Article
Chemistry, Multidisciplinary
Jay Thakkar, Winters Kexi Guo, Michael J. Janik, Xueyi Zhang
Summary: The computational evaluation of the separation of butanes and butenes using MOF-74 revealed that the selectivity between C-4 alkene and alkane is determined by pi-d chemical interactions, while the selectivity differences among butenes arise from steric implications.
Article
Engineering, Chemical
Tong-Chuan Li, Xiang-Jing Kong, Yabo Xie, Tao He, Guang-Rui Si, Xiang-Yu Li, Wei Wu, Minjian Zhao, Jian-Rong Li
Summary: This study functionalized IRMOF-74-IV using a ligand substitution strategy to create multivariate MOF catalysts. By adjusting the contents of the ligand and the type of metal ion, the researchers found that IRMOF-74-IV-PBHB45%-Cu exhibited the highest efficiency in photocatalytic CO2 conversion. The mixed-ligand approach used in this work allows for tailoring of existing MOFs and opens up new opportunities for their applications.
SEPARATION AND PURIFICATION TECHNOLOGY
(2022)
Article
Materials Science, Multidisciplinary
Xiaojiao You, Jian Yang, Chengyi Dan, Han Chen, Yuchi Cui, Haowei Wang, Mingliang Wang, Zhe Chen
Summary: The mechanism of deformation banding in cold rolling Al-Mg alloy was investigated with a focus on local lattice rotation and related dislocation slip. It was found that the formation of deformation bands is orientation dependent, with a strong presence in grains close to certain crystallographic directions. The activation of secondary slips and their associated lattice rotation contribute to the formation of deformation bands.
MATERIALS CHARACTERIZATION
(2022)
Article
Chemistry, Multidisciplinary
Guangchao Li, Christopher Foo, Xianfeng Yi, Wei Chen, Pu Zhao, Pan Gao, Tatchamapan Yoskamtorn, Yao Xiao, Sarah Day, Chiu C. Tang, Guangjin Hou, Anmin Zheng, Shik Chi Edman Tsang
Summary: This study provides the first direct experimental observation of induced active sites in zeolites, which contradicts traditional views. Evidence shows that under the action of strong polar adsorbates, typical acid sites in pristine zeolites can transform into new induced structures.
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2021)
Article
Chemistry, Physical
Minghao Hua, Xuelei Tian, Shuo Li, Anchen Shao, Xiaohang Lin
Summary: This study investigates the surface aggregation of Pt atoms on the Pt/Ag(111) surface under different conditions using density functional theory calculations and Monte Carlo simulations. The results reveal the decisive influence of CO-CO interactions and the competition between CO-metal interactions and CO-CO repulsion. Two methods for synthesizing the surface Pt atomic system are found, and the Pt distribution can be controlled by adjusting the concentration. An ordered structure with the maximized number of Pt monomers and homogeneous distribution on the surface is observed. The ordered Pt3Ag(111) surface shows a lower overpotential compared to pure Pt(111), suggesting its potential as a candidate for ORR catalysts with rich active sites and a low overpotential.
PHYSICAL CHEMISTRY CHEMICAL PHYSICS
(2022)
Article
Engineering, Environmental
Chuan Yu, Shenyu Lan, Sentai Cheng, Lixi Zeng, Mingshan Zhu
Summary: This study utilized Ba-substituted SrTiO3 piezoelectric materials for the piezocatalytic degradation of CBZ in water, with Ba0.5Sr0.5TiO3 (BSTO-2) showing the optimal performance. The enhanced piezocatalytic activity of BSTO-2 was attributed to its distorted structure and modified conductivity, resulting in a higher piezoelectric response and faster interfacial charge transfer. This research provides valuable insights for developing highly efficient piezocatalysts and highlights the potential of piezocatalysis in water remediation.
JOURNAL OF HAZARDOUS MATERIALS
(2022)
Article
Physics, Applied
Lizhong Huang, Jianzhong Lin, Ruijin Wang, Chun Shao
Summary: We explore the changes in wall shear stress caused by migrating soft particles modeled as capsules in a channel. It is interesting to note that the wall shear stress shows a roughly linear increase in both its maximum value and variation magnitude as the normalized overall lateral position of the capsules increases when they form a linear train. Furthermore, for a single stable capsule in the channel, the streamlines exhibit an M-like shape in the upper part and a W-like shape in the lower part. The vertical velocity is used to explain the peak-valley-peak structure in the wall shear stress profile, and for multiple capsules, the contours of vertical velocity can determine the locations of the peaks or valleys in the wall shear stress.
APPLIED PHYSICS LETTERS
(2023)
Article
Chemistry, Physical
Elisabeth M. Dietze, Henrik Groenbeck
Summary: In this study, the adsorption and desorption processes of CO on Pt(111) surface are investigated using density functional theory calculations combined with Monte Carlo simulations. The results show that the average adsorption energy determines the adsorption process, while the low energy part of the adsorbate stability distribution describes the desorption process.
JOURNAL OF CHEMICAL THEORY AND COMPUTATION
(2023)
Article
Chemistry, Physical
Yang He, Junyan Zhang, Felipe Polo-Garzon, Zili Wu
Summary: Since the 1970s, researchers have been studying the strong metal-support interactions (SMSIs) in supported metal catalysts to enhance stability and create novel catalytic sites. They have discovered that SMSIs are more common than initially thought and that various adsorbed species can promote SMSI in catalytic systems. The understanding of SMSIs has implications for catalyst stability, catalytic rates, and product selectivity in heterogeneous catalysis.
JOURNAL OF PHYSICAL CHEMISTRY LETTERS
(2023)
Article
Chemistry, Physical
Omer Tayfuroglu, Abdulkadir Kocak, Yunus Zorlu
Summary: Metal-organic frameworks (MOFs) with their exceptional porous and organized structures have been widely studied. However, predicting their properties accurately is still a challenge due to their hybrid structures. In this work, a neural network potential (NNP) is constructed to predict the properties of the isoreticular metal-organic framework (IRMOF) series. The NNP successfully predicts the properties of both fragments and bulk MOFs, and reveals some odd behaviors of selected MOFs.
PHYSICAL CHEMISTRY CHEMICAL PHYSICS
(2022)
Article
Physics, Applied
Hui-Yu Chen, Fumito Araoka, Fang-Yu Lee, Chi Lee, Jui Jiun Chen
Summary: The nonlinear optical response of the blue-phase liquid crystals was investigated using a SHG microscope. It was found that the internal coupling between polarization and structural deformation can be visualized quickly with the aid of the SHM. The induced polarization and SHG intensity in the blue phase were dependent on the electric field strength and transition to the chiral nematic phase.
JOURNAL OF PHYSICS D-APPLIED PHYSICS
(2023)
Article
Nanoscience & Nanotechnology
Shangguo Liu, Yaxiang Chang, Na He, Shenglin Zhu, Lianbao Wang, Xien Liu
Summary: The oxygen evolution reaction (OER) is a critical step in water splitting for hydrogen production, and understanding its mechanism is crucial for developing efficient OER electrocatalysts. However, the mechanism of OER, especially in a water-solvent environment, is still not well understood for the widely studied rutile Ru-based oxide. It is still debated whether the adsorbate evolving mechanism (AEM) competes with the lattice oxygen mechanism (LOM) for OER.
ACS APPLIED MATERIALS & INTERFACES
(2023)
Article
Materials Science, Multidisciplinary
Lifeng Zhang, Zejian Dong, Shuangbao Wang, Langli Luo
Summary: The compositional and phase segregation on the surface of an alloy can alter its functionality, especially in applications where surface structure and chemistry are crucial. The atomic processes during gas molecule-induced segregation remain elusive.
SCIENCE CHINA-MATERIALS
(2021)
Article
Geosciences, Multidisciplinary
Weiyu Zheng, Zhong Lu, Roger P. Denlinger, Jin-Woo Kim
Summary: Wastewater disposal can cause detectable surface uplift, posing a threat to infrastructure due to potential ground instability. To better understand this geohazard, the study combines Interferometric Synthetic Aperture Radar (InSAR) measurements, injection information, and a poroelastic finite element model with a Bayesian Monte Carlo approach to constrain local hydro-geomechanical parameters. The analysis of Sentinel-1A/B imagery from 2014 to 2020 in Winkler county, West Texas, USA, reveals under-reported volumes in a well near the deformation center. The inversion results provide improved constraints on the parameters compared to using cumulative spatial deformation or temporal development alone.
GEOPHYSICAL RESEARCH LETTERS
(2023)
Article
Materials Science, Multidisciplinary
E. Iaparova, L. Heller, O. Tyc, P. Sittner
Summary: The functional behavior of nanocrystalline NiTi shape memory wires with different austenitic microstructures was investigated. Three phenomena were reported and discussed: the elongation and subsequent shortening of martensitic NiTi wire under low applied stresses due to thermally induced martensite reorientation, the martensite stabilization by deformation caused by change of martensite variant microstructures, and the generation of unrecovered plastic strains and dislocation defects during martensitic transformation/reorientation/detwinning processes.
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
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
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
Sabyasachi Roy Chowdhury, Ngan Nguyen, Bess Vlaisavljevich
Summary: This study reports a computational investigation of the molecular geometries of a pair of manganese(III) spin-crossover complexes. Density functionals overestimate Mn-Namine bond distances for the high-spin state but accurately describe the geometry for the intermediate-spin state. Restricted open-shell Moller-Plesset perturbation theory (MP2) appropriately describes the high-spin geometry while extended multistate complete active space second-order perturbation theory (XMS-CASPT2) provides a good description of the geometry for the intermediate-spin state. Coupled cluster methods (i.e., DLPNO-CCSD(T)) yield bond distances in agreement with experiment.
JOURNAL OF PHYSICAL CHEMISTRY A
(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
Chemistry, Inorganic & Nuclear
Rina Bhowmick, Sabyasachi Roy Chowdhury, Bess Vlaisavljevich
Summary: Copper corroles have unique multiconfigurational electronic structures in the ground state, which are influenced by the transfer of electrons from the π orbitals of the corrole to the d-orbital of copper. The choice of functional heavily affects the determination of the ground spin state and its energetics. Extended multireference perturbation theory methods (XMS-CASPT2) can assess the functional choice. The electronic structure is fundamentally different between density functional theory (DFT) and XMS-CASPT2.
INORGANIC CHEMISTRY
(2023)
Article
Chemistry, Physical
Diba Behnoudfar, Cory M. Simon, Joshua Schrier
Summary: This study proposes a graph-regularized logistic matrix factorization (GR-LMF) approach to predict the miscibility of solutions in aqueous, two-phase systems (ATPSs). By incorporating pairwise miscibility experiments and the categorical relationships of solutes, GR-LMF outperforms traditional methods in predicting missing miscibility outcomes.
JOURNAL OF PHYSICAL CHEMISTRY B
(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
Yutong Pang, ChoongSze Lee, Bess Vlaisavljevich, Christopher P. Nicholas, Paul J. Dauenhauer
Summary: Dehydration of methyl lactate to acrylic acid and methyl acrylate was efficiently achieved over a Na-FAU zeolite catalyst impregnated with multifunctional diamines. 12BPE and 44TMDP with a loading of 40 wt% or two molecules per Na-FAU supercage showed a dehydration selectivity of 96%, with 44TMDP achieving the highest reported yield of 92% at a selectivity of 96% by tuning the weighted hourly space velocity.
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.
