IP Library Granted Patent US 9,755,248
Granted Patent B2
US 9,755,248 · App. 14/375,602 · Granted Sep 5, 2017

Use of mesoporous graphite particles for electrochemical applications

Inventors: Ferdi Schüth (Mülheim an der Ruhr, DE); Diana Carolina Galeano Nunez (Mülheim an der Ruhr, DE); Hans-Josef Bongard (Mülheim an der Ruhr, DE); Stefano Mezzavilla (Mülheim an der Ruhr, DE); Karl J. Mayrhofer (Düsseldorf, DE); Josef C. Meier (Düsseldorf, DE); Claudio Baldizzone (Düsseldorf, DE); Jean-Francois Drillet (Mannheim, DE); Sakthivel Mariappan (Frankfurt am Main, DE); Tadios Tesfu (Frankfurt am Main, DE); Volker Peinecke (Mülheim an der Ruhr, DE)
Assignee: STUDIENGESELLSCHAFT KOHLE MBH
H01M4/926B01J21/18B01J23/06B01J23/08B01J23/14B01J23/16B01J23/40B01J23/42B01J23/44B01J23/48B01J23/50B01J23/52B01J23/626B01J23/6525B01J23/6562B01J23/70B01J23/745B01J23/892B01J23/8906B01J23/8913B01J23/8926B01J23/8966B01J35/002B01J35/006B01J35/008B01J35/0033B01J35/0046B01J35/0086B01J35/08B01J35/1028B01J35/1061B01J37/0203B01J37/0244B01J37/084B01J37/18B01J37/343C01B31/04H01M4/8605H01M4/8842H01M4/8882H01M4/9041H01M4/9083H01M8/1018H01M12/04H01M12/08B01J29/0325B01J35/0006C01P2004/32C01P2006/12H01M2008/1095H01M2300/0082
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Quick Facts
Patent No.
US 9,755,248
App. No.
14/375,602
Granted
Sep 5, 2017
Kind
B2
Abstract

The present invention relates to the use of mesoporous graphitic particles having a loading of sintering-stable metal nanoparticles for fuel cells and further electrochemical applications, for example as constituent of layers in electrodes of fuel cells and batteries.

Claims (20)

1. A process comprising conducting an electrochemical reaction in the presence of a catalyst, said catalyst comprising mesoporous graphitic particles having a loading of sintering-stable metal nanoparticles (M-HGS) in an interconnected 3D mesopore structure, wherein the mesoporous graphitic particles having a loading of sintering-stable metal nanoparticles (M-HGS) in an interconnected 3D mesopore structure are obtainable by a process comprising:

(a) impregnating particles having a mesoporous base framework with a graphitizable organic compound to yield impregnated particles;

(b) subjecting the impregnated particles to a high-temperature graphitization step in order to yield graphitized particles having graphitic framework in the mesoporous base framework;

(c) subjecting the graphitized particles to a process for removing the mesoporous base framework in order to yield mesoporous graphitic particles having a mesoporous graphitic framework;

(d) impregnating the mesoporous graphitic particles with a solution of a salt of a catalytically active metal to yield impregnated mesoporous graphitic particles;

(e) subjecting the impregnated mesoporous graphitic particles to a hydrogenation step in order to yield metal-loaded impregnated mesoporous graphitic particles having catalytically active metal particles in mesopores of the metal-loaded impregnated mesoporous graphitic particles; and

(f) calcining the metal-loaded impregnated mesoporous graphitic particles in a temperature range of from 600° C. to 1000° C. in order to obtain said mesoporous graphitic particles having a loading of sintering-stable metal nanoparticles (M-HGS) in mesopores in an interconnected 3D mesopore structure;

and wherein said mesoporous graphitic particles having a loading of sintering-stable metal nanoparticles (M-HGS) in an interconnected 3D mesopore structure comprise a hollow sphere structure comprising a mesoporous graphitic shell having a layer thickness of from 20 nm to 50 nm and a hollow core having a diameter of from 60 nm to 440 nm, and the mesoporous graphitic shell is loaded with the catalytically active metal, and the catalytically active metal is selected from among Ti, V, Cr, Mn, Fe, Co, Ni, Cu, Zn, Al, Mo, Se, Sn, Pt, Ru, Pd, W, Ir, Os, Rh, Nb, Ta, Pb, Bi, Au, Ag, Sc, Y, and combinations thereof in from 5-50% by weight based on the total weight of the mesoporous graphitic particles having a loading of sintering-stable metal nanoparticles (M-HGS) in mesopores in an interconnected 3D mesopore structure.

2. The process as claimed in claim 1 , wherein the catalyst is a constituent of an electrode in an electrochemical cell.

3. The process as claimed in claim 2 , wherein the catalyst is an oxidation catalyst anode constituent of an electrochemical cell.

4. The process as claimed in claim 2 , wherein the catalyst is a reduction catalyst cathode of an electrochemical cell.

5. The process as claimed in claim 1 , wherein the catalyst is a layer constituent in a layer structure of a membrane-electrode assembly (MEA) of a fuel cell, electrochemical cell, or electrochemical reformer or is a constituent of an electrode layer of a battery.

6. The process as claimed in claim 1 , wherein the catalytically active metal is selected from Pt with at least one of Fe, Co, Ni, Cu, Ru, Pd, Au, Ag, Sn, Mo, Mn, Y, and Sc.

7. A process comprising conducting an electrochemical reaction in the presence of mesoporous graphitic particles without a loading of sintering-stable metal nanoparticles (n-HGS), wherein the mesoporous graphitic particles without a loading of sintering-stable metal nanoparticles (M-HGS) are obtainable by a process comprising:

(a) impregnating particles having a mesoporous base framework with a graphitizable organic compound to yield impregnated particles;

(b) subjecting the impregnated particles to a high-temperature graphitization step in order to yield graphitized particles having graphitic framework in the mesoporous base framework;

(c) subjecting the graphitized particles to a process for removing the mesoporous base framework in order to yield said mesoporous graphitic particles without a loading of sintering-stable metal nanoparticles (n-HGS);

and wherein said mesoporous graphitic particles without a loading of sintering-stable metal nanoparticles (n-HGS) comprise a hollow sphere structure comprising a mesoporous graphitic shell having a layer thickness of from 20 nm to 50 nm and a hollow core having a diameter of from 60 nm to 440 nm.

8. The process according to claim 7 , wherein the electrochemical reaction occurs in a fuel cell, at an anode or at a cathode.

9. Process according to claim 1 , wherein the metal-loaded impregnated mesoporous graphitic particles obtained in step e) have catalytically active metal sites on the metal-loaded impregnated mesoporous graphitic particles.

Assignments (2)
CHANGE OF NAME Recorded Feb 27, 2023
From: STUDIENGESELLSCHAFT KOHLE MBH
To: STUDIENGESELLSCHAFT KOHLE GGMBH
Reel/Frame 062876/0181 →
ASSIGNMENT OF ASSIGNOR'S INTEREST Recorded Sep 16, 2014
From: SCHÜTH, FERDI; GALEANO NUNEZ, DIANA CAROLINA; BONGARD, HANS-JOSEF; MEZZAVILLA, STEFANO; MAYRHOFER, KARL; MEIER, JOSEF C.; BALDIZZONE, CLAUDIO; DRILLET, JEAN-FRANCOIS; MARIAPPAN, SAKTHIVEL; TESFU, TADIOS; PEINECKE, VOLKER
To: STUDIENGESELLSCHAFT KOHLE MBH
Reel/Frame 033744/0660 →
Priority Claims (2)
EP 12154508 · Feb 8, 2012 · regional
DE 10 2012 102 120 · Mar 13, 2012 · national
Continuity (1)
Related Publication 20150017555A1 · Jan 15, 2015