A General Method for Constructing Two-Dimensional Layered Mesoporous Mono- and Binary-Transition-Metal Nitride/Graphene as an Ultra-Efficient Support to Enhance Its Catalytic Activity and Durability for Electrocatalytic Application.
A General Method for Constructing Two-Dimensional Layered Mesoporous Mono- and Binary-Transition-Metal Nitride/Graphene as an Ultra-Efficient Support to Enhance Its Catalytic Activity and Durability for Electrocatalytic Application.
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DOI：
10.1021/acsami.6b03747
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发表时间：
2016-07
影响因子：
9.5
通讯作者：
Baocang Liu;L. Huo;R. Si;Jian Liu;Jun Zhang
中科院分区：
文献类型：
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作者：
Baocang Liu;L. Huo;R. Si;Jian Liu;Jun Zhang
我们首次通过一种高效和通用的纳米铸造策略，构建了一系列二维层状介孔单相和二元过渡金属氮化物/石墨烯纳米复合材料(TMN/G，Tm=Ti，Cr，W，Mo，TICR，TiW和TiMo)。二维层状介孔TMN/G是由细小的TMN纳米颗粒与石墨烯纳米片复合而成，具有较大的比表面积和较高的孔隙率。通过修饰分散良好的铂纳米颗粒，可以得到在酸性和碱性介质中对甲醇电氧化反应(MOR)和氧气还原反应(ORR)表现出良好催化活性和稳定性的二维层状介孔催化剂。二维层状介孔双孔催化剂的催化活性优于单一的铂/TMN/G、无石墨烯的铂/TMN、铂/G和铂/C催化剂。可喜的是，2D层状介孔铂/Ti0.5Cr0.5N/G催化剂对MOR和ORR都表现出最好的电催化性能。铂/Ti0.5Cr0.5N/G催化剂优异的电催化性能源于其大的比表面积、高的孔隙率、铂、Ti0.5Cr0.5N和石墨烯之间的强相互作用、N掺杂的石墨烯促进的良好的电子转移性能以及铂和Ti0.5Cr0.5N纳米晶的小尺寸。优异的催化性能为二维层状介孔铂/Ti0.5Cr0.5N/G催化剂在酸性和碱性介质中直接甲醇燃料电池提供了广泛的应用前景。该合成方法可用于构建其他2D层状介孔金属氮化物、碳化物和磷化物。
We constructed a series of two-dimensional (2D) layered mesoporous mono- and binary-transition-metal nitride/graphene nanocomposites (TMN/G, TM = Ti, Cr, W, Mo, TiCr, TiW, and TiMo) via an efficient and versatile nanocasting strategy for the first time. The 2D layered mesoporous TMN/G is constituted of small TMN nanoparticles composited with graphene nanosheets and has a large surface area with high porosity. Through decoration with well-dispersed Pt nanoparticles, 2D layered mesoporous Pt/TMN/G catalysts can be obtained that display excellent catalytic activity and stability for methanol electro-oxidation reactions (MOR) and oxygen reduction reactions (ORR) in both acidic and alkaline media. The 2D layered mesoporous binary-Pt/TMN/G catalysts possess catalytic activity superior to that of mono-Pt/TMN/G, graphene free Pt/TMN, Pt/G, and Pt/C catalysts. Encouragingly, the 2D layered mesoporous Pt/Ti0.5Cr0.5N/G catalyst exhibits the best electrocatalytic performance for both MOR and ORR. The outstanding electrocatalytic performance of the Pt/Ti0.5Cr0.5N/G catalyst is rooted in its large surface area, high porosity, strong interaction among Pt, Ti0.5Cr0.5N, and graphene, an excellent electron transfer property facilitated by N-doped graphene, and the small size of Pt and Ti0.5Cr0.5N nanocrystals. The outstanding catalytic performance provides the 2D layered mesoporous Pt/Ti0.5Cr0.5N/G catalyst with a wide range of application prospects in direct methanol fuel cells in both acidic and alkaline media. The synthetic method may be available for constructing other 2D layered mesoporous metal nitrides, carbides, and phosphides.