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Köleli, Fatih; Atilan, T.; Palamut, N.; Gizir, A. Murat; Aydın, Rezzan; Hamann, C. H.

doi:10.1023/a:1024471513136

Cited by 146 publications

(102 citation statements)

References 13 publications

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“…The ''poisoning'' of copper cathodes for CO 2 reduction has been widely reported [2,3] and deactivation of tin cathodes has also been observed [7,8]. In the present work, the SEM images and EDX spectra of new and used cathodes in Figure 7 show a progressive loss of tin from the cathode surface that probably accounts for the effect of cathode age.…”

Section: Main and Interaction Effectssupporting

confidence: 68%

“…De-activation of the cathode over time (e.g. 1 h) has been observed for CO 2 reduction on copper electrodes [2,3], and some effects of this type have been indicated on lead and tin [7,8].…”

Section: Introductionmentioning

confidence: 99%

“…low exchange current density for hydrogen evolution), such as indium, lead, mercury and tin [3][4][5][6][7]. The exchange current densities for CO 2 reduction to formate at 293 K (in 0.95 M KCl + 0.05 M NaHCO 3 ) on In, Hg and Sn are reported respectively as: 1 · 10 )7 , 5 · 10 )10 and 1 · 10 )8 kA m )2 [8], with the primary electro-active species in the cathode reaction being CO 2 (aq), engaged in a multi-step adsorption/ reaction process involving the intermediate radical anion CO .)…”

Section: Introductionmentioning

confidence: 99%

“…70 mM at STP), coupled with the CO 2 (aq)/HCO 3 ) /CO 3 2) equilibria, creates a mass transfer constraint on the reaction that limits the primary (steady-state) current density to a maximum value of the order 0.1 kA m )2 (i.e. 10 mA cm )2 ) under the typical laboratory reaction conditions, with 100 kPa(abs) CO 2 pressure at 298 K [2][3][4][5][6][7][8]9]. The intrinsic reaction order with respect to the CO 2 pressure is 0.6-1.0 (depending on the cathode material and potential) with partial current densities ranging up to 1.6 kA m )2 (i.e.…”

Section: Introductionmentioning

confidence: 99%

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The Electro-Reduction of Carbon Dioxide in a Continuous Reactor

2005

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This paper reports an investigation into the electro-reduction of CO 2 in a laboratory bench-scale continuous reactor with co-current flow of reactant gas and catholyte liquid through a flow-by 3D cathode of 30 # mesh tinned-copper. Factorial and parametric experiments were carried out in this apparatus with the variables: current (1-8 A), gas phase CO 2 concentration (16-100 vol%) and operating time (10-180 min), using a cathode feed of [CO 2 + N 2 ] gas and 0.45 M KHCO 3 (aq) with an anolyte feed of 1 M KOH(aq), in operation near ambient conditions (ca. 115 kPa(abs), 300 K). The primary and secondary reactions here were respectively the reduction of CO 2 to formate (HCOO ) ) and of water to hydrogen, while up to ca. 5% of the current went to production of CO, CH 4 and C 2 H 4 . The current efficiency for formate depended on the current density and CO 2 pressure, coupled with the hydrogen over-potential plus mass transfer capacity of the cathode, and decreased with operating time, as tin was lost from the cathode surface. For superficial current densities ranging from 0.22 to 1.78 kA m )2 , the measured values of the performance indicators are: current efficiency for HCOO ) = 86-13%, reactor voltage = 3-6 Volt, specific energy for HCOO ) = 300-1300 kWh kmol )1 , space-time yield of HCOO ) = 2 · 10 )4 -6 · 10 )4 kmol m )3 s )1 , conversion of CO 2 = 20-80% and yield of organic products from CO 2 = 6-17%. Nomenclature a specific surface area of cathode, m )1 a k Tafel constant for reaction k, V a 2Cu Tafel constant for reaction 2 on copper, V a 2Sn Tafel constant for reaction 2 on tin, V CD current density, kA m )2 CE k current efficiency for reaction k, -D diffusion coefficient of CO 2 (aq), m 2 s )1 d wire diameter in cathode mesh, m d b bubble diameter, m E electrode potential, V(SHE) E cell full-cell operating voltage (absolute value), V E r,k reversible electrode potential of reaction k, V(SHE) E o k standard electrode potential of reaction k, V(SHE) DE voltage window in operation of 3D flow-by electrode, V F Faraday's number, kC kmol )1 G gas load in 3D flow-by electrode, kg m )2 s )1 h liquid hold-up in 3D flow-by electrode, -I current, kA i superficial current density, kA m )2i iL mass transfer limited superficial current density for reaction 1, kA m )2 j k partial real current density of reaction k, kA m )2 j 1L mass transfer limited real current density for reaction 1, kA m )2 K¢, K 0 , K 1 reaction equilibrium constants, -, M kPa )1 , M k F mass transfer coefficient due to forced convection, m s )1 k G mass transfer coefficient due to gas (H 2 ) generation, m s )1 k M combined mass transfer coefficient, m s )1 L liquid load in 3D flow-by electrode, kg m )2 s )1 P total pressure, kPa(abs) p CO 2 partial pressure of CO 2 , kPa(abs) p H 2 partial pressure of H 2 , kPa(abs) R gas constant, kJ kmol )1 K )1 Re bReynolds' number for bubble generation at electrode, -Re g Reynolds' number for gas flow = v g d q g / l g , -Re l Reynolds' number for liquid flow = v l d q l / l l , -SE specific energy for formate p...

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Section: Main and Interaction Effectssupporting

confidence: 68%

“…De-activation of the cathode over time (e.g. 1 h) has been observed for CO 2 reduction on copper electrodes [2,3], and some effects of this type have been indicated on lead and tin [7,8].…”

Section: Introductionmentioning

confidence: 99%

Section: Introductionmentioning

confidence: 99%

Section: Introductionmentioning

confidence: 99%

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The Electro-Reduction of Carbon Dioxide in a Continuous Reactor

2005

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“…As reported, with modification of the electrolyte at ambient temperature and pressure, the formation of CO 2 reduction products can be enhanced with respect to faradaic efficiency. For example, on changing the electrolyte from K 2 CO 3 to KHCO 3 , HCOOH has been detected as a predominant product in the working potential ranges (from −1.5 to −1.8 V vs. SCE) for both Pb and Sn electrodes [113].…”

Section: Effects Of Supporting Electrolytesmentioning

confidence: 99%

Transformation of Carbon Dioxide to Useable Products through Free Radical‐Induced Reactions

Dey¹

2014

Green Carbon Dioxide

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Emerging Carbon‐Based Heterogeneous Catalysts for Electrochemical Reduction of Carbon Dioxide into Value‐Added Chemicals

et al. 2018

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The electrocatalytic reduction of CO2 provides a sustainable way to mitigate CO2 emissions, as well as store intermittent electrical energy into chemicals. However, its slow kinetics and the lack of ability to control the products of the reaction inhibit its industrial applications. In addition, the immature mechanistic understanding of the reduction process makes it difficult to develop a selective, scalable, and stable electrocatalyst. Carbon‐based materials are widely considered as a stable and abundant alternative to metals for catalyzing some of the key electrochemical reactions, including the CO2 reduction reaction. In this context, recent research advances in the development of heterogeneous nanostructured carbon‐based catalysts for electrochemical reduction of CO2 are summarized. The leading factors for consideration in carbon‐based catalyst research are discussed by analyzing the main challenges faced by electrochemical reduction of CO2. Then the emerging metal‐free doped carbon and aromatic N‐heterocycle catalysts for electrochemical reduction of CO2 with an emphasis on the formation of multicarbon hydrocarbons and oxygenates are discussed. Following that, the recent progress in metal–nitrogen–carbon structures as an extension of carbon‐based catalysts is scrutinized. Finally, an outlook for the future development of catalysts as well as the whole electrochemical system for CO2 reduction is provided.

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Untitled

Cited by 146 publications

References 13 publications

The Electro-Reduction of Carbon Dioxide in a Continuous Reactor

The Electro-Reduction of Carbon Dioxide in a Continuous Reactor

Transformation of Carbon Dioxide to Useable Products through Free Radical‐Induced Reactions

Emerging Carbon‐Based Heterogeneous Catalysts for Electrochemical Reduction of Carbon Dioxide into Value‐Added Chemicals

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