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 as an irreplaceable chemical has been widely demanded to keep the sustainable development of the modern society. However, its industrial production consumes huge energy and releases extraordinary green-house gases, leading to various environmental issues. To achieve the green production of ammonia is a great challenge that has been extensively pursued recently. In the review, a most promising strategy, electrochemical nitrate reduction reaction (e-NO3RR) for the purpose is comprehensively investigated to give a full understanding of its development and mechanism and provide guidance for future directions. Particularly, the development of electrocatalysts is focused to realize the high ammonia yield rate and Faraday efficiency for industrial applications. The recent-developed catalysts, including noble metallic materials, alloys, metal compounds, single-metal-atom catalysts, and metal-free materials, are systematically discussed to review the effects of various factors on the catalytic performance in e-NO3RR. Accordingly, the strategies, including defects engineering, coordination environment modulating, surface controlling, and hybridization, are carefully discussed to improve the catalytic performance, such as the intrinsic activity and selectivity. Finally, perspectives and challenges are given out. This review shall provide insightful guidance on the development of advanced catalytic systems for the production of green ammonia efficiently in the industry. 

Recent Advances in Electrocatalysts for Efficient Nitrate Reduction to Ammonia

Lithium-sulfur (Li-S) batteries are supposed to be one of the most potential next-generation batteries owing to their high theoretical capacity and low cost. Nevertheless, the shuttle effect of firm multi-step two-electron reaction between sulfur and lithium in liquid electrolyte makes the capacity much smaller than the theoretical value. Many methods were proposed for inhibiting the shuttle effect of polysulfide, improving corresponding redox kinetics and enhancing the integral performance of Li-S batteries. Here, we will comprehensively and systematically summarize the strategies for inhibiting the shuttle effect from all components of Li-S batteries. First, the electrochemical principles/mechanism and origin of the shuttle effect are described in detail. Moreover, the efficient strategies, including boosting the sulfur conversion rate of sulfur, confining sulfur or lithium polysulfides (LPS) within cathode host, confining LPS in the shield layer, and preventing LPS from contacting the anode, will be discussed to suppress the shuttle effect. Then, recent advances in inhibition of shuttle effect in cathode, electrolyte, separator, and anode with the aforementioned strategies have been summarized to direct the further design of efficient materials for Li-S batteries. Finally, we present prospects for inhibition of the LPS shuttle and potential development directions in Li-S batteries. 

Engineering Strategies for Suppressing the Shuttle Effect in Lithium–Sulfur Batteries

The rapid rise of triboelectric nanogenerators (TENGs), which are emerging energy conversion devices in advanced electronics and wearable sensing systems, has elevated the interest in high‐performance and multifunctional triboelectric materials. Among them, cellulosic materials, affording high efficiency, biodegradability, and customizability, are becoming a new front‐runner. The inherently low dielectric constant limits the increase in the surface charge density. However, owing to its unique structure and excellent processability, cellulose shows great potential for dielectric modulation, providing a strong impetus for its advanced applications in the era of Internet of Things and artificial intelligence. This review aims to provide comprehensive insights into the fabrication of dielectric‐enhanced cellulosic triboelectric materials via dielectric modulation. The exceptional advantages and research progress in cellulosic materials are highlighted. The effects of the dielectric constant, polarization, and percolation threshold on the charge density are systematically investigated, providing a theoretical basis for cellulose dielectric modulation. Typical dielectric characterization methods are introduced, and their technical characteristics are analyzed. Furthermore, the performance enhancements of cellulosic triboelectric materials endowed by dielectric modulation, including more efficient energy harvesting, high‐performance wearable electronics, and impedance matching via material strategies, are introduced. Finally, the challenges and future opportunities for cellulose dielectric modulation are summarized.

https://onlinelibrary.wiley.com/doi/pdfdirect/10.1002/advs.202206243

Fabrication of Advanced Cellulosic Triboelectric Materials via Dielectric Modulation

Physicochemical confinement and catalytic conversion of lithium polysulfides (LiPSs) are crucial to suppress the shuttle effect and enhance the redox kinetics of lithium-sulfur (Li-S) batteries. In this study, a NH4Cl-assisted pyrolysis strategy is developed to fabricate highly mesoporous N-rich carbon (designed as NC(p)) featuring thin outer shells and porous inner networks, on which single-Ni atoms are anchored to form an excellent sulfur host (designed as Ni-NC(p)) for Li-S batteries. During pyrolysis, the pyrolytic HCl from confined NH4Cl within ZIF-8 will in situ etch ZIF-8 to produce rich mesopores in the carbonized product NC(p). The mesoporous Ni-NC(p) enables favorable electron/ion transfer, high sulfur loading, and effective confinement of LiPSs, while the catalytic effect of single-Ni species enhances the redox kinetics of LiPSs. As a result, the sulfur cathode based on the Ni-NC(p) host delivers obviously improved Li-S battery performance with high specific capacity, good rate capability, and cycling stability.

Mesoporous N-rich Carbon with Single-Ni Atoms as a Multifunctional Sulfur Host for Li-S Batteries.

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

Favorable pore size distribution of biomass-derived N, S dual-doped carbon materials for advanced oxygen reduction reaction

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

Ordered mesoporous carbon fiber bundles with high-density and accessible Fe-NX active sites as efficient ORR catalysts for Zn-air batteries

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