The development of electrocatalysts capable of efficient reduction of nitrate (NO3-) to ammonia (NH3) is drawing increasing interest for the sake of low carbon emission and environmental protection. Herein, we present a CuCo bimetallic catalyst able to imitate the bifunctional nature of copper-type nitrite reductase, which could easily remove NO2- via the collaboration of two active centers. Indeed, Co acts as an electron/proton donating center, while Cu facilitates NOx- adsorption/association. The bio-inspired CuCo nanosheet electrocatalyst delivers a 100 ± 1% Faradaic efficiency at an ampere-level current density of 1035 mA cm-2 at -0.2 V vs. Reversible Hydrogen Electrode. The NH3 production rate reaches a high activity of 4.8 mmol cm-2 h-1 (960 mmol gcat-1 h-1). A mechanistic study, using electrochemical in situ Fourier transform infrared spectroscopy and shell-isolated nanoparticle enhanced Raman spectroscopy, reveals a strong synergy between Cu and Co, with Co sites promoting the hydrogenation of NO3- to NH3 via adsorbed *H species. The well-modulated coverage of adsorbed *H and *NO3 led simultaneously to high NH3 selectivity and yield. 

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Ampere-level current density ammonia electrochemical synthesis using CuCo nanosheets simulating nitrite reductase bifunctional nature

Designing genuine electrocatalysts that selectively reduce nitrate/nitrite (NOx−) is becoming ever more vital to produce ammonia (NH3) sustainably, safeguard the environment, and even rebalance the Earth’s nitrogen cycle. Since 2020, the aim of NH3 electrosynthesis from NOx− has been pursued, and with electrode design explosion, the field has been able to progressively distinguish effective strategies. Collective knowledge of state-of-the-art catalytic systems is indisputably essential for implementing this clean technology in industry. Hence, we present an overview of nicely constructed denitrifying electrocatalysts along with structural features that are more favorable for turning NOx− into NH3, focusing on performance, mechanisms, upgraded devices, etc. Key NH3-evolving efficiency optimization ideas with critical insights are identified and highlighted. We discuss high-quality works that exemplify gaps separating studies from large-scale deployment and proposed relevant bridging solutions. Outlook on challenges faced by NOx−-to-NH3 electrolysis systems are emphasized to inspire future works. Designing genuine electrocatalysts that selectively reduce nitrate/nitrite (NOx−) is becoming ever more vital to produce ammonia (NH3) sustainably, safeguard the environment, and even rebalance the Earth’s nitrogen cycle. Since 2020, the aim of NH3 electrosynthesis from NOx− has been pursued, and with electrode design explosion, the field has been able to progressively distinguish effective strategies. Collective knowledge of state-of-the-art catalytic systems is indisputably essential for implementing this clean technology in industry. Hence, we present an overview of nicely constructed denitrifying electrocatalysts along with structural features that are more favorable for turning NOx− into NH3, focusing on performance, mechanisms, upgraded devices, etc. Key NH3-evolving efficiency optimization ideas with critical insights are identified and highlighted. We discuss high-quality works that exemplify gaps separating studies from large-scale deployment and proposed relevant bridging solutions. Outlook on challenges faced by NOx−-to-NH3 electrolysis systems are emphasized to inspire future works. 

Advances in ammonia electrosynthesis from ambient nitrate/nitrite reduction

Natural nitrogen cycle has been severely disrupted by anthropogenic activities. The overuse of N-containing fertilizers induces the increase of nitrate level in surface and ground waters, and substantial emission of nitrogen oxides causes heavy air pollution. Nitrogen gas, as the main component of air, has been used for mass ammonia production for over a century, providing enough nutrition for agriculture to support world population increase. In the last decade, researchers have made great efforts to develop ammonia processes under ambient conditions to combat the intensive energy consumption and high carbon emission associated with the Haber-Bosch process. Among different techniques, electrochemical nitrate reduction reaction (NO3 RR) can achieve nitrate removal and ammonia generation simultaneously using renewable electricity as the power, and there is an exponential growth of studies in this research direction. Here we provide a timely and comprehensive review on the important progresses of electrochemical NO3 RR, covering the rational design of electrocatalysts, emerging C-N coupling reactions, and advanced energy conversion and storage systems. Moreover, future perspectives are proposed to accelerate the industrialized NH3 production and green synthesis of chemicals, leading to a sustainable nitrogen cycle via prosperous N-based electrochemistry. This article is protected by copyright. All rights reserved.

Electrochemical Nitrate Reduction: Ammonia Synthesis and the Beyond.

Artificial electrocatalytic ammonia (NH3) synthesis is recently becoming a research hotspot. It can couple with clean renewable electricity, which is considered an energy-efficient and sustainable approach for regulating the recirculation of nitrogen species and meanwhile promoting the growth of a circular nitrogen economy. In this Account, we review recent advances in electrocatalytic ammonia synthesis. Firstly, we briefly introduce the research background and significance of three electrochemical NH3 synthesis routes: electrocatalytic nitrogen reduction, nitric oxide reduction, and nitrate/nitrite reduction. And then we give a detailed discussion of the latest research advances in electrocatalysts for ambient NH3 synthesis, mainly involving catalytic mechanisms, theoretical advances, and electrochemical performance. Finally, the existing challenges and future research needs for artificial electrosynthesis of NH3 are also highlighted. 

Recent advances in electrocatalytic ammonia synthesis

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

Flower-like open-structured polycrystalline copper with synergistic multi-crystal plane for efficient electrocatalytic reduction of nitrate to ammonia

Electro-triggered Joule heating method to synthesize single-phase CuNi nano-alloy catalyst for efficient electrocatalytic nitrate reduction toward ammonia

Atomic catalyst supported on oxygen defective MXenes for synergetic electrocatalytic nitrate reduction to ammonia: A first principles study

Dopamine D1 receptor agonist treatment alleviates morphine-exposure-induced learning and memory impairments.

Objective: The objective of this article is to study the role of the dopamine (DA) D1 receptor in the midbrain periaqueductal grey (PAG) on learning and memory in morphine-addicted rats.Methods: DA...

A dopamine D1 receptor agonist improved learning and memory in morphine-treated rats.

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