DOE OSTI · 2583415
Robust Oxygen‐Vacancy‐Engineered Co(OH) 2 /Cu Heterostructures Boost Nitrate Electroreduction to Ammonia beyond 2 A cm −2
Abstract
Electrocatalytic nitrate reduction reaction (NO 3 RR) presents a sustainable paradigm for green NH 3 synthesis and NO 3 − wastewater valorization. However, overcoming sluggish NO 3 RR kinetics under industrial-current operation persists as a critical challenge. Herein, robust oxygen vacancy-enriched heterostructures (O v -Co(OH) 2 /Cu) are engineered through in situ electrochemical reconstruction. By coupling Cu-mediated NO 3 − -to-NO 2 − conversion with O v -Co(OH) 2 -accelerated NO 2 − -to-NH 3 transformation, this heterostructured system delivers an unprecedented NH 3 yield rate of 167.8 mg h −1 cm −2 and 97.7% Faradaic efficiency at >2 A cm −2 , while maintaining exceptional current tolerance over 25 h. Operando spectroscopic characterizations and theoretical calculations reveal that the introduction of O v in Co(OH) 2 synergistically accelerates water dissociation to ensure continuous hydrogen supply and optimizes *NOOH adsorption, reducing the energy barrier for the rate-limiting step (*NO 2 to *NOOH). To demonstrate practical viability, a membrane-electrode-assembly electrolyzer integrating NO 3 RR with glycerol oxidation reaction achieves highly effective co-production of NH 3 and formate alongside wastewater treatment. In conclusion, this work offers new insights into the rational design of electrocatalysts through in situ reconstruction-induced vacancy engineering for scalable and practical NO 3 RR applications.
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Mei, Weijie [Tianjin Univ. (China); Haihe Laboratory of Sustainable Chemical Transformations, Tianjin (China)], Chang, Chun‐Wai [Oregon State Univ., Corvallis, OR (United States)], Li, Zhiguo [Tianjin Univ. (China); Haihe Laboratory of Sustainable Chemical Transformations, Tianjin (China)], Wang, Xinyu [Tianjin Univ. (China); Haihe Laboratory of Sustainable Chemical Transformations, Tianjin (China)], Qie, Yaning [Tianjin Univ. (China); Haihe Laboratory of Sustainable Chemical Transformations, Tianjin (China)], Liu, Qi [Oregon State Univ., Corvallis, OR (United States)], Davis, Ryan C. [SLAC National Accelerator Laboratory (SLAC), Menlo Park, CA (United States). Stanford Synchrotron Radiation Lightsource (SSRL)], Wu, Zhitan [Tianjin Univ. (China); Haihe Laboratory of Sustainable Chemical Transformations, Tianjin (China)], Yue, Yunpei [Tianjin Univ. (China); Haihe Laboratory of Sustainable Chemical Transformations, Tianjin (China)], Yang, Chenxu [Tianjin Univ. (China); Haihe Laboratory of Sustainable Chemical Transformations, Tianjin (China)], Li, Siqi [Tianjin Univ. (China); Haihe Laboratory of Sustainable Chemical Transformations, Tianjin (China)], Han, Daliang [Tianjin Univ. (China); Haihe Laboratory of Sustainable Chemical Transformations, Tianjin (China)], Yang, Quan‐Hong [Tianjin Univ. (China); Haihe Laboratory of Sustainable Chemical Transformations, Tianjin (China)], Feng, Zhenxing [Oregon State Univ., Corvallis, OR (United States)] (ORCID:0000000175985076), Weng, Zhe [Tianjin Univ. (China); Haihe Laboratory of Sustainable Chemical Transformations, Tianjin (China)] (ORCID:0000000260059552). 2025-07-15. Robust Oxygen‐Vacancy‐Engineered Co(OH) 2 /Cu Heterostructures Boost Nitrate Electroreduction to Ammonia beyond 2 A cm −2. https://doi.org/10.1002/adma.202507363
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