Enhanced activity of Co catalysts supported on tungsten carbide-activated carbon for CO2 reforming of CH4 to produce syngas
Enhanced activity of Co catalysts supported on tungsten carbide-activated carbon for CO2 reforming of CH4 to produce syngas
复制标题
增强碳化钨-活性炭负载 Co 催化剂用于 CO2 重整 CH4 生产合成气的活性
DOI：
10.1016/j.ijhydene.2021.06.085
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发表时间：
2021-08
影响因子：
7.2
通讯作者：
Lv Yongkang
中科院分区：
文献类型：
--
作者：
Li Sheng;Zhang Guojie;Wang Jiming;Liu Jun;Lv Yongkang
碳材料因其优异的性能而被广泛用作催化剂或载体。本文通过在AC基体上原位渗碳的方法成功制备了碳化钨-活性炭(WC-AC)复合载体，其特点是WC共价锚固在AC载体上。将活性金属Co负载在WC-AC上用于甲烷干重整(DRM)。通过 N2 物理吸附测量、XRD、XPS、H2-TPR、H2-TPD、CH4&CO2-TPSR、TG-DTG 对样品进行分析。 WC-AC稳定了AC中C的扰动，减轻了CO2的气化效应，增加了CH4裂解的活性位点。此外，WC提供了适合Co3+→Co2+的无电阻桥，从而在催化剂表面上产生高Co2+/Co3+比率。这增强了 Co 物质和 WC-AC 之间的相互作用，从而增强了 CH4 活化。在WC-AC促进Co3+→Co2+的过程中，催化剂表面伴随着氧空位的产生。这可以增强WC-钴氧化物表面CO2的解离吸附，同时增加催化剂表面吸附氧的相对比例，从而有效抑制焦炭的形成。然而，由于WC和Co的强耦合而产生的少量石墨碳是Co/WC-AC失活的主要原因。
Carbon materials are widely used as catalysts or supports due to their excellent properties. In this paper, the tungsten carbide-activated carbon (WC-AC) composite support was successfully prepared byin-situcarburizing on AC matrix, which is characterized by the covalent anchoring of WC on the AC support. The active metal Co was supported on WC-AC for dry reforming of methane (DRM). Samples were analyzed by N2physisorption measurements, XRD, XPS, H2-TPR, H2-TPD, CH4&CO2-TPSR, TG-DTG. The WC-AC stabilizes the disturbance of C in AC, alleviates the gasification effect of CO2and increases the active sites for CH4cracking. Moreover, WC provides a resistance-less bridge suitable for the Co3+→ Co2+, resulting in a high Co2+/Co3+ratio on the catalyst surface. This enhances the interaction between the Co species and the WC-AC, thereby enhancing the CH4activation. In the process of WC-AC promoting Co3+→Co2+, the catalyst surface is accompanied by the generation of oxygen vacancies. This can enhance the dissociative adsorption of CO2on surface of the WC-cobalt oxide, and at the same time increase the relative proportion of adsorbed oxygen on the catalyst surface, thereby effectively inhibiting the formation of coke. However, the small amount of graphitic carbon generated due to the strong coupling of WC and Co is the main reason for deactivation of Co/WC-AC.
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