Realizing stable and efficient overall water splitting is highly desirable for sustainable and efficient hydrogen production yet challenging because of the rapid deactivation of electrocatalysts during the acidic oxygen evolution process. Here, we report that the single-site Pt-doped RuO
2
hollow nanospheres (SS Pt-RuO
2
HNSs) with interstitial C can serve as highly active and stable electrocatalysts for overall water splitting in 0.5 M H
2
SO
4
. The performance toward overall water splitting have surpassed most of the reported catalysts. Impressively, the SS Pt-RuO
2
HNSs exhibit promising stability in polymer electrolyte membrane electrolyzer at 100 mA cm
−2
during continuous operation for 100 hours. Detailed experiments reveal that the interstitial C can elongate Ru-O and Pt-O bonds, and the presence of SS Pt can readily vary the electronic properties of RuO
2
and improve the OER activity by reducing the energy barriers and enhancing the dissociation energy of
*
O species.
Amorphous materials have attracted increasing attention in diverse fields due to their unique properties, yet their controllable fabrications still remain great challenges. Here, we demonstrate a top-down strategy for the fabrications of amorphous oxides through the amorphization of hydroxides. The versatility of this strategy has been validated by the amorphizations of unitary, binary and ternary hydroxides. Detailed characterizations indicate that the amorphization process is realized by the variation of coordination environment during thermal treatment, where the M–OH octahedral structure in hydroxides evolves to M–O tetrahedral structure in amorphous oxides with the disappearance of the M–M coordination. The optimal amorphous oxide (FeCoSn(OH)6-300) exhibits superior oxygen evolution reaction (OER) activity in alkaline media, where the turnover frequency (TOF) value is 39.4 times higher than that of FeCoSn(OH)6. Moreover, the enhanced OER performance and the amorphization process are investigated with density functional theory (DFT) and molecule dynamics (MD) simulations. The reported top-down fabrication strategy for fabricating amorphous oxides, may further promote fundamental research into and practical applications of amorphous materials for catalysis.
Developing a versatile electrocatalyst with remarkable performance viable for pH-universal overall water splitting is increasingly important for the industrial production of renewable energy conversion. Herein, our theoretical calculations predicate that...
The physicochemical properties and catalytic performance
of transition
metals are highly phase-dependent. Ru-based nanomaterials are superior
catalysts toward hydrogen evolution reaction (HER) and hydrogen oxidation
reaction (HOR), but studies are mostly limited to conventional hexagonal-close-packed
(hcp) Ru, mainly arising from the difficulty in synthesizing Ru with
pure face-centered-cubic (fcc) phase. Herein, we report a crystal-phase-dependent
catalytic study of MoO
x
-modified Ru (MoO
x
-Ru fcc and MoO
x
-Ru hcp) for bifunctional HER and HOR. MoO
x
-Ru fcc is proven to outperform MoO
x
-Ru hcp in catalyzing both HER and HOR with much higher catalytic
activity and more durable stability. The modification effect of MoO
x
gives rise to optimal adsorption of H and
OH especially on fcc Ru, which thus has resulted in the superior catalytic
performance. This work highlights the significance of phase engineering
in constructing superior electrocatalysts and may stimulate more efforts
on phase engineering of other metal-based materials for diversified
applications.
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