Abstract
Boron has been explored as p-block catalysts for nitrogen reduction reaction (NRR) by density functional theory. Unlike transition metals, on which the active centers need empty d orbitals to accept the lone-pair electrons of the nitrogen molecule, the sp 3 hybrid orbital of the boron atom can form B-to-N π -back bonding. This results in the population of the N-N π∗ orbital and the concomitant decrease of the N-N bond order. We demonstrate that the catalytic activity of boron is highly correlated with the degree of charge transfer between the boron atom and the substrate. Among the 21 concept-catalysts, single boron atoms supported on graphene and substituted into h-MoS 2 are identified as the most promising NRR catalysts, offering excellent energy efficiency and selectivity against hydrogen evolution reaction.
| Original language | English |
|---|---|
| Pages (from-to) | 2884-2888 |
| Number of pages | 5 |
| Journal | Journal of the American Chemical Society |
| Volume | 141 |
| Issue number | 7 |
| DOIs | |
| Publication status | Published - 1 Jan 2019 |
Cite this
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Single-Boron Catalysts for Nitrogen Reduction Reaction. / Liu, Chuangwei; Li, Qinye; Wu, Chengzhang; Zhang, Jie; Jin, Yonggang; Macfarlane, Douglas R.; Sun, Chenghua.
In: Journal of the American Chemical Society, Vol. 141, No. 7, 01.01.2019, p. 2884-2888.Research output: Contribution to journal › Article › Research › peer-review
TY - JOUR
T1 - Single-Boron Catalysts for Nitrogen Reduction Reaction
AU - Liu, Chuangwei
AU - Li, Qinye
AU - Wu, Chengzhang
AU - Zhang, Jie
AU - Jin, Yonggang
AU - Macfarlane, Douglas R.
AU - Sun, Chenghua
PY - 2019/1/1
Y1 - 2019/1/1
N2 - Boron has been explored as p-block catalysts for nitrogen reduction reaction (NRR) by density functional theory. Unlike transition metals, on which the active centers need empty d orbitals to accept the lone-pair electrons of the nitrogen molecule, the sp 3 hybrid orbital of the boron atom can form B-to-N π -back bonding. This results in the population of the N-N π∗ orbital and the concomitant decrease of the N-N bond order. We demonstrate that the catalytic activity of boron is highly correlated with the degree of charge transfer between the boron atom and the substrate. Among the 21 concept-catalysts, single boron atoms supported on graphene and substituted into h-MoS 2 are identified as the most promising NRR catalysts, offering excellent energy efficiency and selectivity against hydrogen evolution reaction.
AB - Boron has been explored as p-block catalysts for nitrogen reduction reaction (NRR) by density functional theory. Unlike transition metals, on which the active centers need empty d orbitals to accept the lone-pair electrons of the nitrogen molecule, the sp 3 hybrid orbital of the boron atom can form B-to-N π -back bonding. This results in the population of the N-N π∗ orbital and the concomitant decrease of the N-N bond order. We demonstrate that the catalytic activity of boron is highly correlated with the degree of charge transfer between the boron atom and the substrate. Among the 21 concept-catalysts, single boron atoms supported on graphene and substituted into h-MoS 2 are identified as the most promising NRR catalysts, offering excellent energy efficiency and selectivity against hydrogen evolution reaction.
UR - http://www.scopus.com/inward/record.url?scp=85061527693&partnerID=8YFLogxK
U2 - 10.1021/jacs.8b13165
DO - 10.1021/jacs.8b13165
M3 - Article
VL - 141
SP - 2884
EP - 2888
JO - Journal of the American Chemical Society
JF - Journal of the American Chemical Society
SN - 0002-7863
IS - 7
ER -