Composition-Designed Multielement Perovskite Oxides for Oxygen Evolution Catalysis
Composition-Designed Multielement Perovskite Oxides for Oxygen Evolution Catalysis
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DOI：
10.1021/acs.chemmater.2c02986
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发表时间：
2022-12-07
影响因子：
8.6
通讯作者：
Yamada，Ikuya
中科院分区：
文献类型：
--
作者：
Okazaki，Yuichi;Fujita，Yushi;Yamada，Ikuya
析氧反应(OER)催化剂在能量转换电化学反应中起着至关重要的作用。近年来，高熵氧化物(HEO)被认为是实现高活性和低成本的OER催化剂的潜在候选者。由于HEOS巨大的组成空间需要付出相当大的努力才能找到有前景的催化剂，因此还没有实现从等摩尔组成这样简单的化学组成的进一步发展。在本研究中，我们利用贝叶斯优化方法对具有高OER催化活性的钙钛矿La(Cr，Mn，Fe，Co，Ni)O_3进行了快速高效的设计，找出了化学组成与OER催化活性之间的关系。优化组成的多元钙钛矿催化剂的活性远高于已报道的等摩尔LaCr1/5Mn1/5Fe1/5Co1/5Ni1/503催化剂。贝叶斯优化调整了高含量的过氧活性元素Fe、Co、Ni的浓度，以提高催化活性。优化结果还表明，钙钛矿中的OER非活性元素(铬和锰)甚至促进了OER活性。这些发现表明，基于数据的预测的解决方案，以改善多元过渡金属氧化物的催化性能。
Oxygen evolution reaction (OER) catalysts play an essential role in energy-conversion electrochemical reactions. High-entropy oxides (HEOs) were recently investigated as promising candidates to realize highly active and cost-effective OER catalysts. Since the vast composition space for the HEOs needs considerable efforts to find promising catalysts, the further development beyond simple chemical compositions like equimolar ones has not been achieved yet. In this study, we conducted the fast and efficient design of the perovskite of La(Cr, Mn, Fe, Co, Ni)O3with high OER catalytic activity using Bayesian optimization and found the relationship between chemical compositions and OER catalytic activities. The multielement perovskites with the optimized compositions exhibited much higher activities than the equimolar LaCr1/5Mn1/5Fe1/5Co1/5Ni1/5O3, which was previously reported as an active catalyst. Bayesian optimization adjusted the concentrations of OER active elements of Fe, Co, and Ni in high contents to enhance the catalytic activities. The optimization also indicates that the OER inactive elements (Cr and Mn) in perovskites even promote the OER activities. These findings suggest the solution of data-based predictions to improve catalytic performances in multielement transition-metal oxides.