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. 2016 Sep 2:7:12697.
doi: 10.1038/ncomms12697.

Metallic tin quantum sheets confined in graphene toward high-efficiency carbon dioxide electroreduction

Fengcai Lei  1 , Wei Liu  2 , Yongfu Sun  1   3 , Jiaqi Xu  1 , Katong Liu  1 , Liang Liang  1 , Tao Yao  2   3 , Bicai Pan  1 , Shiqiang Wei  2   3 , Yi Xie  1   3
Affiliations

Metallic tin quantum sheets confined in graphene toward high-efficiency carbon dioxide electroreduction

Fengcai Lei et al. Nat Commun. .

Abstract

Ultrathin metal layers can be highly active carbon dioxide electroreduction catalysts, but may also be prone to oxidation. Here we construct a model of graphene confined ultrathin layers of highly reactive metals, taking the synthetic highly reactive tin quantum sheets confined in graphene as an example. The higher electrochemical active area ensures 9 times larger carbon dioxide adsorption capacity relative to bulk tin, while the highly-conductive graphene favours rate-determining electron transfer from carbon dioxide to its radical anion. The lowered tin-tin coordination numbers, revealed by X-ray absorption fine structure spectroscopy, enable tin quantum sheets confined in graphene to efficiently stabilize the carbon dioxide radical anion, verified by 0.13 volts lowered potential of hydroxyl ion adsorption compared with bulk tin. Hence, the tin quantum sheets confined in graphene show enhanced electrocatalytic activity and stability. This work may provide a promising lead for designing efficient and robust catalysts for electrolytic fuel synthesis.

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Figures

Figure 1
Figure 1. Scheme.
Schematic illustration depicts the several advantages of ultrathin metal layers confined in graphene for CO2 electroreduction into hydrocarbon fuels.
Figure 2
Figure 2. Formation process and characterizations of the Sn quantum sheets confined in graphene.
(a) Scheme illustration for the formation of Sn quantum sheets confined in graphene, (b) TEM image, (c) HRTEM image, (d–f) AFM image, the corresponding height profile and scheme illustration and (g) micro-Raman spectrum of the Sn quantum sheets confined in graphene. (h) TG analysis of Sn quantum sheets confined in graphene, 15 nm Sn nanoparticles and 15 nm Sn nanoparticles mixed with graphene. The scale bars in (b–d) are 100, 10 and 200 nm, respectively. The inset circles in (c) denote the presence of Sn quantum sheets.
Figure 3
Figure 3. Synchrotron radiation XAFS measurements.
(a) Sn K-edge extended XAFS oscillation function k3χ(k), (b) the corresponding Fourier transforms FT(k3χ(k)) for the graphene confined Sn quantum sheets, 15 nm Sn nanoparticles and bulk Sn, respectively.
Figure 4
Figure 4. CO2 electroreduction performances.
(a) Linear sweep voltammetric curves in the CO2-saturated 0.1 M NaHCO3 aqueous solution, (b) Faradaic efficiencies for formate at each applied potentials for 4 h, (c) Tafel plots for producing formate, (d) Chrono-Amperometry results at the potentials of −1.8 V versus SCE for the Sn quantum sheets confined in graphene, 15 nm Sn nanoparticles mixed with graphene, 15 nm Sn nanoparticles and bulk Sn. The error bars in b represent the standard deviations of five independent measurements of the same sample.
Figure 5
Figure 5. Advantages of the Sn quantum sheets confined in graphene.
(a) Charging current density differences plotted against scan rates; (b) CO2 adsorption isotherms; (c) Nyquist plots; (d) single oxidative LSV scans in N2-saturated 0.1 M NaOH for the Sn quantum sheets confined in graphene, 15 nm Sn nanoparticles mixed with graphene, 15 nm Sn nanoparticles and bulk Sn.
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