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Article
Qian Peng
Nankai University
Corresponding Author
ORCiD: https://orcid.org/0000-0002-1218-5976
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This work is licensed under a CC BY 4.0 License. Read Full License
Ammonia synthesis from N2 under mild conditions is a long-term pursuit and goal, which theoretically limited by the Brønsted–Evans–Polanyi (BEP) relation in industrial transformation via the N2 dissociation. Here we show that the Fe2 catalyst combined with the “vicinal nonmetallic sites” may break the BEP limitation to fulfill the efficient ammonia synthesis. The catalyst supported on boron doped graphitic carbon nitride (Fe2/B/mpg-C3N4) strongly favors hydrogenation of N2 to form a NHNH2 species, which leads to low energy barriers for N-H formation (0.57eV) and N-N dissociation (0.51eV). Constructed B-N “Lewis pairs” on the mpg-C3N4 serve as nonmetallic sites can activate and transfer hydrogen, which reduce the competitive adsorption of N2 and H2. Through co-activated H2 on the vicinal site, synergistic Fe2 catalyst shows a significant advantage among Fen/mpg-C3N4 (n=2, 3, 4) catalysts and thus can avoid harsh reaction condition for the thermal conversion of N2 to NH3.
Keywords
Brønsted–Evans–Polanyi Relation, Industrial Transformation, N2 Dissociation, B-N Lewis Pairs, Competitive Adsorption
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There is NO Competing Interest.
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Scheme 1. (a) Synthetic ammonia in thermal catalysis and (b) Schematic diagram of theoretical prediction of high efficiency iron catalyst.
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This preprint is under consideration at a Nature Portfolio Journal. A preprint is a preliminary version of a manuscript that has not completed peer review at a journal. Research Square does not conduct peer review prior to posting preprints. The posting of a preprint on this server should not be interpreted as an endorsement of its validity or suitability for dissemination as established information or for guiding clinical practice.
Nature journals have partnered with Research Square to offer In Review, a journal-integrated preprint deposition service.
Article
Qian Peng
Nankai University
Corresponding Author
ORCiD: https://orcid.org/0000-0002-1218-5976
Badges
Prescreen
This manuscript passed our Prescreen assessment
Complete author information
Appropriate declaration statements
Potential risks to human health
Prescreen
Peer Review Timeline
CURRENT STATUS: Under Review
Version 1
Posted 22 Mar, 2021
Metrics
Comments: 0
PDF Downloads: ...
HTML Views: ...
Subject Areas
Catalysis
License:
This work is licensed under a CC BY 4.0 License. Read Full License
Ammonia synthesis from N2 under mild conditions is a long-term pursuit and goal, which theoretically limited by the Brønsted–Evans–Polanyi (BEP) relation in industrial transformation via the N2 dissociation. Here we show that the Fe2 catalyst combined with the “vicinal nonmetallic sites” may break the BEP limitation to fulfill the efficient ammonia synthesis. The catalyst supported on boron doped graphitic carbon nitride (Fe2/B/mpg-C3N4) strongly favors hydrogenation of N2 to form a NHNH2 species, which leads to low energy barriers for N-H formation (0.57eV) and N-N dissociation (0.51eV). Constructed B-N “Lewis pairs” on the mpg-C3N4 serve as nonmetallic sites can activate and transfer hydrogen, which reduce the competitive adsorption of N2 and H2. Through co-activated H2 on the vicinal site, synergistic Fe2 catalyst shows a significant advantage among Fen/mpg-C3N4 (n=2, 3, 4) catalysts and thus can avoid harsh reaction condition for the thermal conversion of N2 to NH3.
Figure 1
Figure 2
Figure 3
Figure 4
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Figure 6
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Figure 9
Figure 10
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