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This is a very rare case of a metal phosphite incorporating both N\u2010 and O\u2010donor ligands. The tetradentate TIMB linker bound to zinc atoms of the isolated zincophosphite hexamers to form a 3D open\u2010framework structure by crosslinking structural components of 1D chains and 2D layers. Here, the TPDC ligand acts as a monodentate binding model to functionalize its porous structure with the uncoordinated S atom and COO<jats:sup>\u2212<\/jats:sup> group. Interestingly, this compound demonstrates the highest H<jats:sub>2<\/jats:sub> storage capacity among organic\u2013inorganic hybrid metal phosphates (and phosphites), and a good CO<jats:sub>2<\/jats:sub> capture at 298\u2005K compared with the majority of crystalline materials. The possible adsorption sites and selectivity for CO<jats:sub>2<\/jats:sub> over H<jats:sub>2<\/jats:sub>, N<jats:sub>2<\/jats:sub>, and CO at 298\u2005K were calculated by using density functional theory (DFT), the ideal adsorption solution theory (IAST), and fitting experimental pure\u2010component adsorption data.<\/jats:p>","DOI":"10.1002\/chem.202200732","type":"journal-article","created":{"date-parts":[[2022,4,16]],"date-time":"2022-04-16T12:37:12Z","timestamp":1650112632000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":2,"title":["Genuine Pores in a Stable Zinc Phosphite for High H<sub>2<\/sub> Adsorption and CO<sub>2<\/sub> Capture"],"prefix":"10.1002","volume":"28","author":[{"given":"Ju\u2010Ying","family":"Chen","sequence":"first","affiliation":[{"name":"Department of Bioscience and Biotechnology National Taiwan Ocean University  Keelung Taiwan 202 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