Bottom-Up Synthesis Strategies Enabling the Investigation of Metal Catalyst-Carbon Support Interactions
Bottom-Up Synthesis Strategies Enabling the Investigation of Metal Catalyst-Carbon Support Interactions
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DOI：
10.3390/c8030037
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发表时间：
2022-06
期刊：
影响因子：
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通讯作者：
H. Bateni;Prathamesh T. Prabhu;Hannah E. Gebur;J. Tessonnier
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作者：
H. Bateni;Prathamesh T. Prabhu;Hannah E. Gebur;J. Tessonnier
碳材料结构的多功能性和活跃的表面化学性质为通过调节界面金属-载体相互作用（MSI）来调整负载金属纳米颗粒的催化性能提供了巨大的机会。MSI的几何和结构效应对这些材料都有很好的记录。然而，其他潜在的支持效应，如电子金属-碳相互作用，仍然知之甚少。这些限制与常用的碳材料（如活性炭）固有的限制（例如，微孔）以及通常用于其合成的自上而下的方法有关。尽管如此，了解碳负载金属催化剂的结构、性质和性能之间的相互作用对于合理设计它们是至关重要的。本研究探讨了有前途和可扩展的自下而上的合成方法，即热液碳化（HTC）和蒸发诱导自组装（EISA），它们为控制碳结构提供了很大的灵活性。讨论了这些方法的机会和局限性，特别着重于利用氧官能团的力量。EISA法合成介孔碳的产率达到了32.8%。此外，这些碳材料的外表面积为316±19 m2/g，平均孔径为10.0±0.1 nm，同时可以灵活地将氧浓度控制在5-26 wt%的范围内。该研究为进一步研究金属-碳载体相互作用和合理设计催化剂提供了基础。
The structural versatility and vibrant surface chemistry of carbon materials offer tremendous opportunities for tailoring the catalytic performance of supported metal nanoparticles through the modulation of interfacial metal-support interactions (MSI). MSI’s geometric and structural effects are well documented for these materials. However, other potential support effects such as electronic metal-carbon interactions remain poorly understood. Such limitations are tied to constraints intrinsic to commonly available carbon materials such as activated carbon (e.g., microporosity) and the top-down approach that is often used for their synthesis. Nonetheless, it is crucial to understand the interplay between the structure, properties, and performance of carbon-supported metal catalysts to take steps toward rationalizing their design. The present study investigates promising and scalable bottom-up synthesis approaches, namely hydrothermal carbonization (HTC) and evaporation-induced self-assembly (EISA), that offer great flexibility for controlling the carbon structure. The opportunities and limitations of the methods are discussed with a particular focus on harnessing the power of oxygen functionalities. A remarkable production yield of 32.8% was achieved for mesoporous carbons synthesized via EISA. Moreover, these carbon materials present similar external surface areas of 316 ± 19 m2/g and average pore sizes of 10.0 ± 0.1 nm while offering flexibility to control the oxygen concentration in the range of 5–26 wt%. This study provides the cornerstone for future investigations of metal-carbon support interactions and the rational design of these catalysts.