Since last decade, single atom catalysts have massive development in the field of propane dehydrogenation (PDH). In this study, both the catalytic activity and reaction mechanism of 3d, 4d, and 5d transition metal atom anchored on C₂N (TM-C₂N) for non-oxidative PDH are studied in detail using the density functional theory methods. Firstly, six stable catalysts (Cr-, Mn-, Fe-, Co-, Cu-, and Ag-C₂N) are screened out by calculating the difference between the formation energy of the single atom and the cohesive energy of the corresponding bulk metal. Combining the results of adsorption energy and density of states, it is demonstrated that propane and propylene can be stably adsorbed on all screened TM-C₂N. The calculated activation barrier and reaction energy of elementary reactions involved in PDH indicate that the initial C−H bond breaking step is determined as the rate-determining step on almost all the screened TM-C₂N catalysts. Among all studied TM-C₂N, the Fe-C₂N possesses excellent catalytic activity even better than other promising catalysts. In addition, the d-band center values of transition metal atoms in screened TM-C₂N show a stronger liner relationship with the interaction energy, suggesting that the d-band center may be served as a priority descriptor for the interaction energy between reaction species and catalyst surface rather than for the adsorption energy of reaction species.

近十年来，单原子催化剂在丙烷脱氢（PDH）领域取得了长足的发展。本研究采用密度泛函理论方法详细研究了锚定在C ₂ N（TM-C ₂ N）上的3d、4d和5d过渡金属原子对非氧化性PDH的催化活性和反应机理。首先，通过计算单个原子的形成能与相应原子的内聚能之差，筛选出六种稳定的催化剂（Cr-、Mn-、Fe-、Co-、Cu-和Ag-C ₂ N）。大块金属。结合吸附能和态密度的结果，证明丙烷和丙烯可以稳定地吸附在所有经过筛选的TM-C _2上。N. 计算的 PDH 中涉及的基本反应的活化能垒和反应能表明，在几乎所有筛选的 TM-C ₂ N 催化剂上，初始 C-H 键断裂步骤被确定为速率决定步骤。在所有研究的TM-C ₂ N中，Fe-C ₂ N具有优异的催化活性，甚至优于其他有前途的催化剂。此外，筛选的TM-C ₂ N中过渡金属原子的d带中心值与相互作用能表现出更强的线性关系，表明d带中心可以作为反应之间相互作用能的优先描述符。物种和催化剂表面而不是反应物种的吸附能量。