2024 New's Items

Complete miscibility of immiscible elements at the nanometre scale

Chen PC
Gao M
McCandler CA
Song C
Jin J
Yang Y
Maulana AL
Persson KA
Yang P
2024

Understanding the mixing behaviour of elements in a multielement material is important to control its structure and property. When the size of a multielement material is decreased to the nanoscale, the miscibility of elements in the nanomaterial often changes from its bulk counterpart. However, there is a lack of comprehensive and quantitative experimental insight into this process. Here we explored how the miscibility of Au and Rh evolves in nanoparticles of sizes varying from 4 to 1 nm and composition changing from 15% Au to 85% Au. We found that the two immiscible elements exhibit a...

Nanometre-resolved observation of electrochemical microenvironment formation at the nanoparticle–ligand interface

Shan Y
Zhao X
Guzman MF
Jana A
Chen S
Yu S
Ng KC
Roh I
Chen H
Altoe V
Corder SG
Bechtel HA
Qian J
Salmeron MB
Yang P
2024

The dynamic response of surface ligands on nanoparticles (NPs) to external stimuli critically determines the functionality of NP–ligand systems. For example, in electrocatalysis the collective dissociation of ligands on NP surfaces can lead to the creation of an NP/ordered-ligand interlayer, a microenvironment that is highly active and selective for CO2-to-CO conversion. However, the lack of in situ characterization techniques with high spatial resolution hampers a comprehensive molecular-level understanding of the mechanism of interlayer formation. Here we...

Crystalline Polyphenylene Covalent Organic Frameworks

Han X
Zhou Z
Wang K
Zheng Z
Neumann SE
Zhang H
Ma T
Yaghi OM
2023

The synthesis of crystalline polyphenylene covalent organic frameworks (COFs) was accomplished by linking fluorinated tris(4-acetylphenyl)benzene building units using aldol cyclotrimerization. The structures of the two COFs, reported here, were confirmed by powder X-ray diffraction techniques, Fourier transform infrared, and solid-state 13C CP/MAS NMR spectroscopy. The results showed that the COFs were porous and chemically stable in corrosive, harsh environments for at least 1 week. Accordingly, postsynthetically modified derivatives of these COFs using primary amines showed...

Harvesting Water from Air with High-Capacity, Stable Furan-Based Metal–Organic Frameworks

Alawadhi AH
Chheda S
Stroscio GD
Rong Z
Kurandina D
Nguyen HL
Rampal N
Zheng Z
Gagliardi L
Yaghi OM
2024

We synthesized two isoreticular furan-based metal–organic frameworks (MOFs), MOF-LA2-1(furan) and MOF-LA2-2(furan) with rod-like secondary building units (SBUs) featuring 1D channels, as sorbents for atmospheric water harvesting (LA = long arm). These aluminum-based MOFs demonstrated a combination of high water uptake and stability, exhibiting working capacities of 0.41 and 0.48 gwater/gMOF (under isobaric conditions of 1.70 kPa), respectively. Remarkably, both MOFs showed a negligible loss in water uptake after 165 adsorption–desorption cycles. These working...

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,...