Evaluation of electrocatalytic dinitrogen reduction performance on diamond carbon via density functional theory

Guo, Z; Qiu, S; Li, H; Xu, Y; Langford, SJ; Sun, C

Evaluation of electrocatalytic dinitrogen reduction performance on diamond carbon via density functional theory

Guo, Z Qiu, S Li, H Xu, Y Langford, SJ Sun, C

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Publisher:: Elsevier BV
Publication Type:: Journal Article
Citation:: Diamond and Related Materials, 2021, 111, pp. 108210
Issue Date:: 2021-01-01

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Field	Value	Language
dc.contributor.author	Guo, Z
dc.contributor.author	Qiu, S
dc.contributor.author	Li, H
dc.contributor.author	Xu, Y
dc.contributor.author	Langford, SJ
dc.contributor.author	Sun, C
dc.date.accessioned	2022-02-01T00:12:13Z
dc.date.available	2022-02-01T00:12:13Z
dc.date.issued	2021-01-01
dc.identifier.citation	Diamond and Related Materials, 2021, 111, pp. 108210
dc.identifier.issn	0925-9635
dc.identifier.uri	http://hdl.handle.net/10453/154015
dc.description.abstract	Carbon-based electrocatalysts for nitrogen fixation under ambient conditions has attracted tremendous attention but still encounter great challenges of low Faradic efficiency (FE) and a sluggish kinetics. Inspired by intrinsic defects (vacancies, edges and dislocation) on graphene showing activity towards oxygen reduction reaction (ORR) and nitrogen reduction reaction (NRR), here, two commonly exposed surfaces of diamond carbon, i.e., C(111) & C(110), were calculated for electrocatalytic nitrogen reduction reaction (eNRR) by the density functional theory (DFT) method, and calculations show that, compared with C(110), C(111) could be highly promising towards eNRR with a low over-potential (η) of 0.57 V (ΔGmax = 0.73 eV, η = 0.57 V), which are distinctly less than that (ΔGmax = 1.08 eV, η = 0.92 V) of flat benchmark Ru(0001) catalysts. Importantly, these two surfaces are shown to exhibit the suppression of hydrogen evolution reaction (HER). This work is the first reported indication that the low-coordinated carbons (LCCs) on sp3-hybridized diamond-carbon framework are active for eNRR, which gives a brand-new direction of designing/synthesizing sp3-configured diamond-carbon-composited catalysts for eNRR.
dc.language	en
dc.publisher	Elsevier BV
dc.relation.ispartof	Diamond and Related Materials
dc.relation.isbasedon	10.1016/j.diamond.2020.108210
dc.rights	info:eu-repo/semantics/embargoedAccess
dc.subject	0904 Chemical Engineering, 0910 Manufacturing Engineering, 0912 Materials Engineering
dc.subject.classification	Applied Physics
dc.title	Evaluation of electrocatalytic dinitrogen reduction performance on diamond carbon via density functional theory
dc.type	Journal Article
utslib.citation.volume	111
utslib.for	0904 Chemical Engineering
utslib.for	0910 Manufacturing Engineering
utslib.for	0912 Materials Engineering
pubs.organisational-group	/University of Technology Sydney
pubs.organisational-group	/University of Technology Sydney/Faculty of Science
pubs.organisational-group	/University of Technology Sydney/Faculty of Science/School of Mathematical and Physical Sciences
utslib.copyright.status	open_access	*
utslib.copyright.embargo	2023-01-01T00:00:00+1000Z
dc.date.updated	2022-02-01T00:12:12Z
pubs.publication-status	Published
pubs.volume	111

Abstract:

Carbon-based electrocatalysts for nitrogen fixation under ambient conditions has attracted tremendous attention but still encounter great challenges of low Faradic efficiency (FE) and a sluggish kinetics. Inspired by intrinsic defects (vacancies, edges and dislocation) on graphene showing activity towards oxygen reduction reaction (ORR) and nitrogen reduction reaction (NRR), here, two commonly exposed surfaces of diamond carbon, i.e., C(111) & C(110), were calculated for electrocatalytic nitrogen reduction reaction (eNRR) by the density functional theory (DFT) method, and calculations show that, compared with C(110), C(111) could be highly promising towards eNRR with a low over-potential (η) of 0.57 V (ΔGmax = 0.73 eV, η = 0.57 V), which are distinctly less than that (ΔGmax = 1.08 eV, η = 0.92 V) of flat benchmark Ru(0001) catalysts. Importantly, these two surfaces are shown to exhibit the suppression of hydrogen evolution reaction (HER). This work is the first reported indication that the low-coordinated carbons (LCCs) on sp3-hybridized diamond-carbon framework are active for eNRR, which gives a brand-new direction of designing/synthesizing sp3-configured diamond-carbon-composited catalysts for eNRR.

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http://hdl.handle.net/10453/154015