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However, the practical application of plasmonic nanometal is hindered by challenge of energetic electrons extraction and low selectivity. The energetic carriers generated in nanometal under illumination have extremely short lifetimes, leading to rapid energy loss. In this work, silver nanometals modified with five distinct sulfhydryl ligands (re\u2010Ag\u2010S\u2010R) were synthesized via photoreduction of superlattice precursors. Modified surface efficiently extracts and preserves excited state electrons of plasmonic nanometals. By modulation the local charge density at catalytic active sites through substituents with varying electron\u2010donating and electron\u2010withdrawing properties, the selectivity of the photocatalytic carbon dioxide reduction reaction and hydrogen evolution reaction was influenced. The results demonstrated opposite selectivity between methoxy\u2010modified re\u2010Ag\u2010S\u2010OCH<jats:sub>3<\/jats:sub> (CO selectivity of 96.73\u2009%) and amino\u2010modified re\u2010Ag\u2010S\u2010NH<jats:sub>2<\/jats:sub> (H<jats:sub>2<\/jats:sub> selectivity of 96.66\u2009%) despite their similar structures. The changes in excited states and surface contact potentials induced by LSPR were monitored using femtosecond transient absorption (fs\u2010TA) spectroscopy and Kelvin probe force microscopy (KPFM). Meanwhile, the detailed discussion of the LSPR mechanism in plasmonic nanometals will serve as valuable references and foundational elements for future research in this area.<\/jats:p>","DOI":"10.1002\/anie.202422034","type":"journal-article","created":{"date-parts":[[2025,1,16]],"date-time":"2025-01-16T01:39:42Z","timestamp":1736991582000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":17,"title":["Light\u2010induced Enhancement of Energetic Charge Carrier Extraction and Modulation of Local Charge Density to Impact Selectivity in Plasmonic Nanometals"],"prefix":"10.1002","volume":"64","author":[{"given":"Yanjun","family":"Liu","sequence":"first","affiliation":[{"name":"Department of Chemistry Key Laboratory of Advanced Energy Material Chemistry Frontiers Science Center for New Organic Matter State Key Laboratory of Advanced Chemical Power Sources College of Chemistry Nankai University  Tianjin 300071 P. R. 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China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0003-0396-1846","authenticated-orcid":false,"given":"Peng","family":"Cheng","sequence":"additional","affiliation":[{"name":"Department of Chemistry Key Laboratory of Advanced Energy Material Chemistry Frontiers Science Center for New Organic Matter State Key Laboratory of Advanced Chemical Power Sources College of Chemistry Nankai University  Tianjin 300071 P. R. 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