Dual-Doping Promotes the Carbon Dioxide Electroreduction Activity of MoS₂ Nanosheet Array

Abstract

Electrocatalytic reduction of CO2 (ECR) to valuable fuels and chemicals using spare renewable energy offers a promising strategy to realize the artificial carbon cycle. Significant advances in ECR have been achieved, but challenges remain, such as accelerating the rate-limiting CO desorption step required for MoS2. Here, a N,P-codoped MoS2 nanosheet array was synthesized via a hydrothermal method, followed by an NH3-etching treatment. It can effectively catalyze CO2 reduction to CO with the highest faradaic efficiency of 91.5% at −0.9 V vs RHE in an ionic liquid electroyte. Meanwhile, the catalyst can maintain the ECR activity for 30 h with negligible decay. The theoretical calculations indicate that the dopants synergistically promote the desorption of the *CO moiety, thus resulting in an enhanced ECR activity. This work opens a new avenue for designing MoS2-based materials for the electroreduction of CO2 to CO.

Ionic Liquid‐Assisted Electrocatalytic NO Reduction to NH3 by P‐Doped MoS2

“…−1 ) as compared to NRR, because NO is a polar molecule with weaker bond energy [25,26] . Two‐dimensional metal chalcogenides, especially MoS 2 , have attracted considerable interest in various electrochemical reactions due to their unique and remarkable electrical, chemical, mechanical and thermal performances [26–30] . One recent study from Sun's group confirmed that MoS 2 nanosheets array could catalyze NORR with a maximal NH 3 yield rate of 99.6 μmol h −1 cm −2 at −0.7 V versus the reversible hydrogen electrode (vs RHE) (while the obtained Faradaic efficiency (FE) is less than 30 %) [31] .…”

Boosting the electrochemiluminescence of luminol by high-intensity focused ultrasound pretreatment combined with 1T/2H MoS2 catalysis to construct a sensitive sensing platform

“…For example, the narrow band gap of MoS 2 endows it have photoelectric effect [28] , thus, it is promising in photocatalysis [29] , [30] . Furthermore, MoS 2 shows electrocatalytic activity because of unique electronic structure, and it has been expected to be a wonderful catalyst for hydrogen evolution reaction (HER) [31] , CO 2 [32] or N 2 [33] reduction reactions. MoS 2 has various crystal phase structures due to different coordination of atoms [34] .…”

Electrochemical CO2 Reduction over a MoS2/Mo Electrode

“…In particular, MoS 2 exhibits a high activity for photocatalyzed and electrocatalyzed hydrogen evolution reactions (HER) [4][5][6][7][8]10,11]. However, the MoS 2 -assisted catalytic CO 2 reduction process has been rarely experimentally explored [12][13][14][15][16][17][18][19][20][21][22][23][24][25][26][27]. According to previous studies, CO is obtained as the major product of the photocatalytic reduction of CO 2 over MoS 2 (prepared by chemical vapor deposition) [12].…”

“…For example, theoretically, the catalytic activity of a single-atom Ni 1 /MoS 2 catalyst for electrocatalytic CO 2 reduction to produce methanol is higher than that of other metals [26]. Moreover, ionic liquids are used in EC CO 2 R experiments [19][20][21][22][23]. Asadi et al [20] demonstrated that MoS 2 exhibits a high Faradaic efficiency (FE) for CO production in an ionic liquid owing to the presence of Mo-terminated edges with a high density of d electrons and low work function (3.9 eV) [20].…”

“…Asadi et al [20] demonstrated that MoS 2 exhibits a high Faradaic efficiency (FE) for CO production in an ionic liquid owing to the presence of Mo-terminated edges with a high density of d electrons and low work function (3.9 eV) [20]. N, P-co-doped MoS 2 nanosheet ar-rays also exhibit a high FE (91.5 %) for CO production [21]. Lv et al [22] showed that the CO/H 2 syngas can be produced with a tunable ratio using fluorosilane-decorated MoS 2 via EC CO 2 R in a CO 2saturated ionic liquid.…”