TY - JOUR
T1 - A General Method for Transition Metal Single Atoms Anchored on Honeycomb-Like Nitrogen-Doped Carbon Nanosheets
AU - Zhang, Xiaoyan
AU - Zhang, Shan
AU - Yang, Yong
AU - Wang, Liguang
AU - Mu, Zijie
AU - Zhu, Haishuang
AU - Zhu, Xiaoqing
AU - Xing, Huanhuan
AU - Xia, Hongyin
AU - Huang, Bolong
AU - Li, Jing
AU - Guo, Shaojun
AU - Wang, Erkang
PY - 2020/3/12
Y1 - 2020/3/12
N2 - Excavating and developing highly efficient and cost-effective nonnoble metal single-atom catalysts for electrocatalytic reactions is of paramount significance but still in its infancy. Herein, reported is a general NaCl template-assisted strategy for rationally designing and preparing a series of isolated transition metal single atoms (Fe/Co/Ni) anchored on honeycomb-like nitrogen-doped carbon matrix (M1-HNC-T1-T2, M = Fe/Co/Ni, T1 = 500 °C, T2 = 850 °C). The resulting M1-HNC-500-850 with M-N4 active sites exhibits superior capability for oxygen reduction reaction (ORR) with the half-wave potential order of Fe1-HNC-500-850 > Co1-HNC-500-850 > Ni1-HNC-500-850, in which Fe1-HNC-500-850 shows better performance than commercial Pt/C. Density functional theory calculations reveal a choice strategy that the strong p–d-coupled spatial charge separation results the Fe-N4 effectively merges active electrons for elevating d-band activity in a van-Hove singularity like character. This essentially generalizes an optimal electronic exchange-and-transfer (ExT) capability for boosting sluggish alkaline ORR activity. This work not only presents a universal strategy for preparing single-atom electrocatalyst to accelerate the kinetics of cathodic ORR but also provides an insight into the relationship between the electronic structure and the electrocatalytical activity.
AB - Excavating and developing highly efficient and cost-effective nonnoble metal single-atom catalysts for electrocatalytic reactions is of paramount significance but still in its infancy. Herein, reported is a general NaCl template-assisted strategy for rationally designing and preparing a series of isolated transition metal single atoms (Fe/Co/Ni) anchored on honeycomb-like nitrogen-doped carbon matrix (M1-HNC-T1-T2, M = Fe/Co/Ni, T1 = 500 °C, T2 = 850 °C). The resulting M1-HNC-500-850 with M-N4 active sites exhibits superior capability for oxygen reduction reaction (ORR) with the half-wave potential order of Fe1-HNC-500-850 > Co1-HNC-500-850 > Ni1-HNC-500-850, in which Fe1-HNC-500-850 shows better performance than commercial Pt/C. Density functional theory calculations reveal a choice strategy that the strong p–d-coupled spatial charge separation results the Fe-N4 effectively merges active electrons for elevating d-band activity in a van-Hove singularity like character. This essentially generalizes an optimal electronic exchange-and-transfer (ExT) capability for boosting sluggish alkaline ORR activity. This work not only presents a universal strategy for preparing single-atom electrocatalyst to accelerate the kinetics of cathodic ORR but also provides an insight into the relationship between the electronic structure and the electrocatalytical activity.
KW - NaCl template-assisted strategy
KW - oxygen reduction reaction
KW - p–d-coupled spatial charge separation
KW - single-atom electrocatalysts
UR - http://www.scopus.com/inward/record.url?scp=85078828835&partnerID=8YFLogxK
UR - https://www.scopus.com/record/pubmetrics.uri?eid=2-s2.0-85078828835&origin=recordpage
U2 - 10.1002/adma.201906905
DO - 10.1002/adma.201906905
M3 - RGC 21 - Publication in refereed journal
SN - 0935-9648
VL - 32
JO - Advanced Materials
JF - Advanced Materials
IS - 10
M1 - 1906905
ER -