Single‐Mn‐Atom Chains Anchored on Carbon Nanotubes for Efficient Naphthalene Hydrocracking

ABSTRACT The design of efficient catalysts with high atomic utilization is crucial for effective conversion of polycyclic aromatic hydrocarbons (PAHs) in heavy oil of petroleum. Inspired by recent experimental advances in the successful synthesis of single‐metal‐atom chains confined within 2D semiconductors [ Nat. Commun . 2025, 16, 4924], we design a series of single metal atoms arranged along nanoscale substrates as space‐tunable single‐metal‐atom chain catalysts for heavy oil hydrocracking. Using naphthalene as a prototypical PAH, we perform first‐principles calculations combined with rational screening over transition metal series (TM = Ti, V, Cr, Mn, Fe, Co, Ni, Cu, Zn, Zr, Nb, Mo, W) to identify the most promising candidate of single atom chains anchored on CNTs(n, n) (n = 4, 6, 8, 10). Our results show that MnN 4 @CNT(8, 8) emerges as the most promising candidate for a high‐performance catalyst, demonstrating excellent hydrogenation activity with a low energy barrier of 1.47 eV for the rate‐determining step (2 β → 3 β ), as well as efficient C─C bond cleavage in tetralin with an energy barrier of 1.92 eV. This work demonstrates the potential of single‐metal‐atom chains as superior catalysts for heavy oil hydrocracking.