethylene using a tandem reactor.
Single-atom catalysts reveal the dinuclear characteristic of active sites in NO selective reduction with NH3
Identification of active sites is one key prerequisite for rational design of efficient catalysts. Here, the authors achieve a common feature of catalytic active sites for NO selective reduction with NH3, which assists precise identification of active sites and effective design of optimal catalysts.
Nanocatalysts and single‐atom catalysts are generally considered as two categories with distinct performances. Here, in situ TEM study of catalytic methane pyrolysis over nanoporous Au reveals a highly dynamic process where co‐catalysis exists among various catalyst forms.
Long-lived carbon nitride radicals have been used in several photocatalytic reactions. Herein, long-lived potassium poly(heptazine imide) radicals enable synthesis of γ,γ-dichloroketones from enones by addition of CHCl2 moiety, generated from chloroform, to the C=C bond.
Formation of peptide bonds in cold gas-phase environments might represent a prebiotic synthesis route of polypeptides. Here, the authors show the formation of up to tetra-peptide species in the collision of He2+ ions, with kinetic energies typical for solar wind ions, with cold β-alanine clusters.
Electron affinity (EA) is a key parameter in determining the chemical behavior of the elements, but challenging to measure for unstable atoms. Here the authors succeed in measuring the EA of astatine, the heaviest naturally occurring halogen, and compare it with predictions from relativistic calculations.
The mechanisms of formation of the (6-4) photoproducts in DNA damage by sunlight is still debated. Here the authors show, by optical spectroscopies and computations, the details of the formation of a (6-4) photoadduct via the thietane intermediate in a single-stranded DNA oligonucleotide.
The geometric phase effect associated with a conical intersection between the ground and first excited electronic state has been predicted in the H3 system below the conical intersection energy. The authors, by a crossed molecular beam technique and quantum dynamic calculations, provide experimental evidence and insight into its origin.
Nano-FTIR spectroscopy allows chemical characterization of composite surfaces, but its capability in subsurface analysis is not much explored. The authors show that spectra from thin surface layers differ from those of subsurface layers of the same organic material, and establish a method for distinguishing them in experiments.
Setting benchmarks for modelling gas–surface interactions using coherent control of rotational orientation states
A fundamental and predictive understanding of molecule-surface interactions is challenging to obtain. Here the authors report an experimental technique allowing direct measurement of the scattering matrix, which reports on the coherent evolution of quantum states of a molecule scattering from a surface.
Excited-state structural and electronic changes, observed in molecules, are hampered in nanomaterials. Here the authors identify structural distortion and electron redistribution in three photoexcited gold nanoclusters, connecting molecular and nanocrystal regimes, enabled by flexibility of the tetrahedral core units.
Geometric and electronic structure probed along the isomerisation coordinate of a photoactive yellow protein chromophore
Resolving concerted nuclear and electronic motion in real-time is a primary goal in chemistry. The authors monitor nuclear and valence electronic dynamics in the excited state single-bond isomerisation of a chromophore of photoactive yellow protein, using time-resolved photoelectron imaging and electronic structure calculations.
Interaction of strong laser fields with matter provides powerful tools to image transient dynamics with high spatiotemporal resolution. The authors investigate strong-field ionisation of laser-aligned molecules showing the effect of molecular alignment on the photoelectron dynamics and the resulting influence of the molecular frame in imaging experiments.
Exosomes are used as disease biomarkers, but their characterization in biological samples is challenging. Here the authors achieve simultaneous characterization of size and zeta potential of individual nanoparticles and particle mixtures at physiological salinity conditions, exploiting a salt gradient in a capillary channel.
Light-driven heating of plasmonic metal nanoparticles can activate temperature-sensitive reactions at the nanoscale. Here, the authors exploit such nanoscale plasmonic reactors to drive, control, and spectroscopically track the growth of single metal@semiconductor core@shell nanoparticles.
Quintulene, a quintuple non-graphitic cycloarene, is challenging to synthesize. Here, the authors synthesize and characterize the cone-shaped extended quintulene and its bilayer dimer, and disclose its dimerization as an entropy-driven, second-order reaction with a substantial activation energy.
Superlattices of nanoparticles promise new properties emerging from the periodic order. Here, the authors describe the synthesis of superlattices of plasmonic gold nanoparticles with high crystallinity and demonstrate how new plasmon-polariton modes appear in the structures.
Nested polyhedra are compelling but incredibly complex synthetic targets in cluster chemistry. Here, the authors synthesize a Ag90 nanocluster comprising three concentric polyhedra with apparently incompatible octahedral (Oh) and icosahedral (Ih) symmetry, a mathematical oddity that is solved by the shells’ symmetric arrangement around rotational 2- and 3-fold axes.
Stable diradicals are generally based on two s/p-localized or π-delocalized unpaired electrons (radicals). Here, the authors report a dication diradical that is based on two Se∴Se three-electron σ-bonds.
Structurally divergent reactions on racemic mixtures, which produce distinct chemical species from an enantiomeric mixture, are extremely rare in the literature. Here, the authors are able to use a dynamic combinatorial approach to yield structurally divergent, non-isomeric catenanes from an enantiomeric mixture.
The discovery of atomically precise metal nanoclusters is generally unpredictable, and there are few examples of their rational synthesis. Here, the authors report the de novo design of Au36(SR)24 nanoclusters, from theoretical prediction to experimental synthesis and characterization of physicochemical properties.
Heteroatom-bearing molecular loops and belts are fascinating but generally difficult to synthesize. Here, the authors demonstrate that O,S-bridged double-stranded molecular belts—cyclophenoxathiins—can be successfully constructed and employed as versatile supramolecular hosts.
Many Zintl ions with a single endohedrally encapsulated transition metal ion are known, but relatively few where clusters of two or more metals are present. Here, the authors report the synthesis and characterization of two clusters, [Au8Pb33]6− and [Au12Pb44]12−, which contain Au8 and Au12 cores surrounded by Pb shells.
Precise assembly of heterometallic complexes is a challenge. Here, the authors design a heterometallic triangular necklace through a highly efficient threading-and-ring-closing approach driven by metal-ligand coordination, which shows strong bacterium-binding and cell wall/plasma membrane-disrupting capacity for killing bacterial cells.