Prats Hector, Stamatakis Michail
Department of Chemical Engineering, University College London Roberts Building, Torrington Place London WC1E 7JE UK
Nanoscale Adv. 2023 May 25;5(12):3214-3224. doi: 10.1039/d3na00231d. eCollection 2023 Jun 13.
Small particles of transition metals (TM) supported on transition metal carbides (TMC) - TM@TMC - provide a plethora of design opportunities for catalytic applications due to their highly exposed active centres, efficient atom utilisation and the physicochemical properties of the TMC support. To date, however, only a very small subset of TM@TMC catalysts have been tested experimentally and it is unclear which combinations may best catalyse which chemical reactions. Herein, we develop a high-throughput screening approach to catalyst design for supported nanoclusters based on density functional theory, and apply it to elucidate the stability and catalytic performance of all possible combinations between 7 monometallic nanoclusters (Rh, Pd, Pt, Au, Co, Ni and Cu) and 11 stable support surfaces of TMCs with 1 : 1 stoichiometry (TiC, ZrC, HfC, VC, NbC, TaC, MoC and WC) towards CH and CO conversion technologies. We analyse the generated database to unravel trends or simple descriptors in their resistance towards metal aggregate formation and sintering, oxidation, stability in the presence of adsorbate species, and study their adsorptive and catalytic properties, to facilitate the discovery of novel materials in the future. We identify 8 TM@TMC combinations as promising catalysts, all of them being new for experimental validation, thus expanding the chemical space for efficient conversion of CH and CO.
负载于过渡金属碳化物(TMC)上的过渡金属(TM)小颗粒——TM@TMC,由于其高度暴露的活性中心、高效的原子利用率以及TMC载体的物理化学性质,为催化应用提供了大量的设计机会。然而,迄今为止,仅有极少数的TM@TMC催化剂经过了实验测试,尚不清楚哪些组合可能最适合催化哪些化学反应。在此,我们基于密度泛函理论开发了一种用于负载型纳米团簇催化剂设计的高通量筛选方法,并将其应用于阐明7种单金属纳米团簇(Rh、Pd、Pt、Au、Co、Ni和Cu)与11种化学计量比为1:1的稳定TMC载体表面(TiC、ZrC、HfC、VC、NbC、TaC、MoC和WC)之间所有可能组合对于CH和CO转化技术的稳定性及催化性能。我们分析生成的数据库,以揭示它们在抵抗金属聚集体形成和烧结、氧化、在吸附质存在下的稳定性方面的趋势或简单描述符,并研究它们的吸附和催化性能,以便在未来促进新型材料的发现。我们确定了8种TM@TMC组合为有前景的催化剂,所有这些组合都是有待实验验证的新组合,从而扩展了CH和CO高效转化的化学空间。