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Inspired by the catalytic mechanism of FLPs, we identify a previously overlooked pattern of frustrated br\u00f8nsted pairs (FBPs) in HZSM\u20105 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\u2010involved reactions and exhibiting unique dynamic behavior. Simulations of the methanol\u2010to\u2010hydrocarbons process, including isomerization, addition, decomposition, and substitution reactions, reveal that FBPs can dramatically smooth the free\u2010energy profile and reduce the energy span by nearly 1.00\u00a0eV. This work establishes the novel catalytic pattern of FBPs and uncovers its pivotal role in zeolite catalysis.<\/jats:p>","DOI":"10.1002\/anie.5832908","type":"journal-article","created":{"date-parts":[[2026,5,4]],"date-time":"2026-05-04T12:08:47Z","timestamp":1777896527000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":0,"title":["Frustrated Br\u00f8nsted Pairs: A Kind of Highly Active but Neglected Site in HZSM\u20105 Zeolite"],"prefix":"10.1002","volume":"65","author":[{"given":"Han\u2010Xuan","family":"Liu","sequence":"first","affiliation":[{"name":"State Key Laboratory of Fluorine &amp; Nitrogen Chemicals School of Chemical Engineering and Technology Xi'an Jiaotong University  Xi'an China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Zheng\u2010Qing","family":"Huang","sequence":"additional","affiliation":[{"name":"State Key Laboratory of Fluorine &amp; Nitrogen Chemicals School of Chemical Engineering 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