• 专利标题:   Nitrogen-doped mesoporous graphene microsphere useful in preparing oxygen reduction electrode of alkaline fuel cells, prepared by e.g. adding sodium metal in hexachlorobutadiene, reacting, centrifuging, and mixing microspheres with urea.
  • 专利号:   CN103831121-A, CN103831121-B
  • 发明人:   JIN H, WANG J, WANG S
  • 专利权人:   UNIV WENZHOU
  • 国际专利分类:   B01J027/24, B01J035/08, H01M004/90
  • 专利详细信息:   CN103831121-A 04 Jun 2014 B01J-027/24 201452 Pages: 12 Chinese
  • 申请详细信息:   CN103831121-A CN10683949 12 Dec 2013
  • 优先权号:   CN10683949

▎ 摘  要

NOVELTY - Nitrogen-doped mesoporous graphene microsphere prepared by (i) adding sodium metal in hexachlorobutadiene, reacting at 200-300 degrees C for 10-40 hours in sealed condition, centrifuging, discarding the supernatant, adding anhydrous ethanol, centrifuging by adding aqueous ethanol solution and anhydrous ethanol, removing precipitate, and drying; and (ii) under inert gas protection, mixing the resulting microspheres with urea, or purging ammonia gas, reacting for 0.5-4 hours under sealed condition, centrifuging the reaction mixture, depositing, using water for washing, and drying, is claimed. USE - The microsphere is useful in preparing oxygen reduction electrode of alkaline fuel cells (claimed). ADVANTAGE - The microsphere: has high activity, low cost and long service life; and is suitable for non-platinum oxygen reduction catalyst for fuel cells. DETAILED DESCRIPTION - Nitrogen-doped mesoporous graphene microsphere prepared by (i) adding sodium metal in hexachlorobutadiene, reacting at 200-300 degrees C under pressure of 15 MPa for 10-40 hours in sealed condition, centrifuging, discarding the supernatant, adding anhydrous ethanol, centrifuging by adding 50 vol.% aqueous ethanol solution and anhydrous ethanol, removing precipitate, and drying at 240 degrees C to obtain mesoporous graphene microspheres, where the mass ratio of sodium metal and hexachlorobutadiene is 1:70-600; and (ii) under inert gas protection, mixing the resulting microspheres with urea or purging ammonia gas through the microspheres, reacting at 700-1200 degrees C for 0.5-4 hours under sealed condition, centrifuging the reaction mixture, depositing, using water for washing, and drying to obtain nitrogen-doped mesoporous graphene microspheres, is claimed. The mass ratio of mesoporous graphene microspheres and urea is 1:5-50, and the mass ratio of mesoporous graphene microsphere and ammonia gas is 20:1. An INDEPENDENT CLAIM is also included for preparing the nitrogen-doped mesoporous graphene microsphere, comprising (a) adding sodium metal b to the container, then injecting hexachlorobutadiene b into the inner container, opening plug of the container, sealing the opening of the container with copper film, immersing the container in hexachlorobutadiene c, reacting at 200-330 degrees C for 10-40 hours under sealed condition, centrifuging the reaction product, in turn adding anhydrous ethanol, removing supernatant, centrifuging by using 50 vol.% aqueous ethanol and anhydrous ethanol, finally drying the centrifuged precipitate at 240 degrees C for 1 hour to obtain mesoporous graphene microspheres b, where the container is metal container which does not react with sodium, ceramic container or glass container, the mass ratio of sodium metal b and hexachlorobutadiene b is 1:70-600, and (b) under protection of inert gas, mixing the resulting microspheres b with urea or purging ammonia gas through the resulting microspheres b, reacting at 700-1200 degrees C for 0.5-4 hours under sealed condition, centrifuging the reaction mixture, washing the precipitate, and drying to obtain nitrogen-doped mesoporous graphene microspheres b, where the mass ratio of the mesoporous graphene microspheres and urea is 1:5-50, and the mass ratio of ammonia gas b and mesoporous graphene microspheres b is 1-20:1.