No abstract

In hydrogen production, the anodic oxygen evolution reaction (OER) limits the energy conversion efficiency and also impacts stability in proton-exchange membrane water electrolyzers. Widely used Ir-based catalysts suffer from insufficient activity, while more active Ru-based catalysts tend to dissolve under OER conditions. This has been associated with the participation of lattice oxygen (lattice oxygen oxidation mechanism (LOM)), which may lead to the collapse of the crystal structure and accelerate the leaching of active Ru species, leading to low operating stability. Here we develop Sr–Ru–Ir ternary oxide electrocatalysts that achieve high OER activity and stability in acidic electrolyte. The catalysts achieve an overpotential of 190 mV at 10 mA cm–2 and the overpotential remains below 225 mV following 1,500 h of operation. X-ray absorption spectroscopy and 18O isotope-labeled online mass spectroscopy studies reveal that the participation of lattice oxygen during OER was suppressed by interactions in the Ru–O–Ir local structure, offering a picture of how stability was improved. The electronic structure of active Ru sites was modulated by Sr and Ir, optimizing the binding energetics of OER oxo-intermediates.

The electrocatalytic urea oxidation reaction (UOR) provides more economic electrons than water oxidation for various renewable energy‐related systems owing to its lower thermodynamic barriers. However, it is limited by sluggish reaction kinetics, especially by CO2 desorption steps, masking its energetic advantage compared with water oxidation. Now, a lattice‐oxygen‐involved UOR mechanism on Ni4+ active sites is reported that has significantly faster reaction kinetics than the conventional UOR mechanisms. Combined DFT, 18O isotope‐labeling mass spectrometry, and in situ IR spectroscopy show that lattice oxygen is directly involved in transforming *CO to CO2 and accelerating the UOR rate. The resultant Ni4+ catalyst on a glassy carbon electrode exhibits a high current density (264 mA cm−2 at 1.6 V versus RHE), outperforming the state‐of‐the‐art catalysts, and the turnover frequency of Ni4+ active sites towards UOR is 5 times higher than that of Ni3+ active sites.

Aerogels are synthetic porous materials derived from sol-gel materials in which the liquid component has been replaced with gas to leave intact solid nanostructures without pore collapse. Recently, aerogels based on natural or synthetic polymers, called polymer or organic aerogels, have been widely explored due to their porous structures and unique properties, such as high specific surface area, low density, low thermal conductivity and dielectric constant. This paper gives a comprehensive review about the most recent progresses in preparation, structures and properties of polymer and their derived carbon-based aerogels, as well as their potential applications in various fields including energy storage, adsorption, thermal insulation and flame retardancy. To facilitate further research and development, the technical challenges are discussed, and several future research directions are also suggested in this review.

Self-standing membranes of porous carbon nanofiber (PCNF)@MoS2 core/sheath fibers have been facilely obtained through a combination of electrospinning, high-temperature carbonization and the solvothermal reaction. PCNF fibers with porous channels are used as building blocks for the construction of hierarchical PCNF@MoS2 composites where thin MoS2 nanosheets are uniformly distributed on the PCNF surface. Thus, a three-dimensional open structure is formed, which provides a highly conductive pathway for rapid charge-transfer reactions, as well as greatly improving the surface active sites of MoS2 for fast lithiation/delithiation of Li(+) ions. The highly flexible PCNF@MoS2 composite membrane electrode exhibits synergistically improved electrochemical performance with a high specific capacity of 954 mA h g(-1) upon the initial discharge, a high rate capability of 475 mA h g(-1) even at a high current density of 1 A g(-1), and good cycling stability with almost 100% retention after 50 cycles, indicating its potential application as a binder-free anode for high-performance lithium-ion batteries.