Boosting nitrogen reduction to ammonia on Fe–N3S sites by introduction S into defect graphene

Chen, Shaona; Bu, Mengke; Zhou, Zikai; Liang, Yanhua; Dai, Zhongxu; Shi, Jinjin

doi:10.1016/j.mtener.2022.100954

Cited by 8 publications

(6 citation statements)

References 31 publications

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“…with maximum Faradaic efficiency of 54.5±1.1 %, outperforming most of the reported results for catalytic N 2 fixation under ambient conditions. Some of the recent ENRR, PNRR, and PENRR catalysts have been listed in Table 2, [60,90–99] Table 3, [62,77,100–105] and Table 4, [27,106–109] respectively, for comparison. Most catalysts developed today are composites of two or more materials containing semiconductors such as carbon nitride (C 3 N 4 ), reduced graphene oxide (RGO), titania, etc.…”

Section: Cof‐based Catalysts For Renewable Ammonia Synthesismentioning

confidence: 99%

“…with maximum Faradaic efficiency of 54.5 � 1.1 %, outperforming most of the reported results for catalytic N 2 fixation under ambient conditions. Some of the recent ENRR, PNRR, and PENRR catalysts have been listed in Table 2, [60,[90][91][92][93][94][95][96][97][98][99] Table 3, [62,77,[100][101][102][103][104][105] and Table 4, [27,[106][107][108][109] respectively, for comparison. Most catalysts…”

Section: Cnt-based Cof Catalystmentioning

confidence: 99%

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Covalent Organic Framework: An Emerging Catalyst for Renewable Ammonia Production

2023

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Ammonia (NH3), a fertilizer feedstock and clean energy carrier, is produced primarily by the Haber‐Bosch method, which is environmentally hazardous and energy intensive. Therefore, there is an immediate need for a benign alternative, like catalytic nitrogen fixation, such as catalytic nitrogen reduction reaction (NRR). NRR must involve active, selective, scalable, and long‐lived catalysts to become a sustainable source of ammonia production. Recently, covalent organic frameworks (COFs) and COF‐based functional materials have been proposed as promising catalysts for NRR. COFs comprise repeating units of organic molecules connected by strong covalent bonds. By fine‐tuning the building blocks, various COFs can be designed with numerous active sites. This class of materials offers excellent modularity, porosity, stability, and low density. A novel type of nitrogen‐abundant COFs called covalent triazine framework (CTF) has been noted for its high electron density and ultra‐stability. This review examines the state‐of‐the‐art for the NRR using different COF‐based catalysts and discusses design principles for advancing it. The underlying mechanism of NRR with different strategies adopted for renewable ammonia production is also discussed for a clear understanding of the process. Furthermore, key parameters for improving ammonia synthesis‘s photo/electrocatalytic efficiency will also be highlighted to present new possibilities to this emerging field.

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Section: Cof‐based Catalysts For Renewable Ammonia Synthesismentioning

confidence: 99%

Section: Cnt-based Cof Catalystmentioning

confidence: 99%

Covalent Organic Framework: An Emerging Catalyst for Renewable Ammonia Production

2023

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Section: Electrocatalytic Applications and The Dynamic Coordination S...mentioning

confidence: 99%

“…have prepared Fe SACs with Fe–N 3 S moiety toward NRR. [ 150 ] Electrochemical measurements in 0.1 m KOH electrolyte revealed the enhanced NRR activity with highest FE of 23.7% and NH 3 yield rate of approximately 14.9 µg h −1 mg cat −1 at −0.1 V versus RHE (Figure 13e). Beyond the investigation of Fe SACs, J. Pennycook's group successfully prepared effective Cu SACs with mixed Cu–N 2 and Cu–N 4 /N 3 C structure as the NRR electrocatalysts.…”

Section: Electrocatalytic Applications and The Dynamic Coordination S...mentioning

confidence: 99%

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Dynamic Coordination Structure Evolutions of Atomically Dispersed Metal Catalysts for Electrocatalytic Reactions

Tan

Wang

Lin

et al. 2022

Adv Materials Inter

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and high-efficient renewable energy conversion devices such as fuel cells and batteries. Hence, the development of costeffective catalysts in facilitating various electrocatalytic reactions with high activity and selectivity is urgently needed. [2,3] In the last two decades, nanoparticles have been preferred as the efficient catalysts for various heterogeneous catalysis process. [4,5] However, it should be noted that only the surface atoms would participate in the electrocatalysis process, while metal atoms embedded in nanoparticles cannot be fully utilized. Hence, downsizing the metal sizes of nanoparticles to atomically dispersed metal atoms to form single-atom catalysts (SACs) is a promising strategy, which aims to achieve a comparable electrocatalytic performance to nanoparticles but with maximized atom efficiency and greatly reduced cost of catalyst preparation. [5][6][7] The concept of "SACs" was first developed in heterogeneous catalysis by Zhang et al. in 2011, they used coprecipitation method to synthesize isolated Pt single atoms anchored onto FeO substrates, which exhibited extraordinary activity in CO oxidation. [8] This pioneering work sheds light on using SACs as promising electrocatalysts for the improved activity in the crucial energy-conversion electrochemical reactions.Due to the extremely high surface energy, the single metal atoms in SACs are likely to migrate and aggregate under synthetic and electrocatalytic conditions, and they are generally stabilized by a support matrix such as MOFs [9,10] and graphene-like carbon nitride. [11][12][13] Therefore, the interaction of the single-atom sites with the ideal supports and the electronic properties of SACs can be regulated through changing the host or doping heteroatom. Note that, the metal sites and local coordination environments including the metal-support interaction (MSI) play a crucial synergistic role in dominating electrocatalytic reactions, which is closely correlated to the activity and stability of SACs. [14] Hence, understanding the coordination structure-performance correlation in SACs is the paramount guidance for the development of highly efficient SACs for electrocatalytic reactions.Although many breakthroughs on fabrication strategies and characterization techniques of SACs in various electrocatalytic reactions have been recorded, [15][16][17][18][19][20] a deeper understanding of the dynamic nature of single metal active sites with local coordination structures under realistic working conditions is still poorly studied. In most studies, the isolated metal centers in the SACs with the static atomic configurations based on ex situ Single-atom catalysts (SACs) are regarded as promising electrocatalysts for various reactions in the field of energy conversion and storage owing to their maximized atom utilization efficiency and unique electronic properties. The modifications of local coordination structures of single metal centers play significant roles in dominating catalytic performances, thus the SACs are resurveyed with different l...

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Screening MXene-based single-atom catalysts for selective nitrate-to-ammonia electroreduction

Wang

et al. 2023

Sci. China Mater.

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Boosting nitrogen reduction to ammonia on Fe–N3S sites by introduction S into defect graphene

Cited by 8 publications

References 31 publications

Covalent Organic Framework: An Emerging Catalyst for Renewable Ammonia Production

Covalent Organic Framework: An Emerging Catalyst for Renewable Ammonia Production

Dynamic Coordination Structure Evolutions of Atomically Dispersed Metal Catalysts for Electrocatalytic Reactions

Screening MXene-based single-atom catalysts for selective nitrate-to-ammonia electroreduction

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