skip to main content
US FlagAn official website of the United States government
dot gov icon
Official websites use .gov
A .gov website belongs to an official government organization in the United States.
https lock icon
Secure .gov websites use HTTPS
A lock ( lock ) or https:// means you've safely connected to the .gov website. Share sensitive information only on official, secure websites.

Explore Research Products in the PAR
It may take a few hours for recently added research products to appear in PAR search results.


  • NSF Public Access
  • Search Results
  • A generative artificial intelligence framework based on a molecular diffusion model for the design of metal-organic frameworks for carbon capture
Title: A generative artificial intelligence framework based on a molecular diffusion model for the design of metal-organic frameworks for carbon capture
Abstract Metal-organic frameworks (MOFs) exhibit great promise for CO2capture. However, finding the best performing materials poses computational and experimental grand challenges in view of the vast chemical space of potential building blocks. Here, we introduce GHP-MOFassemble, a generative artificial intelligence (AI), high performance framework for the rational and accelerated design of MOFs with high CO2adsorption capacity and synthesizable linkers. GHP-MOFassemble generates novel linkers, assembled with one of three pre-selected metal nodes (Cu paddlewheel, Zn paddlewheel, Zn tetramer) into MOFs in a primitive cubic topology. GHP-MOFassemble screens and validates AI-generated MOFs for uniqueness, synthesizability, structural validity, uses molecular dynamics simulations to study their stability and chemical consistency, and crystal graph neural networks and Grand Canonical Monte Carlo simulations to quantify their CO2adsorption capacities. We present the top six AI-generated MOFs with CO2capacities greater than 2m mol g−1, i.e., higher than 96.9% of structures in the hypothetical MOF dataset.  more » « less
Award ID(s):
2209892
PAR ID:
10490845
Author(s) / Creator(s):
; ; ; ; ; ; ;
Publisher / Repository:
Nature Publishing Group
Date Published:
Journal Name:
Communications Chemistry
Volume:
7
Issue:
1
ISSN:
2399-3669
Format(s):
Medium: X
Sponsoring Org:
National Science Foundation
More Like this
  1. ; ; ; ; ; ; ; (, Advanced Functional Materials)
    Abstract Global reliance on fossil fuel combustion for energy production has contributed to the rising concentration of atmospheric CO2, creating significant global climate challenges. In this regard, direct air capture (DAC) of CO2from the atmosphere has emerged as one of the most promising strategies to counteract the harmful effects on the environment, and the further development and commercialization of this technology will play a pivotal role in achieving the goal of net‐zero emissions by 2050. Among various DAC adsorbents, metal–organic frameworks (MOFs) show great potential due to their high porosity and ability to reversibly adsorb CO2at low concentrations. However, the adsorption efficiency and cost‐effectiveness of these materials must be improved to be widely deployed as DAC sorbents. To that end, this perspective provides a critical discussion on several types of benchmark MOFs that have demonstrated high CO2capture capacities, including an assessment of their stability, CO2capture mechanism, capture‐release cycling behavior, and scale‐up synthesis. It then concludes by highlighting limitations that must be addressed for these MOFs to go from the research laboratory to implementation in DAC devices on a global scale so they can effectively mitigate climate change. 
    more » « less
  2. ; ; ; ; ; ; ; ; ; ; et al (, Advanced Materials)
    Abstract Metal–organic frameworks (MOFs) are promising materials for electrocatalysis; however, lack of electrical conductivity in the majority of existing MOFs limits their effective utilization in the field. Herein, an excellent catalytic activity of a 2D copper (Cu)‐based conductive MOF, copper tetrahydroxyquinone (CuTHQ), is reported for aqueous CO2reduction reaction (CO2RR) at low overpotentials. It is revealed that CuTHQ nanoflakes (NFs) with an average lateral size of 140 nm exhibit a negligible overpotential of 16 mV for the activation of this reaction, a high current density of ≈173 mA cm−2at −0.45 V versus RHE, an average Faradaic efficiency (F.E.) of ≈91% toward CO production, and a remarkable turnover frequency as high as ≈20.82 s−1. In the low overpotential range, the obtained CO formation current density is more than 35 and 25 times higher compared to state‐of‐the‐art MOF and MOF‐derived catalysts, respectively. The operando Cu K‐edge X‐ray absorption near edge spectroscopy and density functional theory calculations reveal the existence of reduced Cu (Cu+) during CO2RR which reversibly returns to Cu2+after the reaction. The outstanding CO2catalytic functionality of conductive MOFs (c‐MOFs) can open a way toward high‐energy‐density electrochemical systems. 
    more » « less
  3. ; ; ; ; ; ; ; ; (, Chemistry – A European Journal)
    Abstract Charge‐separated metal–organic frameworks (MOFs) are a unique class of MOFs that can possess added properties originating from the exposed ionic species. A new charge‐separated MOF, namely, UNM‐6 synthesized from a tetrahedral borate ligand and Co2+cation is reported herein. UNM‐6 crystalizes into the highly symmetricP43nspace group with fourfold interpenetration, despite the stoichiometric imbalance between the B and Co atoms, which also leads to loosely bound NO3−anions within the crystal structure. These NO3−ions can be quantitatively exchanged with various other anions, leading to Lewis acid (Co2+) and Lewis base (anions) pairs within the pores and potentially cooperative catalytic activities. For example, UNM‐6‐Br, the MOF after anion exchange with Br−anions, displays high catalytic activity and stability in reactions of CO2chemical fixation into cyclic carbonates. 
    more » « less
  4. ; ; ; ; ; (, Molecular Systems Design & Engineering)
    Widespread use of methane-powered vehicles likely requires the development of efficient on-board methane storage systems. A novel concept for methane storage is the nanoporous microtank, which is based on a millimeter-sized nanoporous pellet (the core) surrounded by an ultrathin membrane (the shell). Mixture adsorption simulations in idealized pores indicate that by combining a pellet that features large, hydrophobic pores with a membrane featuring small, hydrophilic pores, it would be possible to trap a large amount of “pressurized” methane in the pellet while keeping the external pressure low. The methane would be trapped by sealing the surrounding membrane with the adsorption of a hydrophilic compound such as methanol. Additional simulations in over 2000 hypothesized metal–organic frameworks (MOFs) indicate that the above design concept could be exploited using real nanoporous materials. Structure–property relationships derived from these simulations indicate that MOFs suitable for the core (storing over 250 cc(STP) CH4 per cc) should have a pore size in the 12–14 Å range and linkers without appreciably hydrophilic moieties. On the other hand, MOFs suitable for the shell should have a pore size less than 9 Å and linkers with hydrophilic functional groups such as –CN, –NO 2 , –OH and –NH 2 . Simulation snapshots suggest that the hydrogen bonding between these groups and hydrophilic moieties of methanol would be critical for the sealing function. 
    more » « less
  5. ; ; ; (, Chem)
    Water is the most abundant and cleanest natural resource on earth, and it is the driving force of all nature. It not only affects food security, human health, and ecosystem integrity and maintenance, but is also an important driver of energy in industrial production and life. Importantly, water adsorption applications are considered to be highly energy-efficient and environmentally friendly technologies,1 including atmospheric water harvesting,2-4 desiccation of clean gases,5 indoor humidity control,6,7 and adsorptive heat transformation.8,9 However, current water adsorption-related applications are still constrained by properties of adsorbents, such as their low water uptake capacities, poor cyclic stabilities, limited feasibilities over a range of humidity conditions, and minimal commercial availabilities. Conventional nanoporous materials (e.g., silica gels, zeolites, and clays) were the first adsorbents used in water capture applications due to their low cost, commercial availability, and favorable water adsorption kinetics. However, these materials generally suffer from either low water uptake capacities or high regeneration temperature, limiting their use in practical water absorption applications.1,10 Metal-organic frameworks (MOFs), a class of crystalline porous materials, are assembled from inorganic nodes and organic linkers through coordination bonds.11,12 Benefiting from their exceptional porosity and surface area, tunable pore size and geometry, and highly tailorable and designable structures and functionalities, MOFs show considerable potential for gas storage and separation, heterogeneous catalysis, and other energy and environmental sustainability applications.13-17 In recent years, MOFs have also shown great potential for water vapor adsorption because of a growing understanding of the relationship between MOFs and water, as well as an increasing number of reports detailing MOFs that exhibit high water stability.1,4,9 Moreover, judicious design of the MOF structures enables control over their water adsorption properties and the water uptake capacities, which make MOFs ideal candidates for water adsorption-related applications. This review aims to provide an overview of recent advances in the development of MOFs for water adsorption, as well as to offer proposed guidelines to develop even better water adsorption materials. First, we briefly introduce the fundamentals of water adsorption, including how to ascertain key insights based on the shapes of water adsorption isotherms, descriptions of various water adsorption mechanisms, and a discussion on the stability of MOFs in water systems. Next, we discuss several recent reports have detailed how to improve water uptake capacity through the design and synthesis of MOFs. In particular, we highlight the importance of reticular chemistry in the designed synthesis of MOF-based water adsorbent materials. We then shift our focus to discussing the enormous potential of MOFs for use in selective water vapor adsorption applications with both theoretical and practical considerations considered. Finally, we offer our thoughts on the future development of this field in three aspects: chemistry and materials design, process engineering, and commercialization of MOFs for water adsorption. We hope that this review will provide fundamental insights for chemists and inspire them to synthesize MOFs with better water adsorption performance; and provide assistance to engineers researching MOF-based water adsorption devices and working towards the development of highly energy-efficient and environmentally friendly technologies with reduced carbon footprints. 
    more » « less
  • Citation Formats
  • MLA
  • APA
  • Chicago
  • BibTeX
  • Save / Share this Record
  • Send to Email