Efficient Electrochemical Hydrogenation of Furfural to Furfuryl Alcohol Using an Anion-Exchange Membrane Electrolysis Cell.

The electrochemical hydrogenation (ECH) of furfural (FF) offers a promising pathway for the production of furfuryl alcohol (FA) while aligning with sustainability and environmental considerations. However, this technology has primarily been studied in half-cell configurations operating at high cell voltages and low current densities. Herein, we employ a membrane electrode assembly (MEA) system with an anion-exchange membrane for the ECH of FF and systematically investigate various parameters, including the ionomer content in the cathode catalyst, electrolyte type, electrolyte concentration, and flow rate. Under optimal conditions, our MEA system with non-noble metal-based catalysts exhibits a current density of 30 mA cm-2 with a Faradaic efficiency for FA production of 66% at a cell voltage of 2 V, maintaining operational durability for 5 h. This study highlights the potential of electrochemical FA production for practical applications to realize the decarbonization of the hydrogenation industry.

Nanocluster Surface Microenvironment Modulates Electrocatalytic CO2 Reduction.

The catalytic activity and product selectivity of the electrochemical CO2 reduction reaction (eCO2RR) depend strongly on the local microenvironment of mass diffusion at the nanostructured catalyst and electrolyte interface. Achieving a molecular-level understanding of the electrocatalytic reaction requires the development of tunable metal-ligand interfacial structures with atomic precision, which is highly challenging. Here, the synthesis and molecular structure of a 25-atom silver nanocluster interfaced with an organic shell comprising 18 thiolate ligands are presented. The locally induced hydrophobicity by bulky alkyl functionality near the surface of the Ag25 cluster dramatically enhances the eCO2RR activity (CO Faradaic efficiency, FECO: 90.3%) with higher CO partial current density (jCO) in an H-cell compared to Ag25 cluster (FECO: 66.6%) with confined hydrophilicity, which modulates surface interactions with water and CO2. Remarkably, the hydrophobic Ag25 cluster exhibits jCO as high as -240 mA cm-2 with FECO >90% at -3.4 V cell potential in a gas-fed membrane electrode assembly device. Furthermore, this cluster demonstrates stable eCO2RR over 120 h. Operando surface-enhanced infrared absorption spectroscopy and theoretical simulations reveal how the ligands alter the neighboring water structure and *CO intermediates, impacting the intrinsic eCO2RR activity, which provides atomistic mechanistic insights into the crucial role of confined hydrophobicity.

Surface Electrochemistry of Carbon Electrodes and Faradaic Reactions in Capacitive Deionization.

Recent advances in electrochemical desalination techniques have paved way for utilization of saline water. In particular, capacitive deionization (CDI) enables removal of salts with high energy efficiency and economic feasibility, while its applicability has been challenged by degradation of carbon electrodes in long-term operations. Herein, we report a thorough investigation on the surface electrochemistry of carbon electrodes and Faradaic reactions that are responsible for stability issues of CDI systems. By using bare and membrane CDI (MCDI) as model systems, we identified various electrochemical reactions of carbon electrodes with water or oxygen, with thermodynamics and kinetics governed by the electrode potential and pH. As a result, a complete overview of the Faradaic reactions taking place in CDI was constructed by tracing the physicochemical changes occurring in CDI and MCDI systems.

Self-supported mesoscopic tin oxide nanofilms for electrocatalytic reduction of carbon dioxide to formate.

Here we report a self-supported SnO2 nanofilm prepared by a robust electrochemical process as an electrocatalyst for the CO2 reduction reaction. The SnO2 film had a large surface area originating from its nano-architecture and manifested high selectivity toward formate (over 60%), which resulted in CO2-to-formate current density up to 33.66 mA cm-2 that is among the state-of-the-art. We unveiled that the high performance of the SnO2 nanofilm is attributable to the presence of a metastable oxide under reductive conditions in addition to the abovementioned advantages.

Less strained and more efficient GaN light-emitting diodes with embedded silica hollow nanospheres.

Light-emitting diodes (LEDs) become an attractive alternative to conventional light sources due to high efficiency and long lifetime. However, different material properties between GaN and sapphire cause several problems such as high defect density in GaN, serious wafer bowing, particularly in large-area wafers, and poor light extraction of GaN-based LEDs. Here, we suggest a new growth strategy for high efficiency LEDs by incorporating silica hollow nanospheres (S-HNS). In this strategy, S-HNSs were introduced as a monolayer on a sapphire substrate and the subsequent growth of GaN by metalorganic chemical vapor deposition results in improved crystal quality due to nano-scale lateral epitaxial overgrowth. Moreover, well-defined voids embedded at the GaN/sapphire interface help scatter lights effectively for improved light extraction, and reduce wafer bowing due to partial alleviation of compressive stress in GaN. The incorporation of S-HNS into LEDs is thus quite advantageous in achieving high efficiency LEDs for solid-state lighting.