In2O3 Nanocrystals for CO2 Fixation: Atomic-Level Insight into the Role of Grain Boundaries
Lirong Wang,
Jinyan Cai,
Yangcenzi Xie,
Jiasheng Guo,
Lingxiao Xu,
Shuyi Yu,
Xusheng Zheng,
Jian Ye,
Junfa Zhu,
Leijie Zhang,
Shuquan Liang,
Liangbing Wang
Affiliations
Lirong Wang
School 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
Jinyan Cai
National Synchrotron Radiation Laboratory, University of Science and Technology of China, Hefei, Anhui 230029, P. R. China
Yangcenzi Xie
School 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
Jiasheng Guo
School 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
Lingxiao Xu
School 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
Shuyi Yu
School 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
Xusheng Zheng
National Synchrotron Radiation Laboratory, University of Science and Technology of China, Hefei, Anhui 230029, P. R. China; Corresponding author
Jian Ye
National Synchrotron Radiation Laboratory, University of Science and Technology of China, Hefei, Anhui 230029, P. R. China
Junfa Zhu
National Synchrotron Radiation Laboratory, University of Science and Technology of China, Hefei, Anhui 230029, P. R. China
Leijie Zhang
National Synchrotron Radiation Laboratory, University of Science and Technology of China, Hefei, Anhui 230029, P. R. China
Shuquan Liang
School 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 author
Liangbing Wang
School 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 author
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
