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Herein, we proposed a new strategy of controlling the electrocatalytic pathways by lateral adsorbate interaction for the bio\u2010polyol oxidation. Redox\u2010innocent 1,1,1,3,3,3\u2010hexafluoro\u20102\u2010propanol (HFIP) anion possesses the alcoholic property that facilely adsorbs on the nickel oxyhydroxide catalyst, but is resistant to oxidation due to the electron\u2010withdrawing trifluoromethyl groups. The alien HFIP adsorbents can compete with bio\u2010polyols and form a mixed adsorbate layer that creates lateral adsorbate interaction via hydrogen bonding, which achieved a &gt;2\u2010fold enhancement of the oxalate selectivity to 55\u2009% for the representative glycerol oxidation and can be extended to various bio\u2010polyol substrates. Through in situ spectroscopic analysis and DFT calculation on the glycerol oxidation, we reveal that the hydrogen\u2010bonded adsorbate interaction can effectively tune the adsorption energies and tailor the oxidation capabilities toward the targeted products. This work offers an additional perspective of tuning electrocatalytic reactions via introducing redox\u2010innocent adsorbates to create lateral adsorbate interactions.<\/jats:p>","DOI":"10.1002\/anie.202403466","type":"journal-article","created":{"date-parts":[[2024,3,7]],"date-time":"2024-03-07T09:38:20Z","timestamp":1709804300000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":16,"title":["Regulating Lateral Adsorbate Interaction for Efficient Electroreforming of Bio\u2010polyols"],"prefix":"10.1002","volume":"63","author":[{"given":"Jianxiang","family":"Wu","sequence":"first","affiliation":[{"name":"Collaborative Innovation Center of Chemistry for Energy Materials (iChEM) Department of Chemistry and Shanghai Key Laboratory of Molecular Catalysis and Innovative Materials Fudan University  Shanghai 200438 P. R. 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