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近年来,单一原子或单一位点催化剂因其独特的结构和电子特性受到催化研究人员的广泛关注.目前,多种无机固体材料被用作限域该类单原子催化剂,包括传统的金属氧化物、沸石分子筛以及金属有机框架配合物等.载体的性质会显著地影响单原子的催化性能,因此具有独特物理化学性质的二维材料无疑是限域单原子的一类理想介质,并逐渐引起了人们在该领域的研究兴趣.二维材料兴起于石墨烯的成功剥离,随后其他类似物如氮化硼、氮化碳以及二硫化钼等蓬勃发展起来.结构简单明确且性质独特的二维材料自身就是一类新颖的催化剂,其与单原子的结合将会为催化带来更多新的可能.二维材料限域单原子催化剂的潜在优势如下:(1)二维材料独特的电子结构对单原子中心的电子特性有显著的调变作用,使其催化性能更为独特;(2)二维材料通常具有巨大的比表面积,这允许其锚定更多的单原子从而显著提高其活性位密度;(3)单原子层二维材料有利于反应物分子从双向接触其表面限域的单原子位点,增加碰撞几率并降低传质阻力;(4)二维材料限域单原子催化剂可被视为理想的模型催化剂,其结构均一的活性中心有利于催化剂构效关系的研究;(5)二维材料限域的单原子能够反过来促进或激活二维材料的本征催化活性.在这里,我们总结了二维材料限域单原子催化剂的最新进展,其中二维材料主要涉及石墨烯、氮化碳和硫化钼.我们围绕在二维材料限域单原子催化剂中什么是真正的活性位点及其如何协同催化等问题进行了讨论,进而展望了二维材料限域单原子催化剂的应用前景和挑战.
In recent years, single-atom or single-site catalysts have attracted the attention of catalytic researchers due to their unique structural and electronic properties.At present, a variety of inorganic solid materials are used to confine such monatomic catalysts, including traditional metal oxides , Zeolites and metal-organic framework complexes, etc. The nature of the support will significantly affect the catalytic performance of the monatomic, so the two-dimensional material with unique physicochemical properties is undoubtedly a kind of ideal medium for limiting the single atom and gradually induces People in the field of research interest.Dimensional material rose in the successful dissection of graphene, followed by the development of other analogues such as boron nitride, carbonitride and molybdenum disulfide, etc. Structure simple and clear and unique two-dimensional material It is a kind of novel catalyst in itself, and its combination with monoatoms will bring more new possibilities for catalysis. The potential advantages of two-dimensional materials in confining monatomic catalysts are as follows: (1) The unique electronic structure of 2D materials The electronic properties of monatomic centers have a remarkable modulation effect, making their catalytic properties more unique. (2) Two-dimensional materials usually have huge specific surface area, which Allowing it to anchor more monatomic atoms to significantly increase its active site density. (3) The monolayer of two-dimensional material facilitates the bi-directional contact of reactant molecules with the monomolecular sites of its surface confinement, increasing the probability of collisions and decreasing the mass transfer (4) The single-atom catalyst with two-dimensional material confinement can be regarded as the ideal model catalyst. The uniform active sites in the structure contribute to the study of the structure-activity relationship of the catalyst. (5) Which in turn promotes or activates the intrinsic catalytic activity of two-dimensional materials. Here, we summarize recent advances in two-dimensional material-confined monoatomic catalysts, where the two-dimensional materials are mainly related to graphene, carbon nitride and molybdenum sulfide. What are the true active sites in the two-dimensional material confined monatomic catalyst and how they are synergistically catalyzed are discussed, and then the application prospects and challenges of the two-dimensional material confined monatomic catalyst are prospected.