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Herein, the hetero-nanocrystals between monodispersed Pt (~\u20092\u00a0nm) and Ni<jats:sub>3<\/jats:sub>S<jats:sub>2<\/jats:sub> (~\u20099.6\u00a0nm) are constructed as active electrocatalysts through interfacial electronic modulation, which exhibit superior bi-functional activities for methanol selective oxidation and H<jats:sub>2<\/jats:sub> generation. The experimental and theoretical studies reveal that the asymmetrical charge distribution at Pt\u2013Ni<jats:sub>3<\/jats:sub>S<jats:sub>2<\/jats:sub> could be modulated by the electronic interaction at the interface of dual-monodispersed heterojunctions, which thus promote the adsorption\/desorption of the chemical intermediates at the interface. As a result, the selective conversion from CH<jats:sub>3<\/jats:sub>OH to formate is accomplished at very low potentials (1.45\u00a0V) to attain 100\u00a0mA\u00a0cm<jats:sup>\u22122<\/jats:sup> with high electronic utilization rate (~\u200998%) and without CO<jats:sub>2<\/jats:sub> emission. Meanwhile, the Pt\u2013Ni<jats:sub>3<\/jats:sub>S<jats:sub>2<\/jats:sub> can simultaneously exhibit a broad potential window with outstanding stability and large current densities for hydrogen evolution reaction (HER) at the cathode. Further, the excellent bi-functional performance is also indicated in the coupled methanol oxidation reaction\u00a0(MOR)\/\/HER reactor by only requiring a cell voltage of 1.60\u00a0V to achieve a current density of 50\u00a0mA\u00a0cm<jats:sup>\u22122<\/jats:sup> with good reusability.<\/jats:p>","DOI":"10.1007\/s40820-023-01282-4","type":"journal-article","created":{"date-parts":[[2024,1,11]],"date-time":"2024-01-11T16:02:22Z","timestamp":1704988942000},"update-policy":"https:\/\/doi.org\/10.1007\/springer_crossmark_policy","source":"Crossref","is-referenced-by-count":67,"title":["Interfacial Electronic Modulation of Dual-Monodispersed Pt\u2013Ni3S2 as Efficacious Bi-Functional Electrocatalysts for Concurrent H2 Evolution and Methanol Selective Oxidation"],"prefix":"10.1007","volume":"16","author":[{"given":"Qianqian","family":"Zhao","sequence":"first","affiliation":[],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Bin","family":"Zhao","sequence":"additional","affiliation":[],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Xin","family":"Long","sequence":"additional","affiliation":[],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Renfei","family":"Feng","sequence":"additional","affiliation":[],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Mohsen","family":"Shakouri","sequence":"additional","affiliation":[],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Alisa","family":"Paterson","sequence":"additional","affiliation":[],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Qunfeng","family":"Xiao","sequence":"additional","affiliation":[],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Yu","family":"Zhang","sequence":"additional","affiliation":[],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Xian-Zhu","family":"Fu","sequence":"additional","affiliation":[],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Jing-Li","family":"Luo","sequence":"additional","affiliation":[],"role":[{"vocabulary":"crossref","role":"author"}]}],"member":"297","published-online":{"date-parts":[[2024,1,11]]},"reference":[{"key":"1282_CR1","doi-asserted-by":"publisher","first-page":"43","DOI":"10.1038\/nature11115","volume":"486","author":"MK Debe","year":"2012","unstructured":"M.K. 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