Unsupported medium entropy alloy catalysts

Patent metadata

Field	Value
Publication number	US-2025332582-A1
Application number	US-202418650606-A
Country	US
Kind code	A1
Filing date	Apr 30, 2024
Priority date	Apr 30, 2024
Publication date	Oct 30, 2025
Grant date	—

Abstract

Compositions and methods for the catalysis of methane pyrolysis. Compositions include a catalyst that includes a medium entropy alloy particle. Methods include catalyzing the pyrolysis of methane using the catalyst.

First claim

What is claimed is:

1 . A catalyst comprising:
a medium entropy alloy (MEA) particle, wherein the MEA particle comprises
a first principal metal,
a second principal metal, and
a third principal metal, wherein each of the principal metals is independently selected without repetition from the group consisting of Co, Cr, Fe, Mn, Ni, Al, Cu, Zn, Ti, Zr, Mo, V, Ru, Rh, Pd, Ag, W, Re, Ir, Pt, Au, Ce, Y, Yb, Sn, Ga, In, and Be.

2 . The catalyst of claim 1 , wherein one of the first principal metal, the second principal metal, or the third principal metal is present in the MEA particle at 30 atomic percent (at %) or more.

3 . The catalyst of claim 1 , wherein the MEA particle includes a promoter, wherein the promoter is selected from the group consisting of molybdenum, calcium, cesium, In 2 O 3 , Cr 2 O 3 , and rare earth metals, and any combination thereof.

4 . The catalyst of claim 3 , wherein the atomic percentage (at %) of the promoter in the MEA particle is from about 0.5 at % to about 10 at %.

5 . The catalyst of claim 1 , wherein the MEA particle further comprises a non-reducible metal oxide selected from the group consisting of Li 2 O, K 2 O, Na 2 O, Cs 2 O, BeO, MgO, CaO, SrO, BaO, P 2 O 5 , Al 2 O 3 , Al 2 O 4 , In 2 O 3 , SiO 2 , TiO 2 , ZrO 2 , CeO 2 , Y 2 O 3 , La 2 O 3 , and Er 2 O 3 , and any combination thereof.

6 . The catalyst of claim 5 , wherein the atomic percentage (at %) of the non-reducible metal oxide in the MEA particle is less than about 20 at %.

7 . The catalyst of claim 1 , wherein the catalyst includes a metal chloride selected from the group consisting of metal chlorides of Li, Na, Ca, K, Cs, or Fr, or chlorides of Fe, Co, Mn, Mg, Al, Ni, Mo, Cu, Pd, Pt, Ce, Mg, La, Nd, Ge, and Re, and any combination thereof.

8 . The catalyst of claim 7 , wherein the atomic percentage (at %) of the metal chloride in the MEA particle is less than about 20 at %.

9 . The catalyst of claim 1 , wherein the MEA particle further comprises a non-reducible and high-temperature-stable compound selected from the group consisting of carbides, borides, boron carbides, nitrides, boron nitrides, silicide, aluminides, phosphides, phosphates, sulfides, sulfates, hydrides, hydrates, carbonitrides, graphene, graphene oxide, carbon nanotubes, graphite, and any combinations thereof.

10 . The catalyst of claim 9 , wherein the non-reducible and high-temperature-stable compound is selected from the group consisting of Fe 3 C, KBr, NaNO 3 , B 4 C, BN, Na 4 Si 4 , Na 2 Al 2 O 4 , FeP, Na 3 PO 4 , FeS, Na 2 SO 4 , MgH 2 , and C 3 N 4 , and any combination thereof.

11 . The catalyst of claim 9 , wherein the atomic percentage (at %) of the non-reducible and high-temperature-stable compound in the MEA particle is less than about 20 at %.

12 . The catalyst of claim 1 , wherein the MEA particle is from about 1 nm to about 10 μm in diameter.

13 . The catalyst of claim 1 , wherein the MEA particle further comprises a fourth principal metal, wherein the fourth principal metal is independently selected without repetition from the group consisting of Co, Cr, Fe, Mn, Ni, Al, Cu, Zn, Ti, Zr, Mo, V, Ru, Rh, Pd, Ag, W, Re, Ir, Pt, Au, Ce, Y, Yb, Sn, Ga, In, and Be.

14 . The catalyst of claim 13 , wherein one of the first principal metal, the second principal metal, the third principal metal, or the fourth principal metal is present in the MEA particle at 30 atomic percent (at %) or more.

15 . The catalyst of claim 13 , wherein the MEA particle includes a promoter, wherein the promoter is selected from the group consisting of molybdenum, calcium, cesium, In 2 O 3 , Cr 2 O 3 , and rare earth metals, and any combination thereof.

16 . The catalyst of claim 15 , wherein the atomic percentage (at %) of the promoter in the MEA particle is from about 0.5 at % to about 10 at %.

17 . The catalyst of claim 13 , wherein the MEA particle further comprises a non-reducible metal oxide selected from the group consisting of Li 2 O, K 2 O, Na 2 O, Cs 2 O, BeO, MgO, CaO, SrO, BaO, P 2 O 5 , Al 2 O 3 , Al 2 O 4 , In 2 O 3 , SiO 2 , TiO 2 , ZrO 2 , CeO 2 , Y 2 O 3 , La 2 O 3 , and Er 2 O 3 , and any combination thereof.

18 . The catalyst of claim 17 , wherein the atomic percentage (at %) of the non-reducible metal oxide in the MEA particle is less than about 20 at %.

19 . The catalyst of claim 13 , wherein the catalyst includes a metal chloride selected from the group consisting of metal chlorides of Li, Na, Ca, K, Cs, or Fr, or chlorides of Fe, Co, Mn, Mg, Al, Ni, Mo, Cu, Pd, Pt, Ce, Mg, La, Nd, Ge, and Re, and any combination thereof.

20 . The catalyst of claim 19 , wherein the atomic percentage (at %) of the metal chloride in the MEA particle is less than about 20 at %.

21 . The catalyst of claim 13 , wherein the MEA particle further comprises a non-reducible and high-temperature-stable compound selected from the group consisting of carbides, borides, boron carbides, nitrides, boron nitrides, silicide, aluminides, phosphides, phosphates, sulfides, sulfates, hydrides, hydrates, carbonitrides, graphene, graphene oxide, carbon nanotubes, graphite, and any combinations thereof.

22 . The catalyst of claim 21 , wherein the non-reducible and high-temperature-stable compound is selected from the group consisting of Fe 3 C, KBr, NaNO 3 , B 4 C, BN, Na 4 Si 4 , Na 2 Al 2 O 4 , FeP, Na 3 PO 4 , FeS, Na 2 SO 4 , MgH 2 , and C 3 N 4 , and any combination thereof.

23 . The catalyst of claim 21 , wherein the atomic percentage (at %) of the non-reducible and high-temperature-stable compound in the MEA particle is less than about 20 at %.

24 . The catalyst of claim 13 , wherein the MEA particle is from about 1 nm to about 10 μm in diameter.

25 . A method of producing a catalyst, the method comprising:
placing a first principal metal, a second principal metal, and a third principal metal, and zirconia media in a ball mill, wherein each of the principal metals is independently selected without repetition from the group consisting Co, Cr, Fe, Mn, Ni, Al, Cu, Zn, Ti, Zr, Mo, V, Ru, Rh, Pd, Ag, W, Re, Ir, Pt, Au, Ce, Y, Yb, Sn, Ga, In, and Be; rotating the ball mill to produce the catalyst; and separating the produced catalyst from the zirconia media.

26 . The method of claim 25 , further comprising placing a fourth principal metal in the ball mill before rotating the ball mill, wherein the fourth principal metal is independently selected without repetition from the group consisting of Co, Cr, Fe, Mn, Ni, Al, Cu, Zn, Ti, Zr, Mo, V, Ru, Rh, Pd, Ag, W, Re, Ir, Pt, Au, Ce, Y, Yb, Sn, Ga, In, and Be.

27 . The method of claim 25 , wherein the ball mill is rotated for about 2 days at about 1100 rpm.

28 . The method of claim 25 , further comprising placing a non-reducible metal oxide in the ball mill before rotating the ball mill, wherein the non-reducible metal oxide is selected from the group consisting of Li 2 O, K 2 O, Na 2 O, Cs 2 O, BeO, MgO, CaO, SrO, BaO, P 2 O 5 , Al 2 O 3 , Al 2 O 4 , In 2 O 3 , SiO 2 , TiO 2 , ZrO 2 , CeO 2 , Y 2 O 3 , La 2 O 3 , and Er 2 O 3 , and any combination thereof.

29 . The method of claim 25 , further comprising placing a metal chloride in the ball mill before rotating the ball mill, wherein the metal chloride is selected from the group consisting of metal chlorides of Li, Na, Ca, K, Cs, or Fr, or chlorides of Fe, Co, Mn, Mg, Al

Assignees

• Saudi Arabian Oil Co

Inventors

• Wang Xiaoxing
• Liang Feng

Classifications

• B01J35/45

  Nanoparticles · CPC title

• B01J23/745

  Iron · CPC title

• C01B3/40

  characterised by the catalyst · CPC title

• B01J37/0036

  Grinding · CPC title

• B01J35/40

  characterised by dimensions, e.g. grain size (in a colloidal state B01J35/23; crystallite size B01J35/77) · CPC title