Article
Green & Sustainable Science & Technology
Huajian Chen, Jinquan Wan, Zhicheng Yan, Yongwen Ma, Yan Wang, Yongchang Xie, Jin Hou
Summary: In this study, different small molecule acids were used as modulators to prepare high-activity defective Fe(II)-MOFs with unsaturated coordination sites. The addition of the modulators created more unsaturated sites for PS activation, leading to enhanced degradation of sulfamethoxazole. Citric acid was found to be the most effective modulator, improving the crystallinity, porosity, and coordination of the Fe(II)-MOFs. The study also proposed a degradation pathway for sulfamethoxazole in the Fe(II)-MOF-CA/PS system and proposed a possible catalytic mechanism based on experimental results.
JOURNAL OF CLEANER PRODUCTION
(2022)
Article
Materials Science, Multidisciplinary
Sung Gu Kang
Summary: This study systematically examined the band gaps of several metal-organic frameworks and calculated their stabilities, revealing that the band gap of methylammonium barium formate was the highest while that of methylammonium copper formate was the lowest. Additionally, the effects of charge transfer and pressure on the band gaps of methylammonium nickel formate were explored.
MATERIALS RESEARCH BULLETIN
(2021)
Article
Chemistry, Physical
Ying Wei, Anwen Tang, Xiaojie He, Hong Chen, Huimin Yin, Yi Li, Yongfan Zhang, Shuping Huang
Summary: The potassium storage performance of UiO-66 derivatives was investigated using density functional theory calculations. The results showed that modifying the metal atoms in the UiO-66 nodes can affect the band gap and charge transfer processes. Proper modification can improve the electronic and ionic conductivity of UiO-66 when used as an anode material in potassium ion batteries.
JOURNAL OF PHYSICAL CHEMISTRY C
(2022)
Article
Chemistry, Multidisciplinary
Qing Luo, Zhen Ding, Huamin Sun, Zhen Cheng, Naien Shi, Chuanyuan Song, Min Han, Daqing Gu, Mingdong Yi, Yujie Sun, Linghai Xie, Wei Huang
Summary: The study presents a solution-processed approach based on SDS for the synthesis of well-dispersed 2D MOF nanosheets, which opens up new possibilities for shape control and mass production of MOF materials.
Article
Chemistry, Physical
Jiemin Wang, Inhar Imaz, Daniel Maspoch
Summary: The ability to miniaturize metal-organic frameworks (MOFs) into smaller sizes offers unique characteristics and properties such as large outer surface area/volume ratios and size-dependent flexibility or catalytic performance. It also allows for the shaping of MOFs into unconventional morphologies like 2D nanosheets, leading to new possibilities for applications in porous materials. Ongoing research in shrinking MOFs through nanotechnology is expected to produce novel materials with unprecedented structural and functional properties.
Review
Chemistry, Inorganic & Nuclear
Douchao Mei, Lijia Liu, Bing Yan
Summary: This paper provides a comprehensive review on the enrichment and removal of U(VI) from seawater and wastewater using metal-organic frameworks (MOFs) and covalent organic frameworks (COFs). It discusses the synthetic approach, influencing factors, adsorption mechanism, and compares the performance of MOFs and COFs with other materials. The paper also points out the current problems and discusses the future directions for MOFs and COFs in uranium treatment.
COORDINATION CHEMISTRY REVIEWS
(2023)
Article
Chemistry, Physical
Peng Wu, Yu Shen, Hongfeng Li, Wenxiong Shi, Lulu Zhang, Ting Pan, Wenbo Pei, Weina Zhang, Fengwei Huo
Summary: Metal nanoparticles supported on metal-organic frameworks have shown excellent performance in catalytic reactions. By controlling the growth behavior of nanoparticles on specific binding sites of MOFs, improved reaction performance can be achieved, providing insights into the structure-activity relationship.
Article
Chemistry, Physical
Weixiang Geng, Tianchun Li, Xiaorong Zhu, Yu Jing
Summary: This study investigates the potential of Mo-3(C6O6)(2) monolayers as electrocatalysts for the CO2 reduction reaction (CRR) using first principles calculations. The Mo centers are found to be active sites that selectively promote CRR and produce methane. Coordination with hydroxyl further enhances the catalytic activity and lowers the thermodynamic barrier.
PHYSICAL CHEMISTRY CHEMICAL PHYSICS
(2022)
Article
Chemistry, Applied
Larissa L. Lima, Sergio R. Tavares, Carla Soares, Guillaume Maurin, Alexandre A. Leita
Summary: Metal Organic Frameworks (MOFs) with versatile chemical functionality and tunable pore structures are attractive for various applications. In this study, the doping of the Ti12O15 inorganic node of MIP-177(Ti) MOF with different transition metals (Fe, Ru, and Zr) is systematically explored using computational methods. The results show that the doping metals preferentially substitute the corner-sharing trimers of Ti octahedra, and the band gap can be significantly tuned by low concentrations of metal doping. This computational work is important for the development of mixed metal MOFs with controllable electronic properties for potential photocatalysis applications.
MICROPOROUS AND MESOPOROUS MATERIALS
(2023)
Article
Chemistry, Multidisciplinary
Anastasia Terzopoulou, Mario Palacios-Corella, Carlos Franco, Semih Sevim, Thomas Dysli, Fajer Mushtaq, Maria Romero-Angel, Carlos Marti-Gastaldo, De Gong, Jun Cai, Xiang-Zhong Chen, Martin Pumera, Andrew J. DeMello, Bradley J. Nelson, Salvador Pane, Josep Puigmarti-Luis
Summary: Biotemplating is an effective method for manufacturing small-scale devices, as demonstrated in the assembly of metal-organic framework nanocrystals on Spirulina platensis. By coating the magnetic surface with gelatin, MOF nanocrystals can be successfully assembled on helical biotemplates, creating highly integrated magnetically driven microrobots with multiple functionalities for potential applications in biomedicine and environmental remediation.
ADVANCED FUNCTIONAL MATERIALS
(2022)
Article
Chemistry, Multidisciplinary
Jianting Zhang, Jingbo Shi, Hang Zhao, Jinbo Bai, Xiaolin Li, Kunyue Leng
Summary: This study reports a crystal growth blocking strategy for the preparation of hierarchical UiO-66 MOFs using a solvent-free method. The addition of FeCl3 limits the overgrowth of UiO-66 crystals, resulting in particles with a size of approximately 12 nm. After removing Fe, these small particles loosely aggregate and gain intercrystalline mesopores. The optimized sample Mes-UiO-66 exhibits a well-developed hierarchical structure, with a BET surface area of 1161.9 m2 g-1 and a mesopore volume of 1.21 cm3 g-1. The catalytic performance and stability of Mes-UiO-66 are demonstrated by the oxidation of DBT, achieving a DBT conversion of over 99% with only a slight decrease after five cycles. This finding provides a novel platform for efficiently fabricating hierarchical MOFs for large-molecule catalysis.
CRYSTAL GROWTH & DESIGN
(2023)
Article
Engineering, Chemical
Stephen J. Percival, Leo J. Small, William B. Bachman, Mara E. Schindelholz, Tina M. Nenoff
Summary: Nanoporous materials, including MOFs and inorganic zeolites, are being explored as gas sensor materials due to their selectivity and durability. Long-term testing under varying conditions is crucial to evaluate their stability and response. In this study, nanoporous materials-based sensors were tested for 3 months under dry or humid conditions, and the results showed relative stability in dry conditions but degradation in the humid environment. These findings highlight the need for long-term testing of emerging nanoporous sensors under specific environmental conditions.
INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
(2023)
Review
Chemistry, Multidisciplinary
Thibault De Villenoisy, Xiaoran Zheng, Vienna Wong, Sajjad S. Mofarah, Hamidreza Arandiyan, Yusuke Yamauchi, Pramod Koshy, Charles C. Sorrell
Summary: Materials derived from metal-organic frameworks (MOFs) have shown exceptional structural variety and complexity and can be synthesized using low-cost scalable methods. However, their inherent instability and low electrical conductivity limit their applications. MOF-derived metal-based derivatives (MDs) provide a superior alternative with higher stability and electrical conductivity, while retaining the complex nanostructures of MOFs. This work comprehensively reviews the synthesis and nanostructural design of MDs, aiming to identify the parameters for optimal compositions, structures, nanostructures, and performance, and provide a platform for designing and processing these materials for specific applications. The study is supported by figures summarizing reported approaches and a comprehensive tabular coverage of the studies.
ADVANCED MATERIALS
(2023)
Article
Multidisciplinary Sciences
Ryunosuke Hayashi, Shohei Tashiro, Masahiro Asakura, Shinya Mitsui, Mitsuhiko Shionoya
Summary: The structure of porous molecular crystals can be controlled allosterically by the adsorption of effectors within low-symmetry nanochannels with multiple molecular recognition sites, leading to diverse framework structure conversion and switchable molecular affinity at different recognition sites. These findings may provide guidance for the development of supramolecular materials with flexible and highly-ordered three-dimensional structures for biological applications.
NATURE COMMUNICATIONS
(2023)
Article
Chemistry, Inorganic & Nuclear
Yue Li, Xiaokang Wang, Xinlei Yang, Hongyan Liu, Xianyi Chai, Yutong Wang, Weidong Fan, Daofeng Sun
Summary: The development of high-performance adsorbents is crucial for the low-energy separation of acetylene. In this study, a Fe-MOF with U-shaped channels was synthesized. The adsorption isotherms and breakthrough experiments showed that Fe-MOF has a high acetylene uptake and can effectively separate C2H2/CO2 and C2H2/C2H4 mixtures at normal temperatures. The simulation results also demonstrated the strong interaction between Fe-MOF with U-shaped channels and acetylene.
INORGANIC CHEMISTRY
(2023)
Article
Multidisciplinary Sciences
Hongrui Zhang, David Raftrey, Ying-Ting Chan, Yu-Tsun Shao, Rui Chen, Xiang Chen, Xiaoxi Huang, Jonathan T. Reichanadter, Kaichen Dong, Sandhya Susarla, Lucas Caretta, Zhen Chen, Jie Yao, Peter Fischer, Jeffrey B. Neaton, Weida Wu, David A. Muller, Robert J. Birgeneau, Ramamoorthy Ramesh
Summary: In this study, a novel magnetic ground state, namely Néel-type skyrmion lattice, is observed at room temperature in a single-phase, layered 2D magnet. The relationship between thickness and magnetic domain size follows Kittel's law. The current-induced motion of the skyrmion lattice at room temperature is successfully observed. This discovery provides an important platform for layered device applications and studies of topological and quantum effects in 2D.
Article
Materials Science, Multidisciplinary
Stephen E. Gant, Jonah B. Haber, Marina R. Filip, Francisca Sagredo, Dahvyd Wing, Guy Ohad, Leeor Kronik, Jeffrey B. Neaton
Summary: This study investigates the accuracy of the WOT-SRSH functional as a generalized Kohn-Sham starting point for single-shot GW calculations. The results show that G(0)W(0)@WOT-SRSH provides comparable precision and accuracy in computing band gaps to more advanced methods, and improves the description of states deeper in the valence band manifold. Additionally, G(0)W(0)@WOT-SRSH reduces the sensitivity of computed band gaps to ambiguities in the tuning procedure.
PHYSICAL REVIEW MATERIALS
(2022)
Article
Engineering, Environmental
John Young, Fergus Mcilwaine, Berend Smit, Susana Garcia, Mijndert van der Spek
Summary: Direct air capture using solid adsorbents is crucial for achieving net zero greenhouse gas emissions. Current research mainly focuses on developing new adsorbents, but there is a disconnect between adsorbent design and process performance. This study demonstrates that while CO2 capacity is important for a steam-assisted TVSA process, it does not significantly impact the performance of an amine-functionalised adsorbent in a temperature vacuum swing adsorption process. Factors such as adsorption kinetics, density, and thermal conductivity play a more critical role in energy efficiency and cost reduction. The findings provide guidance for scientists and engineers in improving adsorbent design and intensified DAC processes.
CHEMICAL ENGINEERING JOURNAL
(2023)
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
Nanoscience & Nanotechnology
Aditya Sood, Jonah B. Haber, Johan Carlstrom, Elizabeth A. Peterson, Elyse Barre, Johnathan D. Georgaras, Alexander H. M. Reid, Xiaozhe Shen, Marc E. Zajac, Emma C. Regan, Jie Yang, Takashi Taniguchi, Kenji Watanabe, Feng Wang, Xijie Wang, Jeffrey B. Neaton, Tony F. Heinz, Aaron M. Lindenberg, Felipe H. da Jornada, Archana Raja
Summary: In this study, lattice dynamics in photoexcited WSe2/WS2 heterostructures were directly visualized using femtosecond electron diffraction. It was found that both WSe2 and WS2 were heated simultaneously on a picosecond timescale, which cannot be explained by phonon transport across the interface. First-principles calculations revealed a fast channel involving layer-hybridized electronic states, enabling phonon-assisted interlayer transfer of photoexcited electrons. Phonons were emitted in both layers on the femtosecond timescale via this channel, consistent with the simultaneous lattice heating observed experimentally. Strong electron-phonon coupling via layer-hybridized electronic states was identified as a novel route for controlling energy transport across atomic junctions.
NATURE NANOTECHNOLOGY
(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
Chemistry, Multidisciplinary
Nency P. Domingues, Seyed Mohamad Moosavi, Leopold Talirz, Kevin Maik Jablonka, Christopher P. Ireland, Fatmah Mish Ebrahim, Berend Smit
Summary: In this study, a joint machine learning and experimental approach is used to optimize the synthesis conditions of Al-PMOF, resulting in improved yield and crystallinity. The most important experimental variables that determine the outcome are identified through analysis of failed and partially successful experiments.
COMMUNICATIONS CHEMISTRY
(2022)
Article
Chemistry, Multidisciplinary
Beatriz Mourino, Kevin Maik Jablonka, Andres Ortega-Guerrero, Berend Smit
Summary: Covalent organic frameworks (COFs) are promising organic-based photocatalysts with attractive optoelectronic properties. The CURATED COFs database, which contains experimental COFs, has been largely unexplored for photocatalysis. In this study, a screening process using DFT-based descriptors assesses the cost-effective visible light absorption, thermodynamic feasibility, charge separation, and charge-carrier mobility of COFs. 13 COFs are identified as potential candidates for water splitting, and materials (N-x-COF (x = 0-3)) reported as candidates for hydrogen evolution reaction are also highlighted. Overall, this strategy directs future research towards a selective group of COFs and provides valuable insights for structural design in achieving desired photocatalytic processes.
ADVANCED FUNCTIONAL MATERIALS
(2023)
Article
Chemistry, Multidisciplinary
Patrick Gaeumann, Thomas Rohrbach, Luca Artiglia, Daniele Ongari, Berend Smit, Jeroen A. van Bokhoven, Marco Ranocchiari
Summary: The tandem HF-AC reaction is a highly efficient method for the synthesis of industrially relevant products. Adding Zn-MOF-74 to the cobalt-catalyzed hydroformylation reaction enables tandem HF-AC under milder conditions compared to the aldox process. The addition of Zn-MOF-74 significantly enhances the yield of aldol condensation products.
CHEMISTRY-A EUROPEAN JOURNAL
(2023)
Article
Engineering, Chemical
Elias Moubarak, Seyed Mohamad Moosavi, Charithea Charalambous, Susana Garcia, Berend Smit
Summary: To evaluate the performance of materials for carbon capture, pure component isotherms are used to predict mixture isotherms. Molecular simulations are also used for screening materials. An efficient workflow for sampling pure component isotherms was developed and tested on metal-organic frameworks, proving its reliability. The use of ideal adsorbed solution theory (IAST) is shown to accurately predict CO2 and N2 mixture isotherms, making it a suitable technique for bridging the gap between adsorption data and process modeling.
INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
(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
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
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.