US 1251954 A
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Patented Jan. 1, 1918.
AND THE LIKE.
APPLICATION FILE-I1 Aue.3.1su.
I BEI IGIUS &J.' BIELWILLER. PROCESS FOR PRODUCING LIQUID 0R SOLUBLE O RGANIC COMBINA TIONS FROM HARD GOAL Z many, have invented certainnew and useful which is materially below the pro UNITED STATES PATENT clarionrnmnn'rcn annulus am) JOHN nunwinnnn, be woven, annular,
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To 'allwhom it may concern:
0 Be it known that we, (1) Dr. FRIEDRICH BnRo'IUs and (2) JOHN BILLWILLER, citizens of 1) the German Empire and (2) Switzerland, (St. Gallen,) residing at Hanover, Gerin or Relating to Processes Combinations from Hard Coal and the like, of which the following is a specification.-
This invention relates to. a process of treating carbonaceous material. suchas natural coals or other "products of carboni'-. zation of wood and other vegetable matter,
so as to transform such carbonaceous material into a liquid or into substances of low 'meltingpoint practically without leaving a solid carbonaceous residue in the .form of coke or similar material'. The process of this invention whereby the liquefaction of coal is obtained consists therein that the coal is subjected to the action of hydrogen at high pressure of more than atmospheres and elevated temperatlire not exceeding 600 ,centigrade, preferably at a hydrogen pres sure of-more'than 40 atmospheres, and
at an elevated temperature between 300 and 500 C. The effect of such treatment consists therein that hydrocarbons are formedby" chemical reaction betweenthe hydrogen a and the carbon compounds of the coal, which are either liquid at ordinary temperature or have a low melting point.
of methane at the -working' temperature er,coal
distillation temperature so that in t e process of this invention practically no coal distillation roducts are formed. Notwithstandin this, the amount of liquid products formed y the process is many times greater than that, obtained by the usual coal dis tillation and reaches nearly 100% of the carbonaceous substance of the coal, whereas the liquid roducts of usual coal distillation generally 0 not exceed say 3%.
"iThe; nitrogen contained in the coal is transformed during the hydrogenation procinto ammonia and ammonium. comfd an'd ther same can be recovered in quantitatively.
Specification 0t Letters I'atent. Application fled August a, 1914. Serial No. 854,825.
undergoing carbonization Only a very small, generating substances,
portion of the carbon is volatilized in form Patented Jan. 1,1918.
Some of the organic compounds produced by' the hydrogenation process contain oxygen and are of the phenolic type.' The chief part is recovered as hydrocarbons of differout boiling points, similar to petroleum distillates.
The unliquefied residue is a dark colored substance containing the ash of the original charge and a small proportion of carbonaceous material.
The period of reaction can be shortened and the output increased if a hydrocarbon capable of dissolving or diluting the resulting products, such for example as a heavy commercial grade of benzene, is added to the dry material to be treated. L
The process 'is applicable not only to natural coal and other products of natural carbonization of wood and of other vegetable material, but also to' wood, peat and other vegetable material, these substances during the heating process .according to this invention. Furthermore, the process to the products of coal. distillation such as tar and, pitch, producing therefrom compounds of lower melting-point.
In order to carry through the process an apparatus may be used which allows the treatment of coal under high pressure at an elevated temperature with hydrogen n or hydrogen-containing gases or hydrogenthat is 'to say, substances which are capable bf liberating hydrogen under the operating conditions, as for example the hydrogen compound calcium, CaH
A suitable apparatus is diagrammatically shown on the annexed. drawing.
is applicable also l designates areaction vessel adapted to opens-into a vessel 10. 11 is a circulating plpe having inserted therein a pump 12. 13 1s a cooler. a
. The operation of the device is 'as folsolid residue. Only 15% Thecharging orifice 2 of the reaction vessel is opened. and the material to be treated placed thereim. This material consists either of powdered coal, or of a suspension of coal in a liquid which serves as a diluent for the products of reaction to be formed by the process. After filling the char e into the reaction vessel the orifice 2 is c osed pres? sure-ti ht. Thereafter hydrogen from receptac e 6 is introduced into the reaction vessel 1 and the pressure in the reaction vessel brought to the desired degree. The furnace 5 is started and the metal bath 4 brought to the desired working temperature. The pump 12- is put in operation so that hydrogen is circulated through the reaction vessel and the material therein. The circulation of the hydrogen effects a suitable stirring of the maternal under treatment. Under the efl'ect of heat and pressure hydrocarbons are formed within the .vessel by reaction between the coal and hydrogen under high pressure, and portions of these hydrocarbons erg transported with the circulating stream through the coil 9 and are condensed by the operation of the condenser 13. The condensed/material accumulates within the vessel 10 from which it, 'can be, rembved. The uncondensed'f'gas' consisting nearly entirely of hydrogen is returned by the pump 12 to the reaction-vesse l t The consumed hydrogen is replaced b jfw gas taken from the receptacle 6. Theia'irnnonia sorbent.
escaping from the coal under treatment may be retained within the receptacle 10 in any suitable manner as' by any suitable ab- Ewampls.
1'. 400 kg. powdered coal are filled intoia pressure-resisting. vessel of about 400 liters capacity, which is connected to a tank in which hydrogen is-held under 200 atmos;
pher'es pressure. After 15 hours the connec- ,tion .with the hydrogen tank is turned off and the vessel is emptied. About 10 to 15 kg. of hydrogen have.then been consumed, according to the qualit' of coal used.
From the contents 0 the vessel more than half of the coal can be separated from the solid residue as liquid.
The remaining part of liquid products in 7 the solid residue can be gained by extraction. 7 I e :2. 150 kg. powdered-coa1 are placedwith an equal quantity of heavy benzene in a pressure resisting vessel of about 400 liters capacity and the sameis connected to a" hydrogen tank. For the purpose or sists in subjecting them to thg elevated tem contents stirred and heated to 400.
After 12 hours the vessel is o ened and the liquid produced is separate from the of the weight of coal employed is then left. The remaining 85% is dissolved in the benzene. The con- Sumption of hydrogen is about 5 kg.
3. 400 kg. powdered coal are filled into a pressure resisting vessel of about 400 liters capacity and the same is connected to a tank in which hydrogen is held under 200 atmospheres pressure and heated to about 400. After two hours the operation is intermising, the vessel is either rotated, or the rupted and the material removed from the vessel. It contains onl liquid substance, "whic is separated from the solid -material. The solid material= is extracted'iwith an organic solvent such as benzene, inan extractln apparatus." A.fter distilling the benzene, -t e products gained by ydrogenation process and contained therein, can be extracted. I
. a small quantity of The terms hydrogen containing, and
hydrogen-yielding, as used in the claims, are intended to include, and do in lude, substances, such as liquids or gases, t at impart hydrogen to the unsaturated carbon comounds in the coal, etc., as well as free hydrogen, by which the hydrogenatioxi ofthe 'i'msaturated compounds is eflected, duringthe reaction.
What we claim is: I J 1. The process of treating products of carbonization of vegetable matter which consists in subjecting them to the action of hy-' hydrogen at a temperature fr n3 300 to 500 centigrade and at a pressure of more than 100 atmospheres. until liquid or lowmelting-point reaction. products of the solid carbonaceous matter are formed.
4. The process of treating products of carbonizatlon of vegetable matter which com sists in reacting thereon with hydrogen at rature andhigh pressure until most of e solid carbonaceous substance is t-ransformed\ into liquid 01 low-meltingp int compounds,
v 5. Theprocess of treating products of car-r bonization of vegetable matter which consists in carbonizing vegetable matter in the presence of hydrogen at elevated tempera.- ture and high pressure and continuing the hydrogen treatment until most of the solid carbonaceous substance is transformed into liquid or low-melting-point com ounds.
6. The process of treating prodilcts of carbonization of vegetable matter which consists in reacting upon a mixture or emulsion of the carbonized material in a suspending and diluting medium with hydrogen at elevated temperature and high pressure, said suspended and diluting medium forming a liqhid under working'conditions.
. The process of treating products of carbonization of vegetable matter which consists in subjecting them to the action of by drogen-containin gases at an elevated temperature of less t an 600 centigrade and at a high hydrogen ressure of more than 20 atmospheres unti' liquid or low-meltingpoint reaction products of the solid caronaceous matter are formed.
8. The process of treating products of car bonization of vegetable matter which consists in subjecting them to the action of hydrogen-yielding substances at an elevated temperature of lesscthan 600 Centigrade and at a hi h hydrogen ressure of more than 20 atmosp eres until iquid or low-meltingpoint reaction products of the solid carbo-q naceous matter are formed.
'9. The process of treating coal and similar substances produced by natural or artificial carbonization, to produce liquid compounds, which comprises reacting thereon with hydrogen under increased pressure and at an elevated temperature less than 600 C.
10. The process of treating coal and similar substances produced by natural or artificial carbonization, to produce liquid compounds, which comprises reacting thereon -with hydrogen-containing substances under increased pressure" and at an elevated temperature less than 600 C.
11. The process of treating coal and similarsubstances produced by natural or artificiah'carboniza'tion to produce liquid com pounds, which comprises reacting thereon with h drogen-yield 'ng substances under increase pressure and at an elevated temperature less than 600 C.
-12 The process of treating coal and similar substances produced by natural or artificial carbonization to produce liquid oompounds, which comprises reacting thereon with hydrogen under increased pressure and In testimony whereof, we our signstures in presence of two witn=-=-= DR. FRIEDRICH BERGIUS. JOHN ,BILLWILLER.
S. Hmmr Rm, KARL Eooms.