Novel catalyst mixtures

a catalyst and mixture technology, applied in the field of catalysts, can solve the problems of preventing efficient conversion of carbon dioxide into, lack of catalysts, and high overpotential costs, and achieve the effects of low electron conversion efficiency, high overpotentials, and low rates

Inactive Publication Date: 2011-09-29
DIOXIDE MATERIALS
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  • Summary
  • Abstract
  • Description
  • Claims
  • Application Information

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Benefits of technology

[0015]The invention provides a novel catalyst mixture that can overcome one or more of the limitations of low rates, high overpotentials and low electron conversion efficiencies (i.e. selectivities) for catalytic reactions and high powers for sensors. The catalyst mixture includes at least one Catalytically Active Element, and at least one Helper Catalyst. When the Catalytically Active Element and the Helper Catalyst are combined the rate and / or selectivity of a chemical reaction can be enhanced over the rate seen in the absence of the Helper Catalyst. For example, the overpotential for electrochemical conversion of carbon-dioxide can be substantially reduced and the current efficiency (i.e. selectivity) for CO2 conversion can be substantially increased.

Problems solved by technology

Still according to Bell Basic Research Needs, Catalysis For Energy, US Department Of Energy Report PNNL-17214, 2008), (“The Bell Report”) “The major obstacle preventing efficient conversion of carbon dioxide into energy-bearing products is the lack of catalyst” with sufficient activity at low overpotentials and high electron conversion efficiencies.
Yet, according to The Bell Report “Electron conversion efficiencies of greater than 50 percent can be obtained, but at the expense of very high overpotentials” This limitation needs to be overcome before practical processes can be obtained.
A second disadvantage of many of the catalysts is that they also have low electron conversion efficiency.
At present, these sensors require over 1-5 watts of power, which is too high for portable sensing applications.

Method used

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Examples

Experimental program
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specific example 1

Using a Active Element, Helper Catalyst Mixture including of Platinum and 1-ethyl-3-Methylimidazoilum Tetrafluoroborate (EMIM-BF4) to Lowering the Overpotential for Electrochemical Conversion of CO2 and Raising the Selectivity (Current Efficiency) of the Reaction

[0078]The experiments used the glass three electrode cell shown in FIG. 7. The cell consisted of a Three neck flask (101), to hold the anode (108), and the cathode (109). A silver / 0.01 molar silver ion reference electrode (103) in acetnonitrile was connected to the cell through a Luggin Cappillary (102). The reference electrode (103) was fitted with a vycor frit to prevent any of the reference electrode solution from contaminating the ionic liquid in the capillary. The reference electrode was calibrated against the Fc / Fc+ redox couple. A conversion factor of +535 was used convert our potential axis to reference the Standard Hydrogen Electrode (SHE). A 25×25 mm Platinum gauze (size 52) (113) was connected to the anode while a...

specific example 2

The Effect of Dilution on the Electrochemical Conversion of CO2

[0090]This example shows that water additions speed the formation of CO. The experiment used the Cell and procedures in Example 1, with the following exception: a solution containing 98.55% EMIM-BF4 and 0.45% water was substituted for the 99.9999% EMIM-BF4 used in Example 1, the potential was held for 10 or 30 minutes at −0.6V with respect to RHE, and then the potential was ramped positively at 50 mV / sec. FIG. 10 shows the result. Notice the peak at between 1.2 and 1.5 eV. This is the peak associated with CO formation and is much larger than in example 1. Thus the addition of water has accelerated the formation of CO presumably by acting as a reactant.

specific example 3

Using a Active Element, Helper Catalyst Mixture that include Palladium and choline Iodide to Lowering the Overpotential for Electrochemical Conversion of CO2 in Water

[0091]The next example is to demonstrate that the invention can be practiced using Palladium as an active element and Choline Iodide as a Helper Catalyst.

[0092]The experiment used the cell and procedures in Example 1, with the following exceptions: ii) A 10.3% by weight of a Helper Catalyst, choline iodide in water solution was substituted for the 1-ethyl-3-methylimidazolium tetrafluoroborate and ii) a 0.25 cm2 Pd foil purchased from Alfa Aesar was substituted for the gold plug and platinum black on the cathode, and a silver / silver chloride reference was used.

[0093]FIG. 11 shows a CV taken under these conditions. There is a large negative peak near zero volts with respect with SHE associated with iodine transformations and a negative going peak starting at about 0.8 V associated with conversion of CO2. By comparison the...

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Abstract

Catalysts comprised of at least one catalytically active element and at least one helper catalyst are disclosed. The catalysts may be used to increase the rate, the selectivity or lower the overpotential of chemical reactions. These catalysts may be useful for a variety of chemical reactions including in particular the electrochemical conversion of carbon dioxide to formic acid.

Description

CROSS-REFERENCES TO RELATED APPLICATIONS[0001]This application claims priority to and the benefit under 35 U.S.C. §119(e) to provisional application 61 / 317,955, filed Mar. 26, 2010, the disclosure of which is expressly incorporated herein by reference in its entirety.FIELD OF THE INVENTION[0002]The field of the invention is catalysis and catalysts. The catalysts of this invention are applicable, for example, to the electrochemical conversion of carbon dioxide into formic acid.BACKGROUND[0003]There is a present need to decrease carbon dioxide (CO2) emissions from industrial facilities. Over the years, a number of electrochemical processes have been suggested for the conversion of CO2 into useful products. Processes for CO2 conversion and the catalysts for them are discussed in U.S. Pat. Nos. 3,959,094 4,240,882 4,523,981 4,545,872, 4,595,465 4,608,132 4,608,133 4,609,441 4,609,440, 4,620,906, 4,668,349, 4,673,473, 4,711,708, 4,756,807, 4,756,807, 4,818,353 5,064,733 5,284,563 5,382,3...

Claims

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Application Information

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Patent Type & Authority Applications(United States)
IPC IPC(8): C07C51/15B01J31/02C25B3/25C01B32/40
CPCB01J31/0239B01J31/0268B01J31/0278B01J31/0281G01N33/004B01J31/0288B01J31/0289B01J2231/62C25B3/04B01J31/0284C25B11/04Y02P20/133C25B1/23C25B3/03C25B3/07C25B3/26C25B11/051C25B11/095B01J31/12G01N27/30C25B3/25
Inventor MASEL, RICHARD ISAAC
Owner DIOXIDE MATERIALS
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