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Herein, atomically dispersed transition metal (TM) modified platinum (Pt)\u2010based bimetallic catalysts were designed and synthesized with the atomic layer deposition (ALD) method. Methanol steam reforming (MSR) was selected as a probe reaction to investigate the atomic\u2010level electronic effects of nickel (Ni) and iron (Fe) on Pt species. In situ\/ex situ characterizations, isotope labeling, and DFT calculations reveal that different transition metals and ALD cycles tune the Pt electronic structure, significantly affecting catalytic activity. Notably, the 10cNi\/Pt\n                    <jats:sub>1<\/jats:sub>\n                    \/CeO\n                    <jats:sub>2<\/jats:sub>\n                    catalyst exhibits optimal electronic modification, achieving the highest MSR and water\u2010gas shift (WGS) conversions and the lowest activation energies. Additionally, kinetic isotope effect studies confirm that hydrogen formation proceeds via methanol dehydrogenation coupled with WGS. These findings provide new insights into electronic modifications at atomic scales within the bimetallic components, offering valuable guidance for the design and development of advanced catalytic systems.\n                  <\/jats:p>","DOI":"10.1002\/anie.202514431","type":"journal-article","created":{"date-parts":[[2025,9,27]],"date-time":"2025-09-27T06:30:23Z","timestamp":1758954623000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":11,"title":["Electronic Modification at Atomic Scale: Design and Preparation of Diatomic Structures by Atomic Layer Deposition for Methanol Steam Reforming"],"prefix":"10.1002","volume":"64","author":[{"given":"Jinqiu","family":"Guo","sequence":"first","affiliation":[{"name":"School of Materials Science and Engineering Nankai University  Tianjin 300350 China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Leisheng","family":"Che","sequence":"additional","affiliation":[{"name":"School of Materials Science and Engineering Nankai University  Tianjin 300350 China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Yuyao","family":"Qin","sequence":"additional","affiliation":[{"name":"Sinopec Beijing Research Institute of Chemical Industry  Beijing 100013 China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Yaqi","family":"Hu","sequence":"additional","affiliation":[{"name":"School of Materials Science and Engineering Nankai University  Tianjin 300350 China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Xiaolin","family":"Tai","sequence":"additional","affiliation":[{"name":"Hefei National Laboratory for Physical Sciences at the Microscale Department of Chemistry University of Science and Technology of China  Hefei 230026 China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Jin","family":"Yuan","sequence":"additional","affiliation":[{"name":"School of Materials Science and Engineering Nankai University  Tianjin 300350 China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Li","family":"Jin","sequence":"additional","affiliation":[{"name":"Sinopec Beijing Research Institute of Chemical Industry  Beijing 100013 China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Yue","family":"Lin","sequence":"additional","affiliation":[{"name":"Hefei National Laboratory for Physical Sciences at the Microscale Department of Chemistry University of Science and Technology of China  Hefei 230026 China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-4065-6499","authenticated-orcid":false,"given":"Hongbo","family":"Zhang","sequence":"additional","affiliation":[{"name":"School of Materials Science and Engineering Nankai University  Tianjin 300350 China"}],"role":[{"vocabulary":"crossref","role":"author"}]}],"member":"311","published-online":{"date-parts":[[2025,9,26]]},"reference":[{"key":"e_1_2_9_1_1","doi-asserted-by":"publisher","DOI":"10.1021\/acs.chemrev.1c00412"},{"key":"e_1_2_9_2_1","doi-asserted-by":"publisher","DOI":"10.1038\/nature21672"},{"key":"e_1_2_9_3_1","doi-asserted-by":"publisher","DOI":"10.1038\/s41586-024-08483-w"},{"key":"e_1_2_9_4_1","doi-asserted-by":"publisher","DOI":"10.1126\/science.adt0682"},{"key":"e_1_2_9_5_1","doi-asserted-by":"publisher","DOI":"10.1021\/cr050198b"},{"key":"e_1_2_9_6_1","doi-asserted-by":"publisher","DOI":"10.1039\/D3EY00225J"},{"key":"e_1_2_9_7_1","doi-asserted-by":"publisher","DOI":"10.1021\/jacs.2c09437"},{"key":"e_1_2_9_8_1","doi-asserted-by":"publisher","DOI":"10.1002\/anie.201106591"},{"key":"e_1_2_9_9_1","doi-asserted-by":"publisher","DOI":"10.1002\/anie.201405213"},{"key":"e_1_2_9_10_1","doi-asserted-by":"publisher","DOI":"10.1016\/j.apcatb.2020.119052"},{"key":"e_1_2_9_11_1","doi-asserted-by":"publisher","DOI":"10.1038\/nature01009"},{"key":"e_1_2_9_12_1","doi-asserted-by":"publisher","DOI":"10.1002\/anie.200351664"},{"key":"e_1_2_9_13_1","doi-asserted-by":"publisher","DOI":"10.1021\/acscatal.9b02243"},{"key":"e_1_2_9_14_1","doi-asserted-by":"publisher","DOI":"10.1002\/anie.201209758"},{"key":"e_1_2_9_15_1","doi-asserted-by":"publisher","DOI":"10.1016\/S0021-9517(03)00032-0"},{"key":"e_1_2_9_16_1","doi-asserted-by":"publisher","DOI":"10.1038\/s41467-022-33186-z"},{"key":"e_1_2_9_17_1","volume-title":"Bimetallic Catalysts: Discoveries, Concepts, and Applications","author":"Sinfelt J. 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