Method of producing graphene from liquid metal

摘要

A method for producing a graphene layer on a multilayered plate containing, as the graphene forming matrix, an external layer composed of a metal or a metal alloy and, as a support substrate, the transition metals and/or their alloys and/or metalloids and/or their solutions and compounds, the method involving subjecting the multilayered plate to heat treatment in the following stages: plate heating until the plate reaches a temperature that is between 0.5° C. and 50° C., annealing, at a constant or variable temperature from the temperature range, for a period between 60 and 600 seconds and cooling, with the cooling rate maintained between 0.1 and 2° C./min in the temperature range of 1,200° C.-1,050° C.

主权项

1. A method for producing a graphene layer from a liquid metal matrix on a solid metal or ceramic substrate, wherein a multilayered plate containing, as the graphene forming matrix, an external layer composed of a metal or a metal alloy with a melting point in the range from 1,051° C. and 1,150° C. and, as a support substrate, between 1 and 5 layers made of transition metals and/or their alloys and/or metalloids and/or their solutions and compounds with melting points in the range from 1,151° C. to 3,410° C., is subjected to heat treatment in the following stages:
plate heating until the plate reaches a temperature that is between 0.5° C. and 50° C. higher than the melting point of the forming matrix, annealing, at a constant or variable temperature from the temperature range, for a period between 60 and 600 seconds, concurrently supplying the atmosphere with acetylene at a partial pressure of up to 4 hPa, ethylene at a partial pressure of up to 4 hPa and hydrogen at a partial pressure of up to 2 hPa for a period between 10 and 300 seconds, cooling, partially controlled, with the cooling rate maintained between 0.1 and 2° C./min in the temperature range of 1,200° C.-1,050° C., where consecutive stages of heating, annealing and cooling are conducted in the atmosphere of pure argon at a constant partial pressure varying from 1 hPa to 1,100 hPa, wherein the transition metal is selected from the group consisting of platinum, molybdenum, palladium and nickel, and (1) when the transition metal is platinum, the platinum plate, which is at least 0.2 mm thick and coated by electrolysis on one side with a 0.2 mm thick copper layer, is placed in the chamber of a vacuum furnace, at which point, after removing air from the chamber to the vacuum level of 10−3 hPa, argon is supplied into the furnace chamber in such a way as to maintain the partial pressure of argon throughout the entire process at the level of 20 hPa, whereby concurrently with the commencement of argon supply the plate heating process is initiated and continued until the plate reaches 1,100° C. and the temperature of the plate stabilizes at this level for 2.5 min, with acetylene, ethylene, hydrogen and argon additionally supplied into the furnace chamber for 60 seconds during the period of maintaining constant temperature until the partial pressure reaches 28 hPa, following which the plate is cooled down at a rate of 1° C./min to 1,075° C., at which point rapid uncontrolled cooling to the ambient temperature is continued in the furnace chamber, (2) when the transition metal is molybdenum, a molybdenum plate with a thickness of 4.5 mm and dimensions of 50×50 mm is coated by magnetron sputtering with a 40 μm thick layer of nickel and then a 1.5 mm thick layer of copper and is placed in the chamber of a vacuum furnace, at which point, after removing air from the chamber to the vacuum level of 10−3 hPa, argon is supplied into the furnace chamber in such a way as to maintain the partial pressure of argon throughout the entire process at the level of 1100 hPa, whereby at the same time the plate heating process is initiated and continued until the plate reaches 1,100° C. and then temperature of the plate stabilizes at this level for 10 minutes, with additional hydrogen supplied into the furnace chamber for 120 seconds during the period of heating to the temperature to achieve the partial pressure of 60 hPa, following which the plate is cooled down at a rate of 0.2° C./min to 1,050° C., at which point rapid uncontrolled cooling to the ambient temperature is continued in the furnace chamber, and wherein the metalloid or its compound is silicon or quartz, and when the metalloid or its compound is quartz, a quartz glass plate, which is at least 0.8 mm thick and coated with a 300 nm thick layer of silicon and a 1,000 nm thick layer of copper, is placed in the chamber of a vacuum furnace, at which point, after removing air from the chamber to the vacuum level of 10−3 hPa, argon is supplied into the furnace chamber in such a way as to maintain the partial pressure of argon throughout the entire process at the level of 50 hPa, whereby after 5 minutes the plate heating process is initiated and continued until the plate reaches 1,090° C. and the temperature of the plate stabilizes at this level for 5 minutes, with additional gases supplied into the furnace chamber for 20 seconds during the period of maintaining constant temperature: acetylene—to achieve the partial pressure of 2 hPa, ethylene—to reach the partial pressure of 2 hPa and hydrogen—to attain the partial pressure of 1 hPa, following which the plate is cooled down at a rate of 0.2° C./min to 1,075° C., at which point rapid uncontrolled cooling to the ambient temperature is continued in the furnace chamber.