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Hence, optimizing the  orbital electronic states to achieve enhanced MOR activities are highly desired. Here, cobalt (Co) and iron (Fe) doping are used to modify the  orbital electronic states. Although both dopants can broaden the  orbital; however, Co doping leads to an elevation in the energy level of  highest occupied crystal orbital (HOCO), whereas Fe doping results in its reduction. Such a discrepancy in the regulation of  orbital electronic states stems from the disparate partial electron transfer mechanisms amongst these transition metal ions, which possess distinct energy level and occupancy of <jats:italic>d<\/jats:italic> orbitals. Motivated by this finding, the NiCoFe hydroxide is prepared and exhibited an excellent MOR performance. The results showed that the Co dopants effectively suppress the partial electron transfer from Ni to Fe, combined with the  orbital broadening induced by NiO<jats:sub>6<\/jats:sub> octahedra distortion, endowing NiCoFe hydroxide with high  HOCO and broad  orbital. It is believed that the work gives an in\u2010depth understanding on  orbital electronic states regulation in Ni(OH)<jats:sub>2<\/jats:sub>, which is beneficial for designing Ni(OH)<jats:sub>2<\/jats:sub>\u2010based catalysts with high MOR performance.<\/jats:p>","DOI":"10.1002\/smll.202406829","type":"journal-article","created":{"date-parts":[[2024,10,7]],"date-time":"2024-10-07T05:17:02Z","timestamp":1728278222000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":8,"title":["Modification dx2\u2212y2${{d}_{{{x}^2} - {{y}^2}}}$ Orbital Electronic States in Nickel\u2010Based Hydroxides Via Cobalt\/Iron Co\u2010Doping for High\u2010Efficiency Methanol Electrooxidation"],"prefix":"10.1002","volume":"20","author":[{"given":"Junhua","family":"Li","sequence":"first","affiliation":[{"name":"College of Materials Science and Engineering Sichuan University  Chengdu 610065 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