Materials: Elemental iron (Fe, 99.99%, Sigma Aldrich, USA), red phosphorus powder (P, 100
mesh, 99%, Alfa Aesar, USA), potassium bicarbonate (KHCO3), and sulfur (S, 99.98%,
Aldrich, USA) were purchased. Analytical grade acetone was purchased from Fisher
Scientific and it was distilled and used for the exfoliation of layered Fe2P2S6. The sealing
system (PPS-90, MRVS-1002) was purchased from Partulab Technology Co. Ltd. The water
use throughout all experiments was purified through a Millipore system.

Electrochemical conversion of CO2 into alcohols provides an attractive path toward
achieving a carbon-neutral cycle, while its efficiency is challenged by identifying active
electrocatalysts for the CO2 reduction reaction (CO2RR). In this work, we report the
Fe2P2S6 nanosheet acts as an efficient CO2RR electrocatalytst toward highly selective
hydrogenation of CO2 to alcohols. This catalyst is capable of achieving a high total Faradaic
efficiency (FEmethanol+ ethanol) of 88.3%, with a FEmethanol up to 65.2% at− 0.20 V vs the …