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However, screening compatible guests with appropriate geometries and host\u2013guest interactions that could inhibit the dense packing of building blocks remains a primary challenge. This study presents a novel guest\u2010induced crystallization (GIC) strategy, guided by thermodynamic calculations, to develop porous hydrogen\u2010bonded organic frameworks (HOFs) using structurally challenging tetrazole building units. Thermodynamic principles are established from the crystal structure data and the density functional theory calculation of the formation energy (\n                    <jats:italic>\u0394E<\/jats:italic>\n                    ). This provides criteria to identify available guests in GIC, enabling the successful discovery of a hidden HOF that is kinetically challenging to crystallize. Furthermore, the potential application for\n                    <jats:italic>p<\/jats:italic>\n                    \u2010xylene (PX) separation is predicted by analyzing the\n                    <jats:italic>\u0394E<\/jats:italic>\n                    of guest\u2010induced HOFs. A high PX selectivity (PX\/\n                    <jats:italic>m<\/jats:italic>\n                    \u2010xylene=6.1, PX\/\n                    <jats:italic>o<\/jats:italic>\n                    \u2010xylene=7.2, and PX\/ethylbenzene=4.1) is achieved through selective inclusion of PX from C8 aromatic isomers within the guest\u2010induced HOFs. Significantly, the guest\u2010free HOF (\n                    <jats:bold>HOF\u2010PX\u2010a<\/jats:bold>\n                    ), bearing PX\u2010templated cavities derived from molecular imprinting, shows a record\u2010high PX\/ethylbenzene selectivity (21.7) in liquid adsorption. This work elucidates the underpinning self\u2010assembly rules of GIC for HOF construction, providing exciting new opportunities for the predictable assembly of PCMs for molecular recognition and target\u2010specific separations.\n                  <\/jats:p>","DOI":"10.1002\/anie.202423932","type":"journal-article","created":{"date-parts":[[2025,1,2]],"date-time":"2025-01-02T08:35:07Z","timestamp":1735806907000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":6,"title":["From Guest\u2010Induced Crystallization to Molecular Imprinting: Calculation\u2010Guided Discovery of Hydrogen\u2010Bonded Tetrazole Frameworks for\n                    <i>p<\/i>\n                    \u2010Xylene Separation"],"prefix":"10.1002","volume":"64","author":[{"given":"Yi","family":"Su","sequence":"first","affiliation":[{"name":"Collaborative Innovation Center of Advanced Nuclear Energy Technology Institute of Nuclear and New Energy Technology Tsinghua University  100084 Beijing China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Qiang","family":"Gao","sequence":"additional","affiliation":[{"name":"School of Materials Science and Engineering North Minzu University  750021 Yinchuan China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Xiaojun","family":"Ding","sequence":"additional","affiliation":[{"name":"Collaborative Innovation Center of Advanced Nuclear Energy Technology Institute of Nuclear and New Energy Technology Tsinghua University  100084 Beijing China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-7066-940X","authenticated-orcid":false,"given":"Gang","family":"Ye","sequence":"additional","affiliation":[{"name":"Collaborative Innovation Center of Advanced Nuclear Energy Technology Institute of Nuclear and New Energy Technology Tsinghua University  100084 Beijing China"}],"role":[{"vocabulary":"crossref","role":"author"}]}],"member":"311","published-online":{"date-parts":[[2025,1,10]]},"reference":[{"key":"e_1_2_8_1_1","doi-asserted-by":"publisher","DOI":"10.1021\/acscentsci.7b00146"},{"key":"e_1_2_8_2_1","doi-asserted-by":"publisher","DOI":"10.1002\/adfm.201909842"},{"key":"e_1_2_8_3_1","doi-asserted-by":"publisher","DOI":"10.1039\/D2CC04719E"},{"key":"e_1_2_8_4_1","doi-asserted-by":"publisher","DOI":"10.1039\/D4SC02628D"},{"key":"e_1_2_8_5_1","doi-asserted-by":"publisher","DOI":"10.1039\/D3CS00866E"},{"key":"e_1_2_8_6_1","first-page":"1","volume":"2400101","author":"Liu X.","year":"2024","journal-title":"Adv. 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