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.

Photocatalysis is a promising sustainable technology to remove organic pollution and convert solar energy into chemical energy. Titanium dioxide has drawn extensive attention in this field owing to its high activity under UV light, good chemical stability, large availability, low price and low toxicity. However, the poor quantum efficiency derived from fast electron/hole recombination, the limited utilization of sunlight, and a weak reducing ability still hinder its practical application. Among the modification strategies of TiO2 to enhance its performance, the construction of heterojunctions with other semiconductors is a powerful and versatile way to maximise the separation of photogenerated charge carriers and steer their transport toward enhanced efficiency and selectivity. Here, the research progress and current status of TiO2 modification are reviewed, focusing on heterojunctions. A rapid evolution of the understanding of the different charge transfer mechanisms is witnessed from traditional type II to the recently conceptualised S-scheme. Particular attention is paid to different synthetic approaches and interface engineering methods designed to improve and control the interfacial charge transfer, and several cases of TiO2 heterostructures with metal oxides, metal sulfides and carbon nitride are discussed. The application hotspots of TiO2-based photocatalysts are summarized, including hydrogen generation by water splitting, solar fuel production by CO2 conversion, and the degradation of organic water pollutants. Hints about less studied and emerging processes are also provided. Finally, the main issues and challenges related to the sustainability and scalability of photocatalytic technologies in view of their commercialization are highlighted, outlining future directions of development.

TiO2-based photocatalysts from type-II to S-scheme heterojunction and their applications

100% N2O Inhibition in Photocatalytic NOx Reduction by Carbon Particles over Bi2WO6/TiO2 Z-Scheme Heterojunctions

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

A carbon catalyst doped with Co and N derived from the metal-organic framework hybrid (ZIF-8@ZIF-67) for efficient oxygen reduction reaction

Ion-exchange membranes (IEMs) are used in several electrochemical systems for a wide variety of applications, including water purification, mineral ion recovery, and energy storage and conversion. These materials often dictate...

Ion transport on self-assembled block copolymer electrolytes with different side chain chemistries

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100% N2O Inhibition in Photocatalytic NOx Reduction by Carbon Particles over Bi2WO6/TiO2 Z-Scheme Heterojunctions

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

A carbon catalyst doped with Co and N derived from the metal-organic framework hybrid (ZIF-8@ZIF-67) for efficient oxygen reduction reaction

Ion transport on self-assembled block copolymer electrolytes with different side chain chemistries