Uncovering Two Principles of Multivariate Hierarchical Metal–Organic Framework Synthesis via Retrosynthetic Design
[1];
[3]
- Department of Chemistry, Texas A&M University, College Station, Texas 77843-3255, United States
- Department of Chemistry, Texas A&M University, College Station, Texas 77843-3255, United States, College of Chemistry, Tianjin Normal University, Tianjin, 300387, China, Key Laboratory of Advanced Energy Materials Chemistry (Ministry of Education), Nankai University, Tianjin 300071, China
- Department of Chemistry, Texas A&M University, College Station, Texas 77843-3255, United States, Department of Materials Science and Engineering, Texas A&M University, College Station, Texas 77843-3003, United States
Multivariate (MTV) hierarchical metal-organic frameworks (MOFs), which contain multiple regions arranged in ordered structures, show promise for applications such as gas separation, size-selective catalysis, and controlled drug delivery. However, the complexity of these hierarchical MOFs is limited by a lack of control during framework assembly. Herein, we report the controlled generation of hierarchical MOF-on-MOF structural formation under the guidance of two design principles, surface functionalization and retrosynthetic techniques for stability control. Accordingly, the tunability of spatial distributions, compositions, and crystal sizes has been achieved in these hierarchical systems. The resulting MOF-on-MOF hierarchical structures represent a unique crystalline porous material which contains a controllable distribution of functional groups and metal clusters that are associated together within a framework composite. This general synthetic approach not only expands the scope and tunability of the traditional MTV strategy to multicomponent materials, but also offers a facile route to introduce variants and sequences to sophisticated three-dimensional hierarchical and cooperative systems. As a proof of concept, the photothermal effects of a porphyrinic core-MOF are exploited to trigger the controlled guest release from a shell- MOF with high guest capacity, highlighting the integrated cooperative behaviors in multivariate hierarchical systems.
- Research Organization:
- Energy Frontier Research Centers (EFRC) (United States). Center for Gas Separations Relevant to Clean Energy Technologies (CGS); Texas A & M Univ., College Station, TX (United States); Univ. of California, Berkeley, CA (United States)
- Sponsoring Organization:
- USDOE Office of Science (SC), Basic Energy Sciences (BES); USDOE Office of Fossil Energy and Carbon Management (FECM); USDOE Office of Fossil Energy (FE)
- Grant/Contract Number:
- SC0001015; FE0026472
- OSTI ID:
- 1485532
- Alternate ID(s):
- OSTI ID: 1508811
- Journal Information:
- ACS Central Science, Journal Name: ACS Central Science Vol. 4 Journal Issue: 12; ISSN 2374-7943
- Publisher:
- American Chemical SocietyCopyright Statement
- Country of Publication:
- United States
- Language:
- English
Web of Science
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