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. 2020 Jun 25;5(26):16003-16009.
doi: 10.1021/acsomega.0c01363. eCollection 2020 Jul 7.

Conversion of Methane into Methanol Using the [6,6'-(2,2'-Bipyridine-6,6'-Diyl)bis(1,3,5-Triazine-2,4-Diamine)](Nitrato-O)Copper(II) Complex in a Solid Electrolyte Reactor Fuel Cell Type

Luis M S Garcia  1   2 , Sanil Rajak  2 , Khaoula Chair  2 , Camila M Godoy  1 , Araceli Jardim Silva  1 , Paulo V R Gomes  3 , Edgar Aparecido Sanches  3 , Andrezza S Ramos  1 , Rodrigo F B De Souza  1 , Adam Duong  2 , Almir O Neto  1
Affiliations

Conversion of Methane into Methanol Using the [6,6'-(2,2'-Bipyridine-6,6'-Diyl)bis(1,3,5-Triazine-2,4-Diamine)](Nitrato-O)Copper(II) Complex in a Solid Electrolyte Reactor Fuel Cell Type

Luis M S Garcia et al. ACS Omega. .

Abstract

The application of solid electrolyte reactors for methane oxidation to co-generation of power and chemicals could be interesting, mainly with the use of materials that could come from renewable sources and abundant metals, such as the [6,6'- (2, 2'-bipyridine-6, 6'-diyl)bis (1,3,5-triazine-2, 4-diamine)](nitrate-O)copper (II) complex. In this study, we investigated the optimal ratio between this complex and carbon to obtain a stable, conductive, and functional reagent diffusion electrode. The most active Cu-complex compositions were 2.5 and 5% carbon, which were measured with higher values of open circuit and electric current, in addition to the higher methanol production with reaction rates of 1.85 mol L-1 h-1 close to the short circuit potential and 1.65 mol L-1 h-1 close to the open circuit potential, respectively. This activity was attributed to the ability of these compositions to activate water due to better distribution of the Cu complex in the carbon matrix as observed in the rotating ring disk electrode experiments.

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Conflict of interest statement

The authors declare no competing financial interest.

Figures

Scheme 1
Scheme 1. Molecular Structure of Ligand 1 and Cu-Complex 2
Figure 1
Figure 1
Solid electrolyte reactor.
Figure 2
Figure 2
Cyclic voltammetry of Cu-complex/Carbon Vulcan material in 1 mol L–1 KOH (v = 10 mV s–1).
Figure 3
Figure 3
RRDE voltammograms at 1600 r.p.m. in O2-unsaturated electrolyte with the disk current, ring current, and current corresponding to hydrogen peroxide obtained from the ring current.
Figure 4
Figure 4
H2O2% selectivity as a function of the applied potential.
Figure 5
Figure 5
Polarization curves of a 5 cm2 SEMR-FC at room temperature using Cu-complex/Carbon Vulcan catalyst anodes (5 mg cm–2 catalyst loading) and Pt/C BASF as the cathode in all experiments (1 mg cm–2 Pt catalyst loading with 20 wt % Pt loading on carbon), Nafion 117 membrane treated with KOH 1.0 mol L–1 + CH4 at 50 mL min–1, and O2 flux at 200 mL min- 1.
Figure 6
Figure 6
FT-IR spectra of the effluent of the SEMR-FC at several potentials in 1.0 mol L–1 KOH, and the methane flow was set to 50 mL min–1 for (a) Carbon Vulcan, (b) 1% Cu-complex, (c) 2.5% Cu-complex, (d) 5% Cu-complex, (e) 10% Cu-complex, and (f) 20% Cu-complex.
Figure 7
Figure 7
The reaction rate of methanol production in a SEMR-FC as a function of potential.
See this image and copyright information in PMC

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