Article
Chemistry, Physical
Bor-Rong Chen, Wenhao Sun, Daniil A. Kitchaev, Kevin H. Stone, Ryan C. Davis, Gerbrand Ceder, Laura T. Schelhas, Michael F. Toney
Summary: Pourbaix diagrams can guide the hydrothermal synthesis of transition metal oxides, but conditions often need to exceed phase boundaries to initiate crystallization in a reasonable timescale.
JOURNAL OF MATERIALS CHEMISTRY A
(2021)
Article
Chemistry, Multidisciplinary
Andrew Cashmore, Russell Miller, Hikaru Jolliffe, Cameron J. Brown, Mei Lee, Mark D. Haw, Jan Sefcik
Summary: This article presents an experimental workflow for the rapid assessment of primary and secondary nucleation and crystal growth kinetics under supersaturation conditions. By conducting experiments, researchers can quantify and analyze the effects of supersaturation on the nucleation and growth kinetics of α-glycine in aqueous solutions at isothermal conditions. This approach provides a means to estimate the absolute values of nucleation and growth rates and gain insights into crystallization behavior, which can be used to optimize batch or continuous crystallization processes.
CRYSTAL GROWTH & DESIGN
(2023)
Article
Biochemistry & Molecular Biology
Lie-Ding Shiau
Summary: A linearized integral model is used in this study to determine the interfacial energy and pre-exponential factor. The results show that the calculated values from different methods are consistent for the studied systems.
Article
Crystallography
Josia Tonn, Aishe Grotjohann, Christian Kocks, Andreas Jupke
Summary: Scandium, a critical raw material according to the EU, has low availability but increasing demand. Bauxite residue can be a potential European source. A novel anti-solvent crystallization process is developed to extract scandium from the residue, but it faces challenges in solid-liquid separation due to the formation of small crystals. By studying nucleation kinetics and varying operating parameters, the boundaries for controlling the crystallization process and crystal growth are explored.
Article
Engineering, Chemical
Tong Zhou, Chunzhao Tu, Ya Sun, Linan Ji, Chuangxian Bian, Xiaohua Lu, Changsong Wang
Summary: The experimental determination of the solubility, metastable zone width, and induction time of thiourea in the cooling crystallization process showed the effects under different conditions. The study indicated that homogeneous nucleation could occur at high supersaturation, while heterogeneous nucleation was more likely to occur at low supersaturation.
CHINESE JOURNAL OF CHEMICAL ENGINEERING
(2021)
Article
Crystallography
Zhirong Chen, Rongfan Zhou, Hong Yin, Shenfeng Yuan
Summary: The metastable zone width (MSZW) of DL-methionine aqueous solution for unseeded batch crystallization was measured by turbidity method. The spontaneous nucleation curves at different stirring rates and cooling rates were obtained. The results show that the increase in saturation temperature and stirring rate makes the MSZW narrower, while the increase in cooling rate widens the MSZW due to a time lag between nucleation and turbidity detection. These data are important for controlling crystallization in production and the nucleation kinetics was also studied.
JOURNAL OF CRYSTAL GROWTH
(2023)
Article
Crystallography
Lie-Ding Shiau
Summary: By developing a linearized integral model that considers the combined effect of nucleation and growth rates on crystallite size distribution, this study determined nucleation parameters from the metastable zone width. The proposed model resulted in a lower value of the interfacial energy compared to the classical 3D nucleation theory approach, but exhibited a poorer fit to the data.
JOURNAL OF CRYSTAL GROWTH
(2021)
Article
Engineering, Chemical
Jianxin Zhang, Marjatta Louhi-Kultanen
Summary: The metastable zone width (MSZW) and induction time of CoSO4 in the presence of H2SO4 were measured, and the solubility of CoSO4 was determined using Raman spectroscopy and UV-Vis. Nucleation parameters were estimated using a self-consistent Nyvlt-like approach and classical 3D theory. The results showed that the solubility of CoSO4 decreased with increasing H2SO4 concentration, and the MSZW decreased with higher saturation temperature, mixing speed, H2SO4 concentration, and lower cooling rate. The induction time measurement indicated homogeneous nucleation at high supersaturation and heterogeneous nucleation at low supersaturation. The crystallized product had different shapes depending on the presence of H2SO4, and particle sizes were smaller with higher H2SO4 concentration and cooling rate.
Article
Crystallography
Keshra Sangwal
Summary: Based on classical nucleation theory, final equations regarding the metastable zone width were derived using three deterministic approaches, which were then applied to analyze experimental data from different systems. The analysis compared and discussed trends in nucleation kinetic parameters values obtained from the deterministic integral nucleation model and the conventional stochastic theory. Results showed that the solute-supply approach could explain the dependency of solutions' Delta T-m values on cooling rate at different saturation temperatures and estimate nucleation parameters, while relatively low values of the solid-solution interfacial solution gamma(eff) suggested crystallization by heterogeneous nucleation. The nature of nucleation encountered in the MSZW measurements by the polythermal method was also discussed.
JOURNAL OF CRYSTAL GROWTH
(2021)
Article
Crystallography
Lie-Ding Shiau
Summary: In this study, induction time and metastable-zone-width (MSZW) data for aqueous l-glycine solutions in the presence of l-arginine impurity were experimentally measured using a turbidity probe. Nucleation parameters were compared and the influences of lag time on these parameters were examined. The effects of l-arginine impurity concentration on the nucleation parameters were also investigated in detail based on both induction time and MSZW data.
Article
Crystallography
Christian Kocks, Christina Maria Krekel, Marcel Gausmann, Andreas Jupke
Summary: Electrified downstream processes reduce waste salt generation and enhance the attractiveness of biotechnological production. Understanding the metastable zone width is crucial for designing and controlling electrochemically induced crystallization processes.
Article
Crystallography
Xin Liu, Zhengmin Zhang, Lin Zhang, Shi Bu, Chengcheng Shi, Weigang Xu, Zhiyang Peng, Zhilei Ma, Chen Xu, Hongqi Yao
Summary: The experiment studied the metastable zone width of Na2SO4-NaCl-H2O from high saline water of lead-acid batteries at different temperatures using the conductivity method. Results show that the width of the metastable zone increases with temperature, especially in solutions containing calcium ions. Changes in rotation speed also affect the width of the metastable zone.
JOURNAL OF CRYSTAL GROWTH
(2021)
Article
Chemistry, Multidisciplinary
Shijie Xu, Yixuan Liu, Rong Zhang, Yanfei Wang
Summary: The study investigates the impact of byproducts such as heptanedioic acid and azelaic acid on the nucleation behaviors of succinic acid, finding that increasing carbon chain length and additive concentration widens the metastable zone widths further.
CRYSTAL GROWTH & DESIGN
(2023)
Article
Chemistry, Multidisciplinary
Haoyu Peng, Ningning Tian, Changyou Yu, Ye Gao, Kangli Li, Hui Yan, Pengwei Zhao, Songgu Wu, Mingyang Chen, Junbo Gong
Summary: The experimental metastable zone widths of PE-DPE-H2O systems were measured using a polythermal method, and the nucleation behavior of PE and the influence of DPE on critical nucleus parameters were analyzed based on modified Sangwal's model and classical nucleation theory, respectively. The results show that dissolved DPE molecules can significantly affect the nucleation process.
CRYSTAL GROWTH & DESIGN
(2022)
Article
Chemistry, Multidisciplinary
Zhiyu Liao, Klaas Wynne
Summary: Research on laser-induced crystal nucleation shows that the presence of amorphous intermediates is a general requirement for nucleation.
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2022)
Article
Energy & Fuels
Benben Jiang, Marc D. Berliner, Kun Lai, Patrick A. Asinger, Hongbo Zhao, Patrick K. Herring, Martin Z. Bazant, Richard D. Braatz
Summary: The article proposes a fast-charging Bayesian optimization strategy that efficiently samples without the need for first-principles models, optimizing charging schemes to reduce charging time for lithium-ion batteries by considering degradation constraints. Research shows that the probability-of-improvement acquisition function performs better in reducing charging time compared to lower confidence bound and expected improvement acquisition functions.
Article
Chemistry, Multidisciplinary
Georgios Katsikis, Iris E. Hwang, Wade Wang, Vikas S. Bhat, Nicole L. McIntosh, Omair A. Karim, Bartlomiej J. Blus, Sha Sha, Vincent Agache, Jacqueline M. Wolfrum, Stacy L. Springs, Anthony J. Sinskey, Paul W. Barone, Richard D. Braatz, Scott R. Manalis
Summary: Quantifying the composition of viral vectors is crucial for vaccine development and gene therapy. Traditional methods are time-consuming, while emerging methods using optical or charge properties enable quick measurement of viral vector mass.
Article
Computer Science, Interdisciplinary Applications
Pavan K. Inguva, Kaylee C. Schickel, Richard D. Braatz
Summary: This study introduces a finite difference scheme at the limit of numerical stability, which has very low computational cost and zero discretization error for certain classes of PBMs, showing good performance in various applications.
COMPUTERS & CHEMICAL ENGINEERING
(2022)
Article
Computer Science, Interdisciplinary Applications
Pil Rip Jeon, Moo Sun Hong, Richard D. Braatz
Summary: This article introduces the properties of a compact DANN model structure called the standard normal operator form (SNOF) and its application in the data-driven modelling of nonlinear dynamical systems. The study demonstrates that, compared to popular DANN model structures, SNOF can achieve the same model identification error with fewer neurons. A case study on a multi-stage bioreactor reveals the potential of SNOF in modelling highly nonlinear dynamical systems, suggesting its use as a basis for the design of model-based optimal control systems with theoretical guarantees of closed-loop stability and performance.
COMPUTERS & CHEMICAL ENGINEERING
(2022)
Article
Computer Science, Interdisciplinary Applications
Joachim Schaeffer, Richard D. Braatz
Summary: This article introduces an interactive software, the Latent Variable Demonstrator (LAVADE), for teaching and understanding latent variable methods. LAVADE helps students to choose appropriate methods, tune hyperparameters, and interpret model coefficients, fostering a conceptual understanding of algorithm differences.
COMPUTERS & CHEMICAL ENGINEERING
(2022)
Article
Electrochemistry
Marc D. Berliner, Benben Jiang, Daniel A. Cogswell, Martin Z. Bazant, Richard D. Braatz
Summary: This article introduces General Operating Modes (GOMs) that go beyond conventional modes and allow simulation of novel operating modes for batteries. It also proposes a hybrid solution for constrained charging problem, enabling real-time implementation of nonlinear model predictive control (NMPC) using sophisticated physics-based battery models.
JOURNAL OF THE ELECTROCHEMICAL SOCIETY
(2022)
Article
Automation & Control Systems
Anastasia Nikolakopoulou, Moo Sun Hong, Richard D. Braatz
Summary: This article presents a synthesis method for full dynamic state feedback controllers and state and output observers that have guaranteed properties for systems approximated by dynamic artificial neural networks. The method uses linear matrix inequalities and quadratic Lyapunov function to derive sufficient conditions for controller synthesis and observer design. It is applicable to the practical situation where the steady-state values for the control input are not known.
Review
Biotechnology & Applied Microbiology
Christopher T. Canova, Pavan K. Inguva, Richard D. Braatz
Summary: Viral systems are crucial in biotechnology and medicine, but their commercial-scale production remains inefficient. Computational strategies offer potential for improving process development, optimization, and control, but require mathematical models. This article reviews mechanistic modeling strategies for viral particle production at cellular and bioreactor scales, adapting techniques and models from adjacent fields. These process models can be used for in-silico testing of novel process operating strategies and advanced process control.
BIOTECHNOLOGY AND BIOENGINEERING
(2023)
Article
Computer Science, Interdisciplinary Applications
Pavan K. Inguva, Richard D. Braatz
Summary: Multidimensional population balance models (PBMs) are used to describe chemical and biological processes with distribution over multiple intrinsic properties. We propose a low-cost finite difference scheme based on operator splitting that achieves a discretization error of zero for certain classes of PBMs. The scheme exploits the commutative property of the differential operators and can be computationally efficient.
COMPUTERS & CHEMICAL ENGINEERING
(2023)
Article
Computer Science, Interdisciplinary Applications
Prakitr Srisuma, Ajinkya Pandit, Qihang Zhang, Moo Sun Hong, Janaka Gamekkanda, Fabio Fachin, Nathan Moore, Dragan Djordjevic, Michael Schwaerzler, Tolutola Oyetunde, Wenlong Tang, Allan S. Myerson, George Barbastathis, Richard D. Braatz
Summary: This article presents the design of an observer for a Stefan problem in cell therapy, where frozen cells need to be thawed before injection. The dynamic model is simulated using a finite difference scheme and the method of lines on a moving grid. A Luenberger observer is designed based on the continuous-time moving-boundary moving-grid equations and real-time thermal imaging. Results from simulations and experiments demonstrate that the integrated numerical model and observer can accurately predict the spatiotemporal evolution of thawing with errors of 1%-2% throughout the cell thawing process, providing a reliable approach for state estimation and monitoring of cell thawing.
COMPUTERS & CHEMICAL ENGINEERING
(2023)
Article
Materials Science, Multidisciplinary
J. Lund, H. Wang, R. D. Braatz, R. E. Garcia
Summary: By utilizing a machine learning method based on custom two-step k-nearest neighbor strategy, the properties of materials can be inferred rapidly, significantly faster than traditional approaches. When combined with thermodynamic models, it can be applied to reconstruct CALPHAD formulations and identify new stable and metastable phases for various applications, such as lithium-ion batteries.
MATERIALS ADVANCES
(2022)
Proceedings Paper
Automation & Control Systems
Marc D. Berliner, Daniel A. Cogswell, Martin Z. Bazant, Richard D. Braatz
Summary: This article discusses fast charging for lithium-ion batteries and proposes physics-based operating modes to ensure safety and minimal degradation. By simulating different charging protocols, it is found that physics-based protocols achieve higher charge capacity in a shorter time, with relatively low computational cost.
Review
Chemistry, Multidisciplinary
Marian Chatenet, Bruno G. Pollet, Dario R. Dekel, Fabio Dionigi, Jonathan Deseure, Pierre Millet, Richard D. Braatz, Martin Z. Bazant, Michael Eikerling, Iain Staffell, Paul Balcombe, Yang Shao-Horn, Helmut Schaefer
Summary: This article explores the use of hydrogen as a sustainable energy carrier, focusing on electrocatalytic water splitting. It covers the fundamentals of the process, the latest scientific findings, and the current industrial processes and large-scale applications. The article also discusses strategies for optimizing electrode materials and includes a technoeconomic analysis of water electrolysis. Overall, it aims to promote collaboration and exchange among researchers in different fields.
CHEMICAL SOCIETY REVIEWS
(2022)
Article
Chemistry, Physical
Sanket Diwale, Maximilian K. Eisner, Corinne Carpenter, Weike Sun, Gregory C. Rutledge, Richard D. Braatz
Summary: An augmented Bayesian optimization approach is proposed for materials discovery in the presence of noisy and unreliable measurements. The approach is validated and characterized using a challenging case study of discovering additives for promoting nucleation of polyethylene crystals. The results show that the discovered candidates exhibit nearly optimal performance, and the Bayesian optimization using noise-augmented acquisition function and batched sampling achieves high accuracy and improved robustness against noise.
MOLECULAR SYSTEMS DESIGN & ENGINEERING
(2022)
Proceedings Paper
Automation & Control Systems
Hoang Hai Nguyen, Tim Zieger, Sandra C. Wells, Anastasia Nikolakopoulou, Richard D. Braatz, Rolf Findeisen
Summary: Providing stability guarantees for controllers using neural networks is challenging. A robust control framework is derived to provide stability guarantees for a known nominal system controlled by a learning-based neural network controller. The controller is reformulated into a diagonal nonlinear differential form to establish closed-loop stability conditions based on sector-bounded activation functions and globally bounded slopes.
2021 AMERICAN CONTROL CONFERENCE (ACC)
(2021)
