Electronic Phosphide–Support Interactions in Carbon-Supported Molybdenum Phosphide Catalysts Derived from Metal–Organic Frameworks

IF 9.6 1区材料科学 Q1 CHEMISTRY, MULTIDISCIPLINARY

Nano Letters Pub Date : 2023-11-16 DOI:10.1021/acs.nanolett.3c03217

Juncong Zou, Shaohua Wu, Yan Lin*, Shanying He*, Qiuya Niu, Xiang Li and Chunping Yang*,

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Abstract

Interfacial interaction in carbon-supported catalysts can offer geometric, electronic, and compositional effects that can be utilized to regulate catalytically active sites, while this is far from being systematically investigated in carbon-supported phosphide catalysts. Here, we proposed a novel concept of electronic phosphide–support interaction (EPSI), which was confirmed by using molybdenum phosphide (MoP) supported on nitrogen–phosphorus codoped carbon (NPC) as a model catalyst (MoP@NPC). Such a strong EPSI could not only stabilize MoP in a low-oxidation state under environmental conditions but also regulate its electronic structure, leading to reduced dissociation energy of the oxygen-containing intermediates and enhancing the catalytic activity for oxidative desulfurization. The removal of dibenzothiophene over the MoP@NPC was as high as 100% with a turnover frequency (TOF) value of 0.0027 s^–1, which was 33 times higher than that of MoP without EPSI. This work will open new avenues for the development of high-performance supported phosphide catalysts.

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金属-有机骨架碳负载磷化钼催化剂中的电子磷化-支持相互作用。

碳负载催化剂中的界面相互作用可以提供几何、电子和组成效应，可用于调节催化活性位点，而这在碳负载磷化物催化剂中还远远没有得到系统的研究。在此，我们提出了一个新的电子磷化物-载体相互作用(EPSI)的概念，并通过使用氮磷共掺杂碳(NPC)负载的磷化钼(MoP)作为模型催化剂(MoP@NPC)进行了验证。这种强EPSI不仅可以在环境条件下稳定MoP处于低氧化状态，还可以调节其电子结构，从而降低含氧中间体的解离能，增强氧化脱硫的催化活性。在MoP@NPC上对二苯并噻吩的去除率高达100%，TOF值为0.0027 s-1，是不加EPSI的MoP的33倍。这项工作将为高性能负载型磷化物催化剂的开发开辟新的途径。

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来源期刊

Nano Letters 工程技术-材料科学：综合

CiteScore

16.80

自引率

2.80%

发文量

1182

审稿时长

1.4 months

期刊介绍： Nano Letters serves as a dynamic platform for promptly disseminating original results in fundamental, applied, and emerging research across all facets of nanoscience and nanotechnology. A pivotal criterion for inclusion within Nano Letters is the convergence of at least two different areas or disciplines, ensuring a rich interdisciplinary scope. The journal is dedicated to fostering exploration in diverse areas, including: - Experimental and theoretical findings on physical, chemical, and biological phenomena at the nanoscale - Synthesis, characterization, and processing of organic, inorganic, polymer, and hybrid nanomaterials through physical, chemical, and biological methodologies - Modeling and simulation of synthetic, assembly, and interaction processes - Realization of integrated nanostructures and nano-engineered devices exhibiting advanced performance - Applications of nanoscale materials in living and environmental systems Nano Letters is committed to advancing and showcasing groundbreaking research that intersects various domains, fostering innovation and collaboration in the ever-evolving field of nanoscience and nanotechnology.