Hydrophobic and Electronic Properties of the E‐MoS₂ Nanosheets Induced by FAS for the CO₂ Electroreduction to Syngas with a Wide Range of CO/H₂ Ratios

Abstract

The electrochemical CO2 reduction reaction (CO2RR) to produce CO and H2 (syngas) is a promising method for clean energy, but challenges remain, such as controlling the CO/H2 ratios required for the syngas yield. Herein, hydrophobic exfoliated MoS2 (H‐E‐MoS2) nanosheets are fabricated from bulk MoS2 by a cost‐effective ball‐milling method, followed by decoration with fluorosilane (FAS). H‐E‐MoS2 is a cost‐effective electrocatalyst capable of directly reducing CO2 and H2O for tuneable syngas production with a wide range of CO/H2 ratios (from 1:2 to 4:1). In addition, H‐E‐MoS2 shows a high current density, 61 mA cm−2 at −1.1 V, and the highest CO FE of 81.2% at −0.9 V, which are higher than those of unmodified MoS2. According to density functional theory calculations, FAS decoration on the surface of MoS2 electrode can change the electronic properties of the edge Mo atom, which facilitates the rate‐limiting CO‐desorption step, thus promoting CO2RR. Moreover, the hydrophobic surface of H‐E‐MoS2 depressed the H2 evolution reaction and created abundant three‐phase contact points that provided sufficient CO2. The hydrophobization of the electrode may provide an effective strategy for easily tuning the CO/H2 ratio of syngas in a large range for the direct electroreduction CO2 to syngas with an optimized CO/H2 ratio.

CuxNiy alloy nanoparticles embedded in a nitrogen–carbon network for efficient conversion of carbon dioxide

“…3a). For Cu 1.0 Ni 1.0 /N–C and Cu 4.8 Ni 1.0 /N–C, the increase of current density relates to the HER in the N 2 saturated solution, and the combination of the CO 2 RR and HER in the CO 2 saturated solution 37. The sharp increase of current density in the CO 2 saturated solution compared to that in the N 2 saturated solution indicates that Cu 1.0 Ni 1.0 /N–C and Cu 4.8 Ni 1.0 /N–C are more favorable for the CO 2 RR than the HER.…”

Confined local oxygen gas promotes electrochemical water oxidation to hydrogen peroxide

“…7c, d). Secondly, to demonstrate that the carbon site selectivity for H2O2 formation is not related to the specific surface deposited materials, trimethoxy (1H,1H,2H,2H-heptadecafluorodecyl) silane was used to replace the PTFE to create the similar aerophilic surface to trap O2 gas 32 ( Supplementary Fig. 7e, f).…”

Zn–Cu Alloy Nanofoams as Efficient Catalysts for the Reduction of CO2 to Syngas Mixtures with a Potential‐Independent H2/CO Ratio

“…Previous reports have focusedo nm onometallic molecular [4][5][6] and heterogeneousc atalytic systems, [7][8][9][10][11][12][13][14][15] which have been used fors imultaneous production of CO and H 2 .H owever,s ingle catalytic sites offer limited possibilities for selective tuning of the catalyst. Introducing as econd metal site offers an extra degree of freedom in catalystd esign ando ffers the best route to address the above criteria.…”