In2O3 Nanocrystals for CO2 Fixation: Atomic-Level Insight into the Role of Grain Boundaries
Summary: 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. He...
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doaj-bc882f5c322845eca6e7b2d0412260c82020-11-25T01:09:28ZengElsevieriScience2589-00422019-06-0116390398In2O3 Nanocrystals for CO2 Fixation: Atomic-Level Insight into the Role of Grain BoundariesLirong Wang0Jinyan Cai1Yangcenzi Xie2Jiasheng Guo3Lingxiao Xu4Shuyi Yu5Xusheng Zheng6Jian Ye7Junfa Zhu8Leijie Zhang9Shuquan Liang10Liangbing Wang11School of Materials Science and Engineering, Key Laboratory of Nonferrous Metal Materials Science and Engineering, Ministry of Education, Central South University, Changsha, Hunan 410083, P. R. ChinaNational Synchrotron Radiation Laboratory, University of Science and Technology of China, Hefei, Anhui 230029, P. R. ChinaSchool of Materials Science and Engineering, Key Laboratory of Nonferrous Metal Materials Science and Engineering, Ministry of Education, Central South University, Changsha, Hunan 410083, P. R. ChinaSchool of Materials Science and Engineering, Key Laboratory of Nonferrous Metal Materials Science and Engineering, Ministry of Education, Central South University, Changsha, Hunan 410083, P. R. ChinaSchool of Materials Science and Engineering, Key Laboratory of Nonferrous Metal Materials Science and Engineering, Ministry of Education, Central South University, Changsha, Hunan 410083, P. R. ChinaSchool of Materials Science and Engineering, Key Laboratory of Nonferrous Metal Materials Science and Engineering, Ministry of Education, Central South University, Changsha, Hunan 410083, P. R. ChinaNational Synchrotron Radiation Laboratory, University of Science and Technology of China, Hefei, Anhui 230029, P. R. China; Corresponding authorNational Synchrotron Radiation Laboratory, University of Science and Technology of China, Hefei, Anhui 230029, P. R. ChinaNational Synchrotron Radiation Laboratory, University of Science and Technology of China, Hefei, Anhui 230029, P. R. ChinaNational Synchrotron Radiation Laboratory, University of Science and Technology of China, Hefei, Anhui 230029, P. R. ChinaSchool of Materials Science and Engineering, Key Laboratory of Nonferrous Metal Materials Science and Engineering, Ministry of Education, Central South University, Changsha, Hunan 410083, P. R. China; Corresponding authorSchool of Materials Science and Engineering, Key Laboratory of Nonferrous Metal Materials Science and Engineering, Ministry of Education, Central South University, Changsha, Hunan 410083, P. R. China; Corresponding authorSummary: 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. : Catalysis; Materials Characterization Techniques; Nanomaterials Subject Areas: Catalysis, Materials Characterization Techniques, Nanomaterialshttp://www.sciencedirect.com/science/article/pii/S2589004219301877 |
collection |
DOAJ |
language |
English |
format |
Article |
sources |
DOAJ |
author |
Lirong Wang Jinyan Cai Yangcenzi Xie Jiasheng Guo Lingxiao Xu Shuyi Yu Xusheng Zheng Jian Ye Junfa Zhu Leijie Zhang Shuquan Liang Liangbing Wang |
spellingShingle |
Lirong Wang Jinyan Cai Yangcenzi Xie Jiasheng Guo Lingxiao Xu Shuyi Yu Xusheng Zheng Jian Ye Junfa Zhu Leijie Zhang Shuquan Liang Liangbing Wang In2O3 Nanocrystals for CO2 Fixation: Atomic-Level Insight into the Role of Grain Boundaries iScience |
author_facet |
Lirong Wang Jinyan Cai Yangcenzi Xie Jiasheng Guo Lingxiao Xu Shuyi Yu Xusheng Zheng Jian Ye Junfa Zhu Leijie Zhang Shuquan Liang Liangbing Wang |
author_sort |
Lirong Wang |
title |
In2O3 Nanocrystals for CO2 Fixation: Atomic-Level Insight into the Role of Grain Boundaries |
title_short |
In2O3 Nanocrystals for CO2 Fixation: Atomic-Level Insight into the Role of Grain Boundaries |
title_full |
In2O3 Nanocrystals for CO2 Fixation: Atomic-Level Insight into the Role of Grain Boundaries |
title_fullStr |
In2O3 Nanocrystals for CO2 Fixation: Atomic-Level Insight into the Role of Grain Boundaries |
title_full_unstemmed |
In2O3 Nanocrystals for CO2 Fixation: Atomic-Level Insight into the Role of Grain Boundaries |
title_sort |
in2o3 nanocrystals for co2 fixation: atomic-level insight into the role of grain boundaries |
publisher |
Elsevier |
series |
iScience |
issn |
2589-0042 |
publishDate |
2019-06-01 |
description |
Summary: 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. : Catalysis; Materials Characterization Techniques; Nanomaterials Subject Areas: Catalysis, Materials Characterization Techniques, Nanomaterials |
url |
http://www.sciencedirect.com/science/article/pii/S2589004219301877 |
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