4.8 Article

Origin of Selective Guest-Induced Magnetism Transition in Fe/MOF-74

期刊

JOURNAL OF PHYSICAL CHEMISTRY LETTERS
卷 4, 期 15, 页码 2530-2534

出版社

AMER CHEMICAL SOC
DOI: 10.1021/jz4015103

关键词

-

资金

  1. Korea CCS R&D Center, Basic Science Research [2010-0023018]
  2. WCU program [R31-2008-000-10055-0]
  3. Ministry of Education, Science and Technology of the Korean government
  4. KAIST EEWS Initiative
  5. Ministry of Science, ICT & Future Planning, Republic of Korea [N01130023] Funding Source: Korea Institute of Science & Technology Information (KISTI), National Science & Technology Information Service (NTIS)
  6. National Research Foundation of Korea [2011-0032170] Funding Source: Korea Institute of Science & Technology Information (KISTI), National Science & Technology Information Service (NTIS)

向作者/读者索取更多资源

The experimentally observed selective guest-induced (olefin-induced) magnetism transition from ferromagnetism (FM) to antiferromagnetism (AFM) on Fe/MOF-74 is investigated using the first principles calculations. We reveal that FM in bare MOF is due to direct exchange interaction between neighboring Fe ions while the olefin-adsorbed MOF prefers AFM through the superexchange interaction. We find that geometrical changes (such as Fe-Fe distance and Fe-O-Fe angle) associated with strong interaction of olefin pi-bonds with open metal sites in MOF framework define magnetic coupling while electronic effects such as charge transfer and orbital interaction play a minor role. Additionally, the weak interchain magnetic coupling whose magnitude is smaller than the intrachain coupling by an order of magnitude can be switched by introducing a paramagnetic ligand between metal atoms. This work offers the origin of magnetism in MOFs with open metal sites and its subtle alteration due to selective guest binding that can be used for future design of lightweight porous magnet and magnetic separation of oxygen.

作者

我是这篇论文的作者
点击您的名字以认领此论文并将其添加到您的个人资料中。

评论

主要评分

4.8
评分不足

次要评分

新颖性
-
重要性
-
科学严谨性
-
评价这篇论文

推荐

Article Multidisciplinary Sciences

Controlling hot electron flux and catalytic selectivity with nanoscale metal-oxide interfaces

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

Bimetallic Gold-Silver Nanostructures Drive Low Overpotentials for Electrochemical Carbon Dioxide Reduction

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

Heterogeneous Catalysis in Grammar School

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

Classifying Intermetallic Tetragonal Phase of All-d-Metal Heusler Alloys for Catalysis Applications

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

Automated exploitation of the big configuration space of large adsorbates on transition metals reveals chemistry feasibility

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

Generative Adversarial Networks for Crystal Structure Prediction (vol 6, pg 1412, 2020)

Sungwon Kim, Juhwan Noh, Geun Ho Gu, Alan Aspuru-Guzik, Yousung Jung

ACS CENTRAL SCIENCE (2022)

Article Chemistry, Physical

Perovskite synthesizability using graph neural networks

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

Correlated Local Fluctuations in the Hydrogen Bond Network of Liquid Water

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

Activity Trends of Methane Oxidation Catalysts under Emission Conditions

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.

ACS CATALYSIS (2022)

Article Chemistry, Physical

Metal Encapsulation-Driven Strong Metal-Support Interaction on Pt/Co3O4 during CO Oxidation

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.

ACS CATALYSIS (2023)

Article Chemistry, Physical

A structure translation model for crystal compounds

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

A generalized-template-based graph neural network for accurate organic reactivity prediction (Sept, 10.1038/s42256-022-00526-z, 2022)

Shuan Chen, Yousung Jung

NATURE MACHINE INTELLIGENCE (2022)

Article Computer Science, Artificial Intelligence

A generalized-template-based graph neural network for accurate organic reactivity prediction

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

Alteration of oxygen evolution mechanisms in layered LiCoO2 structures by intercalation of alkali metal ions

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

Engineering vacancy and hydrophobicity of two-dimensional TaTe2 for efficient and stable electrocatalytic N2 reduction

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.

INNOVATION (2022)

暂无数据