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通过中子粉末衍射监测PrBaFeCoO层状钙钛矿上Co-Fe合金纳米颗粒的脱溶及其对甲烷干重整的催化作用。

Exsolution of Co-Fe Alloy Nanoparticles on the PrBaFeCoO Layered Perovskite Monitored by Neutron Powder Diffraction and Catalytic Effect on Dry Reforming of Methane.

作者信息

Managutti Praveen B, Yu Haoran, Hernandez Olivier, Prestipino Carmelo, Dorcet Vincent, Wang Haiqian, Hansen Thomas C, Bahout Mona

机构信息

University of Rennes, CNRS, ISCR (Institut des Sciences Chimiques de Rennes)─UMR 6226, F-35000 Rennes, France.

Chemical Crystallography Laboratory, Khalifa University of Science and Technology, Abu Dhabi, P.O. Box 127788, United Arab Emirates.

出版信息

ACS Appl Mater Interfaces. 2023 May 17;15(19):23040-23050. doi: 10.1021/acsami.2c22239. Epub 2023 Apr 11.

Abstract

Reversible exsolution and dissolution of metal nanoparticles (NPs) in complex oxides have been investigated as an efficient strategy to improve the performance and durability of the catalysts for thermal and electrochemical energy conversion. Here, in situ exsolution of Co-Fe alloy NPs from the layered perovskite PrBaFeCoO (PBFC) and their dissolution back into the oxide host have been monitored for the first time by in situ neutron powder diffraction and confirmed by X-ray diffraction and electron microscopy. Catalytic tests for dry reforming of methane showed stable operation over ∼100 h at 800 °C with negligible carbon deposition (<0.3 mg/g h). The CO and CH conversions are among the highest achieved by layered double perovskites. The cyclability of the PBFC catalyst and the potential to improve the catalytic activity by adjusting the composition, size, and the NP distribution would pave the way for highly efficient energy conversion applications.

摘要

金属纳米颗粒(NPs)在复合氧化物中的可逆析出和溶解已被研究作为一种提高热和电化学能量转换催化剂性能和耐久性的有效策略。在此,首次通过原位中子粉末衍射监测了层状钙钛矿PrBaFeCoO(PBFC)中Co-Fe合金纳米颗粒的原位析出及其重新溶解回氧化物主体,并通过X射线衍射和电子显微镜进行了确认。甲烷干重整的催化测试表明,在800°C下稳定运行约100小时,碳沉积可忽略不计(<0.3毫克/克·小时)。CO和CH转化率是层状双钙钛矿所达到的最高转化率之一。PBFC催化剂的循环性以及通过调整组成、尺寸和纳米颗粒分布来提高催化活性的潜力将为高效能量转换应用铺平道路。

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