当前位置: X-MOL 学术J. CO2 Util. › 论文详情
Our official English website, www.x-mol.net, welcomes your feedback! (Note: you will need to create a separate account there.)
Effect of spinel inversion and metal-support interaction on the site activity of Mg-Al-Ox supported Co catalyst for CO2 reforming of CH4
Journal of CO2 Utilization ( IF 7.7 ) Pub Date : 2019-12-23 , DOI: 10.1016/j.jcou.2019.12.006
Wahab O. Alabi , Kazeem O. Sulaiman , Hui Wang , Yongfeng Hu , Christian Patzig

The active metal–support interaction, as well as spinel inversion was studied for site formation, properties, activity and site resistance to carbon deposition in dry reforming of methane (DRM) using Al-Ox and Mg-Al-Ox supported Ni and Co monometallic catalysts. A change in support from Al-Ox to Mg-Al-Ox led to transformation of hysteresis loop from H2 to H4 as revealed by the N2 adsorption results, while additional MgO phase was observed from the XRD results of the catalysts. Phase quantification of the XRD showed a reduction from 100% to 45% spinel with the introduction of Mg in the support. Al and Mg K-edge XANES results revealed changes in the co-ordination number (CN) of Mg and Al inside the support, leading to spinel inversion, which ultimately affected the distribution of Ni and Co, as well as site formation on the support system. STEM EDX revealed different interaction/distribution of active metals on the support system. Co showed a uniform distribution, while Ni showed a heterogeneous distribution in addition to the isolated NiO formed on the surface of the support. The K-edge XANES results showed that more Ni sites were generated than Co sites during reduction, but Co sites showed better conversion rate for CO2, CH4, in DRM, and resistance to deactivation, which was also confirmed by the calculated TOF. This improved performance of Co sites was attributed to the better basicity per active site generated from its interaction with MgO (from the support) as compared to the Ni sites.



中文翻译:

尖晶石转化和金属-载体相互作用对Mg-Al-Ox负载的Co催化剂对CO 4重整CH 4的位点活性的影响

研究了使用Al-O x和Mg-Al-O x负载的Ni和Ni进行甲烷干重整时,活性金属-载体相互作用以及尖晶石反型的位点形成,性质,活性和位点对碳沉积的抵抗性(DRM)。钴单金属催化剂。N 2揭示了从Al-O x到Mg-Al-O x的支持率变化导致磁滞回线从H2转变为H4吸附结果,而从催化剂的XRD结果观察到另外的MgO相。XRD的相定量表明,在载体中引入Mg后,尖晶石的含量从100%降至45%。Al和Mg的K-edge XANES结果揭示了载体内部Mg和Al的配位数(CN)发生变化,导致尖晶石反转,最终影响了Ni和Co的分布以及载体上的位点形成系统。STEM EDX显示了活性金属在载体系统上的不同相互作用/分布。Co显示出均匀的分布,而Ni除了在载体表面上形成的分离的NiO之外,还显示出不均匀的分布。K-edge XANES结果表明,还原过程中生成的Ni站点比Co站点多,但Co站点显示出更好的CO转化率。图2中的CH 4处于DRM中,并且具有抗失活性,这也通过计算的TOF得到了证实。Co位点性能的提高归因于与Ni位点相比,其与MgO(来自载体)的相互作用产生的每个活性位点具有更好的碱性。

更新日期:2019-12-26
down
wechat
bug