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Metal utilization can be maximized by single\u2010atom catalysts, but catalytic performance is limited by the insufficient activation capability of a single site. Here, N\u2010bridged Zn\u2500Co atomic pairs with compressed Zn\u2500N\/Co\u2500N bonds are constructed to enable continuous orbital coupling near the Fermi level, by which the C\n                    <jats:sub>\u03b2<\/jats:sub>\n                    \u2500O bond of lignin is activated by accepting charge via vacant Co\n                    <jats:italic>d<\/jats:italic>\n                    <jats:sub>xz<\/jats:sub>\n                    \/\n                    <jats:italic>d<\/jats:italic>\n                    <jats:sub>yz<\/jats:sub>\n                    orbitals and the C\n                    <jats:sub>\u03b1<\/jats:sub>\n                    \u2500OH bond is activated by injecting charge via Zn\n                    <jats:italic>d<\/jats:italic>\n                    <jats:sub>xy<\/jats:sub>\n                    orbitals. Hydrogen heterolytic dissociation is also facilitated by the compressed Co\u2500N through polarizing H\n                    <jats:sub>2<\/jats:sub>\n                    to H\n                    <jats:sup>\u03b4\u2212<\/jats:sup>\n                    \u2010H\n                    <jats:sup>\u03b4+<\/jats:sup>\n                    . Consequently, superior activity is exhibited, by which wood is converted to monophenols with a near\u2010theoretical yield and carbohydrates with 92.2% retention at 200\u00b0C, and a TOF of 3.5 h\n                    <jats:sup>\u22121<\/jats:sup>\n                    is achieved, 6.1 times that of benchmark 5%Ru\/C. A scaled\u2010up operation using the produced phenols as solvent is designed, achieving a high monophenol concentration 85.8\u00a0g\/L in the resultant liquid and demonstrating excellent industrial potential. A design concept for non\u2010noble\u2010metal catalysts at the atomic orbital level is thus provided for lignocellulose biorefining.\n                  <\/jats:p>","DOI":"10.1002\/anie.4411028","type":"journal-article","created":{"date-parts":[[2026,9,28]],"date-time":"2026-09-28T02:42:42Z","timestamp":1790563362000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":0,"title":["Orbital Coupling Over N\u2010Bridged Zn\u2500Co Atomic Pairs Enables Lignocellulose Valorization"],"prefix":"10.1002","author":[{"ORCID":"https:\/\/orcid.org\/0009-0008-2893-6317","authenticated-orcid":false,"given":"Zhensheng","family":"Shen","sequence":"first","affiliation":[{"name":"Key Laboratory for Green Chemical Technology of Ministry of Education, School of Chemical Engineering and Technology Institute of Molecular Plus School of Energy Tianjin University  Tianjin China"},{"name":"State Key Laboratory For Development and Utilization of Forest 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