Gu, H., Li, J., Niu, X., Lin, J., Chen, L. W., Zhang, Z., Shi, Z., Sun, Z., Liu, Q., Zhang, P., Yan, W., Wang, Y., Zhang, L., Li, P., Li, X., Wang, D., Yin, P., & Chen, W. (2023). Symmetry-Breaking p-Block Antimony Single Atoms Trigger N-Bridged Titanium Sites for Electrocatalytic Nitrogen Reduction with High Efficiency. ACS Nano, 17(21), 21838-21849. https://doi.org/10.1021/acsnano.3c07857
Gu, Hongfei ; Li, Jiani ; Niu, Xiangfu et al. / Symmetry-Breaking p-Block Antimony Single Atoms Trigger N-Bridged Titanium Sites for Electrocatalytic Nitrogen Reduction with High Efficiency. In: ACS Nano. 2023 ; Vol. 17, No. 21. pp. 21838-21849.
@article{9ffe0f99a41e4c2cb896a58cabe132dc,
title = "Symmetry-Breaking p-Block Antimony Single Atoms Trigger N-Bridged Titanium Sites for Electrocatalytic Nitrogen Reduction with High Efficiency",
abstract = "The electrochemical nitrogen reduction reaction (eNRR) under mild conditions emerges as a promising approach to produce ammonia (NH3) compared to the typical Haber-Bosch process. Herein, we design an asymmetrically coordinated p-block antimony single-atom catalyst immobilized on nitrogen-doped Ti3C2Tx (Sb SA/N-Ti3C2Tx) for eNRR, which exhibits ultrahigh NH3 yield (108.3 μg h-1 mgcat-1) and excellent Faradaic efficiency (41.2%) at −0.3 V vs RHE. Complementary in situ spectroscopies with theoretical calculations reveal that the nitrogen-bridged two titanium atoms triggered by an adjacent asymmetrical Sb-N1C2 moiety act as the active sites for facilitating the protonation of the rate-determining step from *N2 to *N2H and the kinetic conversion of key intermediates during eNRR. Moreover, the introduction of Sb-N1C2 promotes the formation of oxygen vacancies to expose more titanium sites. This work presents a strategy for single-atom-decorated ultrathin two-dimensional materials with the aim of simultaneously enhancing NH3 yield and Faradaic efficiency for electrocatalytic nitrogen reduction.",
keywords = "Sb−NC moiety, TiCT MXene, antimony single atom, asymmetrically coordinated catalyst, nitrogen reduction reaction",
author = "Hongfei Gu and Jiani Li and Xiangfu Niu and Jie Lin and Chen, {Li Wei} and Zedong Zhang and Ziqian Shi and Zhiyi Sun and Qingqing Liu and Peng Zhang and Wensheng Yan and Yu Wang and Liang Zhang and Pengfei Li and Xinyuan Li and Dingsheng Wang and Penggang Yin and Wenxing Chen",
note = "Publisher Copyright: {\textcopyright} 2023 American Chemical Society.",
year = "2023",
month = nov,
day = "14",
doi = "10.1021/acsnano.3c07857",
language = "English",
volume = "17",
pages = "21838--21849",
journal = "ACS Nano",
issn = "1936-0851",
publisher = "American Chemical Society",
number = "21",
}
Gu, H, Li, J, Niu, X, Lin, J, Chen, LW, Zhang, Z, Shi, Z, Sun, Z, Liu, Q, Zhang, P, Yan, W, Wang, Y, Zhang, L, Li, P, Li, X, Wang, D, Yin, P & Chen, W 2023, 'Symmetry-Breaking p-Block Antimony Single Atoms Trigger N-Bridged Titanium Sites for Electrocatalytic Nitrogen Reduction with High Efficiency', ACS Nano, vol. 17, no. 21, pp. 21838-21849. https://doi.org/10.1021/acsnano.3c07857
Symmetry-Breaking p-Block Antimony Single Atoms Trigger N-Bridged Titanium Sites for Electrocatalytic Nitrogen Reduction with High Efficiency. / Gu, Hongfei; Li, Jiani; Niu, Xiangfu et al.
In:
ACS Nano, Vol. 17, No. 21, 14.11.2023, p. 21838-21849.
Research output: Contribution to journal › Article › peer-review
TY - JOUR
T1 - Symmetry-Breaking p-Block Antimony Single Atoms Trigger N-Bridged Titanium Sites for Electrocatalytic Nitrogen Reduction with High Efficiency
AU - Gu, Hongfei
AU - Li, Jiani
AU - Niu, Xiangfu
AU - Lin, Jie
AU - Chen, Li Wei
AU - Zhang, Zedong
AU - Shi, Ziqian
AU - Sun, Zhiyi
AU - Liu, Qingqing
AU - Zhang, Peng
AU - Yan, Wensheng
AU - Wang, Yu
AU - Zhang, Liang
AU - Li, Pengfei
AU - Li, Xinyuan
AU - Wang, Dingsheng
AU - Yin, Penggang
AU - Chen, Wenxing
N1 - Publisher Copyright:
© 2023 American Chemical Society.
PY - 2023/11/14
Y1 - 2023/11/14
N2 - The electrochemical nitrogen reduction reaction (eNRR) under mild conditions emerges as a promising approach to produce ammonia (NH3) compared to the typical Haber-Bosch process. Herein, we design an asymmetrically coordinated p-block antimony single-atom catalyst immobilized on nitrogen-doped Ti3C2Tx (Sb SA/N-Ti3C2Tx) for eNRR, which exhibits ultrahigh NH3 yield (108.3 μg h-1 mgcat-1) and excellent Faradaic efficiency (41.2%) at −0.3 V vs RHE. Complementary in situ spectroscopies with theoretical calculations reveal that the nitrogen-bridged two titanium atoms triggered by an adjacent asymmetrical Sb-N1C2 moiety act as the active sites for facilitating the protonation of the rate-determining step from *N2 to *N2H and the kinetic conversion of key intermediates during eNRR. Moreover, the introduction of Sb-N1C2 promotes the formation of oxygen vacancies to expose more titanium sites. This work presents a strategy for single-atom-decorated ultrathin two-dimensional materials with the aim of simultaneously enhancing NH3 yield and Faradaic efficiency for electrocatalytic nitrogen reduction.
AB - The electrochemical nitrogen reduction reaction (eNRR) under mild conditions emerges as a promising approach to produce ammonia (NH3) compared to the typical Haber-Bosch process. Herein, we design an asymmetrically coordinated p-block antimony single-atom catalyst immobilized on nitrogen-doped Ti3C2Tx (Sb SA/N-Ti3C2Tx) for eNRR, which exhibits ultrahigh NH3 yield (108.3 μg h-1 mgcat-1) and excellent Faradaic efficiency (41.2%) at −0.3 V vs RHE. Complementary in situ spectroscopies with theoretical calculations reveal that the nitrogen-bridged two titanium atoms triggered by an adjacent asymmetrical Sb-N1C2 moiety act as the active sites for facilitating the protonation of the rate-determining step from *N2 to *N2H and the kinetic conversion of key intermediates during eNRR. Moreover, the introduction of Sb-N1C2 promotes the formation of oxygen vacancies to expose more titanium sites. This work presents a strategy for single-atom-decorated ultrathin two-dimensional materials with the aim of simultaneously enhancing NH3 yield and Faradaic efficiency for electrocatalytic nitrogen reduction.
KW - Sb−NC moiety
KW - TiCT MXene
KW - antimony single atom
KW - asymmetrically coordinated catalyst
KW - nitrogen reduction reaction
UR - http://www.scopus.com/inward/record.url?scp=85178348863&partnerID=8YFLogxK
U2 - 10.1021/acsnano.3c07857
DO - 10.1021/acsnano.3c07857
M3 - Article
C2 - 37909679
AN - SCOPUS:85178348863
SN - 1936-0851
VL - 17
SP - 21838
EP - 21849
JO - ACS Nano
JF - ACS Nano
IS - 21
ER -
Gu H, Li J, Niu X, Lin J, Chen LW, Zhang Z et al. Symmetry-Breaking p-Block Antimony Single Atoms Trigger N-Bridged Titanium Sites for Electrocatalytic Nitrogen Reduction with High Efficiency. ACS Nano. 2023 Nov 14;17(21):21838-21849. doi: 10.1021/acsnano.3c07857
