US 11,987,907 B2
Molybdenum disulfide/graphene/carbon composite material and use thereof
Hui Du, Qingdao (CN); Yajing Duan, Qingdao (CN); Zhaojun Chen, Qingdao (CN); Hui Fu, Qingdao (CN); and Jinzhe Fu, Qingdao (CN)
Assigned to QINGDAO UNIVERSITY, Qingdao (CN)
Appl. No. 17/638,208
Filed by QINGDAO UNIVERSITY, Qingdao (CN)
PCT Filed Mar. 3, 2020, PCT No. PCT/CN2020/077517
§ 371(c)(1), (2) Date Feb. 25, 2022,
PCT Pub. No. WO2021/036219, PCT Pub. Date Mar. 4, 2021.
Claims priority of application No. 201910804766.8 (CN), filed on Aug. 28, 2019.
Prior Publication US 2022/0243366 A1, Aug. 4, 2022
Int. Cl. D01F 9/22 (2006.01); D01D 5/00 (2006.01)
CPC D01F 9/22 (2013.01) [D01D 5/0007 (2013.01); D10B 2101/12 (2013.01); Y10T 428/2918 (2015.01); Y10T 428/298 (2015.01)] 4 Claims
OG exemplary drawing
 
1. A molybdenum disulfide/graphene/carbon composite material, wherein the molybdenum disulfide/graphene/carbon composite material is composed of a composite nanofiber with a diameter of 60 nm to 500 nm; in a mass percentage, the composite nanofiber comprises 3% to 35% of molybdenum disulfide, 0.2% to 10% of graphene, and 60% to 95% of carbon; and the composite nanofiber has a hierarchical pore structure distributed along an axial direction, wherein based on a pore volume, in the hierarchical pore structure, a microporous structure accounts for 25% to 60% and a mesoporous structure accounts for 40% to 75%,
wherein the molybdenum disulfide and the graphene both are each uniformly dispersed as monolayer structures in the composite nanofiber based on a carbon nanofiber,
wherein the molybdenum disulfide/graphene/carbon composite material has a specific surface area of 500 m2/g to 3,200 m2/g,
wherein the hierarchical pore structure has a pore diameter continuously distributed between 0.1 nm and 5 μm, and an average pore diameter of the hierarchical pore structure is 1.5 nm to 25 nm,
wherein the microporous structure is distributed on a surface of the composite nanofiber and a pore wall of the mesoporous structure, and
wherein the composite material is prepared by the following method:
(1) adding 0.6 g to 1.5 g of polyacrylonitrile, 0.5 g to 1.2 g of polyvinylpyrrolidone, 0.2 g to 1.0 g of ammonium tetrathiomolybdate, and 0.05 g to 0.2 g of graphene to 10 g to 16 g of N,N-dimethylformamide, stirring a resulting solution for dissolution, and filtering the resulting solution through a 400-mesh stainless steel mesh to obtain a filtrate;
(2) conducting an electrostatic spinning of said filtrate to obtain a composite fiber film;
(3) placing the composite fiber film in a tube furnace, and in a N2/H2 mixed atmosphere with a volume ratio of 9/1, heating the tube furnace to a temperature of 380° C. to 450° C. at a heating rate of 2° C./min to 6° C./min, holding the temperature for 1 hour to 6 hours, cooling the tube furnace to room temperature, and taking a treated composite fiber film out of the tube furnace;
(4) preparing a KOH saturated solution, subjecting the treated composite fiber film to an ultrasonic treatment in the KOH saturated solution for 1 hour and a static impregnation for 48 hours in the KOH saturated solution, and vacuum-drying an impregnated composite fiber film for 8 hours to obtain a dried composite fiber film, wherein a mass ratio of the treated composite fiber film to KOH is 1:(0.4-10); and
(5) placing the dried composite fiber film in the tube furnace, and in an argon atmosphere, heating the tube furnace to 750° C. to 850° C. at a heating rate of 2° C./min to 10° C./min to conduct a high-temperature activation for 1 hour to 16 hours, cooling the tube furnace to room temperature, and taking a product out; and washing the product with a dilute hydrochloric acid solution, and vacuum-drying a washed product for 10 hours to obtain the molybdenum disulfide/graphene/carbon composite material with the hierarchical pore structure.