To restore the natural nitrogen cycle (N-cycle), artificial N-cycle electrocatalysis with flexibility, sustainability, and compatibility can convert intermittent renewable energy (e.g., wind) to harmful or value-added chemicals with minimal carbon emissions. The background of such N-cycles, such as nitrogen fixation, ammonia oxidation, and nitrate reduction, is briefly introduced here. The discussion of emerging nanostructures in various conversion reactions is focused on the architecture/compositional design, electrochemical performances, reaction mechanisms, and instructive tests. Energy device advancements for achieving more functions as well as in situ/operando characterizations toward understanding key steps are also highlighted. Furthermore, some recently proposed reactions as well as less discussed C–N coupling reactions are also summarized. We classify inorganic nitrogen sources that convert to each other under an applied voltage into three types, namely, abundant nitrogen, toxic nitrate (nitrite), and nitrogen oxides, and useful compounds such as ammonia, hydrazine, and hydroxylamine, with the goal of providing more critical insights into strategies to facilitate the development of our circular nitrogen economy.

https://www.sciopen.com/article_pdf/1531201054523838466.pdf

Recent advances in nanostructured heterogeneous catalysts for N-cycle electrocatalysis

Electrochemical ammonia (NH3) synthesis from nitrate (NO3-) reduction offers an intriguing approach for both sustainable ammonia synthesis and environmental denitrification, yet it remains hindered by a complicated reaction pathway with various intermediates. Here we present that the interlayer strain compression in bismuth (Bi) nanocrystals can contribute to both activity and selectivity improvement toward NH3 electrosynthesis from NO3- reduction. By virtue of comprehensive spectroscopic studies and theoretical calculations, we untangle that the interlayer lattice compression shortens Bi-Bi bond to broaden the 6p bandwidth for electron delocalization, promoting the chemical affinities of nitrogen intermediates. Such a manipulation facilitates NO3- activation to reduce the energy barrier for activity improvement, and also alleviates *NO2 desorption to suppress nitrite generation. As a result, a strain-compressive Bi electrocatalyst yields a maximal Faradaic efficiency of 90.6% and high generation rate of 46.5 g h-1 gcat-1 with industrially scalable partial current density up to 300 mA cm-2 for NH3 product at the optimized conditions, respectively.

Governing Interlayer Strain in Bismuth Nanocrystals for Efficient Ammonia Electrosynthesis from Nitrate Reduction.

Abstract As a flourishing member of the two-dimensional (2D) nanomaterial family, MXenes have shown great potential in various research areas. In recent years, the continued growth of interest in MXene derivatives, 2D transition metal borides (MBenes), has contributed to the emergence of this 2D material as a latecomer. Due to the excellent electrical conductivity, mechanical properties and electrical properties, thus MBenes attract more researchers' interest. Extensive experimental and theoretical studies have shown that they have exciting energy conversion and electrochemical storage potential. However, a comprehensive and systematic review of MBenes applications has not been available so far. For this reason, we present a comprehensive summary of recent advances in MBenes research. We started by summarizing the latest fabrication routes and excellent properties of MBenes. The focus will then turn to their exciting potential for energy storage and conversion. Finally, a brief summary of the challenges and opportunities for MBenes in future practical applications is presented. 

/pdf/a-rising-2d-star-novel-mbenes-with-excellent-performance-in-1xnl0q45.pdf

A Rising 2D Star: Novel MBenes with Excellent Performance in Energy Conversion and Storage

There is a strong worldwide effort towards environmentally clean and renewable energy sources. Supercapacitors are among the most promising devices for storing the electric charges collected from those sustainable sources. Recently, 3D graphene-based electrodes have attracted much attention due to their high surface area, open porosity, excellent charge mobility, and good mechanical strength. In the constant effort to increase the energy density of devices, 3D graphene-based structures have been modified with other materials (e.g. heteroatom doping, metal oxides/mixed metal oxides, polymers, etc.). In this review , we survey and discuss the recent substantial progress in 3D-structured graphene/metal oxide-based hybrid materials for supercapacitor electrodes. This discussion is preceded by a report on the main research results for composite 2D graphene-metal oxide electrodes in supercapacitors, highlighting the properties of the most promising graphene-oxide combinations. We then examine the scientific challenges for improving the electrochemical characteristics of 3D graphene-based structures modified with different metal oxides and carbon nanotubes. We finish the review with a brief discussion on the future prospects for research in the field of 3D hybrid supercapacitors. 

Graphene-metal oxide hybrid materials with 2D and 3D morphologies for advanced supercapacitor electrodes: Status, challenges and prospects

Metal-organic gels (MOGs) emerged as a novel class of functional soft materials in which the scaffolding framework is fabricated by metal-ligand coordination in combination with other supramolecular interactions (for example, hydrogen bonding or π-π stacking). Through the combination of organic and inorganic (metal/metal-oxo clusters) building blocks, significant steps forward have been made in the development of new electrochemical sensors, superhydrophobic materials and ion storage devices, among others. These leaps forward are to some extend induced by the intrinsic hierarchical microporous/mesoporous pore structure of these metal-organic materials. Within this review we give an overview of recent developments of this growing field. First, we shed light onto the parallels to the well-established field of conventional gels and outline similarities and differences. Afterwards, we classify different types of MOGs according to their architectural/structural nature: (1) pristine MOGs, (2) hybrid MOGs, (3) crosslinking-based MOGs and (4) MOG-derived materials. Furthermore, we look at the different properties of MOGs and the requirements for the preparation of spatially patterned macro-structured MOGs by emerging additive manufacturing technologies. Moreover, different potential fields of application for MOGs and MOG derived materials are critically evaluated and potential improvements and pitfalls in comparison to traditional gel-based materials are given. Finally, a comprehensive outlook into future directions for the development of MOGs is provided.

Hierarchical porous metal-organic gels and derived materials: from fundamentals to potential applications.

The conversion of nitrogen to ammonia offers a sustainable and environmentally friendly approach for producing precursors for fertilizers and efficient energy carriers. Owing to the large energy de...

Rational Design of Graphene Derivatives for Electrochemical Reduction of Nitrogen to Ammonia

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Rational Design of Graphene Derivatives for Electrochemical Reduction of Nitrogen to Ammonia