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Discovery of High-Entropy Oxide Electrocatalysts: From Thin-Film Material Libraries to Particles
Chemistry of Materials ( IF 8.6 ) Pub Date : 2022-11-17 , DOI: 10.1021/acs.chemmater.2c01455
Valerie Strotkötter 1 , Olga A Krysiak 2 , Jian Zhang 2 , Xiao Wang 1 , Ellen Suhr 1 , Wolfgang Schuhmann 2 , Alfred Ludwig 1, 3
Affiliation  

Discovery of new high-entropy electrocatalysts requires testing of hundreds to thousands of possible compositions, which can be addressed most efficiently by high-throughput experimentation on thin-film material libraries. Since the conditions for high-throughput measurements (“screening”) differ from more standardized methods, it is frequently a concern whether the findings from screening can be transferred to the commonly used particulate catalysts. We demonstrate the successful transfer of results from thin-film material libraries to particles of Cantor alloy oxide (Co-Cr-Fe-Mn-Ni)3O4. The chemical compositions of the libraries, all single-phase spinels, cover a wide compositional range of (Cr8.1–28.0Mn11.6–28.4Fe10.6–39.0Co11.4–36.7Ni13.5–31.4)37.7±0.6O62.3±0.6, with composition-dependent lattice constant values ranging from 0.826 to 0.851 nm. Electrochemical screening of the libraries for the oxygen evolution reaction (OER) identifies (Cr24.6±1.4Mn15.7±2.0Fe16.9±1.8Co26.1±1.9Ni16.6±1.7)37.8±0.8O62.2±1.2 as the most active composition, exhibiting an overpotential of 0.36 V at a current density of 1 mA cm–2. This “hit” in the library was subsequently synthesized in the form of particles with the same composition and crystal structure using an aerosol-based synthesis strategy. The similar OER activity of the most active thin-film composition and the derived catalyst particles validates the proposed approach of accelerated discovery of novel catalysts by screening of thin-film libraries.

中文翻译:

高熵氧化物电催化剂的发现:从薄膜材料库到粒子

发现新的高熵电催化剂需要测试成百上千种可能的成分,这可以通过对薄膜材料库进行高通量实验来最有效地解决。由于高通量测量(“筛选”)的条件与更标准化的方法不同,因此人们经常担心筛选结果是否可以转移到常用的颗粒催化剂上。我们展示了从薄膜材料库到康托合金氧化物 (Co-Cr-Fe-Mn-Ni) 3 O 4颗粒的成功转移。所有单相尖晶石库的化学成分涵盖广泛的成分范围(Cr 8.1–28.0 Mn 11.6–28.4 Fe10.6–39.0 Co 11.4–36.7 Ni 13.5–31.4 ) 37.7±0.6 O 62.3±0.6,与成分相关的晶格常数值范围为 0.826 至 0.851 nm。析氧反应 (OER) 库的电化学筛选确定 (Cr 24.6±1.4 Mn 15.7±2.0 Fe 16.9±1.8 Co 26.1±1.9 Ni 16.6±1.7 ) 37.8±0.8 O 62.2±1.2为最活跃的成分,表现出电流密度为 1 mA cm –2时的过电势为 0.36 V. 随后使用基于气溶胶的合成策略以具有相同组成和晶体结构的颗粒形式合成了库中的这种“命中”。最活跃的薄膜组合物和衍生催化剂颗粒的相似 OER 活性验证了通过筛选薄膜库加速发现新型催化剂的拟议方法。
更新日期:2022-11-17
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