Layered materials as a platform for quantum technologies

2D metallene possess high surface area and excellent electron transport capability, thus enabling efficient application in oxygen reduction reaction (ORR). However, the interface regulation and electronic structure optimization of metallene are still great challenges. Herein, Pd-B/Pd hetero-metallene is constructed by interface engineering and B modification strategies for efficient electrocatalytic ORR. The 2D configuration of Pd-B/Pd hetero-metallene exposes a large number of surface atoms and unsaturated defect sites, thus providing abundant catalytic active sites and exhibiting high electron mobility. More importantly, interface engineering and B modification synergistically optimizing the electronic configuration of the metallene system. This work not only provides an effective strategy for the rational regulation of the electronic configuration of metallene, but also offers a reference for the construction of efficient ORR catalysts. 

Interface Engineering and Boron Modification of Pd-B/Pd Hetero-Metallene Synergistically Accelerate Oxygen Reduction Catalysis.

Surface roughness in chiral plasmonic nanostructures generates asymmetrical localized electromagnetic fields, which hold great promise for applications in chiral recognition, chiroptical spectroscopic sensing, and enantioselective photocatalysis. In this study, we develop a surface topographical engineering approach to precisely manipulate the surface structures of chiral Au nanocrystals. Through carefully controlling the amounts of l- or d-cystine (Cys) and the seed solution in the growth process, we successfully synthesize chiral Au nanocrystals with highly disordered, ordered, and less ordered wrinkled surfaces. An underlying principle governing the relationship between surface roughness, orderliness, and chiroptical response is also proposed. More importantly, the chiral ordered wrinkles on the surfaces of the nanocrystals generate asymmetrical localized electronic fields with enhanced intensity, which achieve excellent plasmon-enhanced chiral discrimination ability for penicillamine (Pen) enantiomers. This work offers exciting prospects for manipulating the surface structures of chiral nanocrystals and designing highly sensitive plasmon-enhanced enantioselective sensors with chiral hot spots. 

Surface Topographical Engineering of Chiral Au Nanocrystals with Chiral Hot Spots for Plasmon-Enhanced Chiral Discrimination.

Under the control of chiral ligand glutathione and in the presence of hexadecyltrimethylammonium bromide, Au deposition on Au seeds is known to give chiral nanostructures. We have previously shown that the protruding chiral patterns, as opposed to flat facets, are likely caused by active surface growth, where nonuniform ligand coverage could be responsible for the focused growth at a few active sites. By pushing the limit of such a growth mode, here, we use decahedral seeds to prepare homochiral nanopropellers with intricate patterns of deep valleys and protruding ridges. Control experiments show that the focused growth depends on the rates of Au deposition by changing either the seed concentration or the reductant concentration, consistent with the proposed mechanism. The dynamic growth competition between the ligand-deficient active sites and the ligand-rich surfaces gradually focuses the growth onto a few active sites, causing the expansion of grooves, squeezing of steep ridges, and a surprising 36° rotation of the pentagonal outline. The imbalanced deposition on the prochiral slopes is responsible for the tilted grooves, the twisted walls, and thus the well-separated and distorted blades, which become the origin of the chiroptical responses. 

Homochiral Nanopropeller via Chiral Active Surface Growth.

Benefiting from both one-dimensional (1D) morphology and alloy composition, metal alloy nanowires have been exploited as advanced electrocatalysts in various electrochemical processes. In this review, the synthesis approaches for metal alloy nanowires are classified into two categories: direct syntheses and syntheses based on preformed 1D nanostructures. Ligand systems that are of critical importance to the formation of alloy nanowires are summarized and reviewed, together with the strategies imposed to achieve the co-reduction of different metals. Meanwhile, different scenarios that form alloy nanowires from pre-synthesized 1D nanostructures are compared and contrasted. In addition, the characterization and electrocatalytic applications of metal alloy nanowires are briefly discussed.

Recent progress on the synthesis of metal alloy nanowires as electrocatalysts.

Interlayer excitons (IXs) in MoSe2-WSe2 heterobilayers have generated interest as highly tunable light emitters in transition metal dichalcogenide (TMD) heterostructures. Previous reports of spectrally narrow (<1 meV) photoluminescence (PL) emission lines at low temperature have been attributed to IXs localized by the moiré potential between the TMD layers. We show that spectrally narrow IX PL lines are present even when the moiré potential is suppressed by inserting a bilayer hexagonal boron nitride (hBN) spacer between the TMD layers. We compare the doping, electric field, magnetic field, and temperature dependence of IXs in a directly contacted MoSe2-WSe2 region to those in a region separated by bilayer hBN. The doping, electric field, and temperature dependence of the narrow IX lines are similar for both regions, but their excitonic g-factors have opposite signs, indicating that the origin of narrow IX PL is not the moiré potential. 

/pdf/localized-interlayer-excitons-in-mose2-wse2-heterostructures-2efgqcbp.pdf

Localized interlayer excitons in MoSe2–WSe2 heterostructures without a moiré potential

It is shown that the chiral ligand glutathione can induce active surface growth in the deposition of Au on Au nanoplates, forming nano-badges with complex surface patterns. The special feature of the growth mode is that the growth materials are diverted to a few active sites, causing deep valleys and high standing walls. The circular dichroism signal depends on the tilting degree of the walls, which likely arises from the different packing of the chiral ligands on the two pro-chiral slopes. As a characteristic sign of the Active Surface Growth mode, low seed concentration is used to promote the rate of deposition, which expands the ridge–valley competition favoring growth at the active sites. The understanding and rational control of the chiral ridges will advance the synthetic control for chiral nanostructures. 

Chiral Active Surface Growth via Glutathione Control

Lattice distortions and defects can lead to a strain effect that greatly affects the electronic structure of the noble metal surface and the chemical adsorption of ligands on the surfaces. Introducing defects is an efficient strategy to improve the activity of noble metal catalysts. Herein, a fusion approach is developed to fine-tune the defects and lattice strain in Au-Pd nanowires. Specifically, braided strands in Au-Pd nanoropes gradually coalesce to form solid nanowires upon H2 O2 treatment and heating, leading to a series of Au-Pd nanowires with various amounts of defects. Owing to the 1D morphology, as well as the optimized lattice strain and surface electronic structure, the intermediate Au-Pd nanowire obtained after 60 min heating (denoted as Au-Pd NW60 ) exhibits excellent catalytic activity and stability toward the oxygen reduction reaction, with the half-wave potential at 0.918 V, 45 mV higher than that of the commercial Pt/C; and specific activity reaches up to 1.7 mA cm-2 , 7.3 times higher than that of the Pt/C.

Coalescence of Au-Pd Nanoropes and their Application as Enhanced Electrocatalysts for the Oxygen Reduction Reaction.

CTAB alone is able to induce Active Surface Growth on gold nanoplates, forming curved tips and steep ridges. 

pdf/gold-nanohexagrams-via-active-surface-growth-under-sole-ctab-4ec60edhjt.pdf

Gold nanohexagrams via active surface growth under sole CTAB control.

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