Accelerated Synthesis of TS‐2 Zeolite via 2D Heterogeneous Nucleation for Efficient H2O2 Production

Abstract MEL type c is crucial for addressing energy and environmental crises, yet efficient synthesis remains a challenge due to thermodynamic and kinetic limitations. In this work, TS‐2 as typical zeolite is successfully synthesized with high efficiency (12 h with 92% yield) by introducing titanate acid (TA) 2D nanosheet into a hydrothermal synthesis system. A newly defined TA/TS‐2 heterostructure is precisely identified as being incorporated into the zeolite framework via a heterogeneous nucleation mechanism. Ab initio molecular dynamics simulations deeply revealed the nucleation and growth mechanisms of the TA/TS‐2 heterostructure. The formation energy barrier of Ti─O─Si structural units (88 kJ mol−1) is much lower than that of Si─O─Si units (119 kJ mol−1), leading to more efficient growth of the Ti─O─Si structure. The polarized electronic properties of Ti─O─Si (negative LUMO orbital and larger polarization) further enhanced the reaction probability and stability of Ti─Si bonding. This obtained TA/TS‐2 heterostructure also demonstrated superior activity for photocatalytic production of hydrogen peroxide, which can be attributed to the abundant conductive band holes and narrow bandgap. This research provides an effective strategy for using 2D nanosheets to accelerate zeolite production, as well as an in‐depth molecular‐level insight into the nucleation and growth processes.