Article
Chemistry, Inorganic & Nuclear
Hui Zhang, Xin Zheng, Li-Ming Yang, Eric Ganz
Summary: The study systematically investigated CO2 adsorption performance and microscopic mechanisms of N,N-dimethylethylenediamine appended M-2(dobpdc) structures, revealing the formation of ammonium carbamate during adsorption. Additionally, the research provided information on the atomic-level mechanism of CO2 adsorption and reaction pathways.
INORGANIC CHEMISTRY
(2021)
Article
Multidisciplinary Sciences
Omid T. Qazvini, Ravichandar Babarao, Shane G. Telfer
Summary: Researchers present a metal-organic framework adsorbent, MUF-16, that efficiently captures CO2 over other competing gases with high selectivity. This adsorbent enables high-purity gas separation under dynamic conditions, making it suitable for the purification of natural gas and industrial feedstocks.
NATURE COMMUNICATIONS
(2021)
Article
Chemistry, Multidisciplinary
Xin Zheng, Hui Zhang, Li-Ming Yang, Eric Ganz
Summary: This study investigated the adsorption energy and reaction path of CO2 capture by N,N-diethylethylenediamine-functionalized MOFs using density functional theory. The results show a strong metal center dependence in both the amine binding energies and CO2 adsorption energies. The process of CO2 adsorption involves two main steps with different energy barriers, highlighting the importance of the initial step in the overall reaction. This work contributes to a fundamental understanding of the microprocess of CO2 capture and provides insights for the design and optimization of efficient CO2 capture materials.
CRYSTAL GROWTH & DESIGN
(2021)
Article
Chemistry, Multidisciplinary
Yanze Liu, Shuai Li, Lu Dai, Jiani Li, Jianning Lv, Zhejiaji Zhu, Anxiang Yin, Pengfei Li, Bo Wang
Summary: 2D conjugated MOFs have gained significant interest due to their unique structural features and promising properties, with HATNA-based ligand contributing to the construction of a highly crystalline and porous framework for electrocatalytic reduction of CO2 to methane with high selectivity.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2021)
Article
Chemistry, Multidisciplinary
Il Son Khan, Diego Mateo, Genrikh Shterk, Tuiana Shoinkhorova, Daria Poloneeva, Luis Garzon-Tovar, Jorge Gascon
Summary: This study presents a highly active and stable Ni-based catalyst derived from a metal-organic framework for the photothermal reduction of CO2 to CH4. The catalyst can be tuned by controlling the pyrolysis process of MOF-74 (Ni), achieving high CH4 production rates under UV-visible-IR irradiation. The catalyst shows no significant loss of activity after multiple reaction cycles and hours of continuous operation, demonstrating its potential for reducing CO2 to CH4 using solar energy in outdoor environments.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2021)
Article
Chemistry, Physical
Hao-Lin Zhu, Jia-Run Huang, Xue-Wen Zhang, Chao Wang, Ning-Yu Huang, Pei-Qin Liao, Xiao-Ming Chen
Summary: In this study, a Cu-based metal-organic framework was introduced as a catalyst for the efficient and selective reduction of CO2 to CH4. The in situ-generated trigonal pyramidal Cu(I)N-3 was identified as the electrochemical active site, while the hydrogen-bonding interactions of adjacent aromatic hydrogen atoms played a key role in stabilizing key intermediates of carbon dioxide reduction and inhibiting the hydrogen evolution reaction, demonstrating a high performance in electroreduction of CO2 to CH4.
Review
Chemistry, Physical
Juan-Ding Xiao, Rui Li, Hai-Long Jiang
Summary: Metal-organic frameworks (MOFs) are crystalline inorganic-organic hybrid materials with tunable semiconducting behavior. They have potential for use in photocatalysis to produce sustainable solar fuels, thanks to their unique structural advantages that allow for a better understanding of the structure-activity relationship. This review focuses on the active sites in MOF-based photocatalysts and discusses their enhanced activity based on the well-defined structure of MOFs, providing deep insights into MOF-based photocatalysis.
Article
Engineering, Environmental
Meili Ding, Pan Ma, Yang Wang, Ying Zhang, Jun Liu, Jianfeng Yao
Summary: This study developed a metal organic framework templating method to prepare bimetallic oxide catalysts with hierarchically porous structures, and regulated the quantity and type of active species by adjusting the coordination environment. The optimized catalyst achieved efficient CO2 conversion under solvent-free mild conditions, and exhibited good chemical stability.
JOURNAL OF ENVIRONMENTAL CHEMICAL ENGINEERING
(2023)
Article
Chemistry, Multidisciplinary
Philip M. M. Stanley, Alice Y. Y. Su, Vanessa Ramm, Pascal Fink, Ceren Kimna, Oliver Lieleg, Martin Elsner, Johannes A. A. Lercher, Bernhard Rieger, Julien Warnan, Roland A. A. Fischer
Summary: A light-harvesting metal-organic framework has been engineered as a catalyst carrier, achieving controllable photocatalytic synthesis of syngas. This study is a significant breakthrough for photocatalytic CO2 reduction and H2 evolution in sustainable energy cycles.
ADVANCED MATERIALS
(2023)
Article
Chemistry, Physical
Mingliang Hu, Jiahao Liu, Shaojia Song, Weiwei Wang, Jiasai Yao, Yixuan Gong, Chenyu Li, Huan Li, Yanjie Li, Xilin Yuan, Zhao Fang, Hao Xu, Weiyu Song, Zhenxing Li
Summary: In this study, an ultra-thin two-dimensional trimetallic metal-organic framework nanosheet was successfully synthesized and used as a photocatalyst for CO2 reduction. The nanosheet exhibited high catalytic activity and selectivity, and Zr and Cu doping were found to enhance its performance.
Article
Nanoscience & Nanotechnology
Kaifei Chen, Ranjeet Singh, Jining Guo, Yalou Guo, Ali Zavabeti, Qinfen Gu, Randall Q. Snurr, Paul A. Webley, Gang Kevin Li
Summary: This study demonstrates for the first time that gas adsorption in microporous materials can be regulated by a moderate external electric field, providing a new method for controlling gas adsorption.
ACS APPLIED MATERIALS & INTERFACES
(2022)
Review
Polymer Science
Suleiman Gani Musa, Zulkifli Merican Aljunid Merican, Omid Akbarzadeh
Summary: With the escalating issue of global warming, efforts are being made towards achieving a carbon-neutral environment by utilizing non-fossil fuel sources such as solar, nuclear, and biomass energy. Metal-organic frameworks are being explored as potential catalysts for converting CO2 into organic carbonates, given their unique features and ease of synthesis.
Article
Chemistry, Multidisciplinary
Hao Wu, Xin Ying Kong, Xiaoming Wen, Siang-Piao Chai, Emma C. Lovell, Junwang Tang, Yun Hau Ng
Summary: Encapsulating Cu2O nanowires in metal-organic frameworks (MOFs) enhances activity and stability, facilitates charge separation and CO2 uptake, leading to selective photocatalytic CO2 reduction into CH4. This work demonstrates an effective strategy for CO2 conversion by integrating MOFs with metal oxide photocatalyst.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2021)
Article
Chemistry, Physical
Bin Wang, Xin Zhang, Hongliang Huang, Zhangjing Zhang, Taner Yildirim, Wei Zhou, Shengchang Xiang, Banglin Chen
Summary: BUT-22 is a microporous aluminum-based MOF with high storage capacities for methane, hydrogen, and carbon dioxide, showing excellent performance under different conditions.
Article
Chemistry, Multidisciplinary
Yulong Ying, Bahareh Khezri, Jiri Kosina, Martin Pumera
Summary: In this study, a bismuth-containing metal-organic framework CAU-17 was prepared and employed as an electrocatalyst for highly selective CO2-to-formate conversion. Morphology engineering was utilized to construct a hierarchical structure for CAU-17-fiber, achieving efficient formate production with high selectivity.
Article
Engineering, Chemical
Susana Garcia, Berend Smit
Summary: Decarbonisation from various industrial and power emission sectors calls for optimized capture technologies that can be integrated into diverse applications as a CO2 feedstock. Advanced tailored sorbent-based technologies offer higher capture capacities and lower energy penalties, accelerating the discovery, development, and deployment of novel materials. The PrISMa project addresses this challenge through coordinated efforts between experimentalists, theoreticians, and process engineers, providing optimally tuned carbon capture solutions for local sources and sinks. This article highlights recent results obtained with the PrISMa platform.
CHEMIE INGENIEUR TECHNIK
(2023)
Article
Multidisciplinary Sciences
Kevin Maik Jablonka, Charithea Charalambous, Eva Sanchez Fernandez, Georg Wiechers, Juliana Monteiro, Peter Moser, Berend Smit, Susana Garcia
Summary: To understand the impact of intermittent operation of a power plant using amine-based carbon capture processes, stress tests were conducted on a plant operating with a mixture of two amines. A machine learning model was developed to forecast emissions and model the impact of interventions. The findings suggest the need for reconsidering mitigation strategies for capture plants using a mixture of amines, as certain interventions have opposite effects on the emissions of solvent components.
Article
Biochemical Research Methods
Dennis Woertge, Matthew Parziale, Jan Claussen, Behzad Mohebbi, Siegfried Stapf, Bernhard Bluemich, Matthew Augustine
Summary: The matrix pencil method (MPM) is tested for quantitatively processing multiexponential low-field nuclear magnetic resonance T1 relaxometry data. The data is obtained from T1 saturation recovery curves measured in a highly inhomogeneous magnetic field. Different concentrations of a Gd3+ contrast agent doped in 0.9% brine solutions are used as test liquids. MPM shows superior performance in separating and quantifying relaxation components, as well as exploring the sensitivity to relative contribution of each component and resolving systems with multiple components.
JOURNAL OF MAGNETIC RESONANCE
(2023)
Article
Chemistry, Multidisciplinary
Seung-Jae Shin, Jamie W. W. Gittins, Matthias J. J. Golomb, Alexander C. C. Forse, Aron Walsh
Summary: The electrochemical interface of Cu-3(HHTP)(2) with an organic electrolyte was investigated using simulations and experimental measurements. The excess charges mainly formed on the organic ligand, and cation-dominated charging mechanisms led to greater capacitance. By changing the ligand, the spatially confined electric double-layer structure and self-diffusion coefficients of in-pore electrolytes were improved. The performance of MOF-based supercapacitors can be controlled by modifying the ligating group.
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2023)
Article
Multidisciplinary Sciences
Yao Fu, Yifeng Yao, Alexander C. Forse, Jianhua Li, Kenji Mochizuki, Jeffrey R. Long, Jeffrey A. Reimer, Gael De Paepe, Xueqian Kong
Summary: Defects in metal-organic frameworks (MOFs) have significant impact on their nanostructure and physicochemical properties. This study reveals the presence of formate defects in MOF-74 originating from decomposed solvent. The defects partially eliminate open metal sites and decrease gas adsorption, and the adsorption mechanism of CO2 in defective MOF-74 is elucidated through in-situ NMR analysis and molecular simulations.
NATURE COMMUNICATIONS
(2023)
Article
Chemistry, Physical
Joel E. Schmidt, Berend Smit, Cong-Yan Chen, Dan Xie, Theo L. M. Maesen
Summary: The need to reduce the lifecycle greenhouse gas emissions of fuels and lubricants has increased attention on hydroisomerization processes. By recognizing the individual alkane hydrocracking pathways, changes to the alkane hydroisomerization and hydrocracking networks can be determined based on catalyst pore topology. Spacious pores allow access to both kinetically favored and thermodynamically favored hydrocracking pathways, while narrower pores enhance isomerization by slowing down access to certain pathways and limiting hydrocracking to specific isomers.
Article
Chemistry, Multidisciplinary
Kevin Maik Jablonka, Andrew S. Rosen, Aditi S. Krishnapriyan, Berend Smit
Summary: Digital reticular chemistry is becoming a crucial aspect of modern chemistry, but there is a need for a common ecosystem to prevent it from being subjective. This article introduces the fundamentals of such an ecosystem and highlights its significance through common pitfalls.
ACS CENTRAL SCIENCE
(2023)
Article
Multidisciplinary Sciences
Yao Fu, Alexander C. Forse, Zhengzhong Kang, Matthew J. Cliffe, Weicheng Cao, Jinglin Yin, Lina Gao, Zhenfeng Pang, Tian He, Qinlong Chen, Qi Wang, Jeffrey R. Long, Jeffrey A. Reimer, Xueqian Kong
Summary: Metal-organic frameworks (MOFs) are flexible and non-periodic soft materials with imperfect crystallinity, abundance of flexibility, disorder, and defects. In this study, advanced nuclear magnetic resonance spectroscopy was used to characterize the mesoscale structures of a defective MOF with a semi-crystalline lattice. It was found that engineered defects can tune the lattice flexibility by combining ordered and disordered compartments. The one-dimensional alignment of correlated defects is crucial for the reversible topological transition. This unique structure exhibits both a rigid framework of nanoporosity and a flexible linkage of high swellability.
Article
Computer Science, Artificial Intelligence
Yeonghun Kang, Hyunsoo Park, Berend Smit, Jihan Kim
Summary: Metal-organic frameworks (MOFs) are crystalline porous materials with tunable building blocks. Machine learning approach can explore the vast chemical space of MOFs by predicting their properties. MOFTransformer, a pre-trained multi-modal transformer, achieves state-of-the-art results for property prediction and provides chemical insights through feature analysis.
NATURE MACHINE INTELLIGENCE
(2023)
Article
Engineering, Biomedical
Frederik Dreyer, Qing Yang, Belal Alnajjar, Daniel Kruger, Bernhard Blumich, Jens Anders
Summary: This article presents a portable NMR relaxometry system optimized for the point-of-care analysis of body liquids, demonstrating excellent concentration sensitivity and making it an ideal candidate for future biomarker detection.
IEEE TRANSACTIONS ON BIOMEDICAL CIRCUITS AND SYSTEMS
(2023)
Article
Chemistry, Multidisciplinary
Ziting Zhu, Surya T. Parker, Alexander C. Forse, Jung-Hoon Lee, Rebecca L. Siegelman, Phillip J. Milner, Hsinhan Tsai, Mengshan Ye, Shuoyan Xiong, Maria V. Paley, Adam A. Uliana, Julia Oktawiec, Bhavish Dinakar, Stephanie A. Didas, Katie R. Meihaus, Jeffrey A. Reimer, Jeffrey B. Neaton, Jeffrey R. R. Long
Summary: Diamine-appended Mg-2(dobpdc) metal-organic frameworks have exceptional CO2 selectivities, high separation capacities, and step-shaped adsorption profiles due to a unique cooperative adsorption mechanism. Diamine-Mg-2(olz) frameworks with diverse bulky substituents exhibit desired single-step CO2 adsorption across a wide range of pressures and temperatures. One particular material, ee-2-Mg-2(olz), shows outstanding CO2 capture performance from a simulated coal flue gas and exceptional thermal and oxidative stability.
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2023)
Article
Chemistry, Multidisciplinary
Zhifei Yan, Kristopher G. Reynolds, Rui Sun, Yongjin Shin, Agnes E. Thorarinsdottir, Miguel I. Gonzalez, Bryan Kudisch, Giulia Galli, Daniel G. Nocera
Summary: This study reports the oxidation chemistry of carbonates, providing concrete pathways for the design of catalysts for carbonate management in energy storage applications.
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2023)
Article
Chemistry, Physical
Niamh A. Hartley, Suzi M. Pugh, Zhen Xu, Daniel C. Y. Leong, Adam Jaffe, Alexander C. Forse
Summary: The demand for cost-effective carbon dioxide capture technology is increasing rapidly in order to limit global temperature increase to 1.5°C within the next century. The current capture technology, amine scrubbing, has limitations such as high regeneration energy, high operational costs, and degradation issues. Electrochemically driven carbon dioxide capture, using redox-active quinone molecules, shows promise in overcoming some of these limitations.
JOURNAL OF MATERIALS CHEMISTRY A
(2023)
Article
Materials Science, Biomaterials
Xiaoli Liu, Nency Patricio Domingues, Emad Oveisi, Clara Coll-Satue, Michelle Maria Theresia Jansman, Berend Smit, Leticia Hosta-Rigau
Summary: Blood transfusions are crucial for patients with acute trauma, undergoing surgery, chemotherapy or severe blood disorders. The use of nanomaterials with enzyme-like properties, particularly gold-based metallic nanoparticles, shows promise in creating novel Hemoglobin-Based Oxygen Carriers (HBOCs) with antioxidant protection. By incorporating gold-based nanozymes into a type of Hb-loaded metal-organic framework nanocarrier, the study demonstrates their ability to catalytically deplete reactive oxygen species (ROS) and reduce methemoglobin content.
BIOMATERIALS SCIENCE
(2023)
Article
Chemistry, Multidisciplinary
Kevin Maik Jablonka, Qianxiang Ai, Alexander Al-Feghali, Shruti Badhwar, Joshua D. Bocarsly, Andres M. Bran, Stefan Bringuier, L. Catherine Brinson, Kamal Choudhary, Defne Circi, Sam Cox, Wibe A. de Jong, Matthew L. Evans, Nicolas Gastellu, Jerome Genzling, Maria Victoria Gil, Ankur K. Gupta, Zhi Hong, Alishba Imran, Sabine Kruschwitz, Anne Labarre, Jakub Lala, Tao Liu, Steven Ma, Sauradeep Majumdar, Garrett W. Merz, Nicolas Moitessier, Elias Moubarak, Beatriz Mourino, Brenden Pelkie, Michael Pieler, Mayk Caldas Ramos, Bojana Rankovic, Samuel G. Rodriques, Jacob N. Sanders, Philippe Schwaller, Marcus Schwarting, Jiale Shi, Berend Smit, Ben E. Smith, Joren Van Herck, Christoph Voelker, Logan Ward, Sean Warren, Benjamin Weiser, Sylvester Zhang, Xiaoqi Zhang, Ghezal Ahmad Zia, Aristana Scourtas, K. J. Schmidt, Ian Foster, Andrew D. White, Ben Blaiszik
Summary: This article presents a hackathon focused on exploring the diverse applications of large language models (LLMs) in molecular and materials science. Participants used LLMs for various applications and generated working prototypes, showcasing the profound impact of LLMs on the future of the fields and their potential benefits across scientific disciplines.