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.

Attention:

The NSF Public Access Repository (PAR) system and access will be unavailable from 11:00 PM ET on Friday, July 11 until 2:00 AM ET on Saturday, July 12 due to maintenance. We apologize for the inconvenience.


Title: Challenges and Opportunities: Metal–Organic Frameworks for Direct Air Capture
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
Award ID(s):
2119433
PAR ID:
10528467
Author(s) / Creator(s):
; ; ; ; ; ; ;
Publisher / Repository:
Wiley-VCH GmbH
Date Published:
Journal Name:
Advanced Functional Materials
ISSN:
1616-301X
Format(s):
Medium: X
Sponsoring Org:
National Science Foundation
More Like this
  1. Abstract Marine carbon dioxide removal (mCDR) is gaining interest as a tool to meet global climate goals. Because the response of the ocean–atmosphere system to mCDR takes years to centuries, modeling is required to assess the impact of mCDR on atmospheric CO2reduction. Here, we use a coupled ocean–atmosphere model to quantify the atmospheric CO2reduction in response to a CDR perturbation. We define two metrics to characterize the atmospheric CO2response to both instantaneous ocean alkalinity enhancement (OAE) and direct air capture (DAC): the cumulative additionality (α) measures the reduction in atmospheric CO2relative to the magnitude of the CDR perturbation, while the relative efficiency (ϵ) quantifies the cumulative additionality of mCDR relative to that of DAC. For DAC,αis 100% immediately following CDR deployment, but declines to roughly 50% by 100 years post-deployment as the ocean degasses CO2in response to the removal of carbon from the atmosphere. For instantaneous OAE,αis zero initially and reaches a maximum of 40%–90% several years to decades later, depending on regional CO2equilibration rates and ocean circulation processes. The global meanϵapproaches 100% after 40 years, showing that instantaneous OAE is nearly as effective as DAC after several decades. However, there are significant geographic variations, withϵapproaching 100% most rapidly in the low latitudes whileϵstays well under 100% for decades to centuries near deep and intermediate water formation sites. These metrics provide a quantitative framework for evaluating sequestration timescales and carbon market valuation that can be applied to any mCDR strategy. 
    more » « less
  2. Abstract Carbon capture and sequestration (CCS) from industrial point sources and direct air capture are necessary to combat global climate change. A particular challenge faced by amine‐based sorbents—the current leading technology—is poor stability towards O2. Here, we demonstrate that CO2chemisorption in γ‐cylodextrin‐based metal–organic frameworks (CD‐MOFs) occurs via HCO3formation at nucleophilic OHsites within the framework pores, rather than via previously proposed pathways. The new framework KHCO3CD‐MOF possesses rapid and high‐capacity CO2uptake, good thermal, oxidative, and cycling stabilities, and selective CO2capture under mixed gas conditions. Because of its low cost and performance under realistic conditions, KHCO3CD‐MOF is a promising new platform for CCS. More broadly, our work demonstrates that the encapsulation of reactive OHsites within a porous framework represents a potentially general strategy for the design of oxidation‐resistant adsorbents for CO2capture. 
    more » « less
  3. Abstract Capturing and sequestering carbon dioxide (CO2) from the atmosphere via large‐scale direct air capture (DAC) deployment is critical for achieving net‐zero emissions. Large‐scale DAC deployment, though, will require significant cost reductions in part through policy and investment support. This study evaluates the impact of policy interventions on DAC cost reduction by integrating energy system optimization and learning curve models. We examine how three policy instruments—incremental deployment, accelerated deployment, and R&D‐driven innovation—impact DAC learning investment, which is the total investment required until the technology achieves cost parity with conventional alternatives or target cost. Our findings show that while incremental deployment demands significant learning investment, R&D‐driven innovation is considerably cheaper at cost reduction. Under a baseline 8% learning rate, incremental deployment may require up to $998 billion to reduce costs from $1,154 to $400/tCO2, while accelerated deployment support could save approximately $7 billion on that investment. In contrast, R&D support achieves equivalent cost reductions at less than half the investment of incremental deployment. However, the effectiveness of R&D intervention varies with learning rates and R&D breakthroughs. R&D yields net benefits in all cases except at extremely low breakthroughs (5%) and very high learning rates (20%), where they are slightly more expensive. For learning rates below 20%, R&D provides net benefits even at minimal breakthroughs. These findings underscore the need for comprehensive public policy strategies that balance near‐term deployment incentives with long‐term innovation investments if we are to ensure DACS becomes a viable technology for mitigating climate change. 
    more » « less
  4. Abstract Scenarios that limit global warming to below 2 °C by 2100 assume significant land-use change to support large-scale carbon dioxide (CO2) removal from the atmosphere by afforestation/reforestation, avoided deforestation, and Biomass Energy with Carbon Capture and Storage (BECCS). The more ambitious mitigation scenarios require even greater land area for mitigation and/or earlier adoption of CO2removal strategies. Here we show that additional land-use change to meet a 1.5 °C climate change target could result in net losses of carbon from the land. The effectiveness of BECCS strongly depends on several assumptions related to the choice of biomass, the fate of initial above ground biomass, and the fossil-fuel emissions offset in the energy system. Depending on these factors, carbon removed from the atmosphere through BECCS could easily be offset by losses due to land-use change. If BECCS involves replacing high-carbon content ecosystems with crops, then forest-based mitigation could be more efficient for atmospheric CO2removal than BECCS. 
    more » « less
  5. Abstract Data-driven materials design often encounters challenges where systems possess qualitative (categorical) information. Specifically, representing Metal-organic frameworks (MOFs) through different building blocks poses a challenge for designers to incorporate qualitative information into design optimization, and leads to a combinatorial challenge, with large number of MOFs that could be explored. In this work, we integrated Latent Variable Gaussian Process (LVGP) and Multi-Objective Batch-Bayesian Optimization (MOBBO) to identify top-performing MOFs adaptively, autonomously, and efficiently. We showcased that our method (i) requires no specific physical descriptors and only uses building blocks that construct the MOFs for global optimization through qualitative representations, (ii) is application and property independent, and (iii) provides an interpretable model of building blocks with physical justification. By searching only ~1% of the design space, LVGP-MOBBO identified all MOFs on the Pareto front and 97% of the 50 top-performing designs for the CO2working capacity and CO2/N2selectivity properties. 
    more » « less