首页|Asymmetric configuration activating lattice oxygen via weakening d-p orbital hybridization for efficient C/N separation in urea overall electrolysis

Asymmetric configuration activating lattice oxygen via weakening d-p orbital hybridization for efficient C/N separation in urea overall electrolysis

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Urea oxidation reaction(UOR)is proposed as an exemplary half-reaction in renewable energy applica-tions because of its low thermodynamical potential.However,challenges persist due to sluggish reaction kinetics and complex by-products separation.To this end,we introduce the lattice oxygen oxidation mechanism(LOM),propelling a novel UOR route using a modified CoFe layered double hydroxide(LDH)catalyst termed CFRO-7.Theoretical calculations and in-situ characterizations highlight the acti-vated lattice oxygen(OL)within CFRO-7 as pivotal sites for UOR,optimizing the reaction pathway and accelerating the kinetics.For the urea overall electrolysis application,the LOM route only requires a low voltage of 1.54 V to offer a high current of 100 mA cm-2 for long-term utilization(＞48 h).Importantly,the by-product NCO-is significantly suppressed,while the CO2/N2 separation is efficiently achieved.This work proposed a pioneering paradigm,invoking the LOM pathway in urea electrolysis to expedite reaction dynamics and enhance product selectivity.

Lattice oxygenUrea oxidation reactionOverall electrolysisProducts selectivity

Chongchong Liu、Peifang Wang、Bin Hu、Xiaoli Liu、Rong Huang、Gang Zhou

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Key Laboratory of Integrated Regulation and Resource Development on Shallow Lake of Ministry of Education,College of Environment,Hohai University,Nanjing 210098,Jiangsu,China

Fundamental Research Funds for the Central UniversitiesKey Program of National Natural Science Foundation of ChinaKey Program of National Natural Science Foundation of ChinaKey Program of National Natural Science Foundation of ChinaNational Science Funds for Creative Research Groups of ChinaPostdoctoral Science Foundations of China and Jiangsu ProvincePostdoctoral Science Foundations of China and Jiangsu ProvincePostdoctoral Science Foundations of China and Jiangsu Province

B220202062920472019204730352102237514210062021M6908612022T1501832021K065A

2024

10.1016/j.jechem.2023.12.028

能源化学
中国科学院大连化学物理研究所 中国科学院成都有机化学研究所

能源化学

CSTPCDEI
影响因子：0.654
ISSN：2095-4956
年,卷(期)：2024.92(5)