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Emissions from Hydrogen Peroxide Disinfection and Their Interaction with Mask Surfaces 过氧化氢消毒排放物及其与面罩表面的相互作用
ACS Engineering Au Pub Date : 2024-01-09 DOI: 10.1021/acsengineeringau.3c00036
Pearl Abue, Nirvan Bhattacharyya, Mengjia Tang, Leif G. Jahn, Daniel Blomdahl, David T. Allen, Richard L. Corsi, Atila Novoselac, Pawel K. Mistzal and Lea Hildebrandt Ruiz*, 
{"title":"Emissions from Hydrogen Peroxide Disinfection and Their Interaction with Mask Surfaces","authors":"Pearl Abue,&nbsp;Nirvan Bhattacharyya,&nbsp;Mengjia Tang,&nbsp;Leif G. Jahn,&nbsp;Daniel Blomdahl,&nbsp;David T. Allen,&nbsp;Richard L. Corsi,&nbsp;Atila Novoselac,&nbsp;Pawel K. Mistzal and Lea Hildebrandt Ruiz*,&nbsp;","doi":"10.1021/acsengineeringau.3c00036","DOIUrl":"10.1021/acsengineeringau.3c00036","url":null,"abstract":"<p >A rise in the disinfection of spaces occurred as a result of the COVID-19 pandemic as well as an increase in people wearing facial coverings. Hydrogen peroxide was among the recommended disinfectants for use against the virus. Previous studies have investigated the emissions of hydrogen peroxide associated with the disinfection of spaces and masks; however, those studies did not focus on the emitted byproducts from these processes. Here, we simulate the disinfection of an indoor space with H<sub>2</sub>O<sub>2</sub> while a person wearing a face mask is present in the space by using an environmental chamber with a thermal manikin wearing a face mask over its breathing zone. We injected hydrogen peroxide to disinfect the space and utilized a chemical ionization mass spectrometer (CIMS) to measure the primary disinfectant (H<sub>2</sub>O<sub>2</sub>) and a Vocus proton transfer reaction time-of-flight mass spectrometer (Vocus PTR-ToF-MS) to measure the byproducts from disinfection, comparing concentrations inside the chamber and behind the mask. Concentrations of the primary disinfectant and the byproducts inside the chamber and behind the mask remained elevated above background levels for 2–4 h after disinfection, indicating the possibility of extended exposure, especially when continuing to wear the mask. Overall, our results point toward the time-dependent impact of masks on concentrations of disinfectants and their byproducts and a need for regular mask change following exposure to high concentrations of chemical compounds.</p>","PeriodicalId":29804,"journal":{"name":"ACS Engineering Au","volume":null,"pages":null},"PeriodicalIF":0.0,"publicationDate":"2024-01-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.acs.org/doi/epdf/10.1021/acsengineeringau.3c00036","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"139412753","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
Modeling of Shear Flows over Superhydrophobic Surfaces: From Newtonian to Non-Newtonian Fluids 超疏水表面剪切流建模:从牛顿流体到非牛顿流体
ACS Engineering Au Pub Date : 2024-01-04 DOI: 10.1021/acsengineeringau.3c00048
Hossein Rahmani, Faïçal Larachi and Seyed Mohammad Taghavi*, 
{"title":"Modeling of Shear Flows over Superhydrophobic Surfaces: From Newtonian to Non-Newtonian Fluids","authors":"Hossein Rahmani,&nbsp;Faïçal Larachi and Seyed Mohammad Taghavi*,&nbsp;","doi":"10.1021/acsengineeringau.3c00048","DOIUrl":"10.1021/acsengineeringau.3c00048","url":null,"abstract":"<p >The design and use of superhydrophobic surfaces have gained special attentions due to their superior performances and advantages in many flow systems, e.g., in achieving specific goals including drag reduction and flow/droplet handling and manipulation. In this work, we conduct a brief review of shear flows over superhydrophobic surfaces, covering the classic and recent studies/trends for both Newtonian and non-Newtonian fluids. The aim is to mainly review the relevant mathematical and numerical modeling approaches developed during the past 20 years. Considering the wide ranges of applications of superhydrophobic surfaces in Newtonian fluid flows, we attempt to show how the developed studies for the Newtonian shear flows over superhydrophobic surfaces have been evolved, through highlighting the major breakthroughs. Despite the fact that, in many practical applications, flows over superhydrophobic surfaces may show complex non-Newtonian rheology, interactions between the non-Newtonian rheology and superhydrophobicity have not yet been well understood. Therefore, in this Review, we also highlight emerging recent studies addressing the shear flows of shear-thinning and yield stress fluids in superhydrophobic channels. We focus on reviewing the models developed to handle the intricate interaction between the formed liquid/air interface on superhydrophobic surfaces and the overlying flow. Such an intricate interaction will be more complex when the overlying flow shows nonlinear non-Newtonian rheology. We conclude that, although our understanding on the Newtonian shear flows over superhydrophobic surfaces has been well expanded via analyzing various aspects of such flows, the non-Newtonian counterpart is in its early stages. This could be associated with either the early applications mainly concerning Newtonian fluids or new complexities added to an already complex problem by the nonlinear non-Newtonian rheology. Finally, we discuss the possible directions for development of models that can address complex non-Newtonian shear flows over superhydrophobic surfaces.</p>","PeriodicalId":29804,"journal":{"name":"ACS Engineering Au","volume":null,"pages":null},"PeriodicalIF":0.0,"publicationDate":"2024-01-04","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.acs.org/doi/epdf/10.1021/acsengineeringau.3c00048","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"139373962","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
Biocompatible Cs2PtX6 (X = Cl, Br, I) Vacancy Ordered Perovskites and Shewanella oneidensis MR-1 Bacteria Hybrid for Potential Photocatalytic Solar Fuel Production 具有生物兼容性的 Cs2PtX6(X = Cl、Br、I)空位有序包晶石与 Shewanella oneidensis MR-1 细菌杂交,用于生产潜在的光催化太阳能燃料
ACS Engineering Au Pub Date : 2023-12-26 DOI: 10.1021/acsengineeringau.3c00061
Shweta Shinde, Muhammed Hamdan, Prerna Bhalla and Aravind Kumar Chandiran*, 
{"title":"Biocompatible Cs2PtX6 (X = Cl, Br, I) Vacancy Ordered Perovskites and Shewanella oneidensis MR-1 Bacteria Hybrid for Potential Photocatalytic Solar Fuel Production","authors":"Shweta Shinde,&nbsp;Muhammed Hamdan,&nbsp;Prerna Bhalla and Aravind Kumar Chandiran*,&nbsp;","doi":"10.1021/acsengineeringau.3c00061","DOIUrl":"10.1021/acsengineeringau.3c00061","url":null,"abstract":"<p >Semiconductor-bacterial hybrid systems have been shown to be effective for photochemical conversion. The combination of two systems delineates the light absorption from the catalytic ability, wherein a semiconductor absorbs light, generating an electron–hole pair, followed by the transfer of photogenerated charges to catalytically active bacteria that assume the roles of carrying out redox reactions. The halide perovskite materials possess excellent optoelectronic properties and, if they exhibit biocompatibility with microorganisms, shall provide an opportunity to carry out environmentally important redox reactions including carbon dioxide conversion to value added products. In this work, we report the biocompatibility of panchromatic visible light absorption and stable vacancy ordered halide perovskite (VOP), Cs<sub>2</sub>PtX<sub>6</sub> (X = halide) with <i>Shewanella oneidensis</i> MR-1 nonphotosynthetic bacterium. This microbe is shown to grow in culture media containing VOP, and the growth rate is found to be unaffected by the presence of semiconductor media. Although <i>Shewanella oneidensis</i> MR-1 is a well-known metal-reducing bacteria, in this work, we find that the vacancy ordered perovskite materials remain intact with this bacterium. With constraint-based metabolic modeling, we report that this biohybrid system shall potentially be used for solar energy conversion of water and carbon dioxide to hydrogen and formate, respectively.</p>","PeriodicalId":29804,"journal":{"name":"ACS Engineering Au","volume":null,"pages":null},"PeriodicalIF":0.0,"publicationDate":"2023-12-26","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.acs.org/doi/epdf/10.1021/acsengineeringau.3c00061","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"139052474","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
Using Active Learning for the Computational Design of Polymer Molecular Weight Distributions 利用主动学习进行聚合物分子量分布的计算设计
ACS Engineering Au Pub Date : 2023-12-25 DOI: 10.1021/acsengineeringau.3c00056
Haifan Zhou, Yue Fang and Hanyu Gao*, 
{"title":"Using Active Learning for the Computational Design of Polymer Molecular Weight Distributions","authors":"Haifan Zhou,&nbsp;Yue Fang and Hanyu Gao*,&nbsp;","doi":"10.1021/acsengineeringau.3c00056","DOIUrl":"10.1021/acsengineeringau.3c00056","url":null,"abstract":"<p >The design of the reaction conditions is essential for controlling polymerization to synthesize polymers with desired properties. However, the experimental screening of the reaction conditions can be time-consuming and costly. Computational methods such as kinetic Monte Carlo (KMC) simulations have been developed to assist with the design of experiments. Nevertheless, when the dimensions of the reaction conditions to be explored are large, the simulation models might still not be able to meet the demand for efficient screening and design. Active learning can be used to tackle this problem by designing data acquisition strategies that can minimize the labeling required to construct a good surrogate model in the design space. In this work, we combined a cluster-maximum model change (CMMC) model with KMC simulations, which can precisely design polymerization conditions at the lowest computational cost for the desired molecular weight distributions. The case study results show that the CMMC model only uses 50 KMC simulations to construct a predictive model with a 10% relative error for a system with 4 design parameters, which greatly reduces the computational cost while maintaining accuracy.</p>","PeriodicalId":29804,"journal":{"name":"ACS Engineering Au","volume":null,"pages":null},"PeriodicalIF":0.0,"publicationDate":"2023-12-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.acs.org/doi/epdf/10.1021/acsengineeringau.3c00056","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"139052379","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
Tailored Platinum Group Metal/Spinel Oxide Catalysts for Dynamically Enhanced Methane Oxidation 用于动态增强甲烷氧化的定制铂族金属/尖晶石氧化物催化剂
ACS Engineering Au Pub Date : 2023-12-23 DOI: 10.1021/acsengineeringau.3c00053
Pak Wing Chen, Debtanu Maiti, Ru-Fen Liu, Lars C. Grabow* and Michael P. Harold*, 
{"title":"Tailored Platinum Group Metal/Spinel Oxide Catalysts for Dynamically Enhanced Methane Oxidation","authors":"Pak Wing Chen,&nbsp;Debtanu Maiti,&nbsp;Ru-Fen Liu,&nbsp;Lars C. Grabow* and Michael P. Harold*,&nbsp;","doi":"10.1021/acsengineeringau.3c00053","DOIUrl":"10.1021/acsengineeringau.3c00053","url":null,"abstract":"<p >A combined experimental and molecular modeling study identifies a family of spinel oxides that in combination with PGM (platinum group metals) provide enhanced methane oxidation activity. With a reduction in greenhouse gas (GHG) emissions urgently needed, there is renewed interest in the use of natural gas vehicles (NGVs) and engines (NGEs) for transportation, commerce, and industrial applications. NGVs and NGEs emit less CO<sub>2</sub> than their petroleum-derived counterparts but may emit uncombusted methane, an even more potent GHG. For stoichiometric engines, methane oxidation catalysts containing PGM and spinel oxide in layered architectures offer increased methane oxidation activity and lower light-off temperatures (<i>T</i><sub>50</sub>). The reducible spinel oxide has direct and indirect roles that are effectively described by the bulk oxygen vacancy formation energy (<i>E</i><sub>vac</sub>). We apply density functional theory (DFT) to identify several earth-abundant, cobalt-rich spinel oxides with favorable <i>E</i><sub>vac</sub>, shown to correlate with dynamic oxygen storage capacity (DOSC) and CO and H<sub>2</sub> oxidation activity. We experimentally rank-order the DFT-identified spinel oxides in combination with Pt+Pd for their methane oxidation activity measurements, under both time-invariant and modulated feed conditions. We show good agreement between the activity and the DFT-computed reducibility of the spinel oxide. The findings suggest spinel reducibility is a key factor in achieving enhanced low-temperature methane conversion, enabled through a balance of methane activation on the PGM sites and subsequent oxidation of the intermediates and byproducts on spinel oxides. In agreement with its computationally predicted <i>E</i><sub>vac</sub>, NiCo<sub>2</sub>O<sub>4</sub> was confirmed to have the highest DOSC and lowest <i>T</i><sub>50</sub> among the tested spinel samples.</p>","PeriodicalId":29804,"journal":{"name":"ACS Engineering Au","volume":null,"pages":null},"PeriodicalIF":0.0,"publicationDate":"2023-12-23","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.acs.org/doi/epdf/10.1021/acsengineeringau.3c00053","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"139029134","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
Optimizing Energy Efficiency of a Twin-Screw Granulation Process in Real-Time Using a Long Short-Term Memory (LSTM) Network 利用长短期记忆(LSTM)网络实时优化双螺杆造粒工艺的能效
ACS Engineering Au Pub Date : 2023-12-21 DOI: 10.1021/acsengineeringau.3c00038
Chaitanya Sampat,  and , Rohit Ramachandran*, 
{"title":"Optimizing Energy Efficiency of a Twin-Screw Granulation Process in Real-Time Using a Long Short-Term Memory (LSTM) Network","authors":"Chaitanya Sampat,&nbsp; and ,&nbsp;Rohit Ramachandran*,&nbsp;","doi":"10.1021/acsengineeringau.3c00038","DOIUrl":"10.1021/acsengineeringau.3c00038","url":null,"abstract":"<p >Traditional pharmaceutical manufacturing processes for solid oral dosage forms can be inefficient and have been known to produce a large amount of undesired product. With the progressing trend of achieving carbon neutrality, there is an impetus to increase the energy efficiency of these manufacturing processes while maintaining the critical quality attributes of the product. One of the important steps in downstream pharmaceutical manufacturing is wet granulation, and within that, twin screw granulation (TSG) is a popular continuous manufacturing technique. In this study, the energy efficiency of the TSG process was maximized by combining a long-term memory (LSTM) model with an optimization algorithm. The LSTM model was trained on time-series process data obtained from the TSG experimental runs. The optimization process, with the objective of maximizing energy efficiency, was performed using a stochastic optimization algorithm, and constraints were enforced on the process parameter design space. Experimental runs at the optimal process parameters were conducted on the TSG equipment with updates occurring at predefined intervals depending on the optimization scenarios. The purpose of these experimental runs was to validate the capability of increasing the overall process energy efficiency when operating at the optimized process parameters. A maximum increase of 27% was obtained between two tested optimization scenarios while maintaining the yield of the granules at the end of the twin-screw granulation process.</p>","PeriodicalId":29804,"journal":{"name":"ACS Engineering Au","volume":null,"pages":null},"PeriodicalIF":0.0,"publicationDate":"2023-12-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.acs.org/doi/epdf/10.1021/acsengineeringau.3c00038","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"138950400","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
Scaling Up 3D-Printed Porous Reactors for the Continuous Synthesis of 2,5-Diformylfuran 放大三维打印多孔反应器以连续合成 2,5-二甲酰基呋喃
ACS Engineering Au Pub Date : 2023-12-18 DOI: 10.1021/acsengineeringau.3c00064
Dionysia Koufou,  and , Simon Kuhn*, 
{"title":"Scaling Up 3D-Printed Porous Reactors for the Continuous Synthesis of 2,5-Diformylfuran","authors":"Dionysia Koufou,&nbsp; and ,&nbsp;Simon Kuhn*,&nbsp;","doi":"10.1021/acsengineeringau.3c00064","DOIUrl":"10.1021/acsengineeringau.3c00064","url":null,"abstract":"<p >The present study investigates the potential for scaling up 3D-printed porous reactors at the millimeter scale by integrating different reactor configurations in series. These reactor configurations, ranging from a single reactor (<i>N</i> = 1) to six reactors in series (<i>N</i> = 6), were evaluated for their performance in terms of axial dispersion in a gas–liquid system, with a focus on identifying potential dead zones. The scaled-up reactor systems exhibited a reduced deviation from plug flow behavior, mainly attributed to improved radial mixing maintained throughout the entire length of the porous structures. Among the various configurations tested, the scaled-up system featuring six reactors displayed the highest coefficient of variation (CoV) at approximately 24% for residence times exceeding 100 s. In all cases, the presence of stagnant zones influenced the shape of the residence time distribution (RTD) curves, although in the scaled-up system these stagnant zones did not significantly impact the overall performance or the yield of 2,5-diformylfuran (DFF). This was due to the narrow RTD and effective mass transfer between the stagnant and active flow compartments. Notably, the selectivity remained at 100%, and the highest yield of DFF (approximately 81%) was achieved for a residence time of 6.61 min in the scaled-up system. Despite introducing mass transfer limitations when operating at the millimeter scale, the scaled-up system achieved DFF productivity levels comparable to microreaction systems at significantly lower energy dissipation.</p>","PeriodicalId":29804,"journal":{"name":"ACS Engineering Au","volume":null,"pages":null},"PeriodicalIF":0.0,"publicationDate":"2023-12-18","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.acs.org/doi/epdf/10.1021/acsengineeringau.3c00064","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"138818502","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 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":null,"pages":null},"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":null,"pages":null},"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":null,"pages":null},"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
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