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Ethyne-Reducing Metal–Organic Frameworks to Control Fabrications of Core/shell Nanoparticles as Catalysts
ACS Catalysis ( IF 11.3 ) Pub Date : 2018-06-20 00:00:00 , DOI: 10.1021/acscatal.8b01691
Chenghua Zhang 1, 2 , Xiaoxue Guo 2 , Qingchun Yuan 3 , Rongle Zhang 1, 2 , Qiang Chang 1, 2 , Ke Li 1, 2 , Bo Xiao 4 , Suyao Liu 1, 2 , Caiping Ma 1, 2 , Xi Liu 1, 2 , Yuqun Xu 1, 2 , Xiaodong Wen 1, 2 , Yong Yang 1, 2 , Yongwang Li 1, 2
Affiliation  

An approach using cobalt metal–organic frameworks (Co–MOF) as precursors is established for the fabrication of cobalt nanoparticles in porous carbon shells (core/shell [email protected]). Chemical vapor deposition of ethyne is used for controlling the reduction of cobalt nanoclusters in the MOF and the spontaneous formation of the porous carbon shells. The metallic cobalt cores formed are up to 4–6 nm with the crystal phase varying between hexagonally close-packed (hcp) and face-center-packed (fcc). The porous carbon shells change from amorphous to graphene with the ethyne deposition temperature increasing from 400 to 600 °C. The core/shell [email protected] nanoparticles exhibit high catalytic activity in selectively converting syngas (CTY 254.1–312.1 μmolCO gCo–1 s–1) into hydrocarbons (4.0–5.2 gHC g-cat–1 h–1) at 260 °C and 3.0 MPa. In addition to the crystal size and phase, the coordination numbers of the cobalt to oxygen and to other cobalt atoms on the surface of the cobalt nanoparticles and the permeability of the porous carbon shell have been related to the catalytic performance in FTS reactions.

中文翻译:

减少乙炔的金属-有机骨架,可控制核/壳纳米颗粒作为催化剂的制备

建立了一种使用钴金属-有机骨架(Co-MOF)作为前体的方法,用于在多孔碳壳(核/壳[受电子邮件保护])中制造钴纳米颗粒。乙炔的化学气相沉积用于控制MOF中钴纳米团簇的减少和多孔碳壳的自发形成。形成的金属钴核长达4–6 nm,晶体相在六方密堆积(hcp)和面心堆积(fcc)之间变化。随着乙炔沉积温度从400°C升高到600°C,多孔碳壳从无定形变为石墨烯。核/壳[受电子邮件保护]的纳米颗粒在选择性转化合成气方面表现出高催化活性(CTY 254.1–312.1μmolCOg Co–1 s –1)在260°C和3.0 MPa的压力下转化为碳氢化合物(4.0–5.2 gHC g-cat –1 h –1)。除了晶体尺寸和相之外,钴与钴纳米颗粒表面上的氧和与其他钴原子的配位数以及多孔碳壳的渗透性还与FTS反应中的催化性能有关。
更新日期:2018-06-20
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