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Effects of extrinsic defects originating from the interfacial reaction of CeO2-x-nickel silicate on catalytic performance in methane dry reforming
Applied Catalysis B: Environment and Energy ( IF 20.2 ) Pub Date : 2020-06-25 , DOI: 10.1016/j.apcatb.2020.119278
Dan Guo , Yao Lu , Yongzhe Ruan , Yifan Zhao , Yujun Zhao , Shengping Wang , Xinbin Ma

Dry reforming of methane is a promising process to convert two greenhouse gases into syngas. Calcinated nickel silicate nanotubes (C-NSNT) as well as CeO2-x interface-confined and nickel silicate nanotubes (NSNT)-derived Ni catalysts, which are marked as λCeO2-x-NSNT (λ = 0.5, 1, 1.5 and 2.25), is prepared and evaluated in dry reforming of methane. Compared with C-NSNT, the λCeO2-x-NSNT samples exhibit improved catalytic performance in dry reforming of methane, which is closely related to Ni-CeSiO2-x interface along with extrinsic defects from the interfacial reaction between CeO2 and NSNT during the reduction process. Extrinsic defects can generate oxygen vacancies that can be accompanied by Ce3+ species. The enhancement of catalytic activity is ascribed to confined effects of extrinsic defects at contact interface of Ni-CeSiO2-x and electronic effects of CeO2-x. Furthermore, Ni-CeSiO2-x interface with rich extrinsic defects can promote the adsorption and activation of CO2 as electron donor on reduced λCeO2-x-NSNT catalysts, which is fast dissociated into CO* and O*. Meanwhile, oxygen vacancies can transfer adsorbed O* species to Ni active sites to promote the carbon gasification reaction, which is responsible for the enhancement of catalytic stability in methane dry reforming for λCeO2-x-NSNT catalysts. 1.5CeO2-x-NSNT sample with more extrinsic defects has particular higher catalytic stability due to the improvement of anti-coking.



中文翻译:

CeO 2-x-硅酸镍界面反应产生的外在缺陷对甲烷干重整催化性能的影响

甲烷的干重整是将两种温室气体转化为合成气的有前途的过程。煅烧的硅酸镍纳米管(C-NSNT)以及CeO 2-x界面受限的和硅酸镍纳米管(NSNT)衍生的Ni催化剂,标记为λCeO2 -x -NSNT(λ= 0.5、1、1.5和(2.25),并在甲烷干重整中进行评估。与C-NSNT相比,λCeO2 -x -NSNT样品在甲烷干重整中表现出改善的催化性能,这与Ni-CeSiO 2-x界面以及CeO 2与NSNT界面反应期间的外在缺陷密切相关。减少过程。外在缺陷会产生氧空位,可能伴随铈3+种。催化活性的提高归因于Ni-CeSiO 2-x接触界面处的外在缺陷的局限作用和CeO 2-x的电子作用。此外,具有丰富的外在缺陷的Ni-CeSiO 2-x界面可以促进还原的λCeO2 -x -NSNT催化剂上作为电子供体的CO 2的吸附和活化,该催化剂迅速分解为CO *和O *。同时,氧空位可以将吸附的O *物种转移到Ni活性位点以促进碳气化反应,这有助于提高λCeO2 -x -NSNT催化剂在甲烷干重整中的催化稳定性。1.5CeO 2-x具有更多非本征缺陷的-NSNT样品由于抗焦化的改进而具有特别高的催化稳定性。

更新日期:2020-06-25
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