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Here we show that K+ doping of Pd\/TiO2 (Pd\/KTiOx) enables concerted control of H2 dissociation and C\u2550O activation, resulting in a switchable hydrogenation chemoselectivity. Pristine Pd\/TiO2 selectively hydrogenates the C\u2550C bond of maleic anhydride to succinic anhydride with 99% selectivity, whereas Pd\/KTiOx hydrogenates both C\u2550C and C\u2550O bonds to \u03b3-butyrolactone with 99% selectivity. On both catalysts, H2 undergoes homolytic cleavage on Pd nanoparticles to generate H\u00b7 species responsible for C\u2550C hydrogenation. Introduction of K+ at the Pd\u2013TiO2 interface strengthens K\u2013O electrostatic interactions and increases the electron density on Pd, which together lower the barrier for heterolytic H2 cleavage at Pd\u2013O sites and generate polarized H\u03b4\u2212\u2013H\u03b4+ pairs. These heterolytic hydrogen species preferentially activate polar C\u2550O bonds, thus redirecting the hydrogenation pathway. This work establishes alkali-metal promotion as a strategy to tune the balance between homolytic and heterolytic H2 activation and, in turn, to control functional-group-dependent hydrogenation selectivity in heterogeneous catalysis.<\/jats:p>","DOI":"10.1021\/jacs.6c10350","type":"journal-article","created":{"date-parts":[[2026,8,10]],"date-time":"2026-08-10T14:02:07Z","timestamp":1786370527000},"page":"34840-34848","source":"Crossref","is-referenced-by-count":1,"title":["Aligning H2 Activation with Functional-Group\nPolarity: K+-Promoted Switchable Hydrogenation on\nPd\/TiO2"],"prefix":"10.1021","volume":"148","author":[{"given":"Jianian","family":"Cheng","sequence":"first","affiliation":[{"name":"Lanzhou University , , , ,","place":["Lanzhou, Gansu, China, 730000"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0001-9303-7002","authenticated-orcid":true,"given":"Yanqing","family":"Liu","sequence":"additional","affiliation":[{"name":"Chinese Academy of Sciences , , , ,","place":["Lanzhou, Gansu, China, 730000"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Jun","family":"Yuan","sequence":"additional","affiliation":[{"name":"Lanzhou University , , , ,","place":["Lanzhou, Gansu, China, 730000"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Junqi","family":"Tian","sequence":"additional","affiliation":[{"name":"Lanzhou University , , , ,","place":["Lanzhou, Gansu, China, 730000"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Zhongyang","family":"Liu","sequence":"additional","affiliation":[{"name":"Lanzhou University , , , ,","place":["Lanzhou, Gansu, China, 730000"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Jieyun","family":"Zhang","sequence":"additional","affiliation":[{"name":"Lanzhou University , , , ,","place":["Lanzhou, Gansu, China, 730000"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Wen","family":"Liu","sequence":"additional","affiliation":[{"name":"Lanzhou University , , , ,","place":["Lanzhou, Gansu, China, 730000"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Zelong","family":"Li","sequence":"additional","affiliation":[{"name":"Lanzhou University , , , ,","place":["Lanzhou, Gansu, China, 730000"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-9301-7850","authenticated-orcid":true,"given":"Can","family":"Li","sequence":"additional","affiliation":[{"name":"Lanzhou University , , , ,","place":["Lanzhou, Gansu, China, 730000"]},{"name":"Dalian National Laboratory for Clean Energy , , , ,","place":["Dalian, Liaoning, China, 116023"]}],"role":[{"vocabulary":"crossref","role":"author"}]}],"member":"316","published-online":{"date-parts":[[2026,8,10]]},"reference":[{"issue":"21","key":"2026081910210931000_cit1","doi-asserted-by":"publisher","first-page":"11986","DOI":"10.1021\/acs.chemrev.0c00797","article-title":"Single-Atom Catalysts\nBased on the Metal\u2013Oxide Interaction","volume":"120","author":"Lang","year":"2020","journal-title":"Chem. 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