首页|Insight into the Role and Evidence of Oxygen Vacancies in Porous Single-Crystalline Oxide to Enhance Catalytic Activity and Durability

Insight into the Role and Evidence of Oxygen Vacancies in Porous Single-Crystalline Oxide to Enhance Catalytic Activity and Durability

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Introducing and stabilizing oxygen vacancies in oxide catalysts is considered to be a promising strategy for improving catalytic activity and durability.Herein,we quantitatively create oxygen vacancies in the lattice of porous single-crystalline β-Ga2O3 monoliths by reduction treatments and stabilize them through the long-range ordering of crystal lattice to enhance catalytic activity and durability.The combination analysis of time-of-flight neutron powder diffraction and extended x-ray absorption fine structure discloses that the preferential generation of oxygen vacancy tends to occur at the site of tetrahedral coordination oxygen ions(OⅢ sites),which contributes to the formation of unsaturated Ga-O coordination in the monoclinic phase.The oxygen vacancies are randomly distributed in lattice even though some of them are present in the form of domain defect in the PSC Ga2O3 monoliths after the reduction treatment.The number of oxygen vacancies in the reduced monoliths gives 2.32 x 1013,2.87 x 1013,and 3.45 x 1013 mg-1 for the Ga2O2.952,Ga2O2.895,and Ga2O2.880,respectively.We therefore demonstrate the exceptionally high C2H4 selectivity of~100%at the C2H6 conversion of~37%for nonoxidative dehydrogenation of C2H6 to C2H4.We further demonstrate the excellent durability even at 620 ℃ for 240 h of continuous operation.

Lingting Ye、Jiaming Ma、Jie Zhang、Wen Yin、Yuanguang Xia、Kui Xie

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Key Laboratory of Optoelectronic Materials Chemistry and Physics,Fujian Institute of Research on the Structure of Matter,Chinese Academy of Sciences,Fuzhou,Fujian 350002,China

Fujian Science& Technology Innovation Laboratory for Optoelectronic Information of China,Fuzhou,Fujian 350108,China

Advanced Energy Science and Technology Guangdong Laboratory,29 Sanxin North Road,Huizhou,Guangdong 116023,China

Spallation Neutron Source Science Center,Dongguan,Guangdong 523803,China

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Natural Science Foundation of ChinaNatural Science Foundation of ChinaNatural Science Foundation of ChinaNatural Science Foundation of ChinaNatural Science Foundation of ChinaYouth Innovation Promotion of Chinese Academy of SciencesNatural Science Foundation of Fujian ProvinceNatural Science Foundation of Fujian Province

223255062237914722002167221012822227-914220233182020J050822020J01113

2024

研究(英文)

研究(英文)

CSTPCD
ISSN:
年,卷(期):2024.2024(2)
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