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Here, the asymmetric charge polarized NiCo prussian blue analogue (NiCo PBA\u2010100) is reported to exhibit remarkable catalytic performance with high current density (210\u00a0mA\u00a0cm<jats:sup>\u22122<\/jats:sup> @1.65\u00a0V vs RHE) and Faraday efficiency (over 90%). Meanwhile, the hybrid water splitting and Zinc\u2013methanol\u2010battery assembled by NiCo PBA\u2010100 display the promoted performance with decent stability. X\u2010ray absorption spectroscopy (XAS) and <jats:italic>operando<\/jats:italic> Raman spectroscopy indicate that the asymmetric charge polarization in NiCo PBA leads to more unoccupied states of Ni and occupied states of Co, thereby facilitating the rapid transformation of the high\u2010active catalytic centers. Density functional theory calculations combining <jats:italic>operando<\/jats:italic> Fourier transform infrared spectroscopy demonstrate that the final reconstructed catalyst derived by NiCo PBA\u2010100 exhibits rearranged d band properties along with a lowered energy barrier of the rate\u2010determining step and favors the desired formate production.<\/jats:p>","DOI":"10.1002\/smll.202311452","type":"journal-article","created":{"date-parts":[[2023,12,25]],"date-time":"2023-12-25T11:47:30Z","timestamp":1703504850000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":8,"title":["Constructing Asymmetric Charge Polarized NiCo Prussian Blue Analogue for Promoted Electrocatalytic Methanol to Formate Conversion"],"prefix":"10.1002","volume":"20","author":[{"given":"Yunxiang","family":"Lin","sequence":"first","affiliation":[{"name":"Institutes of Physical Science and Information Technology School of Materials Science and Engineering 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