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双金属金属有机框架衍生的混合纳米结构作为甲烷干重整的高性能催化剂

Bimetallic Metal-Organic Framework-Derived Hybrid Nanostructures as High-Performance Catalysts for Methane Dry Reforming.

作者信息

Liang Teng-Yun, Senthil Raja Duraisamy, Chin Kah Chun, Huang Chun-Lung, Sethupathi Sumathi A/P, Leong Loong Kong, Tsai De-Hao, Lu Shih-Yuan

机构信息

Department of Chemical Engineering, National Tsing Hua University, Hsinchu 30013, Taiwan, R.O.C.

Lee Kong Chian Faculty of Science and Engineering, Universiti Tunku Abdul Rahman, Jalan Sungai Long 9, Bandar Sungai Long, 43000 Kajang, Selangor, Malaysia.

出版信息

ACS Appl Mater Interfaces. 2020 Apr 1;12(13):15183-15193. doi: 10.1021/acsami.0c00086. Epub 2020 Mar 24.

DOI:10.1021/acsami.0c00086
PMID:32167283
Abstract

Syngas, consisting of equimolar CO and H, is an important feedstock for large-scale production of a wide range of commodity chemicals including aldehyde, methanol, ammonia, and other oxygenated chemicals. Dry reforming of methane (DRM), proceeding by reacting greenhouse gases, CO and CH, at high temperatures in the presence of a metal catalyst, is considered one of the most environmentally friendly routes for syngas production. Nevertheless, nonprecious metal-based catalysts, which can operate at relatively low temperatures for high product yields and selectivities, are required to drive the DRM process for industrial applications effectively. Here, we developed NiCo@C nanocomposites from a corresponding NiCo-based bimetallic metal-organic framework (MOF) to serve as high-performance catalysts for the DRM process, achieving high turnover frequencies (TOF) at low temperatures (>5.7 s at 600 °C) and high product selectivities (H/CO = 0.9 at 700 °C). The incorporation of Co in Ni catalysts improves the operation stability and light-off stability. The present development for MOF-derived nanocomposites opens a new horizon for design of DRM catalysts.

摘要

合成气由等摩尔的一氧化碳和氢气组成,是大规模生产包括醛、甲醇、氨及其他含氧化合物在内的多种商品化学品的重要原料。甲烷干重整(DRM)是在金属催化剂存在下,使温室气体一氧化碳和甲烷在高温下反应进行的,被认为是合成气生产中最环保的途径之一。然而,为了有效推动用于工业应用的DRM过程,需要能在相对低温下运行以实现高产物产率和选择性的非贵金属基催化剂。在此,我们从相应的镍钴基双金属金属有机框架(MOF)开发出镍钴@碳纳米复合材料,用作DRM过程的高性能催化剂,在低温下实现了高周转频率(600℃时>5.7 s⁻¹)和高产物选择性(700℃时H₂/CO = 0.9)。钴掺入镍催化剂中提高了操作稳定性和起燃稳定性。MOF衍生纳米复合材料的当前发展为DRM催化剂的设计开辟了新视野。

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