Surface Facets Reconstruction in Copper-Based Materials for Enhanced Electrochemical CO2 Reduction.

The unavoidable and unpredictable surface reconstruction of metallic copper (Cu) during the electrocatalytic carbon dioxide (CO2) reduction process is a double-edged sword affecting the production of high-value-added hydrocarbon products. It is crucial to control the surface facet reconstruction and regulate the targeted facets/facet interfaces, and further understand the mechanism between activity/selectivity and the reconstructed structure of Cu for CO2 reduction. Based on the current catalyst design methods, a facile strategy combining chemical reduction and electro-reduction is proposed to achieve specified Cu(111) facets and the Cu(110)/(111) interfaces in reconstructed Cu derived from cuprous oxide (Cu2O). The surface facet reconstruction significantly boosted the electrocatalytic conversion of CO2 into multi-carbon (C2+) products comparing to the unmodified catalyst. Theoretical and experimental analyses show that the Cu(110)/(111)s interface between Cu(110) and a small amount of Cu(111) can tailor the reaction routes and lower the reaction energy barrier of C-C coupling to ethylene (C2H4). The work will guide the surface facets reconstruction strategy for Cu-based CO2 electrocatalysts, providing a promising paradigm to understand the structural variation in catalysts.

Rational Design of Silicon Nanodots/Carbon Anodes by Partial Oxidization Strategy with High-Performance Lithium-Ion Storage.

Silicon (Si) is considered a promising anode material for rechargeable lithium-ion batteries (LIBs) due to its high theoretical capacity, low working potential, and safety features. However, the practical use of Si-based anodes is hampered by their huge volume expansion during the process of lithiation/delithiation, and they have relatively low intrinsic electronic conductivity, therefore seriously restricting their application in energy storage. Here, we propose a facile approach to directly transform siliceous biomass (bamboo leaves) into a porous carbon skeleton-wrapped Si nanodot architecture through a partial oxidization strategy and magnesium thermal reaction to obtain a high Si nanodot component composite (denoted as Si/C-O). With the synergistic effect of the porous carbon skeleton structure and uniformly dispersed Si nanodots, the Si/C-O composite anode with a stable structure that can avoid pulverization and accommodate volume expansion during cycling is fabricated. As expected, the biomass-converted Si/C-O anode not only presents a high Si component (59.7 wt %) by TGA but also exhibits an excellent capacity of 1013 mAh g-1 at 0.5 A g-1 and robust cycling stability with a capacity retention of 526 mAh g-1 after 650 cycles. Moreover, the Si/C-O anode demonstrates considerable performance in practical LIBs when assembled with a commercial LiNi0.8Co0.1Mn0.1O2 cathode. This work provides an effective strategy and long-term insights into the utilization of porous Si-based materials converted by biomass to design and synthesize high-performance LIB materials.

Electrolyte additive strategy enhancing the electrochemical performance of a soft-packed LiCoO2//graphite full cell.

During the development of high-capacity, ultra-stable battery electrode materials, battery performance, and safety issues are proved to be related to the properties of the electrolyte used. The employment of electrolyte additives is to improve the battery electrolyte properties. Representative commercial two-electrode LiCoO2//graphite pouch cells are used to study electrolyte additives represented by fluoroethylene carbonate (FEC) to improve the electrochemical stability of a commercial pouch full cell. The study reveals that a 1.5% FEC electrolyte additive has the best stability in the voltage range of 3.0-4.2 V.

Improving SERS Sensitivity toward Trace Sulfonamides: The Key Role of Trade-Off Interfacial Interactions among the Target Molecules, Anions, and Cations on the SERS Active Surface.

In recent years, ensuring the rational use and effective control of antibiotics has been a major focus in the eco-environment, which requires an effective monitoring method. However, on-site rapid detection of antibiotics in water environments remains a challenging issue. In this study, surface-enhanced Raman spectroscopy (SERS) was used to systematically achieve selective, rapid, and highly sensitive detection of sulfonamides, based on their fingerprint characteristics. The results show that the trade-off between the competitive and coadsorption behaviors of target molecules and agglomerates (inorganic salts) on the surface of the SERS substrate determines whether the molecules can be detected with high sensitivity. Based on this, the qualitative differentiation and quantitative detection of three structurally similar antibiotics, sulfadiazine, sulfamerazine, and sulfamethazine, were achieved, with the lowest detectable concentration being 1 µg/L for sulfadiazine and 50 µg/L for sulfamerazine and sulfamethazine.

Batch preparation of gold nanoparticles with highly uniform morphology and tunable plasmonic properties.

The plasmonic properties of individual metallic nanostructures are of great importance for application in surface science, materials science, and nanophotonics. Herein, being facilitated with a home-made flow device and pulsed laser irradiation, we proposed a batch preparation protocol towards spherical Au nanoparticles (Au NPs) and cage shell entrapped spherical core nanoparticles (Au@cAu NPs) with highly uniform morphology and a tunable size distribution. The Fano resonance behavior exhibited by the effective interaction between spherical Au NPs and the silicon surface has great potential for the design of ultrasensitive optical sensing devices. In comparison with the spherical Au NP, the individual Au@cAu NP displayed not only a red-shifted and broadened localized surface plasmon resonance (LSPR) scattering peak, but also a higher electromagnetic field enhancement. Therefore, the Au@cAu NPs offer a better choice for plasmonic enhancement-based applications in the red and near-infrared region. In general, the current work provides a new and easy method for the large-scale preparation of gold-based uniform nanostructures, and offers an avenue to understand the interference of different plasmon modes in plasmonic systems, which has potential applications in surface science.

Improved sensitivity and reproducibility in electrochemical detection of trace mercury (II) by bromide ion & electrochemical oxidation.

Nanostructured gold electrodes have been widely used for electrochemical trace analysis of Hg2+ because Hg2+ has superior specificity for the formation of gold amalgam. However, it is still very challenging to achieve both high sensitivity and reproducibility, especially for real environmental water samples due to surface poisoning by organic residues. In this work, we developed two strategies for addressing these challenges. First, we added NaBr (with a final concentration of 0.01 M) to the analytes; this enhanced the sensitivity by two orders of magnitude and improved the reproducibility to be better than RSD <15% because of the synergetic interaction of Br- with Hg2+ and gold at the interface. Second, we developed a pre-oxidation method using a glassy carbon electrode to remove organic residue from the analyte before Hg2+ analysis. The combination of these two approaches results in an efficient, reliable, and fast electrochemical detection technique for on-site trace analysis of Hg2+ that is in concentrations lower than that required by WHO for drinking water.