ABSTRACT Frustrated Lewis Pairs (FLPs) have been well‐established as highly efficient catalytic sites that function through electron transfer from Lewis base to Lewis acid coupled with substrate activation. Inspired by the catalytic mechanism of FLPs, we identify a previously overlooked pattern of frustrated brønsted pairs (FBPs) in HZSM‐5 zeolite, which function via a concerted proton transfer paradigm. This FBP active site comprises two conjugate structures whose interconversion drives swift hydrogen transfer in substrates, thereby enabling the highly efficient catalysis of a variety of hydrogen‐involved reactions and exhibiting unique dynamic behavior. Simulations of the methanol‐to‐hydrocarbons process, including isomerization, addition, decomposition, and substitution reactions, reveal that FBPs can dramatically smooth the free‐energy profile and reduce the energy span by nearly 1.00 eV. This work establishes the novel catalytic pattern of FBPs and uncovers its pivotal role in zeolite catalysis.
Liu et al. (Mon,) studied this question.
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