Wangting Lu

Co nanoparticles/Co, N, S tri-doped graphene templated from in-situ formed Co, S co-doped g-C3N4 as an active bifunctional electrocatalyst for overall water splitting

The development of high-performance electrocatalyst with earth-abundant elements for water-splitting is a key factor to improve its cost efficiency. Herein, a noble metal-free bifunctional electrocatalyst was synthesized by a facile pyrolysis method using sucrose, urea, Co(NO3)2 and sulfur powder as raw materials. During the fabrication process, Co, S co-doped graphitic carbon nitride (g-C3N4) was first produced, and then this in-situ-formed template further induced the generation of a Co, N, S tri-doped graphene coupled with Co nanoparticles (NPs) in the following pyrolysis process. The effect of pyrolysis temperature (700, 800, and 900 °C) on the physical properties and electrochemical performances of the final product was studied. Thanks to the increased number of graphene layer encapsulated Co NPs, higher graphitization degree of carbon matrix and the existence of hierarchical macro/meso pores, the composite electrocatalyst prepared under 900 °C presented the best activity for both hydrogen evolution reaction (HER) and oxygen evolution reaction (OER) with outstanding long-term durability. This work presented a facile method for the fabrication of non-noble-metal-based carbon composite from in-situ-formed template and also demonstrated a potential bifunctional electrocatalyst for the future investigation and application.

Shape-controlled synthesis of Pd nanocrystals in an aqueous solution by using amphiphilic triblock copolymers as both the stabilizer and the reductant

Palladium nanocrystals (NCs) are highly useful functional materials in many applications, and the performances of Pd NCs were strongly depended on the crystalline facet exposed on their surface. In this work, Pd NCs were synthesized in aqueous solutions by using Na2PdCl4 as the precursor, citric acid as the capping agent, and Pluronic F127 as both stabilizer and reductant. By adjusting the reaction parameters, Pd cuboctahedrons, octahedrons, and triangular nanoplates with well-defined facets can be produced. This study provides a new pathway for the shape-controlled preparation of noble metal NCs.

Stern-Layer Adsorption of Oligonucleotides on Lamellar Cationic Lipid Bilayer Investigated by Polarization-Resolved SFG-VS

The molecular interaction between the oligonucleotides and lipid membranes is the key to the functions of virus, aptamer, and various oligonucleotide-based materials. In this study, the conformational changes of oligonucleotides (dT25) on lamellar cationic 1,2-dimyristoyl-3-trimethylammonium-propane (DMTAP) bilayer were investigated by polarization-resolved sum frequency generation vibrational spectroscopy (SFG-VS) in situ. The SFG-VS spectra within different wavenumber ranges were analyzed to give conformation details of thymine groups, phosphate groups, and OD/OH groups and to provide a comprehensive and fundamental understanding of the oligonucleotide adsorption on a model bilayer. It is shown that the adsorption of dT25 on DMTAP bilayer reaches maximum at CdT ≈ 500 nM. And the conformation of dT25 molecules change significantly when surface charge of DMTAP bilayer reaches the point of zero charge (PZC) at CdT ≈ 100 nM. Combined spectroscopic evidences also indicate that the formation of electric double layer at the DMTAP/dT25 surface follows the Gouy–Chapman–Stern model. The analysis results also show that the symmetric PO2– stretching mode of oligonucleotide molecules can serve as a sensitive vibration molecular probe for quantifying the oligonucleotide/lipid charge ratio and determine the point of zero charge (PZC) of lipid bilayer surface, which may help researchers to control the layer-by-layer assembly of oligonucleotide–lipid complexes and to improve the efficiency genetic therapy against cancer and viral infections.

A Spatially Confined gC3N4–Pt Electrocatalyst with Robust Stability

Metal catalysts (e.g., Pt) have a variety of applications in energy conversion devices including polymer electrolyte fuel cells (PEFCs); however, they commonly confront a crucial issue of poor stability. Herein, a structural model of spatially confining supported Pt nanoparticles is determined to improve the stability of metal catalysts, wherein graphitic carbon nitride (gC3N4) supported Pt nanoparticles (gC3N4-Pt) are spatially confined by carbon nanospheres (CNSs). The resulting CNSs-Pt/gC3N4 catalyst demonstrates a surprising retention rate of electrochemical surface area as high as 85.0%, much higher than that of the commercial Pt/C catalyst (45.2%), and the half-wave potential is reduced by only 11 mV compared with 54 mV for Pt/C after 6000 scanning cycles. In addition, CNSs also serve as a conductive agent to increase electron transfer pathways on Pt surfaces, and the unique spatial confinement structure with an open framework ensures the mass transfer. Moreover, the methanol oxidation reaction (MOR) activity of CNSs-Pt/gC3N4 gets elevated by 2.1 times that of Pt/C in terms of the anodic peak current. The stabilized catalyst model and its derivative structures can be applied to various metal catalyst systems.