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Freestanding Single-Atom-Layer Pd-Based Catalysts: Oriented Splitting of Energy Bands for Unique Stability and Activity
Chem ( IF 19.1 ) Pub Date : 2019-11-21 , DOI: 10.1016/j.chempr.2019.11.003
Jinxia Jiang , Wei Ding , Wei Li , Zidong Wei

Freestanding and self-stabilized single-atom-layer (SAL) palladium (Pd) and palladium-cobalt (PdCo) alloy films were generated in the angstrom-sized interlayer space of layered minerals, where the metal only grows and spreads out in two dimensions. The SAL films display strongly coordinated metallic bonds in two dimensions and dangling bonds in the z direction. Under such absolute two-dimensional coordination, their valence-empty band exhibits an unusual split into a lower-energy band in the x-y plane, which promotes in-plane stability, and a higher-energy band in the z direction, which contributes to reactivity along this axis. This gives rise to exceptional properties and functions that cannot be achieved by analogs of other dimensionalities. Specifically, the SAL PdCo alloy exhibits six times higher mass activity than commercial platinum (Pt) nanoparticles in oxygen reduction. Its mass activity is also eight times higher than that of Pd nanoparticles for formic acid oxidation.



中文翻译:

独立式单原子层钯基催化剂:能带定向分裂,具有独特的稳定性和活性

在层状矿物的埃级夹层空间中生成独立且自稳定的单原子层(SAL)钯(Pd)和钯钴(PdCo)合金膜,其中金属仅以二维生长和扩散。SAL膜在二维方向上显示出高度协调的金属键,并在z方向上显示悬空键。在这样的绝对二维配位下,它们的价空带在xy平面上表现出不同寻常的分裂,形成较低的能带,从而促进了平面内的稳定性,而在z方向则呈现出较高的能带,从而促进了反应性。沿着这个轴。这产生了其他维数无法实现的卓越性能和功能。具体来说,SAL PdCo合金在氧还原方面的质量活性是市售铂(Pt)纳米颗粒的六倍。其质量活性也比用于甲酸氧化的Pd纳米颗粒的质量活性高八倍。

更新日期:2019-11-21
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