Abstract
Although single-atom catalysts significantly improve the atom utilization efficiency, the multistep preparation procedures are complicated and difficult to control. Herein, we demonstrate that one-step in situ synthesis of the single-atom Pt anchored in single-crystal MoC (Pt1/MoC) by using facile and controllable arc-discharge strategy under extreme conditions. The high temperature (up to 4000°C) provides the sufficient energy for atom dispersion and overall stability by forming thermodynamically favourable metal-support interactions. The high-temperature-stabilized Pt1/MoC exhibits outstanding performance and excellent thermal stability as durable catalyst for selective quinoline hydrogenation. The initial turnover frequency of 3710 h−1 is greater than those of previously reported samples by an order of magnitude under 2 MPa H2 at 100°C. The catalyst also shows broad scope activity toward hydrogenation containing unsaturated groups of C=C, C=N, and C=O. The facile, one-step, and fast arc-discharge method provides an effective avenue for single-atom catalyst fabrication that is conventionally challenging.
Highlights
Single-atom catalysts (SACs) with unique electronic/geometric structures exhibit more effective atom utilization and can act as a promising bridge between homogeneous and heterogeneous catalysis [1,2,3,4,5,6,7,8,9,10,11,12,13,14]
molybdenum carbide (MoC) and Pt/MoC were synthesized via the facile one-step high-temperature arc-discharge strategy (Figures 1(a) and S1) [45, 46]
X-ray diffraction (XRD) patterns presented in Figure S4 clearly show the exclusive presence of MoC phase with the face-centered-cubic α-MoC structure [37]
Summary
Single-atom catalysts (SACs) with unique electronic/geometric structures exhibit more effective atom utilization and can act as a promising bridge between homogeneous and heterogeneous catalysis [1,2,3,4,5,6,7,8,9,10,11,12,13,14]. It was reported that the presence of subnanometer clusters in SACs can affect the overall thermal stability [18,19,20,21,22,23]. The multistep procedures and complicated processes generally breed the inevitable difficulty in precise controlling of the atomic dispersion. It can lead to the waste of resources and the generation of environmentally unfriendly by-products. High-temperature-assisted routes (e.g., pyrolysis, fusion, and high-temperature shockwave) have been successfully utilized to synthesize the SACs and attract ever-increasing attention [32,33,34,35,36].
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