ACS Engineering Au最新文献

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A Review on the Modeling and Simulation of Shaft Furnace Hydrogen Metallurgy: A Chemical Engineering Perspective 竖炉氢冶金建模与仿真综述:化学工程视角
ACS Engineering Au Pub Date : 2023-12-12 DOI: 10.1021/acsengineeringau.3c00033
Yang Fei, Xiaoping Guan, Shibo Kuang, Aibing Yu and Ning Yang*, 
{"title":"A Review on the Modeling and Simulation of Shaft Furnace Hydrogen Metallurgy: A Chemical Engineering Perspective","authors":"Yang Fei,&nbsp;Xiaoping Guan,&nbsp;Shibo Kuang,&nbsp;Aibing Yu and Ning Yang*,&nbsp;","doi":"10.1021/acsengineeringau.3c00033","DOIUrl":"10.1021/acsengineeringau.3c00033","url":null,"abstract":"<p >Hydrogen-based shaft furnace technology holds promise for low-carbon hydrogen metallurgy. Since hydrogen-assisted iron ore reduction is highly endothermic, inadequate heat supply relevant to the contact of gas and densely packed ores may reduce the rate and efficiency of reductions. The key to addressing this issue lies in understanding the competition among heat supply, heat transfer, and heat loss driven by the gas flow around ores and reactions within them. Modeling and simulation are crucial for revealing the underlying mechanisms and promoting process scale-up and intensification. This review summarizes previous efforts in physical modeling and model applications for improving the reduction performance. The discrete element method (DEM) and computational fluid dynamics (CFD)–DEM models have been used for particle-scale simulation to investigate inhomogeneous particle descent and relevant particle–particle interactions. For macroscale simulations, steady-state simplified models such as plug flow and REDUCTOR, as well as the Eulerian two-phase model, have been developed by considering heat and mass transfer. Based on these model applications, strategies including the optimization of operating conditions and gas-feeding methods have been proposed to improve the furnace performance. Further numerical efforts are needed to analyze the in-furnace heat evolution and reduction and reveal the competitiveness of flow, transport, and reaction by incorporating multiscale physics in shaft furnaces. Additionally, attention could be paid to the effects of particle sticking and degradation on reduction, which may be more serious when the proportion of lump ores increases. When evaluating relative optimization strategies, comprehensive comparisons are expected in terms of iron ore reduction degree, gas utilization rate, energy consumption, and economic feasibility under various reducing and cooling gas operating conditions and furnace profiles to offer practical guidelines for industrial design and intensification.</p>","PeriodicalId":29804,"journal":{"name":"ACS Engineering Au","volume":"4 2","pages":"145–165"},"PeriodicalIF":0.0,"publicationDate":"2023-12-12","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.acs.org/doi/epdf/10.1021/acsengineeringau.3c00033","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"138581775","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Decarbonizing the Gas-to-Liquid (GTL) Process Using an Advanced Reforming of Methane Process 利用先进的甲烷重整工艺实现气液化 (GTL) 过程的去碳化
ACS Engineering Au Pub Date : 2023-12-11 DOI: 10.1021/acsengineeringau.3c00025
Zeinab Ataya, Mohamed Challiwala, Gasim Ibrahim, Hanif A. Choudhury, Mahmoud M. El-Halwagi and Nimir O. Elbashir*, 
{"title":"Decarbonizing the Gas-to-Liquid (GTL) Process Using an Advanced Reforming of Methane Process","authors":"Zeinab Ataya,&nbsp;Mohamed Challiwala,&nbsp;Gasim Ibrahim,&nbsp;Hanif A. Choudhury,&nbsp;Mahmoud M. El-Halwagi and Nimir O. Elbashir*,&nbsp;","doi":"10.1021/acsengineeringau.3c00025","DOIUrl":"10.1021/acsengineeringau.3c00025","url":null,"abstract":"<p >The gas-to-liquid (GTL) process is a promising technology for converting natural gas into synthetic fuels and chemicals. However, its high carbon dioxide (CO<sub>2</sub>) emissions present significant challenges. Methane reforming contributes up to 60% of GTL’s CO<sub>2</sub> emissions, necessitating decarbonization. Dry reforming of methane (DRM) shows potential for CO<sub>2</sub> conversion. Still, it faces challenges such as high energy requirements, catalyst deactivation, and an incompatible hydrogen-to-carbon monoxide (H<sub>2</sub>/CO) ratio for GTL processing, requiring extensive research. A previous study proposed a two-reactor system known as CARGEN that co-produces solid carbon (in the form of multiwalled carbon nanotubes [MWCNTs]) and syngas, reducing CO<sub>2</sub> emissions by 40% compared to the benchmark autothermal reforming (ATR) process through life cycle assessment (LCA) studies. This paper presents a comprehensive simulation of the advanced DRM process used to retrofit an existing ATR-based GTL plant─initially, a 50,000 bbl./day ATR-based GTL plant is simulated. The advanced reformer process replaces ATR through retrofitting. Comparative analysis shows a remarkable 73% reduction in net CO<sub>2</sub> emissions and the potential coproduction of 243 kg of MWCNTs per barrel of syncrude, equivalent to 12,150 tons/day of MWCNTs. However, the advanced reformer-based GTL plant requires 61% more natural gas feedstock while utilizing 79% less oxygen than the ATR-based plant. Furthermore, a separate techno-economic analysis examines the advanced reformer-based GTL plant based on a calculation for 13,100 tons/day of CO<sub>2</sub> feedstock to co-produce 3,277 tons/day of MWCNTs and 50,000 barrels/day of syncrude. This analysis, considering a 25% tax rate, 25-year plant life, and zero salvage value, demonstrates an attractive 10-year payback period at selling prices of 80 USD/bbl. for syncrude and 10 USD/kg for MWCNTs. These results provide a process system-level perspective, showcasing the advanced reformer-based GTL plant (CARGEN Process) as an effective solution for low-carbon GTL production.</p>","PeriodicalId":29804,"journal":{"name":"ACS Engineering Au","volume":"4 1","pages":"99–111"},"PeriodicalIF":0.0,"publicationDate":"2023-12-11","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.acs.org/doi/epdf/10.1021/acsengineeringau.3c00025","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"138581813","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Electrified Catalysts for Endothermic Chemical Processes: Materials Needs, Advances, and Challenges 用于内热化学过程的电气化催化剂:材料需求、进展与挑战
ACS Engineering Au Pub Date : 2023-12-11 DOI: 10.1021/acsengineeringau.3c00051
Meghana Idamakanti, Elmer B. Ledesma, Ram R. Ratnakar, Michael P. Harold, Vemuri Balakotaiah and Praveen Bollini*, 
{"title":"Electrified Catalysts for Endothermic Chemical Processes: Materials Needs, Advances, and Challenges","authors":"Meghana Idamakanti,&nbsp;Elmer B. Ledesma,&nbsp;Ram R. Ratnakar,&nbsp;Michael P. Harold,&nbsp;Vemuri Balakotaiah and Praveen Bollini*,&nbsp;","doi":"10.1021/acsengineeringau.3c00051","DOIUrl":"10.1021/acsengineeringau.3c00051","url":null,"abstract":"<p >Large-scale endothermic chemical processes, as currently practiced, employ tubular reactors that are heated externally through the combustion of fossil fuels, and are highly carbon-intensive. Joule-heated reactors in which electric currents flowing through the catalyst are used to provide thermal energy <i>directly</i> through internal heating are rapidly emerging as an alternative to these conventional, externally heated reactors. Joule-heated reactors could help significantly improve modularity and also reduce the capital, energy, and carbon footprint associated with these enthalpically demanding processes. Development of these novel types of reactors, however, is predicated on overcoming catalyst design challenges encountered uniquely when supplying heat through the use of electric currents passing through catalyst substrates. We review herein some key advancements in catalyst design that have been achieved in the recent past, and highlight considerations critical to the novel mode of reactor operation proposed. We provide an overview of the various types of electrically heated catalysts proposed, methods used in their synthesis, and reactor performance of Joule-heated catalysts for a variety of applications. Also discussed are key knowledge gaps that will likely need to be addressed in an effort to accelerate deployment of this emerging class of reactors that could play a pivotal role in the decarbonization of energy-intensive large-scale chemical processes.</p>","PeriodicalId":29804,"journal":{"name":"ACS Engineering Au","volume":"4 1","pages":"71–90"},"PeriodicalIF":0.0,"publicationDate":"2023-12-11","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.acs.org/doi/epdf/10.1021/acsengineeringau.3c00051","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"138567047","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Electrocoagulation Process for Recovery of Precious Metals from Cyanide Leachates Using a Low Voltage 低电压电絮凝法回收氰化浸出液中的贵金属
ACS Engineering Au Pub Date : 2023-12-05 DOI: 10.1021/acsengineeringau.3c00041
Juan Carlos Soto-Uribe*, Jesus Leobardo Valenzuela-Garcia*, Maria Mercedes Salazar-Campoy*, José Refugio Parga-Torres, Víctor Manuel Vazquez-Vazquez, Martin Antonio Encinas-Romero and Guadalupe Martinez-Ballesteros, 
{"title":"Electrocoagulation Process for Recovery of Precious Metals from Cyanide Leachates Using a Low Voltage","authors":"Juan Carlos Soto-Uribe*,&nbsp;Jesus Leobardo Valenzuela-Garcia*,&nbsp;Maria Mercedes Salazar-Campoy*,&nbsp;José Refugio Parga-Torres,&nbsp;Víctor Manuel Vazquez-Vazquez,&nbsp;Martin Antonio Encinas-Romero and Guadalupe Martinez-Ballesteros,&nbsp;","doi":"10.1021/acsengineeringau.3c00041","DOIUrl":"10.1021/acsengineeringau.3c00041","url":null,"abstract":"<p >The cyanidation of gold ores with copper content is frequent in gold mines. Copper affects the performance and profits of mineral processing. The current technology for gold recovery from cyanide solutions usually involves the adsorption of the gold-cyanide complex ion on activated carbon; however, the copper affects this process. The process of electrocoagulation (EC) is a promising technique for gold and silver recovery with copper, where all of the metals can be recovered. This work used the electrocoagulation process (EC) to evaluate the metal recovery from a pregnant leach solution (PLS), where EC is a promising technique. This study aimed to determine the optimal parameter to recover the gold and silver and to see the effect of copper concentration in the PLS obtained by simultaneous pressure leaching/oxidation of a gold-bearing pyritic concentrate. EC tests were run to recover gold and silver over copper from PLS using aluminum electrodes and variables like distances between electrodes, pH, potential applied, and feeding flow for continuous EC. The chemical assay of cyanide leachates shows a concentration of 7.15 mg/L of gold, 305 mg/L of silver, and 351.5 mg/L of copper with 1810 mg/L of free cyanide. The results showed that the EC process recovered 99% of gold and copper and 92% of silver at a pH of 11, 8 mm of dE, and a potential applied 3 V in 10 min. However, under this condition in continuous EC with a flow rate of 40 mL/min, the recovery is 66.3% of gold, 85.8% of silver, and 45.3% of copper; compared with the batch process, the gold and silver decrease.</p>","PeriodicalId":29804,"journal":{"name":"ACS Engineering Au","volume":"4 1","pages":"139–144"},"PeriodicalIF":0.0,"publicationDate":"2023-12-05","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.acs.org/doi/epdf/10.1021/acsengineeringau.3c00041","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"138493036","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Mechanism of the Direct Reduction of Chromite Process as a Clean Ferrochrome Technology 铬铁矿直接还原法作为清洁铬铁技术的机理研究
ACS Engineering Au Pub Date : 2023-12-01 DOI: 10.1021/acsengineeringau.3c00057
Dogan Paktunc*, Jason P. Coumans, David Carter, Nail Zagrtdenov and Dominique Duguay, 
{"title":"Mechanism of the Direct Reduction of Chromite Process as a Clean Ferrochrome Technology","authors":"Dogan Paktunc*,&nbsp;Jason P. Coumans,&nbsp;David Carter,&nbsp;Nail Zagrtdenov and Dominique Duguay,&nbsp;","doi":"10.1021/acsengineeringau.3c00057","DOIUrl":"10.1021/acsengineeringau.3c00057","url":null,"abstract":"<p >Direct reduction of chromite (DRC) is a promising alternative process for ferrochrome production with the potential to significantly reduce energy consumption and greenhouse gas emissions compared to conventional smelting. In DRC, chromium (Cr) and iron (Fe) from chromite ore incongruently dissolve into a molten salt, which facilitates mass transfer to a carbon (C) reductant where in situ metallization occurs. Consequently, ferrochrome is produced below the slag melting temperatures, achieving substantial energy savings relative to smelting. However, there are significant knowledge gaps in the kinetics, Cr solubility, speciation, and coordination environment which are critical to understanding the fundamental mechanisms of molten salt-assisted carbothermic reactions. To address these knowledge gaps, we performed pyrometallurgical experiments with variable temperature and residence times and analyzed the composition of chromite, ferrochrome, and slag products along with determining the speciation of Cr. Our results indicate that the DRC mechanism can be explained by the following sequential steps: (1) incongruent dissolution of chromite, (2) reduction of dissolved Cr in molten salt/slag, (3) transport of Cr and Fe species in molten media, and (4) reduction on C particles and metallization as Cr–Fe alloys. The discovery of four types of reduced Cr species in the slag indicates that the reduction of Cr<sup>3+</sup> to Cr<sup>2+</sup> and Cr<sup>0</sup> occurred in the molten phase before metallization on solid carbon particles. Thermodynamically, the reduction of CrO(<i>l</i>) to Cr metal is more feasible at a lower temperature than it is for Cr<sub>2</sub>O<sub>3</sub>(<i>l</i>) corroborating the accelerated reduction efficiency of the DRC process.</p>","PeriodicalId":29804,"journal":{"name":"ACS Engineering Au","volume":"4 1","pages":"125–138"},"PeriodicalIF":0.0,"publicationDate":"2023-12-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.acs.org/doi/epdf/10.1021/acsengineeringau.3c00057","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"138496579","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Carbon Dioxide Capture, Utilization, and Sequestration: Current Status, Challenges, and Future Prospects for Global Decarbonization 二氧化碳的捕获、利用和封存:全球脱碳的现状、挑战和未来前景
ACS Engineering Au Pub Date : 2023-12-01 DOI: 10.1021/acsengineeringau.3c00049
Srinu Nagireddi, Jatin R. Agarwal* and Damodaran Vedapuri, 
{"title":"Carbon Dioxide Capture, Utilization, and Sequestration: Current Status, Challenges, and Future Prospects for Global Decarbonization","authors":"Srinu Nagireddi,&nbsp;Jatin R. Agarwal* and Damodaran Vedapuri,&nbsp;","doi":"10.1021/acsengineeringau.3c00049","DOIUrl":"10.1021/acsengineeringau.3c00049","url":null,"abstract":"<p >This Review provides an in-depth overview of carbon dioxide (CO<sub>2</sub>) capture, utilization, and sequestration (CCUS) technologies and their potential in global decarbonization efforts. The Review discusses the concept of CO<sub>2</sub> utilization, including conversion to fuels, chemicals, and minerals as well as biological processes. It also explores the different types of CO<sub>2</sub> sequestration, including geological, ocean, and mineral storage, and the associated challenges and opportunities such as regulatory issues and public acceptance. The Review highlights the potential of integrating CO<sub>2</sub> CCUS technologies and presents case studies of successful projects. The benefits and limitations of these technologies are discussed, along with areas for further research and development. Overall, this Review underscores the importance of CCUS.</p>","PeriodicalId":29804,"journal":{"name":"ACS Engineering Au","volume":"4 1","pages":"22–48"},"PeriodicalIF":0.0,"publicationDate":"2023-12-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.acs.org/doi/epdf/10.1021/acsengineeringau.3c00049","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"138496581","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
A Review of Traditional and Intensified Hydrometallurgy Techniques to Remove Chromium and Vanadium from Solid Industrial Waste 传统和强化湿法冶金法去除固体工业废物中铬、钒的研究进展
ACS Engineering Au Pub Date : 2023-12-01 DOI: 10.1021/acsengineeringau.3c00046
Aya Saidi, Rebecca El Khawaja and Daria C. Boffito*, 
{"title":"A Review of Traditional and Intensified Hydrometallurgy Techniques to Remove Chromium and Vanadium from Solid Industrial Waste","authors":"Aya Saidi,&nbsp;Rebecca El Khawaja and Daria C. Boffito*,&nbsp;","doi":"10.1021/acsengineeringau.3c00046","DOIUrl":"10.1021/acsengineeringau.3c00046","url":null,"abstract":"<p >The continuous growth of industrial activities, driven by economic expansion and technological advancements, has increased industrial waste generation. These wastes often contain hazardous substances, including heavy metals. Their improper disposal has become a significant environmental and health concern, necessitating global attention. To address this issue and mitigate the scarcity and cost of raw materials, recycling waste materials has emerged as a viable solution, particularly in the synthesis of construction materials. Various methods, such as pyrometallurgical and hydrometallurgical techniques, have been established for recycling industrial waste. This Review focuses on hydrometallurgical techniques, specifically targeting the separation of two highly toxic heavy metals: chromium and vanadium. It comprehensively explores various hydrometallurgical methods, including acid, alkaline, organic, and oxidative leaching, for solid waste materials. Additionally, this Review highlights several intensified leaching processes assisted by electrical fields, supercritical fluids, plasma, microwaves, and ultrasound. The presented methods offer promising approaches to effectively manage industrial waste.</p>","PeriodicalId":29804,"journal":{"name":"ACS Engineering Au","volume":"4 1","pages":"49–70"},"PeriodicalIF":0.0,"publicationDate":"2023-12-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.acs.org/doi/epdf/10.1021/acsengineeringau.3c00046","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"138496582","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Production of Sustainable Low-Layer Graphene by Green Synthesis at Room Conditions for Platinum-Based Direct Methanol Fuel Cell 室温绿色合成法制备铂基直接甲醇燃料电池用可持续低层石墨烯
ACS Engineering Au Pub Date : 2023-11-29 DOI: 10.1021/acsengineeringau.3c00040
Vildan Erduran, Ramazan Bayat, Iskender Isik, Tugba Bayazit and Fatih Şen*, 
{"title":"Production of Sustainable Low-Layer Graphene by Green Synthesis at Room Conditions for Platinum-Based Direct Methanol Fuel Cell","authors":"Vildan Erduran,&nbsp;Ramazan Bayat,&nbsp;Iskender Isik,&nbsp;Tugba Bayazit and Fatih Şen*,&nbsp;","doi":"10.1021/acsengineeringau.3c00040","DOIUrl":"10.1021/acsengineeringau.3c00040","url":null,"abstract":"<p >In this study, a cost-effective and scalable method for the production of low-layer graphene (LLG) using sodium percarbonate (SPC) as a green delamination agent and its application in fuel cells is proposed. The obtained graphene showed a decrease in signal height in XRD analysis, indicating thinner layers. Raman analysis confirmed the presence of 7–8 layers of graphene. Field-emission scanning electron microscopy analysis revealed a uniform crystal structure, making it suitable for various applications. Direct methanol fuel cells (DMFCs) are widely recognized as efficient and environmentally friendly devices for converting chemical energy to electrical energy. The utilization of graphene-supported platinum (Pt) nanoparticles (NPs) as catalysts in DMFCs enhances their performance. In this study, Pt-graphene catalysts were synthesized by the chemical reduction method with graphene obtained by using SPC. Characterization through XRD and SEM analyses confirmed the homogeneous distribution of NPs on the carbon support. As a result of methanol oxidation studies, 57.73 and 21.45 mA/cm<sup>2</sup> values were obtained by using Pt@LLG and Pt catalysts, respectively. As a result of long-term stability and durability tests, it has been found that the Pt@LLG catalyst can be used effectively in metal oxidation experiments.</p>","PeriodicalId":29804,"journal":{"name":"ACS Engineering Au","volume":"3 6","pages":"537–545"},"PeriodicalIF":0.0,"publicationDate":"2023-11-29","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.acs.org/doi/epdf/10.1021/acsengineeringau.3c00040","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"138496580","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
QRChEM: A Deep Learning Framework for Materials Property Prediction and Design Using QR Codes QRChEM:基于QR码的材料性能预测和设计的深度学习框架
ACS Engineering Au Pub Date : 2023-11-27 DOI: 10.1021/acsengineeringau.3c00055
Haripriyan Uthayakumar, Rahul Krishna K, Raj Jain, Rajnish Kumar and Tarak K. Patra*, 
{"title":"QRChEM: A Deep Learning Framework for Materials Property Prediction and Design Using QR Codes","authors":"Haripriyan Uthayakumar,&nbsp;Rahul Krishna K,&nbsp;Raj Jain,&nbsp;Rajnish Kumar and Tarak K. Patra*,&nbsp;","doi":"10.1021/acsengineeringau.3c00055","DOIUrl":"10.1021/acsengineeringau.3c00055","url":null,"abstract":"<p >Machine learning (ML) surrogate models are used for the rapid prediction of materials properties and are promising tools for accelerating new materials design and development. The performance and accuracy of these surrogate models appear to be intricately connected to the molecular representation that is employed. Developing efficient numerical representations of molecules is vital for the success of surrogate models in predicting materials' properties. Here, we propose a new machine-readable molecular representation, namely a molecular quick response (QR) code, for the deep learning of materials structure–property correlations. We built a convolutional deep neural network (CNN) model based on molecular QR codes, which is abbreviated as QRChEM. QRChEM was trained and validated using ∼21 000 data for four representative properties of small molecules, namely specific heat, enthalpy, zero-point vibrational energy, and HOMO–LUMO band gap. We show that QRChEM outperforms the commonly used Morgan fingerprint-based and one-hot encoding (OHE)-based deep learning frameworks. We further performed UMAP (uniform manifold approximation and projection) on the molecular QR codes to demonstrate the differentiability of the molecular topologies, which is vital for high-fidelity surrogate model development.</p>","PeriodicalId":29804,"journal":{"name":"ACS Engineering Au","volume":"4 1","pages":"91–98"},"PeriodicalIF":0.0,"publicationDate":"2023-11-27","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.acs.org/doi/epdf/10.1021/acsengineeringau.3c00055","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"138496578","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Competing Effects of Molecular Additives and Cross-Link Density on the Segmental Dynamics and Mechanical Properties of Cross-Linked Polymers 分子添加剂和交联密度对交联聚合物段动力学和机械特性的竞争效应
ACS Engineering Au Pub Date : 2023-11-09 DOI: 10.1021/acsengineeringau.3c00043
Wenjian Nie, Jack F. Douglas* and Wenjie Xia*, 
{"title":"Competing Effects of Molecular Additives and Cross-Link Density on the Segmental Dynamics and Mechanical Properties of Cross-Linked Polymers","authors":"Wenjian Nie,&nbsp;Jack F. Douglas* and Wenjie Xia*,&nbsp;","doi":"10.1021/acsengineeringau.3c00043","DOIUrl":"10.1021/acsengineeringau.3c00043","url":null,"abstract":"<p >The introduction of molecular additives into thermosets often results in changes in their dynamics and mechanical properties that can have significant ramifications for diverse applications of this broad class of materials such as coatings, high-performance composites, <i>etc</i>. Currently, there is limited fundamental understanding of how such additives influence glass formation in these materials, a problem of broader significance in glass-forming materials. To address this fundamental problem, here, we employ a simplified coarse-grained (CG) model of a polymer network as a model of thermoset materials and then introduce a polymer additive having the same inherent rigidity and polymer–polymer interaction strength as the cross-linked polymer matrix. This energetically “neutral” or “self-plasticizing” additive model gives rise to non-trivial changes in the dynamics of glass formation and provides an important theoretical reference point for the technologically more important case of interacting additives. Based on this rather idealized model, we systematically explore the combined effect of varying the additive mass percentage (<i>m</i>) and cross-link density (<i>c</i>) on the segmental relaxation dynamics and mechanical properties of a model thermoset material with additives. We find that increasing the additive mass percentage <i>m</i> progressively decreases both the glass-transition temperature <i>T</i><sub>g</sub> and the fragility of glass formation, a trend <i>opposite</i> to increasing <i>c</i> so that these thermoset variables clearly have a <i>competing effect</i> on glass formation in these model materials. Moreover, basic mechanical properties (<i>i.e.</i>, bulk, shear, and tensile moduli) likewise exhibit a competitive variation with the increase of <i>m</i> and <i>c</i>, which are strongly correlated with the Debye–Waller parameter ⟨<i>u</i><sup>2</sup>⟩, a measure of material stiffness at a molecular scale. Our findings prove beneficial in the development of structure–property relationships for the cross-linked polymers, which could help guide the design of such network materials with tailored physical properties.</p>","PeriodicalId":29804,"journal":{"name":"ACS Engineering Au","volume":"3 6","pages":"512–526"},"PeriodicalIF":0.0,"publicationDate":"2023-11-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.acs.org/doi/epdf/10.1021/acsengineeringau.3c00043","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"135242811","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
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