Interface Engineering of the Cu1.5Mn1.5O4/CeO2 Heterostructure for Highly Efficient Electrocatalytic Nitrate Reduction to Ammonia

Ruikai Qi; Linfeng Zhang; Siyu Ren; Bingyan Shi; Mengxiao Zhong; Zheng-Jie Chen; Xiaofeng Lu

doi:10.1021/acs.nanolett.4c01904

Interface Engineering of the Cu_1.5Mn_1.5O₄/CeO₂ Heterostructure for Highly Efficient Electrocatalytic Nitrate Reduction to Ammonia

Nano Lett. 2024 Jul 24;24(29):8964-8972. doi: 10.1021/acs.nanolett.4c01904. Epub 2024 Jul 10.

Authors

Ruikai Qi¹, Linfeng Zhang¹, Siyu Ren¹, Bingyan Shi¹, Mengxiao Zhong², Zheng-Jie Chen³, Xiaofeng Lu¹

Affiliations

¹ Alan G. MacDiarmid Institute, College of Chemistry, Jilin University, 2699 Qianjin Street, Changchun 130012, P. R. China.
² State Key Laboratory of Integrated Optoelectronics, Key Laboratory of Advanced Gas Sensors, Jilin Province, College of Electronic Science and Engineering, Jilin University, 2699 Qianjin Street, Changchun 130012, P. R. China.
³ Materials Science and Energy Engineering/Institute of Technology for Carbon Neutrality, Shenzhen Institute of Advanced Technology, Chinese Academy of Sciences, Shenzhen 518055, P. R. China.

PMID: 38985521
DOI: 10.1021/acs.nanolett.4c01904

Abstract

The electrochemical nitrate reduction reaction (NO₃RR) is considered a sustainable technology to convert the nitrate pollutants to ammonia. However, developing highly efficient electrocatalysts is necessary and challenging given the slow kinetics of the NO₃RR with an eight-electron transfer process. Here, a Cu_1.5Mn_1.5O₄ (CMO)/CeO₂ heterostructure with rich interfaces is designed and fabricated through an electrospinning and postprocessing technique. Benefiting from the strong coupling between CMO and CeO₂, the optimized CMO/CeO₂-2 catalyst presents excellent NO₃RR performance, with NH₃ Faraday efficiency (FE) up to 93.07 ± 1.45% at -0.481 V vs reversible hydrogen electrode (RHE) and NH₃ yield rate up to 48.06 ± 1.32 mg cm^-2 h^-1 at -0.681 V vs RHE. Theoretical calculations demonstrate that the integration of CeO₂ with CMO modulates the adsorption/desorption process of the reactants and intermediates, showing a reduced energy barrier in the rate determination step of NO* to N* and achieving an outstanding NO₃RR performance.

Keywords: electrocatalytic nitrate reduction; electrospinning; heterostructure; interface engineering.