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

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

doi:10.1021/acs.chemmater.9b01244

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

Journal Article · Mon Jul 01 00:00:00 EDT 2019 · Chemistry of Materials

DOI:https://doi.org/10.1021/acs.chemmater.9b01244· OSTI ID:1561254

Zhang, Zihao ^[1]; Yang, Shize ^[2]; ^[3]; ^[4]; ^[5]; Liu, Miaomiao ^[4]; Thapaliya, Bishnu Prasad ^[4]; Jie, Kecheng ^[4]; Zhao, Jiahua ^[6]; Liu, Jixing ^[4]; ^[7]; ^[4]; ^[7]; ^[7]; ^[6]; ^[8]

Zhejiang Univ., Hangzhou (China); Oak Ridge National Lab., Oak Ridge, TN (United States); Univ. of Tennessee, Knoxville, TN (United States)
Brookhaven National Lab. (BNL), Upton, NY (United States)
Northwestern Univ., Evanston, IL (United States)
Univ. of Tennessee, Knoxville, TN (United States)
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
Shanghai Jiao Tong Univ. (China)
Zhejiang Univ., Hangzhou (China)
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States); Univ. of Tennessee, Knoxville, TN (United States)

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)O_x-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.

View Accepted Manuscript (DOE)

Research Organization:: Brookhaven National Laboratory (BNL), Upton, NY (United States)

Sponsoring Organization:: 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)

Grant/Contract Number:: SC0012704

OSTI ID:: 1561254

Report Number(s):: BNL--212070-2019-JAAM

Journal Information:: Chemistry of Materials, Journal Name: Chemistry of Materials Journal Issue: 15 Vol. 31; ISSN 0897-4756

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

References (61)

Weakly Ferromagnetic Ordered Mesoporous Co ₃ O ₄ Synthesized by Nanocasting from Vinyl-Functionalized Cubic Ia 3 d Mesoporous Silica Wang, Y.; Yang, C. -M.; Schmidt, W. Advanced Materials, Vol. 17, Issue 1 https://doi.org/10.1002/adma.200400777	journal	November 2004
Nanoarchitectures for Mesoporous Metals Malgras, Victor; Ataee-Esfahani, Hamed; Wang, Hongjing Advanced Materials, Vol. 28, Issue 6 https://doi.org/10.1002/adma.201502593	journal	October 2015
Solvent-Free Self-Assembly to the Synthesis of Nitrogen-Doped Ordered Mesoporous Polymers for Highly Selective Capture and Conversion of CO ₂ Liu, Fujian; Huang, Kuan; Wu, Qin Advanced Materials, Vol. 29, Issue 27 https://doi.org/10.1002/adma.201700445	journal	May 2017
Chemical solvent in chemical solvent: A class of hybrid materials for effective capture of CO ₂ Chen, Feng-Feng; Huang, Kuan; Fan, Jie-Ping AIChE Journal, Vol. 64, Issue 2 https://doi.org/10.1002/aic.15952	journal	September 2017
Synthesis of Hexagonally Packed Mesoporous TiO₂ by a Modified Sol–Gel Method Antonelli, David M.; Ying, Jackie Y. Angewandte Chemie International Edition in English, Vol. 34, Issue 18, p. 2014-2017 https://doi.org/10.1002/anie.199520141	journal	October 1995
A General Approach to Mesoporous Metal Oxide Microspheres Loaded with Noble Metal Nanoparticles Jin, Zhao; Xiao, Manda; Bao, Zhihong Angewandte Chemie International Edition, Vol. 51, Issue 26 https://doi.org/10.1002/anie.201106948	journal	April 2012
Solvent-Free Synthesis of Silicoaluminophosphate Zeolites Jin, Yinying; Sun, Qi; Qi, Guodong Angewandte Chemie International Edition, Vol. 52, Issue 35 https://doi.org/10.1002/anie.201302672	journal	July 2013
Highly Ordered Mesoporous Tungsten Oxides with a Large Pore Size and Crystalline Framework for H ₂ S Sensing Li, Yuhui; Luo, Wei; Qin, Nan Angewandte Chemie International Edition, Vol. 53, Issue 34 https://doi.org/10.1002/anie.201403817	journal	July 2014
Controllable Synthesis of Mesoporous Peapod-like Co ₃ O ₄ @Carbon Nanotube Arrays for High-Performance Lithium-Ion Batteries Gu, Dong; Li, Wei; Wang, Fei Angewandte Chemie International Edition, Vol. 54, Issue 24 https://doi.org/10.1002/anie.201501475	journal	April 2015
Surface-Casting Synthesis of Mesoporous Zirconia with a CMK-5-Like Structure and High Surface Area Gu, Dong; Schmidt, Wolfgang; Pichler, Christian M. Angewandte Chemie International Edition, Vol. 56, Issue 37 https://doi.org/10.1002/anie.201705042	journal	July 2017
Magnetic Nanocomposites with Mesoporous Structures: Synthesis and Applications Liu, Jian; Qiao, Shi Zhang; Hu, Qiu Hong Small, Vol. 7, Issue 4 https://doi.org/10.1002/smll.201001402	journal	January 2011
Crystalline mesoporous transition metal oxides: hard-templating synthesis and application in environmental catalysis Zhen, Ma; Zhou, Bei; Ren, Yu Frontiers of Environmental Science & Engineering, Vol. 7, Issue 3 https://doi.org/10.1007/s11783-012-0472-1	journal	December 2012
Solid-state CTAB-assisted synthesis of mesoporous Fe3O4 and Au@Fe3O4 by mechanochemistry Zhao, Jiahua; Shu, Yuan; Zhang, Pengfei Chinese Journal of Catalysis, Vol. 40, Issue 7 https://doi.org/10.1016/S1872-2067(19)63288-2	journal	July 2019
Mesoporous mixed oxide catalysts via non-hydrolytic sol–gel: A review Debecker, Damien P.; Hulea, Vasile; Mutin, P. Hubert Applied Catalysis A: General, Vol. 451 https://doi.org/10.1016/j.apcata.2012.11.002	journal	January 2013
The effect of metal deposition order on the synergistic activity of Au–Cu and Au–Ce metal oxide catalysts for CO oxidation Nikolaev, S. A.; Golubina, E. V.; Krotova, I. N. Applied Catalysis B: Environmental, Vol. 168-169 https://doi.org/10.1016/j.apcatb.2014.12.030	journal	June 2015
One-pot synthesis of ordered mesoporous NiMo-Al 2 O 3 catalysts for dibenzothiophene hydrodesulfurization Liu, Huan; Li, Yanpeng; Yin, Changlong Applied Catalysis B: Environmental, Vol. 198 https://doi.org/10.1016/j.apcatb.2016.06.004	journal	December 2016
Near ambient pressure XPS investigation of the interaction of ethanol with Co/CeO2(111) Óvári, L.; Krick Calderon, S.; Lykhach, Y. Journal of Catalysis, Vol. 307 https://doi.org/10.1016/j.jcat.2013.07.015	journal	November 2013
Highly crystalline poly(heptazine imides) by mechanochemical synthesis for photooxidation of various organic substrates using an intriguing electron acceptor – Elemental sulfur Savateev, Aleksandr; Dontsova, Dariya; Kurpil, Bogdan Journal of Catalysis, Vol. 350 https://doi.org/10.1016/j.jcat.2017.02.029	journal	June 2017
Evaporation-induced self-assembly synthesis of nanostructured alumina-based mixed metal oxides with tailored porosity Gonçalves, Alexandre Amormino S.; Jaroniec, Mietek Journal of Colloid and Interface Science, Vol. 537 https://doi.org/10.1016/j.jcis.2018.11.044	journal	March 2019
Nanocrystalline multicomponent entropy stabilised transition metal oxides Sarkar, Abhishek; Djenadic, Ruzica; Usharani, Nandhini J. Journal of the European Ceramic Society, Vol. 37, Issue 2 https://doi.org/10.1016/j.jeurceramsoc.2016.09.018	journal	February 2017
Support effect on the structure and CO oxidation activity of Cu-Cr mixed oxides over Al2O3 and SiO2 Pantaleo, G.; Liotta, L. F.; Venezia, A. M. Materials Chemistry and Physics, Vol. 114, Issue 2-3 https://doi.org/10.1016/j.matchemphys.2008.10.006	journal	April 2009
One-pot synthesis of mesoporous Cu–γ-Al2O3 as bifunctional catalyst for direct dimethyl ether synthesis Jiang, Heqing; Bongard, Hans; Schmidt, Wolfgang Microporous and Mesoporous Materials, Vol. 164 https://doi.org/10.1016/j.micromeso.2012.08.004	journal	December 2012
In situ XRD, Raman, and TPR studies of CuO/Al2O3 catalysts for CO oxidation Luo, Meng-Fei; Fang, Ping; He, Mai Journal of Molecular Catalysis A: Chemical, Vol. 239, Issue 1-2 https://doi.org/10.1016/j.molcata.2005.06.029	journal	September 2005
Mechanochemical synthesis of metal–organic frameworks Chen, Dong; Zhao, Jiahua; Zhang, Pengfei Polyhedron, Vol. 162 https://doi.org/10.1016/j.poly.2019.01.024	journal	April 2019
One-Pot Synthesis of MeAl ₂ O ₄ (Me = Ni, Co, or Cu) Supported on γ-Al ₂ O ₃ with Ultralarge Mesopores: Enhancing Interfacial Defects in γ-Al ₂ O ₃ To Facilitate the Formation of Spinel Structures at Lower Temperatures Gonçalves, Alexandre A. S.; Costa, Maria J. F.; Zhang, Liping Chemistry of Materials, Vol. 30, Issue 2 https://doi.org/10.1021/acs.chemmater.7b04353	journal	January 2018
Facile Synthesis of Highly Porous Metal Oxides by Mechanochemical Nanocasting Xiao, Weiming; Yang, Shize; Zhang, Pengfei Chemistry of Materials, Vol. 30, Issue 9 https://doi.org/10.1021/acs.chemmater.7b05405	journal	April 2018
In Situ Synthesis of Nitrogen-Enriched Activated Carbons from Procambarus clarkii Shells with Enhanced CO ₂ Adsorption Performance Cai, Weiquan; Zhang, Shoute; Hu, Xin Energy & Fuels, Vol. 32, Issue 9 https://doi.org/10.1021/acs.energyfuels.8b02097	journal	August 2018
One-Pot Synthesis of Mesoporous Ni–Ti–Al Ternary Oxides: Highly Active and Selective Catalysts for Steam Reforming of Ethanol Gonçalves, Alexandre A. S.; Faustino, Patrícia B.; Assaf, José M. ACS Applied Materials & Interfaces, Vol. 9, Issue 7 https://doi.org/10.1021/acsami.6b15507	journal	February 2017
Hard-Templating Pathway To Create Mesoporous Magnesium Oxide Li, Wen-Cui; Lu, An-Hui; Weidenthaler, Claudia Chemistry of Materials, Vol. 16, Issue 26 https://doi.org/10.1021/cm048759n	journal	December 2004
Hierarchically Porous Metal Oxide Monoliths Prepared by the Nanocasting Route Smått, Jan-Henrik; Weidenthaler, Claudia; Rosenholm, Jarl B. Chemistry of Materials, Vol. 18, Issue 6 https://doi.org/10.1021/cm051880p	journal	March 2006
Mechanochemical Synthesis of Metal−Organic Frameworks: A Fast and Facile Approach toward Quantitative Yields and High Specific Surface Areas Klimakow, Maria; Klobes, Peter; Thünemann, Andreas F. Chemistry of Materials, Vol. 22, Issue 18 https://doi.org/10.1021/cm1012119	journal	September 2010
Facile Synthesis of Ordered Mesoporous Alumina and Alumina-Supported Metal Oxides with Tailored Adsorption and Framework Properties Cai, Weiquan; Yu, Jiaguo; Anand, Chokkalingam Chemistry of Materials, Vol. 23, Issue 5 https://doi.org/10.1021/cm102512v	journal	March 2011
Design of SiO ₂ −Al ₂ O ₃ −MoO ₃ Metathesis Catalysts by Nonhydrolytic Sol−Gel Debecker, Damien P.; Bouchmella, Karim; Poleunis, Claude Chemistry of Materials, Vol. 21, Issue 13 https://doi.org/10.1021/cm900490t	journal	July 2009
Synthesis of Very Small TiO ₂ Nanocrystals in a Room-Temperature Ionic Liquid and Their Self-Assembly toward Mesoporous Spherical Aggregates Zhou, Yong; Antonietti, Markus Journal of the American Chemical Society, Vol. 125, Issue 49 https://doi.org/10.1021/ja0380998	journal	December 2003
Facile Synthesis for Ordered Mesoporous γ-Aluminas with High Thermal Stability Yuan, Quan; Yin, An-Xiang; Luo, Chen Journal of the American Chemical Society, Vol. 130, Issue 11 https://doi.org/10.1021/ja0764308	journal	March 2008
Mesoporous Layer-by-Layer Ordered Nanohybrids of Layered Double Hydroxide and Layered Metal Oxide: Highly Active Visible Light Photocatalysts with Improved Chemical Stability Gunjakar, Jayavant L.; Kim, Tae Woo; Kim, Hyo Na Journal of the American Chemical Society, Vol. 133, Issue 38 https://doi.org/10.1021/ja203388r	journal	September 2011
Container Effect in Nanocasting Synthesis of Mesoporous Metal Oxides Sun, Xiaohong; Shi, Yifeng; Zhang, Peng Journal of the American Chemical Society, Vol. 133, Issue 37 https://doi.org/10.1021/ja2060512	journal	September 2011
Ordered Mesoporous Black TiO ₂ as Highly Efficient Hydrogen Evolution Photocatalyst Zhou, Wei; Li, Wei; Wang, Jian-Qiang Journal of the American Chemical Society, Vol. 136, Issue 26 https://doi.org/10.1021/ja504802q	journal	June 2014
Ordered Mesoporous Alumina-Supported Metal Oxides Morris, Stacy M.; Fulvio, Pasquale F.; Jaroniec, Mietek Journal of the American Chemical Society, Vol. 130, Issue 45 https://doi.org/10.1021/ja806429q	journal	November 2008
Mesoporous Co ₃ O ₄ and Au/Co ₃ O ₄ Catalysts for Low-Temperature Oxidation of Trace Ethylene Ma, Chun Yan; Mu, Zhen; Li, Jin Jun Journal of the American Chemical Society, Vol. 132, Issue 8 https://doi.org/10.1021/ja906274t	journal	March 2010
Highly Ordered Mesoporous Cobalt-Containing Oxides: Structure, Catalytic Properties, and Active Sites in Oxidation of Carbon Monoxide Gu, Dong; Jia, Chun-Jiang; Weidenthaler, Claudia Journal of the American Chemical Society, Vol. 137, Issue 35 https://doi.org/10.1021/jacs.5b06336	journal	August 2015
Graphitic Carbon Conformal Coating of Mesoporous TiO ₂ Hollow Spheres for High-Performance Lithium Ion Battery Anodes Liu, Hao; Li, Wei; Shen, Dengke Journal of the American Chemical Society, Vol. 137, Issue 40 https://doi.org/10.1021/jacs.5b08743	journal	September 2015
Mesoporous Tungsten Oxides with Crystalline Framework for Highly Sensitive and Selective Detection of Foodborne Pathogens Zhu, Yongheng; Zhao, Yong; Ma, Junhao Journal of the American Chemical Society, Vol. 139, Issue 30 https://doi.org/10.1021/jacs.7b04221	journal	July 2017
Radical-Facilitated Green Synthesis of Highly Ordered Mesoporous Silica Materials Feng, Guodong; Wang, Jianyu; Boronat, Mercedes Journal of the American Chemical Society, Vol. 140, Issue 14 https://doi.org/10.1021/jacs.8b00093	journal	March 2018
Heterogeneous Uptake of Sulfur Dioxide On Aluminum and Magnesium Oxide Particles Goodman, A. L.; Li, P.; Usher, C. R. The Journal of Physical Chemistry A, Vol. 105, Issue 25 https://doi.org/10.1021/jp004423z	journal	June 2001
Preparation of Porous Aminopropylsilsesquioxane by a Nonhydrolytic Sol−Gel Method in Ionic Liquid Solvent Liu, Yang; Wang, Meijia; Li, Zhiying Langmuir, Vol. 21, Issue 4 https://doi.org/10.1021/la0475829	journal	February 2005
One-Pot Facile Synthesis of Ant-Cave-Structured Metal Oxide–Carbon Microballs by Continuous Process for Use as Anode Materials in Li-Ion Batteries Ko, You Na; Park, Seung Bin; Jung, Kyeong Youl Nano Letters, Vol. 13, Issue 11 https://doi.org/10.1021/nl4030352	journal	October 2013
Generalized syntheses of large-pore mesoporous metal oxides with semicrystalline frameworks Yang, Peidong; Zhao, Dongyuan; Margolese, David I. Nature, Vol. 396, Issue 6707 https://doi.org/10.1038/24132	journal	November 1998
Solid-state synthesis of ordered mesoporous carbon catalysts via a mechanochemical assembly through coordination cross-linking Zhang, Pengfei; Wang, Li; Yang, Shize Nature Communications, Vol. 8, Issue 1 https://doi.org/10.1038/ncomms15020	journal	April 2017
Thermally stable single atom Pt/m-Al2O3 for selective hydrogenation and CO oxidation Zhang, Zailei; Zhu, Yihan; Asakura, Hiroyuki Nature Communications, Vol. 8, Issue 1 https://doi.org/10.1038/ncomms16100	journal	July 2017
Entropy-stabilized oxides Rost, Christina M.; Sachet, Edward; Borman, Trent Nature Communications, Vol. 6, Issue 1 https://doi.org/10.1038/ncomms9485	journal	September 2015
Direct access to thermally stable and highly crystalline mesoporous transition-metal oxides with uniform pores Lee, Jinwoo; Christopher Orilall, M.; Warren, Scott C. Nature Materials, Vol. 7, Issue 3 https://doi.org/10.1038/nmat2111	journal	January 2008
Self-adjusted synthesis of ordered stable mesoporous minerals by acid–base pairs Tian, Bozhi; Liu, Xiaoying; Tu, Bo Nature Materials, Vol. 2, Issue 3, p. 159-163 https://doi.org/10.1038/nmat838	journal	February 2003
High entropy oxides for reversible energy storage Sarkar, Abhishek; Velasco, Leonardo; Wang, Di Nature Communications, Vol. 9, Issue 1 https://doi.org/10.1038/s41467-018-05774-5	journal	August 2018
An overview of the synthesis of ordered mesoporous materials Li, Wei; Zhao, Dongyuan Chem. Commun., Vol. 49, Issue 10 https://doi.org/10.1039/C2CC36964H	journal	January 2013
In situ hydrogenation and decarboxylation of oleic acid into heptadecane over a Cu–Ni alloy catalyst using methanol as a hydrogen carrier Zhang, Zihao; Yang, Qiwei; Chen, Hao Green Chemistry, Vol. 20, Issue 1 https://doi.org/10.1039/C7GC02774E	journal	January 2018
Entropy-stabilized metal oxide solid solutions as CO oxidation catalysts with high-temperature stability Chen, Hao; Fu, Jie; Zhang, Pengfei Journal of Materials Chemistry A, Vol. 6, Issue 24 https://doi.org/10.1039/C8TA01772G	journal	January 2018
Synthesis of replica mesostructures by the nanocasting strategy Yang, Haifeng; Zhao, Dongyuan Journal of Materials Chemistry https://doi.org/10.1039/b414402c	journal	January 2005
Porous crystals of cubic metal oxides templated by cage-containing mesoporous silica Yue, Wenbo; Zhou, Wuzong Journal of Materials Chemistry, Vol. 17, Issue 47 https://doi.org/10.1039/b709076e	journal	January 2007
Hard template synthesis of crystalline mesoporous anatase TiO2 for photocatalytic hydrogen evolution Zhang, Zhenyu; Zuo, Fan; Feng, Pingyun Journal of Materials Chemistry, Vol. 20, Issue 11 https://doi.org/10.1039/b921157h	journal	January 2010
Ordered mesoporous metal oxides: synthesis and applications Ren, Yu; Ma, Zhen; Bruce, Peter G. Chemical Society Reviews, Vol. 41, Issue 14 https://doi.org/10.1039/c2cs35086f	journal	January 2012

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