SAPO-34 templated growth of hierarchical porous graphene cages as electrocatalysts for both oxygen reduction and evolution
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摘要: 具有三维多级孔道结构的石墨烯材料可以作为氧还原反应、氧析出反应的电催化剂，体现出优异的反应活性。在合成石墨烯的众多方法中，化学气相沉积法（CVD）具有良好的应用前景，但可作为CVD法石墨烯沉积模板的材料十分有限。本文采用磷酸硅铝分子筛（SAPO-34）用作多级孔石墨烯的沉积模板制备石墨烯材料。所得石墨烯材料可完整保留SAPO-34分子筛的立方体颗粒结构，呈现为由具有微孔/介孔结构的超薄石墨烯层围成的微米尺度空心立方体结构。引入氨气煅烧，可以得到原子分数6.84%的氮掺杂量。由于具有独特的孔结构，丰富的缺陷位点以及良好的杂原子掺杂，制得的石墨烯材料体现出高效的双功能氧还原与氧析出反应催化活性。Abstract: Three-dimensional hierarchical porous graphene materials with unique properties are of significant importance for the exploration of advanced electrocatalysts for both the oxygen reduction and evolution reactions (ORR/OER). Templated chemical vapor deposition is a favorable strategy to fabricate this kind of graphene, but the number of effective templates is limited. Here, silicoaluminophosphate (SAPO-34) zeolite crystals were used as the catalytic templates for the deposition of hierarchical porous graphene. The graphene obtained consisted of micron-size hollow cubes with mesoporous/nanoporous facets, and ultrathin walls, precisely replicating the structure of the cube-like SAPO-34 zeolite particles. A high doping level of nitrogen (6.84 at%) was achieved by subsequent annealing at 700℃ under ammonia before template removal. Because of the unique porosity, abundant defects, and favorable N-doping, the N-doped graphene exhibited considerable reactivity for both ORR and OER.
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