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Heterostructures for Electrochemical Hydrogen Evolution Reaction: A Review

Two-dimensional MXenes: From morphological to optical, electric, and magnetic properties and applications

Biosensors with high sensitivity, selectivity and a low limit of detection, reaching nano/picomolar concentrations of biomolecules, are important to the medical sciences and healthcare industry for evaluating physiological and metabolic parameters. Over the last decade, different nanomaterials have been exploited to design highly efficient biosensors for the detection of analyte biomolecules. The discovery of graphene has spectacularly accelerated research on fabricating low-cost electrode materials because of its unique physical properties, including high specific surface area, high carrier mobility, high electrical conductivity, flexibility, and optical transparency. Graphene and its oxygenated derivatives, including graphene oxide (GO) and reduced graphene oxide (rGO), are becoming an important class of nanomaterials in the field of biosensors. The presence of oxygenated functional groups makes GO nanosheets strongly hydrophilic, facilitating chemical functionalization. Graphene, GO and rGO nanosheets can be easily combined with various types of inorganic nanoparticles, including metals, metal oxides, semiconducting nanoparticles, quantum dots, organic polymers and biomolecules, to create a diverse range of graphene-based nanocomposites with enhanced sensitivity for biosensor applications. This review summarizes the advances in two-dimensional (2D) and three-dimensional (3D) graphene-based nanocomposites as emerging electrochemical and fluorescent biosensing platforms for the detection of a wide range of biomolecules with enhanced sensitivity, selectivity and a low limit of detection. The biofunctionalization and nanocomposite formation processes of graphene-based materials and their unique properties, surface functionalization, enzyme immobilization strategies, covalent immobilization, physical adsorption, biointeractions and direct electron transfer (DET) processes are discussed in connection with the design and fabrication of biosensors. The enzymatic and nonenzymatic reactions on graphene-based nanocomposite surfaces for glucose- and cholesterol-related electrochemical biosensors are analyzed. This review covers a very broad range of graphene-based electrochemical and fluorescent biosensors for the detection of glucose, cholesterol, hydrogen peroxide (H2O2), nucleic acids (DNA/RNA), genes, enzymes, cofactors nicotinamide adenine dinucleotide (NADH) and adenosine triphosphate (ATP), dopamine (DA), ascorbic acid (AA), uric acid (UA), cancer biomarkers, pathogenic microorganisms, food toxins, toxic heavy metal ions, mycotoxins, and pesticides. The sensitivity and selectivity of graphene-based electrochemical and fluorescent biosensors are also examined with respect to interfering analytes present in biological systems. Finally, the future outlook for the development of graphene based biosensing technology is outlined.

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A review on graphene-based nanocomposites for electrochemical and fluorescent biosensors

Exposing the highly active facets and hybridizing the photocatalyst with appropriate cocatalysts with right placement have been regarded as a powerful approach to high performance photocatalysts. Herein, TiO2 nanosheets (NSs) are in situ grown on highly conductive Ti3C2 MXene and then MoS2 NSs are deposited on the (101) facets of TiO2 NSs with mainly exposed high-active (001) facets through a two-step hydrothermal method. And a unique 2D-2D-2D structure of Ti3C2@TiO2@MoS2 composite is achieved. With an optimized MoS2 loading amounts (15 wt%), the Ti3C2@TiO2@MoS2 composite shows a remarkable enhancement in the photocatalytic H2 evolution reaction compared with Ti3C2@TiO2 composite and TiO2 NS. It also shows good stability under the reaction condition. This arises from: (i) the in situ growth of TiO2 NSs construct strong interfacial contact with excellent electronic conductivity of Ti3C2, which facilitates the separation of carriers; (ii) the coexposed (101) and (001) facets can form a surface heterojunction within single TiO2 NS, which is beneficial for the transfer and separation of charge carriers; and (iii) the MoS2 NSs are deposited on the electrons-rich (101) facets of TiO2 NSs, which not only effectively reduces the charge carriers recombination rate by capturing photoelectrons, but also makes TiO2 NSs expose more highly active (001) facets to afford high-efficiency photogeneration of electron-hole pairs.

2D/2D/2D heterojunction of Ti3C2 MXene/MoS2 nanosheets/TiO2 nanosheets with exposed (001) facets toward enhanced photocatalytic hydrogen production activity

Seeking for a suitable cocatalyst to realize highly efficient photocatalytic hydrogen (H2) production is a great challenge in the field of solar energy conversion. Herein, hollow cobalt sulfide (Co...

Hollow CoSx Polyhedrons Act as High-Efficiency Cocatalyst for Enhancing the Photocatalytic Hydrogen Generation of g-C3N4

In this study, a novel surface initiated polymerization (SIP) method was developed from organic-inorganic hybrid persistent initiator coating (PIC) that embeds initiator molecules into inorganic silica sol-gel layer. Comparing with traditional silane initiator surface that prepared by chemical vapor deposition (CVD) method, the PIC can effectively improve the mechanical stability of initiator that was able to endure ten-thousand times of friction cycles. Besides, it allows polymer grafting from sub-surface and so the grafted brushes, poly 3-sulfopropyl methacrylate potassium salt (pSPMA) on the PIC were also much more wear-resisting than those prepared by the traditional ways. More importantly, the PIC could still trigger new polymerization reaction when the grafted brushes were worn off. In addition, the PIC is universal and can be covered on different substrates including glass, metals and plastics, etc. to realize functionalization of these materials. The approach may pave technological way for the application of surface grafted polymer brushes. 

Repeatedly Regenerating Mechanically Robust Polymer Brushes from Persistent Initiator Coating (PIC)

Single-atom catalysts are a family of heterogeneous electrocatalysts widely used in energy storage and conversion. The determination of the local structure of the active metal sites is challenging, which limits the establishment of the reliable structure-property relationship of single-atom catalysts. A carbon black-conjugated complex can be used as the model catalyst to probe the intrinsic activity of metal sites with certain local structures. In this work, we prepared carbon black-conjugated [Co(phenanthroline)Cl2], [Co(o-phenylenediamine)Cl2] and [Co(salophen)]. In these catalysts, the Co complexes with well-defined structures are anchored on the edge of carbon black by pyrazine moieties. The number of electrochemical accessible Co sites can be measured from the area of the redox peaks of pyrazine linkers in the cyclic voltammetry curve. Then, the intrinsic electrocatalytic activity of one Co site can be obtained. The catalytic performances of the three catalysts towards oxygen reduction reaction in alkaline conditions were measured. Carbon black-conjugated [Co(salophen)] showed the highest intrinsic activity with the turnover frequency of 0.72 s−1 at 0.75 V vs. the reversible hydrogen electrode. The strategy developed in this work can be used to explore and verify the possible local structure of active sites proposed for single-atom catalysts.

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Carbon-Conjugated Co Complexes as Model Electrocatalysts for Oxygen Reduction Reaction

Deformation characteristics and performance evolution of superalloy capillary drawn by electrically assisted microforming

The filling quality of micro-feature structures has a significant impact on the forming quality of micro-channels. The electrical-assisted forming technology can effectively improve the formability of difficult-to-deform materials. In this research, the electrically driven micro-compression constitutive model of SUS304 stainless steels was established to assign grain boundary and grain interior with different material properties. An electrical–thermal–mechanical coupling model was constructed to simulate the filling process considering the effect of grain boundary and grain size. Compared to the experimental results, the simulation indicated a good agreement in microstructure characteristics and higher filling height for the fine-grained material. The increase in grain boundary density makes the resistivity of the fine grain material larger, causing the current destiny and temperature of the specimen to increase with the decrease in grain size. An ellipsoidal gradient temperature distribution is observed due to the uneven current density. Because of the high geometric dislocation density near the grain boundary, a significant dislocation pile-up causes stress to concentrate. It is observed that the deformation coordination is enhanced between the grain boundary and grain core with the decrease in grain size, thus improving the material formability and forming quality.

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Effect of Grain Sizes on Electrically Assisted Micro—Filling of SUS304 Stainless Steel: Experiment and Simulation

The practical application of electrocatalytic water splitting is hindered by the sluggish anodic oxygen evolution reaction (OER), where the exploration of efficient and stable electrocatalysts toward water oxidation remains a great challenge. Herein, we report an active iron-doped ceria (FeOx/CeO2) catalyst with a highly disordered feature decorated on three-dimensional (3D) nickel foam, which can directly serve as the superior OER electrode in alkaline media. The highly disordered Fe-doped CeO2 catalyst displays remarkable OER performance with a low overpotential of 252 mV to achieve 10 mA cm–2, a small Tafel slope of 45 mV dec–1, and long-term durability for at least 48 h with a stable structure. The superior OER activity of FeOx/CeO2 is attributed to the lattice oxygen activation mechanism facilitated by its disordered structure as well as the high electrochemical surface area. This study provides valuable insights into the rational design of efficient OER catalysts through tailoring the catalyst structure and reaction pathway. 

Yizhe Liu

Papers

Repeatedly Regenerating Mechanically Robust Polymer Brushes from Persistent Initiator Coating (PIC)

Carbon-Conjugated Co Complexes as Model Electrocatalysts for Oxygen Reduction Reaction

Deformation characteristics and performance evolution of superalloy capillary drawn by electrically assisted microforming

Effect of Grain Sizes on Electrically Assisted Micro—Filling of SUS304 Stainless Steel: Experiment and Simulation

Highly Disordered Fe-Doped CeO2 with Oxygen Vacancies Facilitates Electrocatalytic Water Oxidation