Engineering
the morphology and electronic properties simultaneously
of emerging metallene materials is an effective strategy for enhancing
their performance as oxygen reduction reaction (ORR) electrocatalysts.
Herein, a highly efficient and stable ORR electrocatalyst, Fe-doped
ultrathin porous Pd metallene (Fe–Pd UPM) composed of a few
layers of 2D atomic metallene layers, was synthesized using a simple
one pot wet-chemical method and characterized. Fe–Pd UPM was
measured to have enhanced ORR activity compared to undoped Pd metallene.
Fe–Pd UPM exhibits a mass activity of 0.736 A mgPd
–1 with a loss of mass activity of only 5.1% after
10 000 cycles at 0.9 V versus the reversible hydrogen electrode
(vs RHE) in 0.1 M KOH solution. Density functional theory (DFT) calculations
reveal that the stable Fe dopant in the inner atomic layers of Fe–Pd
UPM delivers a much smaller overpotential during O* hydrogenation
into OH*. The morphology, porous structure, and Fe doping were verified
to have enhanced ORR activity. We believe that the rational design
of metallene materials with porous structures and interlayer doping
is promising for the development of efficient and stable electrocatalysts.
We report a synergistic confinement strategy for high-entropy alloys nanoparticles (HEA-NPs) synthesis. The carbon nitride substrate and polydopamine coating layer synergistically confine the NPs growth and contribute to the homogeneous...
Tuning the electronic property of active center to balance the adsorption ability and reactivity of oxygen is essential for achieving 2e− oxygen reduction reaction (ORR) for electrocatalytic synthesis of hydrogen peroxide (H2O2), still represents a grand challenge. Herein, different by‐design building blocks are introduced to regulate the electronic structure of catalytically active centers in covalent organic frameworks (COFs). Theoretical calculation reveals that adsorption ability of oxygen molecule (O2) can be finely tuned by the regulation of electronic structure and the binding strength of O2 is positively correlated with the electron donating ability of active center. As a result, the newly designed TP‐TD‐COF shows higher 2e− ORR activity and selectivity owing to the stronger electron donating ability and the higher adsorption strength of O2 on electron‐rich active center. This study reveals fundamental structure–activity relationship in H2O2 synthesis and offers a strategy for designing metal‐free COF catalysts through rational modulation of their electronic properties at molecular level.
We developed a series of single atom catalysts (SACs) anchored on bipyridine-rich COFs. By tuning the active metal center, the optimal Py-Bpy-COF-Zn shows the highest selectivity of 99.1% and excellent...
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