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Title: Mechanochemical Nonhydrolytic Sol–Gel-Strategy for the Production of Mesoporous Multimetallic Oxides

Abstract

Mesoporous metal oxides with wide pore size, high surface area, and uniform porous structures have demonstrated excellent advantages in various fields. Yet, the state-of-art synthesis approaches are dominated by wet chemistry, accompanied by use of excessive solvent, and the requirement of time-consuming drying process. Herein, we report a mechanochemical solid-state route to synthesize mesoporous Al 2O 3 (meso-Al 2O 3) via aluminum isopropoxide-copolymers assembly. The obtained meso-Al 2O 3 reflects a record high surface area (~644 m 2 g -1) and narrow pore size distribution (centered at ~5 nm). Moreover, a mechanochemical nonhydrolytic sol-gel strategy is introduced to fabricate mesoporous transition metal (Cu, Co, Mn, Fe, Mg, Ni)-aluminum binary oxide by using anhydrous metal chlorides and aluminum isopropoxide interplay. More importantly, four or five metals-aluminum oxide complexes with abundant mesopores and single cubic crystalline phase known as high-entropy ceramics are produced. To the best of our knowledge, mesoporous high-entropy metal oxides have not been prepared before, because the high crystallization temperature would make mesopores collapse. Furthermore, this high-entropy property endows (CuNiFeCoMg)O x-Al 2O 3 with superior SO2-resisting performance (1000 ppm of SO 2 in N 2 at 280 °C) in the catalytic oxidation of CO compared to single CuO-Al 2Omore » 3.« less

Authors:
 [1];  [2]; ORCiD logo [3]; ORCiD logo [4]; ORCiD logo [5];  [4];  [4];  [4];  [6];  [4]; ORCiD logo [7]; ORCiD logo [4]; ORCiD logo [7]; ORCiD logo [7]; ORCiD logo [6]; ORCiD logo [8]
  1. Zhejiang Univ., Hangzhou (China); Oak Ridge National Lab., Oak Ridge, TN (United States); Univ. of Tennessee, Knoxville, TN (United States)
  2. Brookhaven National Lab. (BNL), Upton, NY (United States)
  3. Northwestern Univ., Evanston, IL (United States)
  4. Univ. of Tennessee, Knoxville, TN (United States)
  5. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
  6. Shanghai Jiao Tong Univ. (China)
  7. Zhejiang Univ., Hangzhou (China)
  8. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States); Univ. of Tennessee, Knoxville, TN (United States)
Publication Date:
Research Org.:
Brookhaven National Lab. (BNL), Upton, NY (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22). Chemical Sciences, Geosciences & Biosciences Division; USDOE Office of Energy Efficiency and Renewable Energy (EERE), Vehicle Technologies Office (EE-3V); National Natural Science Foundation of China (NNSFC)
OSTI Identifier:
1561254
Report Number(s):
BNL-212070-2019-JAAM
Journal ID: ISSN 0897-4756
Grant/Contract Number:  
SC0012704
Resource Type:
Journal Article: Accepted Manuscript
Journal Name:
Chemistry of Materials
Additional Journal Information:
Journal Volume: 31; Journal Issue: 15; Journal ID: ISSN 0897-4756
Publisher:
American Chemical Society (ACS)
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE

Citation Formats

Zhang, Zihao, Yang, Shize, Hu, Xiaobing, Xu, Haidi, Peng, Honggen, Liu, Miaomiao, Thapaliya, Bishnu Prasad, Jie, Kecheng, Zhao, Jiahua, Liu, Jixing, Chen, Hao, Leng, Yan, Lu, Xiuyang, Fu, Jie, Zhang, Pengfei, and Dai, Sheng. Mechanochemical Nonhydrolytic Sol–Gel-Strategy for the Production of Mesoporous Multimetallic Oxides. United States: N. p., 2019. Web. doi:10.1021/acs.chemmater.9b01244.
Zhang, Zihao, Yang, Shize, Hu, Xiaobing, Xu, Haidi, Peng, Honggen, Liu, Miaomiao, Thapaliya, Bishnu Prasad, Jie, Kecheng, Zhao, Jiahua, Liu, Jixing, Chen, Hao, Leng, Yan, Lu, Xiuyang, Fu, Jie, Zhang, Pengfei, & Dai, Sheng. Mechanochemical Nonhydrolytic Sol–Gel-Strategy for the Production of Mesoporous Multimetallic Oxides. United States. doi:10.1021/acs.chemmater.9b01244.
Zhang, Zihao, Yang, Shize, Hu, Xiaobing, Xu, Haidi, Peng, Honggen, Liu, Miaomiao, Thapaliya, Bishnu Prasad, Jie, Kecheng, Zhao, Jiahua, Liu, Jixing, Chen, Hao, Leng, Yan, Lu, Xiuyang, Fu, Jie, Zhang, Pengfei, and Dai, Sheng. Mon . "Mechanochemical Nonhydrolytic Sol–Gel-Strategy for the Production of Mesoporous Multimetallic Oxides". United States. doi:10.1021/acs.chemmater.9b01244. https://www.osti.gov/servlets/purl/1561254.
@article{osti_1561254,
title = {Mechanochemical Nonhydrolytic Sol–Gel-Strategy for the Production of Mesoporous Multimetallic Oxides},
author = {Zhang, Zihao and Yang, Shize and Hu, Xiaobing and Xu, Haidi and Peng, Honggen and Liu, Miaomiao and Thapaliya, Bishnu Prasad and Jie, Kecheng and Zhao, Jiahua and Liu, Jixing and Chen, Hao and Leng, Yan and Lu, Xiuyang and Fu, Jie and Zhang, Pengfei and Dai, Sheng},
abstractNote = {Mesoporous metal oxides with wide pore size, high surface area, and uniform porous structures have demonstrated excellent advantages in various fields. Yet, the state-of-art synthesis approaches are dominated by wet chemistry, accompanied by use of excessive solvent, and the requirement of time-consuming drying process. Herein, we report a mechanochemical solid-state route to synthesize mesoporous Al2O3 (meso-Al2O3) via aluminum isopropoxide-copolymers assembly. The obtained meso-Al2O3 reflects a record high surface area (~644 m2 g-1) and narrow pore size distribution (centered at ~5 nm). Moreover, a mechanochemical nonhydrolytic sol-gel strategy is introduced to fabricate mesoporous transition metal (Cu, Co, Mn, Fe, Mg, Ni)-aluminum binary oxide by using anhydrous metal chlorides and aluminum isopropoxide interplay. More importantly, four or five metals-aluminum oxide complexes with abundant mesopores and single cubic crystalline phase known as high-entropy ceramics are produced. To the best of our knowledge, mesoporous high-entropy metal oxides have not been prepared before, because the high crystallization temperature would make mesopores collapse. Furthermore, this high-entropy property endows (CuNiFeCoMg)Ox-Al2O3 with superior SO2-resisting performance (1000 ppm of SO2 in N2 at 280 °C) in the catalytic oxidation of CO compared to single CuO-Al2O3.},
doi = {10.1021/acs.chemmater.9b01244},
journal = {Chemistry of Materials},
issn = {0897-4756},
number = 15,
volume = 31,
place = {United States},
year = {2019},
month = {7}
}

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