Modulation of the superficial electronic structure via metal–support interaction for H2 evolution over Pd catalysts,Chemical Science

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Modulation of the superficial electronic structure via metal–support interaction for H2 evolution over Pd catalysts
Chemical Science ( IF 7.6 ) Pub Date : 2021-1-4 , DOI: 10.1039/d0sc06795d
Jin Wang ₁ , Dan Cheng _{2,

3} , Mengmeng Gao ₁ , Qian Li ₁ , Ying Xin ₁ , Nana Zhang ₁ , Zhaoliang Zhang _{1,

4} , Xuehua Yu ₄ , Zhen Zhao ₄ , Kebin Zhou ₂

Affiliation

Electronic interactions can radically enhance the performance of supported metal catalysts and are critical for fundamentally understanding the nature of catalysts. However, at the microscopic level, the details of such interactions tuning the electronic properties of the sites on the metal particle's surface and metal–support interface remain obscure. Herein, we found polarized electronic metal–support interaction (pEMSI) in oxide-supported Pd nanoparticles (NPs) describing the enhanced accumulation of electrons at the surface of NPs (superficial Pd^δ−) with positive Pd atoms distributed on the interface (interfacial Pd^δ+). More superficial Pd^δ− species mean stronger pEMSI resulting from the synergistic effect of moderate Pd–oxide interaction, high structural fluxionality and electron transport activity of Pd NPs. The surface Pd^δ− species are responsible for improved catalytic performance for H₂ evolution from metal hydrides and formates. These extensive insights into the nature of supported-metal NPs may open new avenues for regulating a metal particle's electronic structure precisely and exploiting high-performance catalysts.

中文翻译：

通过金属-载体相互作用调节表面电子结构，以在Pd催化剂上释放氢气

电子相互作用可以从根本上提高负载型金属催化剂的性能，对于从根本上了解催化剂的性质至关重要。然而，在微观层面上，这种相互作用的细节仍不清楚，这些相互作用调节了金属颗粒表面和金属-载体界面上位点的电子特性。在此，我们在氧化物负载Pd纳米颗粒（NP），其描述在纳米粒子的表面的电子的增强累积发现极化电子的金属-载体相互作用（pEMSI）（浅表的Pd ^{δ -}）具有分布的界面上正的Pd原子（界面的Pd ^{δ +}）。比较浅的钯^{δ -}物种意味着适度的Pd-氧化物相互作用，高结构通量性和Pd NPs的电子传输活性的协同作用导致pEMSI增强。表面的Pd ^{δ -}物种是负责用于h改进的催化性能₂选自金属氢化物和甲进化。对负载金属NPs性质的广泛了解可能会为精确调节金属粒子的电子结构和开发高性能催化剂开辟新途径。

更新日期：2021-01-20

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