Seawater electrolysis driven by offshore renewable energy is a promising avenue for large-scale hydrogen production but faces challenges in designing robust anodes that suppress surface chlorine reactions and corrosion at high current densities. Here we report a strategy by selectively docking PW12-polyoxometalate (PW12-POM) onto Fe sites of CoFe hydroxide anode to modulate the electronic structure of adjacent Co active centers and regulate Cl⁻/OH⁻ adsorption for efficient alkaline seawater oxidation. Our CoFe-based anode achieves low overpotentials, high catalytic selectivity, and notable durability, with continuous operation at 1 A cm⁻² for over 1300 hours and at 2 A cm⁻² more than 600 hours. Theoretical calculations and ex situ/in situ analyses reveal that PW12-POM coordination at Fe sites stabilizes Fe, suppresses its leaching, modulates Co acidity, promotes OH⁻ adsorption, and protects metal sites from Cl⁻ corrosion.
29 December 2018 in Critical Reviews in Analytical Chemistry
The present review focuses on the preparations, properties, and applications of zinc oxide (ZnO) nanomaterials in flexible functional devices. An overview is given on several methods for the growth of ZnO nanomaterials, including sputtering, sol-gel method, atomic layer deposition, all-inkjet-printing approach, electrochemical deposition, hydrothermal method. The broad applications of ZnO nanomaterials in solar cell, supercapacitors, flexible piezoelectric nanogenerators, ultraviolet photodetectors, photodiodes, porous three-dimensional (3-D) ceramics, functional surface coating, and sensors are also discussed.
Electrochemical CO2-reduction reaction (CO2RR) is a promising way to alleviate energy crisis and excessive carbon emission. The Cu-based electrocatalysts have been considered for CO2RR to generate hydrocarbons and alcohols. However, the application of Cu electrocatalysts has been restricted by a high onset potential for CO2RR and low selectivity. In this study, we have designed a series of Cu-based single-atom alloy catalysts (SAAs), denoted as TM1/Cu (111), by doping isolated 3d-transition metal (TM) atom onto the Cu (111) surface. We theoretically evaluated their stability and investigated the activity and selectivity toward CO2RR. Compared to the pure Cu catalyst, the majority TM1/Cu (111) catalysts are more favorable for hydrogenating CO2 and can efficiently avoid the hydrogen-evolution reaction due to the strong binding of carbonaceous intermediates. Based on the density functional theory calculations, instead of the HCOOH or CO products, the initial hydrogenation of CO2 on SAAs would form the *CO intermediate, which could be further hydrogenated to produce methane. In addition, we have identified the bond angle of adsorbed *CO2 can describe the CO2 activation ability of TM1/Cu (111) and the binding energy of *OH can describe the CO2RR activity of TM1/Cu (111). We speculated that the V/Cu (111) can show the best activity and selectivity for CO2RR among all the 3d-TM-doped TM1/Cu (111). This work could provide a rational guide to the design of new type of single-atom catalysts for efficient CO2RR.