Ammonia is not only an important feedstock for chemical industry but also a carbon‐free energy carrier and a safe storage media for hydrogen. Due to the advantages compared to Haber–Bosch process, electrochemical NO3−‐to‐NH3 conversion via nitrate reduction reaction (NO3−RR) received attention. Recently, “green hydrogen” generated from water electrolysis shows promise to become the energy for future but limited by the safety of storage and transportation. This review proposes electrochemical NO3−‐to‐NH3 conversion can store renewable electric energy and “green hydrogen” into NH3, which is a potential solution for solving the puzzle of “green hydrogen” storage and transportation. Moreover, the theoretical insights of NO3−RR and electrocatalyst design are discussed. Finally, the challenges and opportunities in this field are elucidated. This review provides a novel perspective for NO3−RR and accelerates the development of effective electrocatalysts for NO3−‐to‐NH3 conversion.

Emerging Applications, Developments, Prospects, and Challenges of Electrochemical Nitrate‐to‐Ammonia Conversion

In situ interface engineered Co/NC derived from ZIF-67 as an efficient electrocatalyst for nitrate reduction to ammonia.

Electroreduction of nitrate to ammonia reaction (NO3 - RR) is considered as a promising carbon-free energy technique, which can eliminate nitrate from waste-water also produce value-added ammonia. However, it remains a challenge for achieving satisfied ammonia selectivity and Faraday efficiency (FE) due to the complex multiple-electron reduction process. Herein, a novel Tandem electrocatalyst that Ru dispersed on the porous graphitized C3 N4 (g-C3 N4 ) encapsulated with self-supported Cu nanowires (denoted as Ru@C3 N4 /Cu) for NO3 - RR is presented. As expected, a high ammonia yield of 0.249 mmol h-1  cm-2 at -0.9 V and high FENH3 of 91.3% at -0.8 V versus RHE can be obtained, while achieving excellent nitrate conversion (96.1%) and ammonia selectivity (91.4%) in neutral solution. In addition, density functional theory (DFT) calculations further demonstrate that the superior NO3 - RR performance is mainly resulted from the synergistic effect between the Ru and Cu dual-active sites, which can significantly enhance the adsorption of NO3 - and facilitate hydrogenation, as well as suppress the hydrogen evolution reaction, thus lead to highly improved NO3 - RR performances. This novel design strategy would pave a feasible avenue for the development of advanced NO3 - RR electrocatalysts.

Constructing Ru@C3 N4 /Cu Tandem Electrocatalyst with Dual-Active Sites for Enhanced Nitrate Electroreduction to Ammonia.

Nitrate is a reasonable alternative instead of nitrogen for ammonia production due to the low bond energy, large water-solubility, and high chemical polarity for good absorption. Nitrate electroreduction reaction (NO3 RR) is an effective and green strategy for both nitrate treatment and ammonia production. As an electrochemical reaction, the NO3 RR requires an efficient electrocatalyst for achieving high activity and selectivity. Inspired by the enhancement effect of heterostructure on electrocatalysis, Au nanowires decorated ultrathin Co3 O4 nanosheets (Co3 O4 -NS/Au-NWs) nanohybrids are proposed for improving the efficiency of nitrate-to-ammonia electroreduction. Theoretical calculation reveals that Au heteroatoms can effectively adjust the electron structure of Co active centers and reduce the energy barrier of the determining step (*NO → *NOH) during NO3 RR. As the result, the Co3 O4 -NS/Au-NWs nanohybrids achieve an outstanding catalytic performance with high yield rate (2.661 mg h-1 mgcat -1 ) toward nitrate-to-ammonia. Importantly, the Co3 O4 -NS/Au-NWs nanohybrids show an obviously plasmon-promoted activity for NO3 RR due to the localized surface plasmon resonance (LSPR) property of Au-NWs, which can achieve an enhanced NH3 yield rate of 4.045 mg h-1 mgcat -1 . This study reveals the structure-activity relationship of heterostructure and LSPR-promotion effect toward NO3 RR, which provide an efficient nitrate-to-ammonia reduction with high efficiency.

Au Nanowires Decorated Ultrathin Co3 O4 Nanosheets toward Light-Enhanced Nitrate Electroreduction.

Electrochemical nitrate reduction reaction (NO3−RR) to synthesize valuable ammonia (NH3) is considered as a green and appealing alternative to enable an artificial nitrogen cycle. However, as there are other NO3−RR pathways present, selectively guiding the reaction pathway towards NH3 is currently challenged by the lack of efficient catalyst. Here, we demonstrate a novel electrocatalyst for NO3−RR consisting of Au doped Cu nanowires on a copper foam (CF) electrode (Au–Cu NWs/CF), which delivers a remarkable NH3 yield rate of 5336.0 ± 159.2 μg h−1 cm−2 and an exceptional faradaic efficiency (FE) of 84.1 ± 1.0% at −1.05 V (vs. RHE). The 15N isotopic labelling experiments confirm that the yielded NH3 is indeed from the Au–Cu NWs/CF catalyzed NO3−RR process. The XPS analysis and in situ infrared spectroscopy (IR) spectroscopy characterization results indicated that the electron transfer between the Cu and Au interface and oxygen vacancy synergistically decreased the reduction reaction barrier and inhibited the generation of hydrogen in the competitive reaction, resulting in a high conversion, selectivity and FE for NO3−RR. This work not only develops a powerful strategy for the rational design of robust and efficient catalysts by defect engineering, but also provides new insights for selective nitrate electroreduction to NH3.

Electrochemical ammonia synthesis by reduction of nitrate on Au doped Cu nanowires

The electrochemical nitrate reduction reaction (NtRR) under ambient conditions is regarded as a potential approach to achieve NH3 production, which currently heavily relies on the Haber-Bosch process at the cost...

Ambient ammonia production via electrocatalytic nitrate reduction catalyzed by flower-like CuCo2O4 electrocatalyst

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Ambient ammonia production via electrocatalytic nitrate reduction catalyzed by flower-like CuCo2O4 electrocatalyst