Review
Green & Sustainable Science & Technology
Liangxing Zhu, Falu Hu, Bin Sun, Shaonan Gu, Tingting Gao, Guowei Zhou
Summary: Solar energy-driven CO2 reduction and H-2 evolution using multivariate metal organic frameworks (MTV-MOFs) show promise in addressing energy shortage and environmental issues. MTV-MOFs have attracted significant attention in photocatalytic CO2 reduction and H-2 evolution due to their structural stability, light-absorption abilities, and catalytic performance. This review focuses on incorporating different functional ligands or metals into MOFs to enhance the photocatalytic performance of MTV-MOFs. It provides an overview of the synthesis and advantages of MTV-MOF-based photocatalysts, and summarizes recent advances in solar-to-chemical energy conversion using MTV-MOFs.
ADVANCED SUSTAINABLE SYSTEMS
(2023)
Article
Chemistry, Physical
Nicholas A. Jose, Jithin John Varghese, Samir H. Mushrif, Hua Chun Zeng, Alexei A. Lapkin
Summary: The study focused on the effects of different solvent environments on the structure and aggregation dynamics of two-dimensional metal organic framework nanosheets, revealing that solvent-surface interactions can control oriented attachment and impact adsorption properties. Liquid cell transmission electron microscopy provided insights into these interactions, while density functional theory calculations suggested the role of binding energy in this behavior. The research highlights the potential of solvent-mediated mechanisms in manipulating the properties of MOF nanomaterials.
JOURNAL OF PHYSICAL CHEMISTRY C
(2021)
Article
Nanoscience & Nanotechnology
B. Akdim, C. Woodward, S. Rao, E. Antillon
Summary: Recent studies have shown that chemically-complex solid-solution alloys produce equilibrium dislocations at high temperatures, leading to kinks and pinning points that significantly increase strength. Atomistic studies and chemical analysis can help understand the effects of different alloy compositions on dislocation formation.
SCRIPTA MATERIALIA
(2021)
Article
Nanoscience & Nanotechnology
Eric Chapman, Saif Ullah, Hao Wang, Liang Feng, Kunyu Wang, Hong-Cai Zhou, Jing Li, Timo Thonhauser, Kui Tan
Summary: This study demonstrates a novel strategy to increase the gas adsorption selectivity of metal organic framework materials by coadsorbing NH3 molecules and shows that strongly coadsorbed species might not always undermine the performance in adsorbing or separating weakly bound target molecules in nanoporous materials.
ACS APPLIED MATERIALS & INTERFACES
(2021)
Article
Chemistry, Physical
Rafaela Maria Giappa, Emmanuel Tylianakis, Marco Di Gennaro, Konstantinos Gkagkas, George E. Froudakis
Summary: By combining multi-scale calculations with machine learning, this study investigates how ligand functionalization affects the hydrogen storage performance of Metal Organic Frameworks. The results show that certain functional groups significantly enhance the interaction strength with hydrogen. The use of ab-initio calculations and machine learning provides a promising approach for predicting and improving hydrogen storage properties in porous materials.
INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
(2021)
Article
Materials Science, Multidisciplinary
Luis E. Gonzalez, David J. Gonzalez
Summary: The static and dynamic properties of several bulk liquid 4d transition metals near their respective melting points have been evaluated using ab-initio molecular dynamics simulations. The results demonstrate the existence of ordered structures and special collective excitations, and further study several transport coefficients.
INTERNATIONAL JOURNAL OF REFRACTORY METALS & HARD MATERIALS
(2022)
Article
Chemistry, Physical
Shuo Cao, Gang Zhao, Dehua Wang
Summary: Using fully ab initio molecular dynamics simulations, this study investigates the inherent structure of water and its temperature dependence. The results reveal three types of translational ordering in the second oxygen coordination shell, leading to the classification of local structures in water into three types. These findings provide ab initio evidence for the mixture model of water and shed light on the temperature dependence of its inherent structure.
PHYSICAL CHEMISTRY CHEMICAL PHYSICS
(2023)
Article
Nanoscience & Nanotechnology
Paul Iacomi, Guillaume Maurin
Summary: Zeolitic imidazolate frameworks (ZIFs) are a prominent subset of metal-organic frameworks (MOFs) known for their good thermal and chemical stability and attractive properties for diverse applications. These materials exhibit significant structural changes in response to external stimuli, making them stimuli-responsive materials.
ACS APPLIED MATERIALS & INTERFACES
(2021)
Article
Chemistry, Physical
Swaroop Chandra, Nandalal Mahapatra, Nagarajan Ramanathan, Kalyanasundaram Sundararajan
Summary: This study reexamines the geometries of nitromethane homodimers and presents concrete evidence for the prevalence of O=N center dot center dot center dot O pnicogen bonding, contrary to previous claims. The formation of a nitromethane dimer with pnicogen bonding stabilization is confirmed using matrix isolation infrared spectroscopy and computations. The study also characterizes the interactions within homodimers using various methods, highlighting the prevalence of hydrogen and pnicogen bonds.
JOURNAL OF PHYSICAL CHEMISTRY A
(2022)
Article
Chemistry, Multidisciplinary
Dong Liu, Rui Li, Juan Ren, Yongjun Cheng, Bing Yan, Yong Wu, Jian Guo Wang, Song Bin Zhang
Summary: This study investigates the electronic structures of diatomic dications, specifically focusing on dication HF2+, achieving good agreement with available references. In addition to common physical quantities, nonadiabatic radial coupling and diabatic potentials are presented. Further examination of predissociation states and shape resonances in collisions is conducted using WKB and scattering methods.
Article
Chemistry, Multidisciplinary
Chang Jun Park, One Heo, Hyeon Seok Lee, Kyung Suh Lee, Sang Hak Lee
Summary: In this study, it was found through theoretical simulation that adding extra excess electrons to the anionic nitrogen atoms in a model system of a nitrogen-containing polycyclic aromatic hydrocarbon significantly increased the reactivity of carbon dioxide reduction, leading to chemical reactions occurring in all the nitrogen atoms in the complexes. This suggests that the efficiency of CO2 reduction can be enhanced by increasing the anionic properties of nitrogen atoms in the presence of more electrons.
Article
Materials Science, Multidisciplinary
Aurash Karimi, Michael Auinger
Summary: This study systematically investigates the diffusion of nitrogen in Ferrite and Austenite using a robust multiscale model combining Density Functional Theory and Kinetic Monte Carlo. Quantitative predictions are made for nitrogen diffusion in vacancy-rich iron crystals, providing valuable insights for nitriding manufacturers. The enhanced diffusion models may play a crucial role in improving existing processes and avoiding common manufacturing problems.
Article
Chemistry, Physical
Stefan K. Kolev, Hristiyan A. Aleksandrov, Victor A. Atanasov, Valentin N. Popov, Teodor Milenov
Summary: The study focused on investigating the surface chemistry of reduced graphene oxide modified with different chemical groups through computational chemistry. Results showed that reactions depend on the proximity of chemical groups and the possibility of H-atom transfer. The presence of sp(2) carbon atoms on the surface plays a crucial role in decreasing the scission energy of C-C bonds during reactions. Additionally, decarboxylation reactions were found to be energetically favorable both at the edge and surface of the carbon material.
APPLIED SURFACE SCIENCE
(2021)
Article
Chemistry, Applied
Jose P. Ceron-Carrasco, Natalia Sanchez, Denis Jacquemin
Summary: In this study, curcuminoid analogues were combined with cisplatin to design a series of prodrugs that can be photo-activated by visible light. The simulations revealed two novel complexes absorbing in the first phototherapeutic window (600-800 nm). The optimization of these structures for photoactivated chemotherapy is discussed.
Article
Chemistry, Physical
Juqin Zeng, Michele Re Fiorentin, Marco Fontana, Micaela Castellino, Francesca Risplendi, Adriano Sacco, Giancarlo Cicero, M. Amin Farkhondehfal, Filippo Drago, Candido F. Pirri
Summary: In this study, a SbCu2O material was synthesized via one-pot microwave-assisted solvothermal route and its catalytic performance in electrochemical reduction of CO2 was investigated. The Sb-Cu2O bimetallic catalyst exhibited high CO selectivity and good stability.
APPLIED CATALYSIS B-ENVIRONMENTAL
(2022)
Article
Multidisciplinary Sciences
Si Woo Lee, Jong Min Kim, Woonghyeon Park, Hyosun Lee, Gyu Rac Lee, Yousung Jung, Yeon Sik Jung, Jeong Young Park
Summary: The interaction between metal and oxides is a crucial factor influencing the selectivity of a desirable reaction. Designing a well-formed metal-oxide interface in a heterogeneous catalyst is important for understanding selectivity and surface electronic excitation at the interface. The study demonstrates the real-time detection of hot electron flow and impact of metal-oxide interface on catalytic selectivity in a nanoscale catalytic Schottky diode.
NATURE COMMUNICATIONS
(2021)
Article
Nanoscience & Nanotechnology
Joon Woo Park, Woong Choi, Juhwan Noh, Woonghyeon Park, Geun Ho Gu, Jonghyeok Park, Yousung Jung, Hyunjoon Song
Summary: Alloy formation is an advanced approach that improves properties beyond what monoelements can achieve. The Au-Ag alloy nanostructures exhibit prominent catalytic properties in the electrochemical carbon dioxide reduction reaction (eCO(2)RR), with superior performance compared to pure elements. The optimal configuration of the active intermediate *COOH involves a bidentate coordination structure where C binds to Au and O binds to Ag, in agreement with experimental results. This study offers new insights into the synergistic roles of Au and Ag in eCO(2)RR and provides a direction for rational design of bimetallic catalysts.
ACS APPLIED MATERIALS & INTERFACES
(2022)
Article
Chemistry, Physical
Johannes T. Margraf, Zachary W. Ulissi, Yousung Jung, Karsten Reuter
Summary: The discovery of new catalytically active materials is crucial for advancing renewable energy sources and reducing energy consumption in the chemical industry. However, computational catalyst discovery is challenging due to uncertainties in material stability and synthesizability. This perspective proposes the use of generative grammars as a new approach to overcome this challenge and outlines research directions to make this technology applicable to real materials.
JOURNAL OF PHYSICAL CHEMISTRY C
(2022)
Article
Chemistry, Applied
Taewon Jin, Yousung Jung
Summary: Heusler alloys are predicted for phase stability using simple descriptors with an accuracy of 86% and it is discovered that 66% of the alloys have scaling relations between electron occupancy and spin moments, allowing cost-saving evaluation without density functional calculations. This phase classification model has the potential to reduce computational costs for the high throughput screening of Heusler compounds in various catalysis applications.
TOPICS IN CATALYSIS
(2022)
Article
Multidisciplinary Sciences
Geun Ho Gu, Miriam Lee, Yousung Jung, Dionisios G. Vlachos
Summary: An automated framework is introduced to predict stable configurations on transition metal surfaces, providing experimental evidence for different catalysts stabilizing different structures.
NATURE COMMUNICATIONS
(2022)
Correction
Chemistry, Multidisciplinary
Sungwon Kim, Juhwan Noh, Geun Ho Gu, Alan Aspuru-Guzik, Yousung Jung
ACS CENTRAL SCIENCE
(2022)
Article
Chemistry, Physical
Geun Ho Gu, Jidon Jang, Juhwan Noh, Aron Walsh, Yousung Jung
Summary: Perovskite is an important material in geophysics and technology, but the number of synthetic perovskites is small. To speed up the discovery of perovskites, we propose a graph neural network model to assess their synthesizability. Our model outperforms empirical rule-based methods and has been validated through literature synthesis results.
NPJ COMPUTATIONAL MATERIALS
(2022)
Article
Chemistry, Multidisciplinary
Yonghwan Yun, Rustam Z. Khaliullin, Yousung Jung
Summary: Recent studies have provided support for the hypothesis that liquid water can separate into two phases in the supercooled state, but there is ongoing debate about whether this structural inhomogeneity extends to ambient conditions. This study uses highly sensitive quantum mechanical calculations to detect a strong correlation in the time evolution of nearby hydrogen bonds in liquid water, revealing a direct mechanism for the appearance of short-range structural fluctuations in the hydrogen bond network. This correlated dynamics is closely connected to the static structural picture.
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2022)
Article
Chemistry, Physical
Gi Joo Bang, Geun Ho Gu, Juhwan Noh, Yousung Jung
Summary: This study develops a workflow based on a microkinetic model to elucidate the mechanism of methane oxidation and successfully screens possible catalysts for methane oxidation. The proposed workflow can be extended to explore other industrial catalysts.
Article
Chemistry, Physical
Daeho Kim, Dongmin Park, Hee Chan Song, Beomgyun Jeong, Jouhahn Lee, Yousung Jung, Jeong Young Park
Summary: The strong metal-support interaction (SMSI) has a significant impact on the catalytic performance of supported metal catalysts, playing a central role in the modern chemical industry. However, understanding SMSI under realistic conditions remains challenging. This study provides evidence of SMSI between Pt and Co3O4 using both three-dimensional and two-dimensional model catalysts. The presence of Pt-Co3O4 interface, demonstrated by the formation of a Co3O4 overlayer on Pt nanoparticles, enhances catalytic activity and offers insights for designing high-performance heterogeneous catalysts.
Article
Chemistry, Physical
Sungwon Kim, Juhwan Noh, Taewon Jin, Jaewan Lee, Yousung Jung
Summary: High-throughput virtual screening for crystals discovers new materials by evaluating the property of every virtual candidate exhaustively, with the computational bottleneck being the costly structural relaxation using DFT calculations. A generative domain translation framework is proposed to map the unrelaxed structural domains to the relaxed domains, enabling data-driven structural translations. This framework accurately predicts the materials formation energy without DFT relaxations and produces atomic coordinates consistent with DFT relaxed structures.
NPJ COMPUTATIONAL MATERIALS
(2023)
Correction
Computer Science, Artificial Intelligence
Shuan Chen, Yousung Jung
NATURE MACHINE INTELLIGENCE
(2022)
Article
Computer Science, Artificial Intelligence
Shuan Chen, Yousung Jung
Summary: This study introduces a chemistry-inspired graph neural network that accurately predicts organic reaction products by learning generalized reaction templates, thereby significantly simplifying reaction rules and exhibiting high accuracy. Despite being simplified, the generalized reaction templates are shown to represent a large percentage of existing reactions.
NATURE MACHINE INTELLIGENCE
(2022)
Article
Chemistry, Physical
Yohan Kim, Seongmin Kim, Minyoung Shim, Yusik Oh, Kug-Seung Lee, Yousung Jung, Hye Ryung Byon
Summary: Two oxygen evolution reaction (OER) mechanisms were demonstrated on layered lithium cobalt oxide (LiCoO2 and LCO) by inserting various alkali metal ions. The insertion of large cations resulted in structural transformations and changes in average Co valence states, which enhanced OER activity. Density functional theory (DFT) calculations supported the formation of OER active sites with partial intercalation of K+ ions. Additionally, Cs+ insertion showed superior OER activity with lattice-oxygen-mediated mechanism.
JOURNAL OF MATERIALS CHEMISTRY A
(2022)
Article
Multidisciplinary Sciences
Zhenqing Zhao, Jongseo Park, Changhyeok Choi, Song Hong, Xiangchao Hui, Hao Zhang, Tsz Woon Benedict Lo, Alex W. Robertson, Zengxiang Lv, Yousung Jung, Zhenyu Sun
Summary: This study successfully increased the efficiency of ambient NRR for ammonia production by tuning the Te vacancies and surface hydrophobicity of two-dimensional TaTe2 nanosheets. It achieved remarkable NH3 faradic efficiency and maintained high stability, with the edge plane of TaTe2 and VTe identified as the main active sites for NRR.