H₂S Sensing and Splitting on Atom‐Functionalized Carbon Nanotubes: A Theoretical Study

Strategies that can manipulate the electronic and chemical properties of carbon nanotubes (CNT) to meet a target application are challenging, and the introduction of atom functionalization is one path toward this goal. Herein, two types of Fe‐atom‐functionalized CNTs, Fe‐adsorbed CNTs (Fe@CNT) and Fe‐welded CNTs, the latter is a new hybrid material combining the merits of both carbon nanotubes and functional welding metals, are examined in terms of their sensitivity toward detecting hydrogen sulfide (H 2 S) and their selective activity toward chemically converting H 2 S into valuable fuel resources, for example, elemental sulfur and H 2 , in the framework of density functional theory (DFT) and the non‐equilibrium Green's function (NEGF) method. The catalytic center formed by the metal and the neighboring under‐coordinated carbon atoms in the Fe‐welded CNT provide an easy pathway for the splitting reaction of H 2 S molecules and sheds light on the design of efficient atom‐functionalized nanomaterials for other challenging chemical reactions.