§ Longcheng Zhang and Jie Liang contributed equally to this work. Benzoate anions-intercalated NiFe-LDH nanosheet on carbon cloth (BZ-NiFe-LDH/CC) behaves as a highly efficient and durable electrocatalyst for alkaline seawater oxidation. In alkaline seawater, it attains the current density of 500 mA cm -2 at a low overpotential of 610 mV for 100-h uninterrupted electrolysis with no obvious structural change, reflecting significantly boosted activity and resistance toward chlorine species corrosion.
Electrocatalytic two‐electron oxygen reduction has emerged as a promising alternative to the energy‐ and waste‐intensive anthraquinone process for distributed H2O2 production. This process, however, suffers from strong competition from the four‐electron pathway leading to low H2O2 selectivity. Herein, we report using a superhydrophilic O2‐entrapping electrocatalyst to enable superb two‐electron oxygen reduction electrocatalysis. The honeycomb carbon nanofibers (HCNFs) are robust and capable of achieving a high H2O2 selectivity of 97.3 %, much higher than that of its solid carbon nanofiber counterpart. Impressively, this catalyst achieves an ultrahigh mass activity of up to 220 A g−1, surpassing all other catalysts for two‐electron oxygen reduction reaction. The superhydrophilic porous carbon skeleton with rich oxygenated functional groups facilitates efficient electron transfer and better wetting of the catalyst by the electrolyte, and the interconnected cavities allow for more effective entrapping of the gas bubbles. The catalytic mechanism is further revealed by in situ Raman analysis and density functional theory calculations.
Direct
electrosynthesis of H2O2 via a two-electron
oxygen reduction reaction (2e– ORR) under ambient
conditions is emerging as a promising solution toward on-site applications
for the replacement of the energy-consuming, waste-intensive, and
indirect anthraquinone process. To date, state-of-the-art 2e– ORR catalysis is mostly performed with transition-metal-based materials,
while main-group element-based catalysts are much less established,
for which there is an urgent need of proper understanding. Herein,
we report a conductive two-dimensionally layered Mg3(hexaiminotriphenylene)2 electrocatalyst for selective hydrogenation of O2 to synthesize H2O2 (selectivity >90%) with
a robust high catalytic efficiency. In situ spectroscopic monitoring
of the catalytic reactions and kinetic studies not only illustrate
the reaction mechanisms on Mg3(hexaiminotriphenylene)2 but confirm that the Mg2+ center serving as the
real active site is responsible for the critical intermediate OOH*
forming event. Additionally, in-depth density functional theory calculations
further discuss the excellent activity and selectivity of Mg3(hexaiminotriphenylene)2 for H2O2 production.
Electrocatalytic N2 reduction is a sustainable alternative to the Haber-Bosch process for ambient NH3 synthesis, but it needs efficient and stable catalysts. Herein, a hybrid of TiO2 and juncus effusus-derived...
The exploration of high-efficiency, robust and low-cost electrocatalysts for the hydrogen peroxide (H2O2) production receives increasing attention due to its key role in developing a new alternative to replace the...
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