Yaqi Jiang

Synthesis of Tin Dioxide Octahedral Nanoparticles with Exposed High-Energy {221} Facets and Enhanced Gas-Sensing Properties

National Natural Science Foundation of China [20725310, 20721001, 20673085, 20801045]; National Basic Research Program of China [2007CB15303, 2009CB939804]

Unique Excavated Rhombic Dodecahedral PtCu3 Alloy Nanocrystals Constructed with Ultrathin Nanosheets of High-Energy {110} Facets

Ultrathin crystalline nanosheets give an extremely high surface area of a specific crystal facet with unique physical and chemical properties compared with normal three-dimensionally polyhedral nanocrystals (NCs). However, the ultrathin metal nanosheets tend to curl themselves or assemble with each other sheet by sheet, which may reduce the effective surface area and accordingly the catalytic activity to a great extent. Here we report a facile wet-chemical route that allows the fabrication of novel excavated rhombic dodecahedral (ERD) PtCu3 alloy NCs with ultrathin nanosheets of high-energy {110} facets. The surface area was measured to be 77 m(2) g(-1) by CO stripping, although the particle size is about 50 nm. Electrochemical characterizations showed that the ERD PtCu3 NCs exhibit excellent electrocatalytic performance and high antipoisoning activity in comparison with commercial Pt black and PtCu3 alloy NCs with {111} surfaces.

Graphene and graphene-based nanomaterials: the promising materials for bright future of electroanalytical chemistry

Similar to its popular older cousins of fullerene and carbon nanotubes (CNTs), the latest form of nanocarbon, graphene, is inspiring intensive research efforts in its own right. As an atomically thin layer of sp(2)-hybridized carbon, graphene possesses spectacular electronic, optical, magnetic, thermal and mechanical properties, which make it an exciting material in a variety of important applications. In this review, we present the current advances in the field of graphene electroanalytical chemistry, including the modern methods of graphene production, and graphene functionalization. Electrochemical (bio) sensing developments using graphene and graphene-based materials are summarized in more detail, and we also speculate on their future and discuss potential progress for their applications in electroanalytical chemistry.

Intrinsic peroxidase-like catalytic activity of nitrogen-doped graphene quantum dots and their application in the colorimetric detection of H2O2 and glucose

In this paper, the highly intrinsic peroxidase-like catalytic activity of nitrogen-doped graphene quantum dots (N-GQDs) is revealed. This activity was greatly dependent on pH, temperature and H2O2 concentration. The experimental results showed that the stable N-GQDs could be used for the detection of H2O2 and glucose over a wide range of pH and temperature, offering a simple, highly selective and sensitive approach for their colorimetric sensing. The linearity between the analyte concentration and absorption ranged from 20 to 1170 μM for H2O2 and 25 to 375 μM for glucose with a detection limit of 5.3 μM for H2O2 and 16 μM for glucose. This assay was also successfully applied to the detection of glucose concentrations in diluted serum and fruit juice samples.

Controlled Synthesis and Enhanced Catalytic and Gas‐Sensing Properties of Tin Dioxide Nanoparticles with Exposed High‐Energy Facets

A morphology evolution of SnO(2) nanoparticles from low-energy facets (i.e., {101} and {110}) to high-energy facets (i.e., {111}) was achieved in a basic environment. In the proposed synthetic method, octahedral SnO(2) nanoparticles enclosed by high-energy {111} facets were successfully synthesized for the first time, and tetramethylammonium hydroxide was found to be crucial for the control of exposed facets. Furthermore, our experiments demonstrated that the SnO(2) nanoparticles with exposed high-energy facets, such as {221} or {111}, exhibited enhanced catalytic activity for the oxidation of CO and enhanced gas-sensing properties due to their high chemical activity, which results from unsaturated coordination of surface atoms, superior to that of low-energy facets. These results effectively demonstrate the significance of research into improving the physical and chemical properties of materials by tailoring exposed facets of nanomaterials.

Silver–Gold Alloy Nanoclusters as a Fluorescence-Enhanced Probe for Aluminum Ion Sensing

In this paper, the development of a simple method is described for preparing highly red fluorescent mercaptosuccinic acid stabilized AgAu alloy nanoclusters (MSA-AgAu NCs) through the core etching of Ag nanoparticles (NPs) and a galvanic exchange reaction using nonorganic solvent and no multistep centrifuge washing. The as-prepared MSA-AgAu NCs were characterized using spectroscopic and microscopic techniques. After covalently attaching methoxy-poly(ethylene glycol)-NH2 (m-PEG-NH2), PEGylated MSA-AgAu NCs were still stable even in 1 M NaCl. Probably based on the deposition of Al(3+)-enhanced fluorescence, the PEGylated MSA-AgAu NCs offered highly selective and sensitive sensing of Al(3+) in aqueous solution with a detection limit of 0.8 μM.

Controlled synthesis of concave Cu2O microcrystals enclosed by {hhl} high-index facets and enhanced catalytic activity

Due to the fact that crystal facets with high surface energy usually exhibit superior performance in many fields, such as catalysis, the importance of the synthesis of micro/nano-crystals with exposed high surface energy facets is becoming a hot research field. In this article, concave Cu2O microcrystals mainly enclosed by {hhl} high-index facets have been successfully prepared by reducing Cu(CH3COO)2 with glucose in the presence of sodium dodecyl sulphate (SDS). SDS was proved to be important in the formation of the concave Cu2O microcrystals. The concave degree of truncated octahedra can be controlled by adjusting the concentration of SDS. In addition, we found the reaction rate also affected the morphology of Cu2O microcrystals. Octahedron-based branched particles, truncated concave octahedra and truncated octahedra can be obtained by adjusting the concentration of glucose. In the catalytic oxidation of CO, truncated concave octahedral Cu2O enclosed by {332} high-index facets exhibited the highest catalytic activity among the high-index {332} facets, low index {111} and {100} facets, due to the existence of high density steps on {332} facets and the CO catalytic activities of the crystal facets are in the sequence: {332} > {111} > {100}.

Excavated Cubic Platinum-Tin Alloy Nanocrystals Constructed from Ultrathin Nanosheets with Enhanced Electrocatalytic Activity.

Excavated polyhedral noble-metal materials that were built by the orderly assembly of ultrathin nanosheets have both large surface areas and well-defined facets, and therefore could be promising candidates for diverse important applications. In this work, excavated cubic Pt-Sn alloy nanocrystals (NCs) with {110} facets were constructed from twelve nanosheets by a simple co-reduction method with the assistance of the surface regulator polyvinylpyrrolidone. The specific surface area of the excavated cubic Pt-Sn NCs is comparable to that of commercial Pt black despite their larger particle size. The excavated cubic Pt-Sn NCs exhibited superior electrocatalytic activity in terms of both the specific area current density and the mass current density towards methanol oxidation.

Underpotential Deposition-Induced Synthesis of Composition-Tunable PtCu Nanocrystals and Their Catalytic Properties

Pt-Cu alloy octahedral nanocrystals (NCs) have been synthesized successfully by using N,N-dimethylformamide as both the solvent and the reducing agent in the presence of cetyltrimethylammonium chloride. Cu underpotential deposition (UPD) is found to play a key role in the formation of the Pt-Cu alloy NCs. The composition in the Pt-Cu alloy can be tuned by adjusting the ratio of metal precursors in solution. However, the Cu content in the Pt-Cu alloy NCs cannot exceed 50%. Due to the fact that Cu precursor cannot be reduced to metallic copper and the Cu content cannot exceed 50%, we achieved the formation of the Pt-Cu alloy by using Cu UPD on the Pt surface. In addition, the catalytic activities of Pt-Cu alloy NCs with different composition were investigated in electrocatalytic oxidation of formic acid. The results reveal that the catalytic performance is strongly dependent on Pt-Cu alloy composition. The sample of Pt(50)Cu(50) exhibits excellent activity in electrocatalytic oxidation of formic acid.

Platinum-nickel alloy excavated nano-multipods with hexagonal close-packed structure and superior activity towards hydrogen evolution reaction

Crystal phase regulations may endow materials with enhanced or new functionalities. However, syntheses of noble metal-based allomorphic nanomaterials are extremely difficult, and only a few successful examples have been found. Herein, we report the discovery of hexagonal close-packed Pt–Ni alloy, despite the fact that Pt–Ni alloys are typically crystallized in face-centred cubic structures. The hexagonal close-packed Pt–Ni alloy nano-multipods are synthesized via a facile one-pot solvothermal route, where the branches of nano-multipods take the shape of excavated hexagonal prisms assembled by six nanosheets of 2.5 nm thickness. The hexagonal close-packed Pt–Ni excavated nano-multipods exhibit superior catalytic property towards the hydrogen evolution reaction in alkaline electrolyte. The overpotential is only 65 mV versus reversible hydrogen electrode at a current density of 10 mA cm−2, and the mass current density reaches 3.03 mA μgPt−1 at −70 mV versus reversible hydrogen electrode, which outperforms currently reported catalysts to the best of our knowledge.