Carbon‐Based Metal‐Free Catalysts for Electrocatalytic Reduction of Nitrogen for Synthesis of Ammonia at Ambient Conditions

Zhao, Shenlong; Lu, Xunyu; Wang, Luyao; Gale, Julian D.; Amal, Rose

doi:10.1002/adma.201805367

Cited by 265 publications

(200 citation statements)

References 70 publications

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“…4 Being a key precursor for industrial chemicals, fertilizer production, convenient hydrogen carrier, and emerging clean fuel, NH 3 production by electrocatalytic reduction of N 2 (NRR) has recently attracted considerable attention. 54 NH 3 possesses about twice the volumetric energy density compared to liquid hydrogen. The well-known Haber-Bosch process for NH 3 production involves the reaction of H 2 (produced from coal) and N 2 (obtained through air refining) at high temperature (350-550°C) and high pressure (150-350 atm), 55 and consumes about 2% of the world's energy and generates 1% of its CO 2 -a detrimental effect on the current energy and environmental landscape.…”

Section: Ten Years' Advancement Of C-mfecsmentioning

confidence: 99%

Ten years of carbon‐based metal‐free electrocatalysts

et al. 2019

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Since the discovery of the first carbon-based metal-free electrocatalysts (C-MFECs, i.e., N-doped carbon nanotubes) for the oxygen reduction reaction in 2009, the field of C-MFECs has grown enormously over the last 10 years.C-MFECs, as alternatives to nonprecious transition metals and/or precious noble metal-based electrocatalysts, have been consistently demonstrated as efficient catalysts for oxygen reduction, oxygen evolution, hydrogen evolution, carbon dioxide reduction, nitrogen reduction, and many other (electro-) chemical reactions. Recent research and development of C-MFECs have indicated their potential applications in fuel cells, metal-air batteries, and hydrogen generation through water oxidation as well as electrochemical production of various commodity chemicals, such as ammonia, alcohols, hydrogen peroxide, and other useful hydrocarbons. Further research and development of C-MFECs would surely revolutionize traditional energy conversion and storage technologies with minimal environmental impact. In this short review article, we summarize the journey of C-MFECs over the past 10 years with an emphasis on materials development and their structure-property characterization for applications in fuel cells and metal-air batteries. Current challenges and future prospects of this emerging field are also discussed. K E Y W O R D Scarbon, electrocatalysis, energy conversion, energy storage, metal-free electrocatalyst

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Section: Ten Years' Advancement Of C-mfecsmentioning

confidence: 99%

Ten years of carbon‐based metal‐free electrocatalysts

et al. 2019

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“…Previous reports regarding the NRR process electrocatalyzed by N-doped carbon as the catalyst reveal that pyridinic and pyrrolic N moieties incorporated in a graphitic layer, together with the generated adjacent atomic vacancy (e.g., C and N), are active sites for adsorbing and activating the N 2 molecule to initiate the conversion of N 2 to NH 3 [13,22]. Thus, we consider the present catalyst similar to those previously reported catalysts in catalytically active sites and a preferable electrochemical reaction pathway for NH 3 synthesis on NC-800.…”

Section: Resultsmentioning

confidence: 99%

“…However, the efficiency of NH 3 production is still far from comparable to that of the Haber-Bosch process, due to the extreme difficulty in breaking the strong N≡N triple bond of N 2 and the competing hydrogen evolution reaction (HER) during the electrocatalysis. Among those developed electrocatalysts, metal-free carbon-based catalysts are more intriguing because of their unique features, such as low-costs, large surface areas, mechanical flexibility with good electronic conductivity, and robust tolerance to acidic and/or alkaline conditions [13]. As a consequence, a number of carbon-based materials have been developed for NRR to NH 3 production, specifically, heteroatom-(e.g., O [14], N [15], S [16], B [17], F [18], Cl [12], and P [19]) doped carbon materials, which demonstrated highly improved catalytic efficiency.…”

Section: Introductionmentioning

confidence: 99%

Biomass-Derived Nitrogen-Doped Porous Carbon for Highly Efficient Ambient Electro-Synthesis of NH3

Chen

Yang

2020

Catalysts

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In this communication, we report a biomass-derived nitrogen-doped porous carbon (named as NC-800) as an electrocatalyst for the ambient conversion of N2 to NH3. The catalyst NC-800 was prepared from naturally renewable and easily available bamboo shoots, with inherently an approximate 8 wt % of N-containing components, such as the N source, in a cost-effective and environmentally benign manner. This exhibited remarkable catalytic activity with a large NH3 yield and a Faradaic efficiency as high as 16.3 μg h−mg-1cat and 27.5%, respectively, at −0.35 V versus a reversible hydrogen electrode (RHE) in 0.1 M HCl solution at ambient conditions. More importantly, the catalyst NC-800 demonstrated excellent electrochemical selectivity and stability.

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“…Nitrogen reduction reaction (also known as nitrogen fixation) converts N 2 to ammonia (NH 3 ) under mild temperature and pressure, playing a vital role in solving the energy issues and food issues. Electrochemical reduction of dinitrogen to ammonia (N 2 + 6H + + 6e − → 2NH 3 (g) E 0 = 0.148 V vs RHE) is six‐proton coupled electron transfer (PCET) steps . Because NN triple bond is very strong, and the first protonation of N 2 (

{normalN}_{2}^{normal*} + {normalH}^{+} + {normale}^{-} \to {NNH}^{normal*}

) is the most difficult step for N 2 RR, the breakage of NN only can occur on the catalysts which have strong adsorption for N 2 .…”

Section: Applications Of Single‐atom Electrocatalystsmentioning

confidence: 99%

Nitrogen‐Doped Porous Carbon Supported Nonprecious Metal Single‐Atom Electrocatalysts: from Synthesis to Application

et al. 2019

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Nonprecious metal single‐atom materials have attracted extensive attention in the field of electrocatalysis due to their low cost, high reactivity, high selectivity, and high atomic utilization. However, the high surface energy of a single atom causes agglomeration during preparation and catalytic measurement, resulting in damage to the catalytic sites. The strong interaction between substrate and monoatoms is the key factor to prevent the aggregation of individual metal atoms, and the geometry and electronic structure of the catalysts can be adjusted to optimize the catalytic activity. Due to the hierarchically pores, high specific surface area, and defect effect, nitrogen‐doped porous carbon (NPC) has been widely studied as an ideal nonprecious metal single‐atom support, which synergistically enhance the electrocatalytic performance toward oxygen reduction reaction, oxygen evolution reaction, hydrogen evolution reaction, carbon dioxide reduction reaction, and nitrogen reduction reaction with non‐noble metal single atoms. This review summarizes the controllable synthesis, characterization, theoretical calculation, and application of M (M = Co, Fe, Ni, Cu, Zn, Mo, etc.) single atoms on nitrogen‐doped porous carbon. Finally, the future development and challenges of nitrogen‐doped porous carbon supported nonprecious metal single‐atom electrocatalysts for practical commercialization are concluded.

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Carbon‐Based Metal‐Free Catalysts for Electrocatalytic Reduction of Nitrogen for Synthesis of Ammonia at Ambient Conditions

Cited by 265 publications

References 70 publications

Ten years of carbon‐based metal‐free electrocatalysts

Ten years of carbon‐based metal‐free electrocatalysts

Biomass-Derived Nitrogen-Doped Porous Carbon for Highly Efficient Ambient Electro-Synthesis of NH3

Nitrogen‐Doped Porous Carbon Supported Nonprecious Metal Single‐Atom Electrocatalysts: from Synthesis to Application

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