2024 New's Items

Water-Enhanced Direct Air Capture of Carbon Dioxide in Metal–Organic Frameworks

Chen OI
Liu C-H
Wang K
Borrego-Marin E
Li H
Alawadhi AH
Navarro JAR
Yaghi OM
2024

We have developed two series of amine-functionalized zirconium (Zr) metal–organic framework-808 (MOF-808), which were produced by postsynthetic modifications to have either amino acids coordinated to Zr ions (MOF-808-AAs) or polyamines covalently bound to the chloro-functionalized structure (MOF-808-PAs). These MOF variants were comprehensively characterized by liquid-state 1H nuclear magnetic resonance (NMR) measurements and potentiometric acid–base titration to determine the amounts of amines, energy-dispersive X-ray spectroscopy to assess the extent of covalent substitution...

Mapping the spatial modulations of excitons in moiré heterostructures

Dandu M
Sankar S
Naik MH
Hays P
Blach D
Barre E
Taniguchi T
Watanabe K
Louie SG
da Jornada FH
Tongay S
Hacktel JA
Ercius P
Raja A
Susarla S
2024

Moiré heterostructures of layered materials such as transition metal dichalcogenides enable periodic arrays of localized quasi-particles with long-range Coulomb interactions which can host a plethora of quantum phenomena. Depending on the lattice mismatch and twist angle across the individual layers, resulting moiré potential modulates the distribution of electronic states, significantly changing the landscape of moiré excitons and their characteristics. We employ simultaneous hyperspectral electron energy loss spectroscopy and annular dark field imaging in a scanning transmission electron...

Image and data mining in reticular chemistry powered by GPT-4V

Zheng Z
He Z
Khattab O
Rampal N
Zaharia MA
Borgs C
Chayes JT
Yaghi OM
2024

The integration of artificial intelligence into scientific research opens new avenues with the advent of GPT-4V, a large language model equipped with vision capabilities. In this study, we demonstrate that GPT-4V, accessible through the ChatGPT web user interface or an API, offers promising possibilities in navigating and mining complex data for metal–organic frameworks (MOFs) especially from graphical sources (e.g. sorption isotherms, powder X-ray diffraction patterns, thermogravimetric analysis graphs, etc.). Our approach involved an...

Mass transfer in atmospheric water harvesting systems

Lassitter T
Hanikel N
Coyle DJ
Hossain MI
Lipinski B
O'Brien M
Hall DB
Hastings J
Borja J
O'Neil T
Neumann SE
Moore DR
Yaghi OM
Glover TG
2024

In this work, the rate-limiting diffusion mechanisms of MOF-303, MOF-333, and a multivariate (MTV) version of these metal–organic frameworks (MOFs), where the organic linkers are present in a 50/50 ratio, are identified and quantified using concentration swing frequency response (CSFR). The data show that the single-atom precision of MOFs allows for precise tuning of the diffusion rate that is not easily achieved in traditional adsorbent materials. The Maxwell-Stefan diffusivity as a function of loading was calculated to decouple the influence of molecular mobility and equilibrium...

Single and Multi-Hop Question-Answering Datasets for Reticular Chemistry with GPT-4-Turbo

Rampal N
Wang K
Burigana M
Hou L
Al-Johani J
Sackmann A
Murayshid HS
AlSumari WA
AlAbdulkarim AM
Alhazmi NE
Alawad MO
Borgs C
Chayes JT
Yaghi OM
2024

The rapid advancement in artificial intelligence and natural language processing has led to the development of large-scale datasets aimed at benchmarking the performance of machine learning models. Herein, we introduce “RetChemQA”, a comprehensive benchmark dataset designed to evaluate the capabilities of such models in the domain of reticular chemistry. This dataset includes both single-hop and multi-hop question-answer pairs, encompassing approximately 45,000 question and answers (Q&As) for each type. The questions have been extracted from an extensive corpus of literature...

Carbon dioxide capture from open air using covalent organic frameworks

Zhou Z
Ma T
Zhang H
Chheda S
Li H
Wang K
Ehrling S
Giovine R
Li C
Alawadhi AH
Abduljawad MM
Alawad MO
Gagliardi L
Sauer J
Yaghi OM
2024

Capture of CO2 from the air offers a promising approach to addressing climate change and achieving carbon neutrality goals1,...

Multilaminate Energy Storage Films from Entropy-Driven Self-Assembled Supramolecular Nanocomposites

Li H
Vargo E
Xie Z
Ma L
Pieters PF
Shelton SW
Alivisatos AP
Xu T
Liu Y
2024

Composite materials comprising polymers and inorganic nanoparticles (NPs) are promising for energy storage applications, though challenges in controlling NP dispersion often result in performance bottlenecks. Realizing nanocomposites with controlled NP locations and distributions within polymer microdomains is highly desirable for improving energy storage capabilities but is a persistent challenge, impeding the in-depth understanding of the structure–performance relationship. In this study, a facile entropy-driven self-assembly approach is employed to fabricate block copolymer-based...

The propensity for covalent organic frameworks to template polymer entanglement

Neumann SE
Kwon J
Gropp C
Ma L
Giovine R
Ma T
Hanikel N
Wang K
Chen T
Jagani S
Ritchie RO
Xu T
Yaghi OM
2024

The introduction of molecularly woven three-dimensional (3D) covalent organic framework (COF) crystals into polymers of varying types invokes different forms of contact between filler and polymer. Whereas the combination of woven COFs with amorphous and brittle polymethyl methacrylate results in surface interactions, the use of the liquid-crystalline polymer polyimide induces the formation of polymer-COF junctions. These junctions are generated by the threading of polymer chains through the pores of the nanocrystals, thus allowing for spatial arrangement of polymer strands. This...

Mapping Composition Evolution through Synthesis, Purification, and Depolymerization of Random Heteropolymers

Yu H
Liu L
Yin R
Jayapurna I
Wang R
Xu T
2024

Random heteropolymers (RHPs) consisting of three or more comonomers have been routinely used to synthesize functional materials. While increasing the monomer variety diversifies the side-chain chemistry, this substantially expands the sequence space and leads to ensemble-level sequence heterogeneity. Most studies have relied on monomer composition and simulated sequences to design RHPs, but the questions remain unanswered regarding heterogeneities within each RHP ensemble and how closely these simulated sequences reflect the experimental outcomes. Here, we quantitatively mapped out the...

Error mitigated metasurface-based randomized measurement schemes

Ren H
Zhang Y
Zheng Z
Ying C
Xu L
Rahmani M
Whaley KB
2024

Estimating properties of quantum states via randomized measurements has become a significant part of quantum information science. In this paper, we design an innovative approach leveraging metasurfaces to perform randomized measurements on photonic qubits, together with error mitigation techniques that suppress realistic metasurface measurement noise. Through fidelity and purity estimation, we confirm the capability of metasurfaces to implement randomized measurements and the unbiased nature of our error-mitigated estimator. Our findings show the potential of metasurface-based...