Journal ArticleDOI
A Review of Electrocatalytic Reduction of Dinitrogen to Ammonia under Ambient Conditions
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In this paper, the authors summarized the recent progress on the electrochemical nitrogen reduction reaction (NRR) at ambient temperature and pressure from both theoretical and experimental aspects, aiming at extracting instructive perceptions for future NRR research activities.Abstract:
DOI: 10.1002/aenm.201800369 reactions involved.[1] In recent years, tremendous progress has been achieved in the field of heterogeneous electrocatalysis, with rapid development of multifarious electocatalysts toward oxygen reduction reaction (ORR), oxygen evolution reaction (OER), hydrogen evolution reaction (HER), and carbon dioxide reduction reaction (CO2RR). However, electrocatalysts for the reduction of dinitrogen (N2) to ammonia (NH3) at room temperature and atmospheric pressure remain largely underexplored, despite the fact that investigations on catalysts and reaction systems for artificial nitrogen fixation have been continued for more than 100 years.[2–4] Ammonia is primarily used for producing fertilizers to sustain the world’s population.[5] It also serves as a green energy carrier and a potential transportation fuel.[6] Currently, ammonia synthesis is dominated by the industrial Haber–Bosch process using heterogeneous iron-based catalysts at high temperature (300–500 °C) and high pressure (150–300 atm),[7] accounting for more than 1% of the world’s energy supply and generating more than 300 million metric tons of fossil fuel–derived CO2 annually.[8,9] Hence, it is desirable to develop alternative processes that have the potential to overcome the limitations of the Haber–Bosch process including harsh conditions, complex plant infrastructure, centralized distribution, high energy consumption, and negative environmental impacts. In nature, biological N2 fixation occurs under mild conditions via nitrogenase enzymes that contain FeMo, FeV, or FeFe cofactor as catalytic active sites.[10,11] Developed man-made catalysts are therefore stimulated to reduce N2 upon the addition of protons and electrons, which is similar to the nitrogenase catalytic process. Transition metal–dinitrogen complexes such as the molybdenum–, iron–, and cobalt–dinitrogen complexes have been proposed as homogeneous catalysts for the reduction of N2 into NH3 under ambient conditions;[12] however, the stability and recycling issues are challenging.[13] On the other hand, electrochemical and photochemical reduction processes using heterogeneous catalysts benefit from clean and renewable energy sources and are promising for achieving NH3 production directly from N2 and water.[14] The electrochemical reduction of N2 to NH3 can be more efficient than the photochemical counterpart. This is because not all of the photons in the photochemical reduction process can The production of ammonia (NH3) from molecular dinitrogen (N2) under mild conditions is one of the most attractive topics in the field of chemistry. Electrochemical reduction of N2 is promising for achieving clean and sustainable NH3 production with lower energy consumption using renewable energy sources. To date, emerging electrocatalysts for the electrochemical reduction of N2 to NH3 at room temperature and atmospheric pressure remain largely underexplored. The major challenge is to achieve both high catalytic activity and high selectivity. Here, the recent progress on the electrochemical nitrogen reduction reaction (NRR) at ambient temperature and pressure from both theoretical and experimental aspects is summarized, aiming at extracting instructive perceptions for future NRR research activities. The prevailing theories and mechanisms for NRR as well as computational screening of promising materials are presented. State-of-the-art heterogeneous electrocatalysts as well as rational design of the whole electrochemical systems for NRR are involved. Importantly, promising strategies to enhance the activity, selectivity, efficiency, and stability of electrocatalysts toward NRR are proposed. Moreover, ammonia determination methods are compared and problems relating to possible ammonia contamination of the system are mentioned so as to shed fresh light on possible standard protocols for NRR measurements.read more
Citations
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Journal ArticleDOI
Recent Advances and Challenges of Electrocatalytic N2 Reduction to Ammonia.
Geletu Qing,Reza Ghazfar,Shane T. Jackowski,Faezeh Habibzadeh,Mona Maleka Ashtiani,Chuan Pin Chen,Milton R. Smith,Thomas W. Hamann +7 more
TL;DR: This review provides a comprehensive account of theoretical and experimental studies on electrochemical nitrogen fixation with a focus on the low selectivity for reduction of N2 to ammonia versus protons to H2.
Journal ArticleDOI
How to explore ambient electrocatalytic nitrogen reduction reliably and insightfully.
Cheng Tang,Shi-Zhang Qiao +1 more
TL;DR: This tutorial review summarizes the present status and challenges in the study of ambient electrocatalytic nitrogen reduction, followed by a thorough discussion of various experimental parameters, and recommends a series of protocols and best practices for experiments.
Journal ArticleDOI
Single-boron catalysts for nitrogen reduction reaction
Chuangwei Liu,Qinye Li,Chengzhang Wu,Jie Zhang,Yonggang Jin,Douglas R. MacFarlane,Chenghua Sun +6 more
TL;DR: Single boron atoms supported on graphene and substituted into h-MoS2 are identified as the most promising NRR catalysts, offering excellent energy efficiency and selectivity against hydrogen evolution reaction.
Journal ArticleDOI
Advanced Electrocatalysts with Single-Metal-Atom Active Sites.
Yuxuan Wang,Hongyang Su,Yanghua He,Ligui Li,Shangqian Zhu,Hao Shen,Pengfei Xie,Xianbiao Fu,Guangye Zhou,Chen Feng,Dengke Zhao,Fei Xiao,Xiaojing Zhu,Yachao Zeng,Minhua Shao,Shaowei Chen,Gang Wu,Jie Zeng,Chao Wang +18 more
TL;DR: This review aims to provide a comprehensive summary on the recent development of single-atom electrocatalysts for various energy-conversion reactions using state-of-the-art microscopic and spectroscopic techniques.
Journal ArticleDOI
Electrochemical nitrogen fixation and utilization: theories, advanced catalyst materials and system design.
TL;DR: Electrochemical techniques for nitrogen fixation and transformation under mild conditions are promising approaches to meet the challenge of efficiently managing and balancing the nitrogen cycle, where the rational design of advanced electrocatalysts from both structural and compositional aspects down to the nanoscale plays the most essential role.
References
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Universality in Oxygen Evolution Electrocatalysis on Oxide Surfaces
Isabela C. Man,Hai-Yan Su,Federico Calle-Vallejo,Heine Anton Hansen,José I. Martínez,Nilay İnoğlu,John R. Kitchin,Thomas F. Jaramillo,Jens K. Nørskov,Jan Rossmeisl +9 more
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Covalent organic frameworks comprising cobalt porphyrins for catalytic CO2 reduction in water
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TL;DR: Modular optimization of covalent organic frameworks (COFs) is reported, in which the building units are cobalt porphyrin catalysts linked by organic struts through imine bonds, to prepare a catalytic material for aqueous electrochemical reduction of CO2 to CO.