am1c03638_si_001.pdf (1.97 MB)
Engineering Ag–Nx Single-Atom Sites on Porous Concave N‑Doped Carbon for Boosting CO2 Electroreduction
journal contribution
posted on 2021-04-08, 14:51 authored by Rui Sui, Jiajing Pei, Jinjie Fang, Xuejiang Zhang, Yufeng Zhang, Feijun Wei, Wenxing Chen, Zheng Hu, Shi Hu, Wei Zhu, Zhongbin ZhuangThe
electrochemical CO2 reduction reaction (CO2RR)
offers an environmentally benign pathway for renewable energy
conversion and further regulation of the environmental CO2 concentration to achieve carbon cycling. However, developing desired
electrocatalysts with high CO Faradaic efficiency (FECO) at an ultralow overpotential remains a grand challenge. Herein,
we report an effective CO2RR electrocatalyst that features
Ag single-atom coordinated with three nitrogen atoms (Ag1–N3) anchored on porous concave N-doped carbon
(Ag1–N3/PCNC), which is identified by
X-ray absorption spectroscopy. Ag1–N3/PCNC shows a low CO2RR onset potential of −0.24
V, high maximum FECO of 95% at −0.37 V, and high
CO partial current density of 7.6 mA cm–2 at −0.55
V, exceeding most of the previous Ag electrocatalysts. The in situ
infrared absorption spectra technique proves that Ag1–N3 single-atom sites have sole linear-adsorbed CO and can easily
desorb *CO species to achieve the highest CO selectivity in comparison
with the corresponding counterparts. This work provides significant
inspiration on boosting CO2RR by tuning the active center
at an atomic level to achieve a specific absorption with an intermediate.