A long-range synergistic effect between Ptn clusters and Zn1 single atoms for efficient selective hydrogenations†

IF 5.3 2区 材料科学 Q2 MATERIALS SCIENCE, MULTIDISCIPLINARY
Haisheng Wei, Jing Li, Xiaorui Yan, Tiantian Liu, Kairui Li, Dan Feng and Yujing Ren
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Abstract

Supported platinum group metal (PGM) catalysts are extensively utilized in catalytic hydrogenations. However, the adsorption energies on single PGM surfaces present the inherent scaling properties, which often lead to increased hydrogenation activity at the expense of selectivity. To address this challenge, we developed a space-separated strategy by confining few-atom Ptn clusters in Zn1-N3 sites decorated with microporous carbon material (Ptn@Zn1-N–C) to break the scaling relationship in selective hydrogenations. In detail, Ptn clusters are more favorable for H2 activation, while the Zn1-N3 single-atom sites can preferentially adsorb functional groups with electron-rich oxygen atoms. Benefiting from this long-range synergistic effect, the Ptn@Zn1-N–C catalyst displays superior catalytic performance in the selective hydrogenation of nitroarenes (>99% selectivity at ∼100% conversion, and sulfur compound-resistant hydrogenations) and excellent stability in the reverse water gas shift reaction (>99% selectivity over 40 hours at 600 °C). Our findings provide a confinement approach for further improving catalytic performance in selective hydrogenations.

Abstract Image

Ptn 簇和 Zn1 单原子之间的长程协同效应促进高效选择性加氢反应
负载型铂族金属 (PGM) 催化剂广泛应用于催化加氢反应。然而,单个铂族金属表面固有的吸附能缩放特性往往会导致氢化活性的提高而牺牲选择性。为了应对这一挑战,我们开发了一种空间隔离策略,通过在 Zn1-N3 位点装饰的微孔碳材料(Ptn@Zn1-N-C)中限制少原子 Ptn 团簇,来打破选择性加氢中的比例关系。具体来说,Ptn 团簇更有利于 H2 的活化,而 Zn1-N3 单原子位点可以优先吸附富含电子氧原子的官能团。得益于这种长程协同效应,Ptn@Zn1-N-C 催化剂在硝基烯烃的选择性加氢反应中表现出卓越的催化性能(99% 的选择性,转化率约为 100%,并具有抗硫化物加氢的特性),并在反向水煤气变换反应中表现出优异的稳定性(在 600°C 下反应 40 小时,99% 的选择性)。我们的研究结果为进一步提高选择性加氢的催化性能提供了一种限制性方法。
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来源期刊
CiteScore
8.30
自引率
3.40%
发文量
1601
期刊介绍: ACS Applied Nano Materials is an interdisciplinary journal publishing original research covering all aspects of engineering, chemistry, physics and biology relevant to applications of nanomaterials. The journal is devoted to reports of new and original experimental and theoretical research of an applied nature that integrate knowledge in the areas of materials, engineering, physics, bioscience, and chemistry into important applications of nanomaterials.
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