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Ni@SiO2核壳型催化剂上孔调控对甲烷干重整催化性能的影响OA北大核心CSTPCD

Effects of pore modulation on catalytic performance of Ni@SiO2 core-shell catalysts for methane dry reforming

中文摘要英文摘要

采用油包水微乳液法制备了Ni@SiO2核壳型催化剂,并添加梯度物质的量的十六烷基三甲基溴化铵(C16TAB)进行后处理,制备了具有不同多孔结构的Ni@SiO2-xC16系列催化剂.结合N2吸/脱附、XRD、TEM、H2-TPR、XPS和Raman光谱等表征方法对催化剂进行了分析,探究了Ni@SiO2-xC16外壳上孔结构对催化剂活性、稳定性以及抗积炭性能的影响.结果表明,Ni@SiO2-xC16具有更大的比表面积和更丰富的孔结构,有助于提高Ni颗粒的分散度和限制Ni颗粒尺寸小于5 nm,并强化Ni颗粒与载体的相互作用.在50 h的稳定性测试中,Ni@SiO2的初始CH4转化率低(68.5%)且稳定性弱,而经过C16TAB后处理的Ni@SiO2-2C16和Ni@SiO2-3C16则具有高初始CH4转化率(均约84.1%)及高稳定性,产物中n(H2)/n(CO)超过0.97,且几乎没有发生失活.经进一步研究发现,Ni@SiO2-xC16中碳物种的类型发生改变,由大量难以消除的石墨碳转化为少量容易清除的无序碳,因此,Ni@SiO2-xC16的抗积炭与抗烧结性能得到了提升.

Ni@SiO2 core-shell catalysts were prepared by oil-in-water microemulsion method.Adding a gradient amount of substance of cetyltrimethylammonium bromide(C16TAB)for post-treatments,Ni@SiO2-x C16 catalysts with distinct porous structures were prepared.By characterization techniques including N2 adsorption/desorption,XRD,TEM,H2-TPR,XPS and Raman spectroscopy,the catalysts were analyzed,and the effects of pore structures on Ni@SiO2-x C16 shell on the activity,stability and anti-coking performance of catalysts were investigated.The results indicate that Ni@SiO2-x C16 has a larger specific surface area and more abundant pore structures,which help to improve the dispersion of Ni particles,limit the size of Ni particles to less than 5 nm and strengthen the interaction between Ni particles and supports.In a 50 h stability test,Ni@SiO2 has a low initial CH4 conversion rate(68.5%)and weak stability,but after C16TAB post-treatment,Ni@SiO2-2C16 and Ni@SiO2-3C16 show high initial CH4 conversion rates(both about 84.1%)and high stability,and n(H2)/n(CO)in products exceeds 0.97 and almost no deactivation occurred.After further study,it is found that the type of carbon species in Ni@SiO2-xC16 changes from a large amount of graphite carbon that is difficult to eliminate to a small amount of disordered carbon that is easy to remove.Therefore,the performances of anti-coking and anti-sintering of Ni@SiO2-xC16 are improved.

冯文磊;杨文师;陈健勇;王超;陈颖;罗向龙

广东工业大学 材料与能源学院,广东 广州 510006

化学工程

甲烷干重整Ni@SiO2多孔结构抗积炭性能

methane dry reformingNi@SiO2porous structuresanti-coking performance

《低碳化学与化工》 2024 (006)

9-16,44 / 9

广东省基础与应用基础研究基金自然科学基金面上项目(2022A1515012035).

10.12434/j.issn.2097-2547.20230378

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