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Although great efforts have been made in homogenous catalysis, it still remains a huge challenge to drive this reaction via heterogeneous catalysts under mild conditions. Herein, a single\u2010atom Au loaded MgAl\u2010layered double hydroxide (Au<jats:sub>1<\/jats:sub>\u2010MgAl\u2010LDH) with a well\u2010defined structure, in which the Au single atoms are located on the top of Al<jats:sup>3+<\/jats:sup> with Au\u2010O<jats:sub>4<\/jats:sub> coordination as revealed by extended x\u2013ray\u2013absorption fine\u2013structure (EXAFS)and density\u2013functional theory (DFT)calculation is reported. The photocatalytic results prove the Au<jats:sub>1<\/jats:sub>\u2010MgAl\u2010LDH is capable of driving benzene oxidation reaction with O<jats:sub>2<\/jats:sub> in water, and exhibits a high selectivity of 99% for phenol. While contrast experiment shows a \u224899% selectivity for aliphatic acid with Au nanoparticle loaded MgAl\u2010LDH (Au\u2010NP\u2010MgAl\u2010LDH). Detailed characterizations confirm that the origin of the selectivity difference can be attributed to the profound adsorption behavior of substrate benzene with Au single atoms and nanoparticles. For Au<jats:sub>1<\/jats:sub>\u2010MgAl\u2010LDH, single Au\u2010C bond is formed in benzene activation and result in the production of phenol. While for Au\u2010NP\u2010MgAl\u2010LDH, multiple Au\uf8ffC bonds are generated in benzene activation, leading to the crack of C\uf8ffC bond.<\/jats:p>","DOI":"10.1002\/smll.202303420","type":"journal-article","created":{"date-parts":[[2023,6,14]],"date-time":"2023-06-14T06:30:03Z","timestamp":1686724203000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":18,"title":["Enabling Specific Benzene Oxidation by Tuning the Adsorption Behavior on Au Loaded MgAl Layered Double Hydroxides"],"prefix":"10.1002","volume":"19","author":[{"given":"Tianyang","family":"Shen","sequence":"first","affiliation":[{"name":"State Key Laboratory of Chemical Resource Engineering Beijing University of Chemical Technology  Beijing 100029 P. R. 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