ACS Nano - Charge Redistribution in High-Entropy Perovskite Oxide Porous Nanotubes Boosts Nitrate Electroreduction to Ammonia

Yao Chen, Cun Chen, Wei-Hsiang Huang*, Chih-Wen Pao, Chun-Chi Chang, Tingjie Mao, Juan Wang, Hui Fu, Feili Lai, Nan Zhang*, Tianxi Liu*

ACS Nano 2024, DOI: 10.1021/acsnano.4c05422

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 mgcat.–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.

Link: https://doi.org/10.1021/acsnano.4c05422