Generalized Approach for Rapid Aqueous MOF Synthesis by Controlling Solution pH

被引:45
作者
Huelsenbeck, Luke [1 ]
Luo, Hongxi [1 ]
Verma, Prince [1 ]
Dane, Jillian [1 ]
Ho, Rachel [1 ]
Beyer, Emily [1 ]
Hall, Hailey [1 ]
Geise, Geoffrey M. [1 ]
Giri, Gaurav [1 ]
机构
[1] Univ Virginia, Dept Chem Engn, Charlottesville, VA 22904 USA
关键词
METAL-ORGANIC FRAMEWORKS; ROOM-TEMPERATURE SYNTHESIS; ZEOLITIC IMIDAZOLATE FRAMEWORK; X-RAY-DIFFRACTION; UIO-66; HKUST-1; NANOCRYSTALS; FABRICATION; MODULATION; ADSORPTION;
D O I
10.1021/acs.cgd.0c00895
中图分类号
O6 [化学];
学科分类号
0703 ;
摘要
Metal-organic frameworks (MOFs) are a promising class of functional materials with applications in catalysis, separations, electronics, and drug delivery, among others. Despite a range of techniques utilized for MOF synthesis, a generalizable and scalable approach has yet to be developed for producing MOFs without using environmentally damaging organic solvents. Here, we look at MOF synthesis as a reaction in an aqueous medium and propose new methods of measuring conversion and selectivity. We show that controlling reactant speciation via pH is a generalizable approach to producing the prototypical MOFs UiO-66, UiO-66-NH2, ZIF-L, and HKUST-1 with space-time yields (STY) of over 2250 kg m(-3) day(-1), which is a 1 order of magnitude improvement for zirconium-based MOFs. We show that UiO-66-NH2 crystallization is complete in 5 min at room temperature, with 70% of the extent of reaction completed by 30 s. Finally, we apply the rapid synthesis approach to coating cotton fabric with up to 20 wt % UiO-66-NH2 using a sequential dip-coating (SQD) technique and demonstrate particulate matter (PM1-4) filtration up to 85%. This work shows a green-chemistry-based, generalizable pathway to rapid synthesis for multiple MOFs and demonstrates its utility for filtration applications. The ability to produce alternative filtration materials is especially relevant under pandemic conditions, where SQD offers a rapid and high-throughput manner of providing air filtration by modifying commonly available textile materials.
引用
收藏
页码:6787 / 6795
页数:9
相关论文
共 76 条
[1]  
American Society of Anesthesiologists, COVID-19 and personal protective equipment
[2]   Cation-Triggered Drug Release from a Porous Zinc-Adeninate Metal-Organic Framework [J].
An, Jihyun ;
Geib, Steven J. ;
Rosi, Nathaniel L. .
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 2009, 131 (24) :8376-+
[3]  
[Anonymous], 2002, UllmannsEncyclopedia of Industrial Chemistry, DOI [10.1002/14356007, DOI 10.1002/14356007.A13283, DOI 10.1002/14356007]
[4]  
[Anonymous], 1972, DISSOCIATION CONSTAN
[5]  
[Anonymous], 2020, STRATEGIES OPTIMIZIN
[6]   High-Throughput Fabrication of Uniform and Homogenous MOF Coatings [J].
Arslan, Hasan K. ;
Shekhah, Osama ;
Wohlgemuth, Jonas ;
Franzreb, Matthias ;
Fischer, Roland A. ;
Woell, Christof .
ADVANCED FUNCTIONAL MATERIALS, 2011, 21 (22) :4228-4231
[7]   Aqueous production of spherical Zr-MOF beads via continuous-flow spray-drying [J].
Avci-Camur, Ceren ;
Troyano, Javier ;
Perez-Carvajal, Javier ;
Legrand, Alexandre ;
Farrusseng, David ;
Imaz, Inhar ;
Maspoch, Daniel .
GREEN CHEMISTRY, 2018, 20 (04) :873-878
[8]  
Brown H.C., 1955, Determination of Organic Structures by Physical Methods, P567, DOI DOI 10.1016/B978-1-4832-3166-2.50018-4
[9]   Tackling the Defect Conundrum in UiO-66: A Mixed-Linker Approach to Engineering Missing Linker Defects [J].
Bueken, Bart ;
Van Velthoven, Niels ;
Krajnc, Andrai ;
Smolders, Simon ;
Taulelle, Francis ;
Mellot-Draznieks, Caroline ;
Mali, Gregor ;
Bennett, Thomas D. ;
De Vos, Dirk .
CHEMISTRY OF MATERIALS, 2017, 29 (24) :10478-10486
[10]   Synthesis, characterization and adsorption ability of UiO-66-NH2 [J].
Cam Loc Luu ;
Thi Thuy Van Nguyen ;
Tri Nguyen ;
Tien Cuong Hoang .
ADVANCES IN NATURAL SCIENCES-NANOSCIENCE AND NANOTECHNOLOGY, 2015, 6 (02)