促进并稳定CO甲烷化的钯铁金属间纳米晶体中的表面铁物种
Surface Iron Species in Palladium-Iron Intermetallic Nanocrystals that Promote and Stabilize CO Methanation.
作者信息
Luo Laihao, Wang Menglin, Cui Yi, Chen Ziyuan, Wu Jiaxin, Cao Yulu, Luo Jie, Dai Yizhou, Li Wei-Xue, Bao Jun, Zeng Jie
机构信息
Hefei National Laboratory for Physical Sciences at the Microscale, National Synchrotron Radiation Laboratory, CAS Key Laboratory of Strongly-Coupled Quantum Matter Physics, Key Laboratory of Surface and Interface Chemistry and Energy Catalysis of Anhui Higher Education Institutes, Department of Chemical Physics, University of Science and Technology of China, Hefei, Anhui, 230026, P. R. China.
出版信息
Angew Chem Int Ed Engl. 2020 Aug 17;59(34):14434-14442. doi: 10.1002/anie.201916032. Epub 2020 May 11.
It is of pivotal importance to develop efficient catalysts and investigate the intrinsic mechanism for CO methanation. Now, it is reported that PdFe intermetallic nanocrystals afforded high activity and stability for CO methanation. The mass activity of fct-PdFe nanocrystals reached 5.3 mmol g h , under 1 bar (CO :H =1:4) at 180 °C, being 6.6, 1.6, 3.3, and 5.3 times as high as that of fcc-PdFe nanocrystals, Ru/C, Ni/C, and Pd/C, respectively. After 20 rounds of successive reaction, 98 % of the original activity was retained for PdFe intermetallic nanocrystals. Further mechanistic studies revealed that PdFe intermetallic nanocrystals enabled the maintenance of metallic Fe species via a reversible oxidation-reduction process in CO methanation. The metallic Fe in PdFe intermetallic nanocrystals induced the direct conversion of CO into CO* as the intermediate, contributing to the enhanced activity.
开发高效催化剂并研究CO甲烷化的内在机制至关重要。现在，有报道称PdFe金属间纳米晶体对CO甲烷化具有高活性和稳定性。在180°C、1 bar（CO:H = 1:4）条件下，fct-PdFe纳米晶体的质量活性达到5.3 mmol g h，分别是fcc-PdFe纳米晶体、Ru/C、Ni/C和Pd/C的6.6倍、1.6倍、3.3倍和5.3倍。经过20轮连续反应后，PdFe金属间纳米晶体保留了98%的原始活性。进一步的机理研究表明，PdFe金属间纳米晶体在CO甲烷化过程中通过可逆的氧化还原过程使金属Fe物种得以维持。PdFe金属间纳米晶体中的金属Fe诱导CO直接转化为中间体CO*，从而提高了活性。
Zotero 插件