# US 11,440,242 B2 · Fused deposition modeling-based additive manufacturing process at low temperatures

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- Number: US 11,440,242 B2
- Document ID: US11440242B2
- Status: Granted
- Kind: B2
- Application number: 16/331,198
- Filed: 2017-09-11
- Published: 2019-07-18
- Granted: 2022-09-13
- Earliest claimed: 2016-09-12
- Assignees: Covestro Deutschland AG
- Applicants: Covestro Deutschland AG
- Inventors: Dirk Achten; Thomas Büsgen; Dirk Dijkstra; Nicolas Degiorgio; Roland Wagner; Levent Akbas; Peter Reichert; Jörg Büchner
- Web page: https://patentgrep.com/patent/US11440242B2

## CPC

- B29C 64/118: using filamentary material being melted, e.g. fused deposition modelling [FDM]
- B29C 64/00: Additive manufacturing, i.e. manufacturing of three-dimensional [3D] objects by additive deposition, additive agglomeration or additive layering, e.g. by 3D printing, stereolithography or selective laser sintering
- B29C 64/10: Processes of additive manufacturing
- B29C 64/176: Sequentially
- B29C 64/182: in parallel batches
- B29C 64/20: Apparatus for additive manufacturing; Details thereof or accessories therefor
- B29C 64/205: Means for applying layers
- B29C 64/227: Driving means
- B29C 64/245: Platforms or substrates (support structures intended to be sacrificed after manufacture B29C64/40)
- B29C 64/25: Housings, e.g. machine housings
- B29C 64/255: Enclosures for the building material, e.g. powder containers
- B29C 64/30: Auxiliary operations or equipment
- B29C 64/307: Handling of material to be used in additive manufacturing
- B29C 64/40: Structures for supporting 3D objects during manufacture and intended to be sacrificed after completion thereof
- B33Y 10/00: Processes of additive manufacturing
- B33Y 30/00: Apparatus for additive manufacturing; Details thereof or accessories therefor
- B33Y 40/00: Auxiliary operations or equipment, e.g. for material handling
- B33Y 40/10: Pre-treatment
- B33Y 40/20: Post-treatment, e.g. curing, coating or polishing
- B33Y 50/00: Data acquisition or data processing for additive manufacturing
- B33Y 70/00: Materials specially adapted for additive manufacturing
- B33Y 80/00: Products made by additive manufacturing
- B33Y 99/00: Subject matter not provided for in other groups of this subclass
- B29K 2995/007: Hardness
- B29C: SHAPING OR JOINING OF PLASTICS; SHAPING OF MATERIAL IN A PLASTIC STATE, NOT OTHERWISE PROVIDED FOR; AFTER-TREATMENT OF THE SHAPED PRODUCTS, e.g. REPAIRING (making preforms B29B11/00; making laminated products by combining previously unconnected layers which become one product whose layers will remain together B32B37/00 - B32B41/00)
- B33Y: ADDITIVE MANUFACTURING, i.e. MANUFACTURING OF THREE-DIMENSIONAL [3D] OBJECTS BY ADDITIVE DEPOSITION, ADDITIVE AGGLOMERATION OR ADDITIVE LAYERING, e.g. BY 3D PRINTING, STEREOLITHOGRAPHY OR SELECTIVE LASER SINTERING
- B29K: INDEXING SCHEME ASSOCIATED WITH SUBCLASSES B29B, B29C OR B29D, RELATING TO MOULDING MATERIALS OR TO MATERIALS FOR {MOULDS, } REINFORCEMENTS, FILLERS OR PREFORMED PARTS, e.g. INSERTS

## Abstract

A process for manufacturing an article comprises the steps of: I) applying a filament of an at least partially fused construction material to a support so as to obtain a layer of the construction material which corresponds to a first selected cross-section of the article; II) applying a filament of the at least partially fused construction material to a previously applied layer of the construction material so as to obtain a further layer of the construction material which corresponds to a further selected cross-section of the article and which is bonded to the previously applied layer; and III) repeating step II) until the article is formed. At least steps II) and III) are carried out in a chamber and the construction material comprises a fusible polymer. The fusible polymer has a fusion range (DSC, differential scanning calorimetry; 2nd heating at a heating rate of 5 K/min.) of ≥20° C. to ≤100° C. The fusible polymer further has a complex viscosity |η*| (determined by viscosity measurement in the melt using a plate-plate oscillating viscometer according to ISO 6721-10 at 100° C. and a shear rate of l/s) of ≥10 Pas to ≤1000000 Pas. Finally, the temperature inside the chamber is ≤50° C. The invention also relates to an article manufactured by the process according to the invention, to an article having a substrate and to an article bonded to the substrate, the article being in the form of an adhesive joint or varnish region, and to the use of a particular polyurethane in fused deposition modeling-based additive manufacturing processes.

## Claims

### Claim 1

A method of producing an article, comprising the steps of:
I) applying a filament of an at least partly molten construction material to a carrier, such that a layer of the construction material is obtained, corresponding to a first selected cross section of the article;
II) applying a filament of the at least partly molten construction material to a previously applied layer of the construction material, such that a further layer of the construction material is obtained, which corresponds to a further selected cross section of the article and which is bonded to the layer applied beforehand;
III) repeating step II) until the article is formed;
where at least steps II) and III) are conducted within a chamber and the construction material includes a fusible polymer;
wherein
the upper melting temperature of the fusible polymer is within a melting range (DSC, differential scanning calorimetry, 2nd heating operation at heating rate 5 K/min.) of >20° C. to <100° C.,
the fusible polymer has a magnitude of the complex viscosity |n*| (determined by viscometry measurement in the melt with a plate/plate oscillation shear viscometer at 100° C. and a shear rate of 1/s) of >1000 Pas to <1 000 000 Pas, wherein the fusible polymer is a polyurethane obtainable from the reaction of a polyisocyanate component and a polyol component, said polyol component comprising a polyesterpolyol having a pour point (ASTM D5985) of >25° C.,
and wherein the temperature within the chamber is <50° C.

### Claim 2 (depends on 1)

The method as claimed in claim 1, wherein the interior of the chamber is cooled at least at times.

### Claim 3 (depends on 1)

The method as claimed in claim 1, wherein the interior of the chamber is not heated at least at times.

### Claim 4 (depends on 1)

The method as claimed in claim 1, wherein the fusible polymer has a Shore hardness (DIN ISO 7619-1) of >40 Shore A to <80 Shore D.

### Claim 5 (depends on 1)

The method as claimed in claim 1, wherein the fusible polymer, after heating to 100° C. and cooling to 20° C. at a cooling rate of 4° C./min, within a temperature interval from 25° C. to 40° C. for >1 minute, has a storage modulus G′ (determined at the respective temperature with a plate/plate oscillation viscometer according to ISO 6721-10 at a shear rate of 1/s) of >100 kPa to <1 MPa and, after cooling to 20° C. and storage at 20° C. for 120 minutes, has a storage modulus G′ (determined at 20° C. with a plate/plate oscillation viscometer according to ISO 6721-10 at a shear rate of 1/s) of >10 MPa.

### Claim 6 (depends on 1)

The method as claimed in claim 1, wherein the article formed is subjected to an aftertreatment selected from the group consisting of mechanical smoothing of the surface, controlled local heating, heating of the entire article, controlled local cooling, cooling of the entire article, contacting of the article with steam, contacting of the article with the vapor of an organic solvent, irradiating the article with electromagnetic radiation, immersing the article into a liquid bath, and a combination of at least two of these.

### Claim 7 (depends on 1)

The method as claimed in claim 1, wherein the article is formed on a substrate and, on conclusion of the method, remains bonded to the substrate.

### Claim 8 (depends on 1)

The method as claimed in claim 1, wherein the polyesterpolyol has a number average molecular weight of from 400 g/mol to 6000 g/mol.