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Immobilization of Iron Phthalocyanine on Pyridine-Functionalized Carbon Nanotubes for Efficient Nitrogen Reduction Reaction
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- Xu, Suxian (author)
- Dalian Univ Technol, DUT KTH Joint Educ & Res Ctr Mol Devices, State Key Lab Fine Chem, Dalian 116024, Peoples R China.
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- Ding, Yunxuan (author)
- Westlake Univ, Ctr Artificial Photosynth Solar Fuels, Sch Sci, Hangzhou 310024, Peoples R China.
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- Du, Jian (author)
- Dalian Univ Technol, DUT KTH Joint Educ & Res Ctr Mol Devices, State Key Lab Fine Chem, Dalian 116024, Peoples R China.
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- Dalian Univ Technol, DUT KTH Joint Educ & Res Ctr Mol Devices, State Key Lab Fine Chem, Dalian 116024, Peoples R China Westlake Univ, Ctr Artificial Photosynth Solar Fuels, Sch Sci, Hangzhou 310024, Peoples R China. (creator_code:org_t)
- 2022-04-25
- 2022
- English.
- In: ACS Catalysis. - : American Chemical Society (ACS). - 2155-5435. ; 12:9, s. 5502-5509
- Journal article (peer-reviewed)
Abstract
Subject headings
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- An electrochemical nitrogen reduction reaction (NRR) under mild conditions offers a promising alternative to the traditional Haber-Bosch process in converting abundant nitrogen (N2) to high value-added ammonia (NH3). In this work, iron phthalocyanine (FePc) was homogeneously immobilized on pyridine-functionalized carbon nanotubes to form a well-tuned electrocatalyst with an FeN5 active center (FePc-Py-CNT). Synchrotron X-ray absorption and Fourier transform infrared spectroscopy proved the presence of an Fe-N coordination bond between FePc and surface-bound pyridine. The resulting hybrid exhibited notably enhanced electrocatalytic NRR performance compared to FePc immobilized on CNTs based on pi-pi stacking interactions (FePc-CNT), resulting in doubled NH3 yield (21.7 mu g 1 h mgcat-1h-1) and Faradaic efficiency (22.2%). Theoretical calculations revealed that the axial coordination on FePc resulted in partial electron transfer from iron to pyridine, which efficiently suppresses the adsorption of H+ and improves the chemisorption of N2 at Fe sites. Meanwhile, the interfacial electron transfer was facilitated by pyridine as an electron transfer relay between FePc and CNTs. This work provides a unique strategy for the design of highly efficient NRR electrocatalysts at the molecular level.
Subject headings
- NATURVETENSKAP -- Kemi -- Organisk kemi (hsv//swe)
- NATURAL SCIENCES -- Chemical Sciences -- Organic Chemistry (hsv//eng)
Keyword
- nitrogen reduction reaction
- axial coordination
- Fe phthalocyanine
- heterogeneous molecular electrocatalysis
- interfacial electron transfer
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- ref (subject category)
- art (subject category)
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- Xu, Suxian
- Ding, Yunxuan
- Du, Jian
- Zhu, Yong
- Liu, Guoquan
- Wen, Zhibing
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- Liu, Xiao
- Shi, Yongbin
- Gao, Hua
- Sun, Licheng, 19 ...
- Li, Fei
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