Heteronuclear
double-atom catalysts, unlike single atom catalysts,
may change the charge density of active metal sites by introducing
another metal single atom, thereby modifying the adsorption energies
of reaction intermediates and increasing the catalytic activities.
First, density functional theory calculations are used to figure out
the best combination by modeling two transition-metal atoms from Fe,
Co, and Ni onto N-doped graphene. Generally, Fe and Co sites are highly
active for the oxygen reduction reaction (ORR) and the oxygen evolution
reaction (OER), respectively. The combination of Co and Fe to form
CoFe–N–C not only further improves the Fe’s ORR
and Co’s OER activities but also greatly enhances the Co site’s
ORR and Fe site’s OER activities. Then, we synthesize the CoFe–N–C
by a two-step pyrolysis process and find that the CoFe–N–C
exhibits exceptional ORR and OER electrocatalytic activities in alkaline
media, significantly superior to Fe–N–C and Co–N–C
and even commercial catalysts.
The ORCID identification number(s) for the author(s) of this article can be found under https://doi.org/10.1002/smll.202202071.
The development of low-Pt catalysts with high activity and durability is critical for fuel cells. Here, Pt-skin wrapped sub-5 nm PtCo intermetallic nanoparticles are successfully mounted on single atom Co-N-C support by exploiting the barrier effect of Co-anchor. According to a collaborative experimental and computational investigation, the increased oxygen reduction reaction activity of PtCo/Co-N-C arises from the direct electron transfer from PtCo to Co-N-C, and the resulting optimal d-band center of Pt. Owing to such unique electronic structure interaction and synergistic effect, the specific and mass activities of PtCo/Co-N-C are up to 4.20 mA cm −2 and 2.71 A mg Pt −1 , respectively, with barely degraded stability after 40 000 CV cycles. The PtCo/ Co-N-C also exhibits outstanding activity as an ethanol electrocatalyst. This work shows a new and effective route to boost the overall efficiency of direct ethanol fuel cells in acidic media by integrating intermetallic low-Pt alloys and single atom carbon support.
Nanostructured high-entropy materials such as alloys, oxides, etc., are attracting extensive attention because of their widely tunable surface electronic structure/catalytic activity through mixing different elements in one system. To further...
We report theoretical evidence of a liquid-liquid phase transition (LLPT) in liquid silicon carbide under nanoslit confinement. The LLPT is characterized by layering transitions induced by confinement and pressure, accompanying the rapid change in density. During the layering transition, the proportional distribution of tetracoordinated and pentacoordinated structures exhibits remarkable change. The tricoordinated structures lead to the microphase separation between silicon (with the dominant tricoordinated, tetracoordinated, and pentacoordinated structures) and carbon (with the dominant tricoordinated structures) in the layer close to the walls. A strong layer separation between silicon atoms and carbon atoms is induced by strong wall-liquid forces. Importantly, the pressure confinement phase diagram with negative slopes for LLPT lines indicates that, under high pressure, the LLPT is mainly confinement-induced, but under low pressure, it becomes dominantly pressure-induced.
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