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The porphyrin\u2010based HOF, PFC\u201045\u2010Co, is assembled from electron\u2010donating 5,10,15,20\u2010tetra(4\u2010carboxyphenyl)porphyrin (Co\u2010TPyP) and electron\u2010accepting cobalt 5,10,15,20\u2010tetra(4\u2010carboxyphenyl)porphyrin (Co\u2010TCPP) through strong O\u2500H\u00b7\u00b7\u00b7N hydrogen bonds, while periodic alternating interlayer \u03c0\u2013\u03c0 stacking generates vertical D\u2013A heterojunctions. Mechanistic studies show that close \u03c0\u2013\u03c0 contacts enable through\u2010space charge transport, and the D\u2013A energy offset drives electron transfer from Co\u2010TPyP to Co\u2010TCPP, producing electron\u2010enriched Co\u2010TCPP sites that promote CO\n                    <jats:sub>2<\/jats:sub>\n                    activation and suppress hydrogen evolution. As a result, PFC\u201045\u2010Co outperforms the single\u2010component HOF PFC\u201072\u2010Co in both neutral and acidic media. In neutral electrolyte, PFC\u201045\u2010Co delivers a CO Faradaic efficiency (FE\n                    <jats:sub>CO<\/jats:sub>\n                    ) of 98.4% at \u22120.9 V versus reversible hydrogen electrode (vs. RHE) and a CO partial current density (\n                    <jats:italic>j<\/jats:italic>\n                    <jats:sub>CO<\/jats:sub>\n                    ) of 31.3 mA cm\n                    <jats:sup>\u22122<\/jats:sup>\n                    at \u22121.2 V versus RHE. In acidic media, it maintains FE\n                    <jats:sub>CO<\/jats:sub>\n                    values of 92%\u201399% and achieves\n                    <jats:italic>j<\/jats:italic>\n                    <jats:sub>CO<\/jats:sub>\n                    of 111.1 mA cm\n                    <jats:sup>\u22122<\/jats:sup>\n                    at \u22121.6 V versus RHE. This work establishes interlayer van der Waals D\u2013A heterojunctions as an effective motif for regulating charge transfer in HOF electrocatalysts.\n                  <\/jats:p>","DOI":"10.1002\/anie.4407565","type":"journal-article","created":{"date-parts":[[2026,9,23]],"date-time":"2026-09-23T08:43:13Z","timestamp":1790152993000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":0,"title":["Engineering van der Waals Heterojunctions Within a 2D Hydrogen\u2010Bonded Organic Framework for Boosting CO\n                    <sub>2<\/sub>\n                    Electroreduction"],"prefix":"10.1002","author":[{"given":"Qiu\u2010Jin","family":"Wu","sequence":"first","affiliation":[{"name":"Fujian Institute of Research on the Structure of Matter Chinese Academy of Sciences  Fujian, Fuzhou P.R. 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R.China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Jia\u2010Tong","family":"Huang","sequence":"additional","affiliation":[{"name":"Fujian Key Laboratory of Polymer Materials Fujian Provincial Key Laboratory of Advanced Materials Oriented Chemical Engineering College of Chemistry &amp; Materials Science Fujian Normal University  Fuzhou P. R.China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-3575-7201","authenticated-orcid":false,"given":"Duan\u2010Hui","family":"Si","sequence":"additional","affiliation":[{"name":"Fujian Institute of Research on the Structure of Matter Chinese Academy of Sciences  Fujian, Fuzhou P.R. China"},{"name":"Fujian Key Laboratory of Polymer Materials Fujian Provincial Key Laboratory of Advanced Materials Oriented Chemical Engineering College of Chemistry &amp; Materials Science Fujian Normal University  Fuzhou P. 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