In2O3 Nanocrystals for CO2 Fixation: Atomic-Level Insight into the Role of Grain Boundaries
Lirong WangJinyan CaiYangcenzi XieJiasheng GuoLingxiao XuShuyi YuXusheng ZhengJian YeJunfa ZhuLeijie ZhangShuquan LiangLiangbing Wang
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N-functionalization of amines with CO2 and H2 is one of the most important processes to make use of CO2. Although noble metal-based catalysts with remarkable performance have been widely used in this process, developing efficient non-noble-metal-based catalysts remains a grand challenge. Herein, we report In2O3 nanocrystals with high density of grain boundaries (HGB-In2O3), which show excellent activity toward methylation of amines. Impressively, HGB-In2O3 achieved the optimal yield of 82.7% for N,N-dimethylaniline with a mass activity of 21.2 mmol·g−1h−1 in methylation of N-methylaniline, comparable to noble-metal-based catalysts. As a bonus, HGB-In2O3 held noticeable stability, remarkable selectivity, and comprehensive applicability. Further mechanistic studies revealed that the presence of high density of grain boundaries not only facilitated the adsorption and activation of CO2 to generate CH3OH as the intermediate but also enhanced the activation of N-H bond in amines, contributing to the attractive activity of HGB-In2O3 toward methylation of amines.Elongated tetrahexahedral Au nanocrystals have been grown in high yields using a seed-mediated growth method. Morphological and structural characterizations show that these Au nanocrystals are single-crystalline and enclosed by 24 high-index {037} facets. They are more electrochemically active than octahedral Au nanocrystals that are enclosed by 8 low-index {111} facets. To date, there have been only a few reports of metal nanocrystals that are enclosed exclusively by high-index facets, including trisoctahedral Au nanocrystals enclosed by 24 {122} facets and tetrahexahedral Pt nanocrystals enclosed by 24 {037} facets. Our tetrahexahedral Au nanocrystals will be an important addition to the family of metal nanocrystals that are enclosed exclusively by high-index facets and will also be useful for fundamental catalytic studies on metal nanocrystals.
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