Patent
US 11,105,009METALLIC SINGLE ATOM-EMBEDDED GRAPHENE MATERIAL, AND PREPARATION METHOD THEREFOR AND APPLICATION THEREOF
Bin LIU
US
Copyright © 2026 Matter42. All rights reserved.
Claims define the patent's legal scope. Independent claims stand alone; dependent claims (nested) narrow them. Click a claim to expand its dependents.
- 26. Canceled
Canceled
A method for preparing a graphene material inlaid with single metal atoms, comprising: a) mixing raw material to obtain a precursor; and b) putting the precursor in an inactive atmosphere for high temperature carbonization to obtain the graphene material inlaid with single metal atoms; wherein the raw material comprises tripolycyanamide and metal salt; or the raw material comprises tripolycyanamide, metal salt and amino acid; or the raw material comprises tripolycyanamide, metal salt, amino acid and conductive carbon material. Currently amended
The method according to Claim 27, wherein the amino acid is at least one selected from the group consisting of cysteine, glycine, alanine, phenylalanine and tryptophan. Previously presented
The method according to Claim 27, wherein the metal salt is at least one selected from the group consisting of nickel salt, cobalt salt, ferric salt and ferrous salt. Previously presented
The method according to Claim 27, wherein the conductive carbon material is at least one selected from the group consisting of acetylene black, carbon fiber, carbon nanotube, carbon dust and Ketjen black. Previously presented
The method according to Claim 27, wherein the mass ratio of the substances in the raw material is: tripolycyanamide: metal salt: amino acid: conductive carbon material = 20 ~ 100: 1 0~ 100: 0 ~ 10. Previously presented
The method according to Claim 27, wherein the mixing is ball milling mixing. Previously presented
The method according to Claim 27, wherein the inactive atmosphere comprises a gas which is at least one selected from the group consisting of nitrogen, argon, helium and xenon. Previously presented
The method according to Claim 27, wherein the high temperature carbonizing uses a[[n]] one step high temperature carbonizing method or a two step high temperature carbonizing method, wherein the one step high temperature carbonizing method comprises: putting the precursor in inactive atmosphere, and heating to a temperature in a range from 800 ° C to 1200 ° C at a heating rate ranging from 1 ° C/min to 5 ° C/min, and then keeping for a time range from 0.5 hours to 5 hours; and the two step high temperature carbonizing method comprises: putting the precursor in inactive atmosphere, and heating to a temperature in a range from 350 ° C to 650 ° C at a heating rate ranging from 1 ° C/min to 2.5 ° C, and then keeping for a time range from 0.5 hours-4 hours; then heating to a temperature in a range from 800 to 1200 ° C at a heating rate ranging from 1 ° C/min to 5° C/min and keeping for a time range from 0.5 hours to 5 hours. Currently amended
The method according to Claim 27, wherein after putting the precursor in the inactive atmosphere for high temperature carbonization; being contacted with an acidic solution for acid treatment; and then being put in the inactive atmosphere and being treated at a high temperature in a range from 700 ° C to 900 ° C for a time range from 10 m in to 120 min, to obtain the graphene material inlaid with single metal atoms. Currently amended
- 40. Canceled
Canceled
Materials described outside the worked examples.
graphene material inlaid with single metal atoms
tripolycyanamide
metal salt
amino acid
amino acid (cysteine, glycine, alanine, phenylalanine, tryptophan)
metal salt (nickel salt, cobalt salt, ferric salt, ferrous salt)
conductive carbon material (acetylene black, carbon fiber, carbon nanotube, carbon dust, Ketjen black)
N-doped graphene
N and S co-doped graphene
single metal atoms (Fe, Co, Ni)
nickel acetate
cobalt acetate
ferrous acetate
ferric acetate
nickel nitrate
cobalt nitrate
ferrous nitrate
ferric nitrate
nickel sulfate
cobalt sulfate
ferrous sulfate
ferric sulfate
Additional fabrication and treatment steps described in the patent.
Performance values and ranges asserted in the specification or claims.
| Property | Value | Material |
|---|---|---|
Faradaic efficiency for CO2 electroreduction to CO | 95 % | graphene material inlaid with single metal atoms |
Reduction current per unit mass at -1.0 V vs. RHE | 1000 mA/mgcatalyst | graphene material inlaid with single metal atoms |
Current at unit area at -1.0 V vs. RHE | 100 mA/cm2 | graphene material inlaid with single metal atoms |
Mass percentage of single metal atoms in graphene material | — | graphene material inlaid with single metal atoms |
Preferred mass percentage of single metal atoms in graphene material | — | graphene material inlaid with single metal atoms |
Temperature | 800–1200 °C | — |
Duration | 0.5–5 hours | — |
Temperature | 350–650 °C | — |
Temperature | 700–900 °C | — |
Temperature | 40–120 °C | — |
Claims define the patent's legal scope. Independent claims stand alone; dependent claims (nested) narrow them. Click a claim to expand its dependents.
- 26. Canceled
Canceled
A method for preparing a graphene material inlaid with single metal atoms, comprising: a) mixing raw material to obtain a precursor; and b) putting the precursor in an inactive atmosphere for high temperature carbonization to obtain the graphene material inlaid with single metal atoms; wherein the raw material comprises tripolycyanamide and metal salt; or the raw material comprises tripolycyanamide, metal salt and amino acid; or the raw material comprises tripolycyanamide, metal salt, amino acid and conductive carbon material. Currently amended
The method according to Claim 27, wherein the amino acid is at least one selected from the group consisting of cysteine, glycine, alanine, phenylalanine and tryptophan. Previously presented
The method according to Claim 27, wherein the metal salt is at least one selected from the group consisting of nickel salt, cobalt salt, ferric salt and ferrous salt. Previously presented
The method according to Claim 27, wherein the conductive carbon material is at least one selected from the group consisting of acetylene black, carbon fiber, carbon nanotube, carbon dust and Ketjen black. Previously presented
The method according to Claim 27, wherein the mass ratio of the substances in the raw material is: tripolycyanamide: metal salt: amino acid: conductive carbon material = 20 ~ 100: 1 0~ 100: 0 ~ 10. Previously presented
The method according to Claim 27, wherein the mixing is ball milling mixing. Previously presented
The method according to Claim 27, wherein the inactive atmosphere comprises a gas which is at least one selected from the group consisting of nitrogen, argon, helium and xenon. Previously presented
The method according to Claim 27, wherein the high temperature carbonizing uses a[[n]] one step high temperature carbonizing method or a two step high temperature carbonizing method, wherein the one step high temperature carbonizing method comprises: putting the precursor in inactive atmosphere, and heating to a temperature in a range from 800 ° C to 1200 ° C at a heating rate ranging from 1 ° C/min to 5 ° C/min, and then keeping for a time range from 0.5 hours to 5 hours; and the two step high temperature carbonizing method comprises: putting the precursor in inactive atmosphere, and heating to a temperature in a range from 350 ° C to 650 ° C at a heating rate ranging from 1 ° C/min to 2.5 ° C, and then keeping for a time range from 0.5 hours-4 hours; then heating to a temperature in a range from 800 to 1200 ° C at a heating rate ranging from 1 ° C/min to 5° C/min and keeping for a time range from 0.5 hours to 5 hours. Currently amended
The method according to Claim 27, wherein after putting the precursor in the inactive atmosphere for high temperature carbonization; being contacted with an acidic solution for acid treatment; and then being put in the inactive atmosphere and being treated at a high temperature in a range from 700 ° C to 900 ° C for a time range from 10 m in to 120 min, to obtain the graphene material inlaid with single metal atoms. Currently amended
- 40. Canceled
Canceled
Materials described outside the worked examples.
graphene material inlaid with single metal atoms
tripolycyanamide
metal salt
amino acid
amino acid (cysteine, glycine, alanine, phenylalanine, tryptophan)
metal salt (nickel salt, cobalt salt, ferric salt, ferrous salt)
conductive carbon material (acetylene black, carbon fiber, carbon nanotube, carbon dust, Ketjen black)
N-doped graphene
N and S co-doped graphene
single metal atoms (Fe, Co, Ni)
nickel acetate
cobalt acetate
ferrous acetate
ferric acetate
nickel nitrate
cobalt nitrate
ferrous nitrate
ferric nitrate
nickel sulfate
cobalt sulfate
ferrous sulfate
ferric sulfate
Additional fabrication and treatment steps described in the patent.
Performance values and ranges asserted in the specification or claims.
| Property | Value | Material |
|---|---|---|
Faradaic efficiency for CO2 electroreduction to CO | 95 % | graphene material inlaid with single metal atoms |
Reduction current per unit mass at -1.0 V vs. RHE | 1000 mA/mgcatalyst | graphene material inlaid with single metal atoms |
Current at unit area at -1.0 V vs. RHE | 100 mA/cm2 | graphene material inlaid with single metal atoms |
Mass percentage of single metal atoms in graphene material | — | graphene material inlaid with single metal atoms |
Preferred mass percentage of single metal atoms in graphene material | — | graphene material inlaid with single metal atoms |
Temperature | 800–1200 °C | — |
Duration | 0.5–5 hours | — |
Temperature | 350–650 °C | — |
Temperature | 700–900 °C | — |
Temperature | 40–120 °C | — |
Claims define the patent's legal scope. Independent claims stand alone; dependent claims (nested) narrow them. Click a claim to expand its dependents.
- 26. Canceled
Canceled
A method for preparing a graphene material inlaid with single metal atoms, comprising: a) mixing raw material to obtain a precursor; and b) putting the precursor in an inactive atmosphere for high temperature carbonization to obtain the graphene material inlaid with single metal atoms; wherein the raw material comprises tripolycyanamide and metal salt; or the raw material comprises tripolycyanamide, metal salt and amino acid; or the raw material comprises tripolycyanamide, metal salt, amino acid and conductive carbon material. Currently amended
The method according to Claim 27, wherein the amino acid is at least one selected from the group consisting of cysteine, glycine, alanine, phenylalanine and tryptophan. Previously presented
The method according to Claim 27, wherein the metal salt is at least one selected from the group consisting of nickel salt, cobalt salt, ferric salt and ferrous salt. Previously presented
The method according to Claim 27, wherein the conductive carbon material is at least one selected from the group consisting of acetylene black, carbon fiber, carbon nanotube, carbon dust and Ketjen black. Previously presented
The method according to Claim 27, wherein the mass ratio of the substances in the raw material is: tripolycyanamide: metal salt: amino acid: conductive carbon material = 20 ~ 100: 1 0~ 100: 0 ~ 10. Previously presented
The method according to Claim 27, wherein the mixing is ball milling mixing. Previously presented
The method according to Claim 27, wherein the inactive atmosphere comprises a gas which is at least one selected from the group consisting of nitrogen, argon, helium and xenon. Previously presented
The method according to Claim 27, wherein the high temperature carbonizing uses a[[n]] one step high temperature carbonizing method or a two step high temperature carbonizing method, wherein the one step high temperature carbonizing method comprises: putting the precursor in inactive atmosphere, and heating to a temperature in a range from 800 ° C to 1200 ° C at a heating rate ranging from 1 ° C/min to 5 ° C/min, and then keeping for a time range from 0.5 hours to 5 hours; and the two step high temperature carbonizing method comprises: putting the precursor in inactive atmosphere, and heating to a temperature in a range from 350 ° C to 650 ° C at a heating rate ranging from 1 ° C/min to 2.5 ° C, and then keeping for a time range from 0.5 hours-4 hours; then heating to a temperature in a range from 800 to 1200 ° C at a heating rate ranging from 1 ° C/min to 5° C/min and keeping for a time range from 0.5 hours to 5 hours. Currently amended
The method according to Claim 27, wherein after putting the precursor in the inactive atmosphere for high temperature carbonization; being contacted with an acidic solution for acid treatment; and then being put in the inactive atmosphere and being treated at a high temperature in a range from 700 ° C to 900 ° C for a time range from 10 m in to 120 min, to obtain the graphene material inlaid with single metal atoms. Currently amended
- 40. Canceled
Canceled
Materials described outside the worked examples.
graphene material inlaid with single metal atoms
tripolycyanamide
metal salt
amino acid
amino acid (cysteine, glycine, alanine, phenylalanine, tryptophan)
metal salt (nickel salt, cobalt salt, ferric salt, ferrous salt)
conductive carbon material (acetylene black, carbon fiber, carbon nanotube, carbon dust, Ketjen black)
N-doped graphene
N and S co-doped graphene
single metal atoms (Fe, Co, Ni)
nickel acetate
cobalt acetate
ferrous acetate
ferric acetate
nickel nitrate
cobalt nitrate
ferrous nitrate
ferric nitrate
nickel sulfate
cobalt sulfate
ferrous sulfate
ferric sulfate
Additional fabrication and treatment steps described in the patent.
Performance values and ranges asserted in the specification or claims.
| Property | Value | Material |
|---|---|---|
Faradaic efficiency for CO2 electroreduction to CO | 95 % | graphene material inlaid with single metal atoms |
Reduction current per unit mass at -1.0 V vs. RHE | 1000 mA/mgcatalyst | graphene material inlaid with single metal atoms |
Current at unit area at -1.0 V vs. RHE | 100 mA/cm2 | graphene material inlaid with single metal atoms |
Mass percentage of single metal atoms in graphene material | — | graphene material inlaid with single metal atoms |
Preferred mass percentage of single metal atoms in graphene material | — | graphene material inlaid with single metal atoms |
Temperature | 800–1200 °C | — |
Duration | 0.5–5 hours | — |
Temperature | 350–650 °C | — |
Temperature | 700–900 °C | — |
Temperature | 40–120 °C | — |
Claims define the patent's legal scope. Independent claims stand alone; dependent claims (nested) narrow them. Click a claim to expand its dependents.
- 26. Canceled
Canceled
A method for preparing a graphene material inlaid with single metal atoms, comprising: a) mixing raw material to obtain a precursor; and b) putting the precursor in an inactive atmosphere for high temperature carbonization to obtain the graphene material inlaid with single metal atoms; wherein the raw material comprises tripolycyanamide and metal salt; or the raw material comprises tripolycyanamide, metal salt and amino acid; or the raw material comprises tripolycyanamide, metal salt, amino acid and conductive carbon material. Currently amended
The method according to Claim 27, wherein the amino acid is at least one selected from the group consisting of cysteine, glycine, alanine, phenylalanine and tryptophan. Previously presented
The method according to Claim 27, wherein the metal salt is at least one selected from the group consisting of nickel salt, cobalt salt, ferric salt and ferrous salt. Previously presented
The method according to Claim 27, wherein the conductive carbon material is at least one selected from the group consisting of acetylene black, carbon fiber, carbon nanotube, carbon dust and Ketjen black. Previously presented
The method according to Claim 27, wherein the mass ratio of the substances in the raw material is: tripolycyanamide: metal salt: amino acid: conductive carbon material = 20 ~ 100: 1 0~ 100: 0 ~ 10. Previously presented
The method according to Claim 27, wherein the mixing is ball milling mixing. Previously presented
The method according to Claim 27, wherein the inactive atmosphere comprises a gas which is at least one selected from the group consisting of nitrogen, argon, helium and xenon. Previously presented
The method according to Claim 27, wherein the high temperature carbonizing uses a[[n]] one step high temperature carbonizing method or a two step high temperature carbonizing method, wherein the one step high temperature carbonizing method comprises: putting the precursor in inactive atmosphere, and heating to a temperature in a range from 800 ° C to 1200 ° C at a heating rate ranging from 1 ° C/min to 5 ° C/min, and then keeping for a time range from 0.5 hours to 5 hours; and the two step high temperature carbonizing method comprises: putting the precursor in inactive atmosphere, and heating to a temperature in a range from 350 ° C to 650 ° C at a heating rate ranging from 1 ° C/min to 2.5 ° C, and then keeping for a time range from 0.5 hours-4 hours; then heating to a temperature in a range from 800 to 1200 ° C at a heating rate ranging from 1 ° C/min to 5° C/min and keeping for a time range from 0.5 hours to 5 hours. Currently amended
The method according to Claim 27, wherein after putting the precursor in the inactive atmosphere for high temperature carbonization; being contacted with an acidic solution for acid treatment; and then being put in the inactive atmosphere and being treated at a high temperature in a range from 700 ° C to 900 ° C for a time range from 10 m in to 120 min, to obtain the graphene material inlaid with single metal atoms. Currently amended
- 40. Canceled
Canceled
Materials described outside the worked examples.
graphene material inlaid with single metal atoms
tripolycyanamide
metal salt
amino acid
amino acid (cysteine, glycine, alanine, phenylalanine, tryptophan)
metal salt (nickel salt, cobalt salt, ferric salt, ferrous salt)
conductive carbon material (acetylene black, carbon fiber, carbon nanotube, carbon dust, Ketjen black)
N-doped graphene
N and S co-doped graphene
single metal atoms (Fe, Co, Ni)
nickel acetate
cobalt acetate
ferrous acetate
ferric acetate
nickel nitrate
cobalt nitrate
ferrous nitrate
ferric nitrate
nickel sulfate
cobalt sulfate
ferrous sulfate
ferric sulfate
Additional fabrication and treatment steps described in the patent.
Performance values and ranges asserted in the specification or claims.
| Property | Value | Material |
|---|---|---|
Faradaic efficiency for CO2 electroreduction to CO | 95 % | graphene material inlaid with single metal atoms |
Reduction current per unit mass at -1.0 V vs. RHE | 1000 mA/mgcatalyst | graphene material inlaid with single metal atoms |
Current at unit area at -1.0 V vs. RHE | 100 mA/cm2 | graphene material inlaid with single metal atoms |
Mass percentage of single metal atoms in graphene material | — | graphene material inlaid with single metal atoms |
Preferred mass percentage of single metal atoms in graphene material | — | graphene material inlaid with single metal atoms |
Temperature | 800–1200 °C | — |
Duration | 0.5–5 hours | — |
Temperature | 350–650 °C | — |
Temperature | 700–900 °C | — |
Temperature | 40–120 °C | — |