Yu Mingquan, Li Guowei, Fu Chenguang, Liu Enke, Manna Kaustuv, Budiyanto Eko, Yang Qun, Felser Claudia, Tüysüz Harun
Max-Planck-Institut für Kohlenforschung, Kaiser-Wilhelm-Platz 1, 45470, Mülheim an der Ruhr, Germany.
Max Planck Institute for Chemical Physics of Solids, Nöthnitzer Straβe 40, 01187, Dresden, Germany.
Angew Chem Int Ed Engl. 2021 Mar 8;60(11):5800-5805. doi: 10.1002/anie.202013610. Epub 2021 Feb 3.
Heusler compounds have potential in electrocatalysis because of their mechanical robustness, metallic conductivity, and wide tunability in the electronic structure and element compositions. This study reports the first application of Co YZ-type Heusler compounds as electrocatalysts for the oxygen evolution reaction (OER). A range of Co YZ crystals was synthesized through the arc-melting method and the e orbital filling of Co was precisely regulated by varying Y and Z sites of the compound. A correlation between the e orbital filling of reactive Co sites and OER activity was found for Co MnZ compounds (Z=Ti, Al, V, and Ga), whereby higher catalytic current was achieved for e orbital filling approaching unity. A similar trend of e orbital filling on the reactivity of cobalt sites was also observed for other Heusler compounds (Co VZ, Z=Sn and Ga). This work demonstrates proof of concept in the application of Heusler compounds as a new class of OER electrocatalysts, and the influence of the manipulation of the spin orbitals on their catalytic performance.
由于赫斯勒化合物具有机械稳定性、金属导电性以及在电子结构和元素组成方面的广泛可调性，它们在电催化领域具有潜力。本研究报道了Co YZ型赫斯勒化合物作为析氧反应（OER）电催化剂的首次应用。通过电弧熔炼法合成了一系列Co YZ晶体，并通过改变化合物的Y和Z位点精确调控了Co的e轨道填充。对于Co MnZ化合物（Z = Ti、Al、V和Ga），发现活性Co位点的e轨道填充与OER活性之间存在相关性，即当e轨道填充接近1时可实现更高的催化电流。对于其他赫斯勒化合物（Co VZ，Z = Sn和Ga），也观察到了钴位点反应性上类似的e轨道填充趋势。这项工作证明了赫斯勒化合物作为一类新型OER电催化剂应用的概念验证，以及自旋轨道调控对其催化性能的影响。
