High-entropy perovskite oxides are promising materials in the field of electrocatalysis due to their advantages such as large spatial composition regulation, entropy effects, and tunable material properties. However, the preparation of high-entropy perovskite oxides with stable and controllable structures still remains challenging. Herein, we fabricated a series of high-entropy perovskite oxide porous nanotubes (PNTs) by electrospinning as efficient electrocatalysts for the nitrate reduction reaction (NO₃RR). We further revealed that the different diffusion and decomposition behaviors of metal ions and polymers during the calcination process are the key to the formation of high-entropy perovskite oxide PNTs. Especially, LaSrNiCoMnFeCuO₃ PNTs show excellent performance of the NO₃RR, achieving the maximum NH₃ Faradaic efficiency of almost 100%, yield rate of 1657.5 μg h^–1 mg_cat.^–1, and durable stability after successive cycling, being one of the best electrocatalysts for the NO₃RR. The mechanism studies show that the charge redistribution induced by the multisite synergistic effect and abundant unsaturated sites in the high-entropy perovskite oxide PNTs favors the adsorption of NO₃^– and key intermediates and reduces the catalytic energy barrier, thus further achieving high NO₃^– conversion efficiency.

中文翻译：

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高熵钙钛矿氧化物多孔纳米管中的电荷重新分布促进硝酸盐电还原为氨


高熵钙钛矿氧化物由于其空间组成调控大、熵效应和材料性能可调等优点，是电催化领域有前途的材料。然而，制备具有稳定可控结构的高熵钙钛矿氧化物仍然具有挑战性。在此，我们通过静电纺丝制备了一系列高熵钙钛矿氧化物多孔纳米管（PNT）作为硝酸盐还原反应（NO ₃ RR）的有效电催化剂。我们进一步揭示了金属离子和聚合物在煅烧过程中不同的扩散和分解行为是高熵钙钛矿氧化物PNT形成的关键。尤其是LaSrNiCoMnFeCuO ₃ PNTs表现出优异的NO ₃ RR性能，实现了几乎100%的最大NH ₃法拉第效率，产率为1657.5 μg h ^–1 mg _cat。 ^–1 ，连续循环后具有持久稳定性，是 NO ₃ RR 的最佳电催化剂之一。机理研究表明，高熵钙钛矿氧化物PNT中的多位点协同效应和丰富的不饱和位点引起的电荷重新分布有利于NO ₃ ^–和关键中间体的吸附，降低催化能垒，从而进一步实现高NO ₃ ^–转换效率。