A new strategy for achieving stable Co single atoms (SAs) on nitrogen-doped porous carbon with high metal loading over 4 wt % is reported. The strategy is based on a pyrolysis process of predesigned bimetallic Zn/Co metal-organic frameworks, during which Co can be reduced by carbonization of the organic linker and Zn is selectively evaporated away at high temperatures above 800 °C. The spherical aberration correction electron microscopy and extended X-ray absorption fine structure measurements both confirm the atomic dispersion of Co atoms stabilized by as-generated N-doped porous carbon. Surprisingly, the obtained Co-Nx single sites exhibit superior ORR performance with a half-wave potential (0.881 V) that is more positive than commercial Pt/C (0.811 V) and most reported non-precious metal catalysts. Durability tests revealed that the Co single atoms exhibit outstanding chemical stability during electrocatalysis and thermal stability that resists sintering at 900 °C. Our findings open up a new routine for general and practical synthesis of a variety of materials bearing single atoms, which could facilitate new discoveries at the atomic scale in condensed materials.

Despite significant advances in the fabrication and applications of graphene-like materials, it remains a challenge to prepare single-layered metallic materials, which have great potential applications in physics, chemistry and material science. Here we report the fabrication of poly(vinylpyrrolidone)-supported single-layered rhodium nanosheets using a facile solvothermal method. Atomic force microscope shows that the thickness of a rhodium nanosheet is o4 Å. Electron diffraction and X-ray absorption spectroscopy measurements suggest that the rhodium nanosheets are composed of planar single-atom-layered sheets of rhodium. Density functional theory studies reveal that the single-layered Rh nanosheet involves a d-bonding framework, which stabilizes the single-layered structure together with the poly(vinylpyrrolidone) ligands. The poly(vinylpyrrolidone)-supported single-layered rhodium nanosheet represents a class of metallic two-dimensional structures that might inspire further fundamental advances in physics, chemistry and material science.

We have studied the adsorption of gas molecules (CO, NO, NO 2 , O 2 , N 2 , CO 2 , and NH 3 ) on graphene nanoribbons (GNRs) using first principles methods. The adsorption geometries, adsorption energies, charge transfer, and electronic band structures are obtained. We find that the electronic and transport properties of the GNR with armchair-shaped edges are sensitive to the adsorption of NH 3 and the system exhibits n-type semiconducting behavior after NH 3 adsorption.Other gas molecules have little effect on modifying the conductance of GNRs. Quantum transport calculations further indicate that NH 3 molecules can be detected out of these gas molecules by GNR based sensor.

First-principles calculations reveal half metallicity in zigzag boron nitride (BN) nanoribbons (ZBNNRs). When the B edge, but not the N edge, of the ZBNNR is passivated, despite being a pure sp-electron system, the ribbon shows a giant spin splitting. The electrons at the Fermi level are 100% spin polarized with a half-metal gap of 0.38 eV and its conductivity is dominated by metallic single-spin states. The two states across at the Dirac point have different molecular origins, which signals a switch of carrier velocity. The ZBNNR should be a good potential candidate for widegap spintronics.

Natural and synthetic nanoparticles composed of fivefold twinned crystal domains have distinct properties. The formation mechanism of these fivefold twinned nanoparticles is poorly understood. We used in situ high-resolution transmission electron microscopy combined with molecular dynamics simulations to demonstrate that fivefold twinning occurs through repeated oriented attachment of ~3-nanometer gold, platinum, and palladium nanoparticles. We discovered two different mechanisms for forming fivefold twinned nanoparticles that are driven by the accumulation and elimination of strain. This was accompanied by decomposition of grain boundaries and the formation of a special class of twins with a net strain of zero. These observations allowed us to develop a quantitative picture of the twinning process. The mechanisms provide guidance for controlling twin structures and morphologies across a wide range of materials.

It is highly desirable but challenging to optimize the structure of photocatalysts at the atomic scale to facilitate the separation of electron–hole pairs for enhanced performance. Now, a highly efficient photocatalyst is formed by assembling single Pt atoms on a defective TiO2 support (Pt1/def‐TiO2). Apart from being proton reduction sites, single Pt atoms promote the neighboring TiO2 units to generate surface oxygen vacancies and form a Pt‐O‐Ti3+ atomic interface. Experimental results and density functional theory calculations demonstrate that the Pt‐O‐Ti3+ atomic interface effectively facilitates photogenerated electrons to transfer from Ti3+ defective sites to single Pt atoms, thereby enhancing the separation of electron–hole pairs. This unique structure makes Pt1/def‐TiO2 exhibit a record‐level photocatalytic hydrogen production performance with an unexpectedly high turnover frequency of 51423 h−1, exceeding the Pt nanoparticle supported TiO2 catalyst by a factor of 591.

NiCo2O4 with higher specific capacitance is an excellent pseudocapacitive material. However, the bulk NiCo2O4 material prevents the achievement of high energy desity and great rate performance due to the limited electroactive surface area. In this work, NiCo2O4 nanosheet arrays were deposited on flexible carbon fabric (CF) as a high-performance electrode for supercapacitors. The NiCo2O4 arrays were constructed by interconnected ultrathin nanosheets (10 nm) with many interparticle pores. The porous feature of NiCo2O4 nanosheets increases the amount of electroactive sites and facilitates the electrolyte penetration. Hence, the NiCo2O4/CF composites exhibited a high specific capacitance of 2658 F g(-1) (2 A g(-1)), good rate performance, and superior cycling life, suggesting the NiCo2O4/CF is a promising electrode material for flexible electrochemical capacitors.

This corrosion: Octahedral Pt-Ni alloy nanoparticles (NPs) are converted into concave Pt(3)Ni NPs by a coordination-assisted chemical-etching process. The corroded concave Pt-Ni NPs have a higher density of low-coordinate atoms in steps sites, a decisive property in heterogeneous catalysis.