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作 者:Chun Zhu Yifei Yang Yike Jing Zhen Zeng Xuesong Yi Wei Sun Fei Yang
出 处:《Nano Research》2025年第1期195-207,共13页纳米研究(英文版)
基 金:supported by Hainan Province Science and Technology Special Fund(No.ZDYF2023GXJS165);National Natural Science Foundation of China(No.22102042);Hainan Province Key Scientific Research Project(No.ZDYF2021GXJS026)。
摘 要:Electrochemical nitrate reduction reaction(NO3RR)to ammonia is a promising approach to address excess Ncontamination in aqueous environment but suffers from a limited ammonia yield and selectivity due to the low concentration and sluggish kinetics.This work reports a three-dimensional porous electrode with binary Co_(2)Cu_(1)hydroxy phosphate embedded into the surface of Ni_(3)Co_(1)oxy/hydroxides(CoCu-PH@NiCo/Ni,“PH”means phosphate-hydroxide),which delivers a yield of 4.13 mg·h^(-1)·cm^(-2)with a high Faraday efficiency of 92.6%under a low nitrate concentration of 40 mM and provide an impressive stability.This embedded structure of the as-prepared catalyst exhibits unique metal coordination ligands and valence states different from the unitary hydroxy-phosphate.The electrochemical in situ infrared spectra and theoretical calculations revealed that the Co sites with the ability to dissociate water molecular to form adsorbed OH*can effectively provide the required protons for the deoxygenation and hydrogenation steps during NO3-conversion,thereby,effectively reducing the energy barrier of the key transition states in the NO3RR process to improve the intrinsic kinetics.We demonstrate that the rational design of binary components with the appropriate ability to activate water molecules as well as the threedimensional porous skeletal structure are expected to promote effectively the low-concentration nitrates conversion to ammonia.
关 键 词:nitrate reduction hydroxy phosphate surface embedded water dissociation active hydroxy adsorbed
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