吉林大学邹晓新团队报道了含有3d, 4d和5d过渡金属的钙钛矿氧化物的电催化水氧化活性-稳定性图。相关研究成果发表在2023年9月27日出版的《德国应用化学》。

在不损失催化稳定性的情况下提高催化活性是在酸性条件下寻找低铱含量析氧电催化剂的核心目标之一。

该文中，研究人员合成了66个具有不同Ti:Ru:Ir原子比的SrBO₃钙钛矿氧化物家族（B=Ti，Ru，Ir），并构建了随组成变化的催化活性稳定性图。这些图谱将多组分钙钛矿分为对酸性析氧反应具有不同催化活性和稳定性的化学基团，并突出了在相对较低的铱水平下同时实现高催化活性和稳定的化学区域。

通过量化多组分钙钛矿的混合过渡金属3d-4d-5d和氧2p轨道的杂化程度，研究人员证明了3d-4d-5d金属和氧原子之间的这种复杂相互作用，可以控制活性和稳定性的趋势，也可以确定是否涉及晶格氧的催化机制。

附：英文原文

Title: Electrocatalytic Water Oxidation Activity-Stability Maps for Perovskite Oxides Containing 3d, 4d and 5d Transition Metals

Author: Xiao Liang, Wensheng Yan, Yinglong Yu, Kexin Zhang, Wei An, Hui Chen, Yongcun Zou, Xiao Zhao, Xiaoxin Zou

Issue&Volume: 2023-09-27

Abstract: Improving catalytic activity without loss of catalytic stability is one of the core goals in search of low-iridium-content oxygen evolution electrocatalysts under acidic conditions. Here, we synthesize a family of 66 SrBO3 perovskite oxides (B = Ti, Ru, Ir) with different Ti:Ru:Ir atomic ratios and construct catalytic activity-stability maps over composition variation. The maps classify the multicomponent perovskites into chemical groups with distinct catalytic activity and stability for acidic oxygen evolution reaction, and highlights a chemical region where high catalytic activity and stability are achieved simultaneously at a relatively low iridium level. By quantifying the extent of hybridization of mixed transition metal 3d-4d-5d and oxygen 2p orbitals for multicomponent perovskites, we demonstrate this complex interplay between 3d-4d-5d metals and oxygen atoms in governing the trends in both activity and stability as well as in determining the catalytic mechanism involving lattice oxygen or not.

DOI: 10.1002/anie.202311606

Source: https://onlinelibrary.wiley.com/doi/10.1002/anie.202311606