Xijun Cheng, Siyang Nie, Yuan Huang, Qingda Liu, Liang Wu, Xun Wang
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引用次数: 0
摘要
将本质上不相容的元素整合到一个单一的亚晶格中,形成单相金属氧化物,具有巨大的科学前景;它揭示了亚纳米材料中被忽视的表面熵可以在热力学上促进均匀单相结构的形成。本文提出了一种简便的方法,通过利用磷钼酸(PMA)团簇捕获无机核的潜力,抑制它们在溶热反应中的后续生长,从而合成多金属氧化物亚纳米颗粒(MMO-PMA SNBs)。实验和理论分析表明,MMO-PMA SNB 中的 PMA 不仅有助于亚纳米结构的形成,还能诱导催化位点的原位修饰。PMA 的电子转移以及过渡金属元素特性的丧失导致了电子析出,从而共同激活了反应位点。这种独特的结构使得五金属氧化物(PMO-PMA SNBs)在 1.34 V 的低电位下电流密度达到 10 mA cm-2,并在 10 mA cm-2 的尿素氧化反应(UOR)中保持稳定 24 小时。卓越的尿素氧化反应催化活性表明,多金属亚纳米结构在能源转换和环境修复方面具有广阔的应用前景。
Electron-Delocalization Across High Surface Entropy Sub-1 nm Nanobelts Toward Enhanced Electrocatalytic Urea Oxidation.
Integration of inherently incompatible elements into a single sublattice, resulting in the formation of monophasic metal oxide, holds great scientific promise; it unveils that the overlooked surface entropy in subnanometer materials can thermodynamically facilitate the formation of homogeneous single-phase structures. Here a facile approach is proposed for synthesizing multimetallic oxide subnanometer nanobelts (MMO-PMA SNBs) by harnessing the potential of phosphomolybdic acid (PMA) clusters to capture inorganic nuclei and inhibiting their subsequent growth in solvothermal reactions. Experimental and theoretical analyses show that PMA in MMO-PMA SNBs not only aids subnanometer structure formation but also induces in situ modifications to catalytic sites. The electron transfer from PMA, coupled with the loss of elemental identity of transition metals, leads to electron delocalization, jointly activating the reaction sites. The unique structure makes pentametallic oxide (PMO-PMA SNBs) achieve a current density of 10 mA cm-2 at a low potential of 1.34 V and remain stable for 24 h at 10 mA cm-2 on urea oxidation reaction (UOR). The exceptional UOR catalytic activity suggests a potential for utilizing multimetallic subnanometer nanostructures in energy conversion and environmental remediation.
期刊介绍:
Small serves as an exceptional platform for both experimental and theoretical studies in fundamental and applied interdisciplinary research at the nano- and microscale. The journal offers a compelling mix of peer-reviewed Research Articles, Reviews, Perspectives, and Comments.
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