TY - JOUR
T1 - Transition metal atom anchored by defective WSSe monolayer as bifunctional single atom catalyst for ORR and OER
AU - Zhang, Xian
AU - Luo, Zhifen
AU - Zhou, Zibo
AU - Wang, Yuwan
AU - Cui, Zichun
AU - Gao, Zhihao
AU - Shi, Junqin
AU - Cao, Tengfei
AU - Fan, Xiaoli
N1 - Publisher Copyright:
© 2022 Elsevier B.V.
PY - 2022/10/1
Y1 - 2022/10/1
N2 - Bifunctional electrocatalysts with high catalytic activity toward oxygen reduction reaction (ORR) and oxygen evolution reaction (OER) are key for developing efficient energy conversion and storage technology. Here, we investigated the ORR and OER electrocatalytic activity of transition metal atoms (TM) anchored at the S and Se vacancy sites of WSSe monolayer (TM@S-WSSe, TM@Se-WSSe) via performing the first-principles calculation. Our result shows that the single atom catalysts (SACs) Pt@S-WSSe and Pt@Se-WSSe have low ORR/OER overpotentials (ηORR/ηOER) of 0.31/0.36 V and 0.43/0.34 V, respectively. The ηORR and ηOER at SAC Pt@S-WSSe are even lower compared with the previously studied SACs. Besides, the Gibbs free energy changes of the key intermediate adsorption are close to the values at ideal catalyst. Our calculations demonstrate the promising potential of Pt@S-WSSe and Pt@Se-WSSe as ORR and OER bifunctional SACs. More importantly, the superior ORR and OER catalytic activity of TM@S-WSSe and TM@Se-WSSe are well explained via the intrinsic feature of SACs as well as the interaction between the TM atom and the intermediates. Especially, we demonstrate that the magnetic moment and the catalytic activity of SACs TM@S-WSSe and TM@Se-WSSe is closely correlated. Our result provides new idea for designing highly effectual ORR and OER bifunctional SACs.
AB - Bifunctional electrocatalysts with high catalytic activity toward oxygen reduction reaction (ORR) and oxygen evolution reaction (OER) are key for developing efficient energy conversion and storage technology. Here, we investigated the ORR and OER electrocatalytic activity of transition metal atoms (TM) anchored at the S and Se vacancy sites of WSSe monolayer (TM@S-WSSe, TM@Se-WSSe) via performing the first-principles calculation. Our result shows that the single atom catalysts (SACs) Pt@S-WSSe and Pt@Se-WSSe have low ORR/OER overpotentials (ηORR/ηOER) of 0.31/0.36 V and 0.43/0.34 V, respectively. The ηORR and ηOER at SAC Pt@S-WSSe are even lower compared with the previously studied SACs. Besides, the Gibbs free energy changes of the key intermediate adsorption are close to the values at ideal catalyst. Our calculations demonstrate the promising potential of Pt@S-WSSe and Pt@Se-WSSe as ORR and OER bifunctional SACs. More importantly, the superior ORR and OER catalytic activity of TM@S-WSSe and TM@Se-WSSe are well explained via the intrinsic feature of SACs as well as the interaction between the TM atom and the intermediates. Especially, we demonstrate that the magnetic moment and the catalytic activity of SACs TM@S-WSSe and TM@Se-WSSe is closely correlated. Our result provides new idea for designing highly effectual ORR and OER bifunctional SACs.
KW - Bifunctional electrocatalyst
KW - Catalytic activity
KW - First-principles method
KW - Janus WSSe monolayer
KW - Single atom catalyst
UR - http://www.scopus.com/inward/record.url?scp=85137161262&partnerID=8YFLogxK
U2 - 10.1016/j.jelechem.2022.116731
DO - 10.1016/j.jelechem.2022.116731
M3 - 文章
AN - SCOPUS:85137161262
SN - 1572-6657
VL - 922
JO - Journal of Electroanalytical Chemistry
JF - Journal of Electroanalytical Chemistry
M1 - 116731
ER -