ACS Engineering Au最新文献

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Magnetowetting Dynamics of Compound Droplets 复合液滴的磁etting动力学
ACS Engineering Au Pub Date : 2024-09-19 DOI: 10.1021/acsengineeringau.4c00023
Debdeep Bhattacharjee, Suman Chakraborty, Arnab Atta
{"title":"Magnetowetting Dynamics of Compound Droplets","authors":"Debdeep Bhattacharjee, Suman Chakraborty, Arnab Atta","doi":"10.1021/acsengineeringau.4c00023","DOIUrl":"https://doi.org/10.1021/acsengineeringau.4c00023","url":null,"abstract":"Understanding the spreading dynamics of compound droplets is crucial for emerging applications like micromixers, microreactors, and mechano-responsive artificial cells. Integrating magnetic fields expands the potential of these technologies in soft robotics and medical imaging. Despite extensive research on individual droplets, the magnetowetting processes of compound droplets on hydrophobic surfaces remain underexplored. To address this gap, we use a finite element framework to conduct numerical simulations, focusing on the spreading behavior of compound droplets on hydrophobic surfaces under magnetic fields. Our approach is validated against experimental and theoretical paradigms from existing single-droplet studies. Additionally, we verify our model for the temporal evolution of compound droplet wetting in the absence of magnetic fields against existing numerical results. This research systematically explores wetting behaviors and shell fluid disintegration by manipulating key parameters, including magnetic field intensity and inner-to-outer droplet size ratios. These findings have significant implications for enhancing magnetically controlled soft fluidic systems, particularly in digital microfluidics and drug development.","PeriodicalId":29804,"journal":{"name":"ACS Engineering Au","volume":null,"pages":null},"PeriodicalIF":0.0,"publicationDate":"2024-09-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142264623","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Synthesis and Characterization of Dy2O3@TiO2 Nanocomposites for Enhanced Photocatalytic and Electrocatalytic Applications 用于增强光催化和电催化应用的 Dy2O3@TiO2 纳米复合材料的合成与表征
IF 4.3
ACS Engineering Au Pub Date : 2024-09-17 DOI: 10.1021/acsengineeringau.4c0002510.1021/acsengineeringau.4c00025
Balachandran Subramanian*, K. Jeeva Jothi, Mohamedazeem M. Mohideen, R. Karthikeyan, A. Santhana Krishna Kumar*, Ganeshraja Ayyakannu Sundaram, K. Thirumalai, Munirah D. Albaqami, Saikh Mohammad and M. Swaminathan*, 
{"title":"Synthesis and Characterization of Dy2O3@TiO2 Nanocomposites for Enhanced Photocatalytic and Electrocatalytic Applications","authors":"Balachandran Subramanian*,&nbsp;K. Jeeva Jothi,&nbsp;Mohamedazeem M. Mohideen,&nbsp;R. Karthikeyan,&nbsp;A. Santhana Krishna Kumar*,&nbsp;Ganeshraja Ayyakannu Sundaram,&nbsp;K. Thirumalai,&nbsp;Munirah D. Albaqami,&nbsp;Saikh Mohammad and M. Swaminathan*,&nbsp;","doi":"10.1021/acsengineeringau.4c0002510.1021/acsengineeringau.4c00025","DOIUrl":"https://doi.org/10.1021/acsengineeringau.4c00025https://doi.org/10.1021/acsengineeringau.4c00025","url":null,"abstract":"<p >Industrial wastewater pollution is a crucial global issue due to the increasing need for clean water. Traditional photocatalytic methods for eliminating harmful dyes are often ineffective and are environmentally damaging. This study introduces a new, efficient photocatalyst combining Dy<sub>2</sub>O<sub>3</sub> with TiO<sub>2</sub> using a single-step hydrothermal approach. Dy<sub>2</sub>O<sub>3</sub>@TiO<sub>2</sub> nanostructures were synthesized and characterized by using XRD, SEM, EDS, TEM, BET, and UV–visible spectroscopy. Dy<sub>2</sub>O<sub>3</sub> was evenly distributed on TiO<sub>2</sub>, preventing clumping and resulting in a larger surface area with more active sites. UV irradiation (365 nm) replaced the traditional thermal energy for photocatalytic dye breakdown, leveraging the varying conductivity of the Dy<sub>2</sub>O<sub>3</sub>@TiO<sub>2</sub> nanocomposites. Incorporating Dy<sub>2</sub>O<sub>3</sub> decreased band gaps, enhancing redox reactions and expanding the range of degradable contaminants. For Rhodamine B dye degradation, the Dy<sub>2</sub>O<sub>3</sub>@TiO<sub>2</sub> composite demonstrated significantly higher degradation rates than Dy<sub>2</sub>O<sub>3</sub> or TiO<sub>2</sub> alone at reaction parameters such as neutral pH (pH 7) and catalyst concentration (2 g L<sup>–1</sup>). The hybrid material also demonstrated improved electrocatalytic activity in oxygen reduction reactions (ORRs) under alkaline conditions with an initial potential of 0.88 V and a Tafel slope of 73 mV dec<sup>–1</sup>. The enhanced catalytic activity and durability are attributed to the synergistic interaction between Dy<sub>2</sub>O<sub>3</sub> and TiO<sub>2</sub>. This novel photocatalyst offers a sustainable alternative for treating industrial effluents while reducing the environmental impact.</p>","PeriodicalId":29804,"journal":{"name":"ACS Engineering Au","volume":null,"pages":null},"PeriodicalIF":4.3,"publicationDate":"2024-09-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.acs.org/doi/epdf/10.1021/acsengineeringau.4c00025","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142437511","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
Synthesis and Characterization of Dy2O3@TiO2 Nanocomposites for Enhanced Photocatalytic and Electrocatalytic Applications 用于增强光催化和电催化应用的 Dy2O3@TiO2 纳米复合材料的合成与表征
ACS Engineering Au Pub Date : 2024-09-17 DOI: 10.1021/acsengineeringau.4c00025
Balachandran Subramanian, K. Jeeva Jothi, Mohamedazeem M. Mohideen, R. Karthikeyan, A. Santhana Krishna Kumar, Ganeshraja Ayyakannu Sundaram, K. Thirumalai, Munirah D. Albaqami, Saikh Mohammad, M. Swaminathan
{"title":"Synthesis and Characterization of Dy2O3@TiO2 Nanocomposites for Enhanced Photocatalytic and Electrocatalytic Applications","authors":"Balachandran Subramanian, K. Jeeva Jothi, Mohamedazeem M. Mohideen, R. Karthikeyan, A. Santhana Krishna Kumar, Ganeshraja Ayyakannu Sundaram, K. Thirumalai, Munirah D. Albaqami, Saikh Mohammad, M. Swaminathan","doi":"10.1021/acsengineeringau.4c00025","DOIUrl":"https://doi.org/10.1021/acsengineeringau.4c00025","url":null,"abstract":"Industrial wastewater pollution is a crucial global issue due to the increasing need for clean water. Traditional photocatalytic methods for eliminating harmful dyes are often ineffective and are environmentally damaging. This study introduces a new, efficient photocatalyst combining Dy<sub>2</sub>O<sub>3</sub> with TiO<sub>2</sub> using a single-step hydrothermal approach. Dy<sub>2</sub>O<sub>3</sub>@TiO<sub>2</sub> nanostructures were synthesized and characterized by using XRD, SEM, EDS, TEM, BET, and UV–visible spectroscopy. Dy<sub>2</sub>O<sub>3</sub> was evenly distributed on TiO<sub>2</sub>, preventing clumping and resulting in a larger surface area with more active sites. UV irradiation (365 nm) replaced the traditional thermal energy for photocatalytic dye breakdown, leveraging the varying conductivity of the Dy<sub>2</sub>O<sub>3</sub>@TiO<sub>2</sub> nanocomposites. Incorporating Dy<sub>2</sub>O<sub>3</sub> decreased band gaps, enhancing redox reactions and expanding the range of degradable contaminants. For Rhodamine B dye degradation, the Dy<sub>2</sub>O<sub>3</sub>@TiO<sub>2</sub> composite demonstrated significantly higher degradation rates than Dy<sub>2</sub>O<sub>3</sub> or TiO<sub>2</sub> alone at reaction parameters such as neutral pH (pH 7) and catalyst concentration (2 g L<sup>–1</sup>). The hybrid material also demonstrated improved electrocatalytic activity in oxygen reduction reactions (ORRs) under alkaline conditions with an initial potential of 0.88 V and a Tafel slope of 73 mV dec<sup>–1</sup>. The enhanced catalytic activity and durability are attributed to the synergistic interaction between Dy<sub>2</sub>O<sub>3</sub> and TiO<sub>2</sub>. This novel photocatalyst offers a sustainable alternative for treating industrial effluents while reducing the environmental impact.","PeriodicalId":29804,"journal":{"name":"ACS Engineering Au","volume":null,"pages":null},"PeriodicalIF":0.0,"publicationDate":"2024-09-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142264629","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Radiofrequency Induction Heating for Green Chemicals Manufacture: A Systematic Model of Energy Losses and a Scale-Up Case-Study 用于绿色化学品生产的射频感应加热:能量损耗系统模型和规模化案例研究
ACS Engineering Au Pub Date : 2024-07-25 DOI: 10.1021/acsengineeringau.4c00009
Jonathan P. P. Noble, Simon J. Bending, Alfred K. Hill
{"title":"Radiofrequency Induction Heating for Green Chemicals Manufacture: A Systematic Model of Energy Losses and a Scale-Up Case-Study","authors":"Jonathan P. P. Noble, Simon J. Bending, Alfred K. Hill","doi":"10.1021/acsengineeringau.4c00009","DOIUrl":"https://doi.org/10.1021/acsengineeringau.4c00009","url":null,"abstract":"Radiofrequency (RF) induction heating has generated much interest for the abatement of carbon emissions from the chemicals sector as a direct electrification technology. Three challenges have held back its deployment at scale: reactors must be built from nonconductive materials which eliminates steel as a design choice; the viability of scale-up is uncertain; and to date the reported energy efficiency has been too low. This paper presents a model that for the first time makes a comprehensive analysis of energy losses that arise from RF induction heating. The maximum energy efficiency for radio frequency induction heating was previously reported to be 23% with a typical frequency range of 200–400 kHz. The results from the model show that an energy efficiency of 65–82% is achieved at a much lower frequency of 10 kHz and a reactor diameter of 0.2 m. Energy efficiency above 90% with reactor diameters above 1 m in diameter are predicted if higher voltage radio frequency sources can be developed. A new location of the work coil inside of the reactor wall is shown to be highly effective. Losses arising from heating a steel reactor wall in this configuration are shown to be insignificant, even when the wall is immediately adjacent to the work coil. This analysis demonstrates that RF induction heating can be a highly efficient and effective industrial technology for coupling high energy demand chemicals manufacture electricity from zero carbon renewables.","PeriodicalId":29804,"journal":{"name":"ACS Engineering Au","volume":null,"pages":null},"PeriodicalIF":0.0,"publicationDate":"2024-07-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141778714","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Radiofrequency Induction Heating for Green Chemicals Manufacture: A Systematic Model of Energy Losses and a Scale-Up Case-Study 用于绿色化学品生产的射频感应加热:能量损耗系统模型和规模化案例研究
IF 4.3
ACS Engineering Au Pub Date : 2024-07-25 DOI: 10.1021/acsengineeringau.4c0000910.1021/acsengineeringau.4c00009
Jonathan P. P. Noble*, Simon J. Bending and Alfred K. Hill*, 
{"title":"Radiofrequency Induction Heating for Green Chemicals Manufacture: A Systematic Model of Energy Losses and a Scale-Up Case-Study","authors":"Jonathan P. P. Noble*,&nbsp;Simon J. Bending and Alfred K. Hill*,&nbsp;","doi":"10.1021/acsengineeringau.4c0000910.1021/acsengineeringau.4c00009","DOIUrl":"https://doi.org/10.1021/acsengineeringau.4c00009https://doi.org/10.1021/acsengineeringau.4c00009","url":null,"abstract":"<p >Radiofrequency (RF) induction heating has generated much interest for the abatement of carbon emissions from the chemicals sector as a direct electrification technology. Three challenges have held back its deployment at scale: reactors must be built from nonconductive materials which eliminates steel as a design choice; the viability of scale-up is uncertain; and to date the reported energy efficiency has been too low. This paper presents a model that for the first time makes a comprehensive analysis of energy losses that arise from RF induction heating. The maximum energy efficiency for radio frequency induction heating was previously reported to be 23% with a typical frequency range of 200–400 kHz. The results from the model show that an energy efficiency of 65–82% is achieved at a much lower frequency of 10 kHz and a reactor diameter of 0.2 m. Energy efficiency above 90% with reactor diameters above 1 m in diameter are predicted if higher voltage radio frequency sources can be developed. A new location of the work coil inside of the reactor wall is shown to be highly effective. Losses arising from heating a steel reactor wall in this configuration are shown to be insignificant, even when the wall is immediately adjacent to the work coil. This analysis demonstrates that RF induction heating can be a highly efficient and effective industrial technology for coupling high energy demand chemicals manufacture electricity from zero carbon renewables.</p>","PeriodicalId":29804,"journal":{"name":"ACS Engineering Au","volume":null,"pages":null},"PeriodicalIF":4.3,"publicationDate":"2024-07-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.acs.org/doi/epdf/10.1021/acsengineeringau.4c00009","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142436610","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
Chemical Recycling of Step-Growth Polymers Guided by Le Chatelier’s Principle 勒夏特列原理指导下的阶跃生长聚合物化学再循环
IF 4.3
ACS Engineering Au Pub Date : 2024-07-15 DOI: 10.1021/acsengineeringau.4c00015
Zhiyong Liu, Youwei Ma
{"title":"Chemical Recycling of Step-Growth Polymers Guided by Le Chatelier’s Principle","authors":"Zhiyong Liu, Youwei Ma","doi":"10.1021/acsengineeringau.4c00015","DOIUrl":"https://doi.org/10.1021/acsengineeringau.4c00015","url":null,"abstract":"","PeriodicalId":29804,"journal":{"name":"ACS Engineering Au","volume":null,"pages":null},"PeriodicalIF":4.3,"publicationDate":"2024-07-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141649026","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Chemical Recycling of Step-Growth Polymers Guided by Le Chatelier’s Principle 勒夏特列原理指导下的阶跃生长聚合物化学再循环
IF 4.3
ACS Engineering Au Pub Date : 2024-07-15 DOI: 10.1021/acsengineeringau.4c0001510.1021/acsengineeringau.4c00015
Zhiyong Liu,  and , Youwei Ma*, 
{"title":"Chemical Recycling of Step-Growth Polymers Guided by Le Chatelier’s Principle","authors":"Zhiyong Liu,&nbsp; and ,&nbsp;Youwei Ma*,&nbsp;","doi":"10.1021/acsengineeringau.4c0001510.1021/acsengineeringau.4c00015","DOIUrl":"https://doi.org/10.1021/acsengineeringau.4c00015https://doi.org/10.1021/acsengineeringau.4c00015","url":null,"abstract":"<p >Although step-growth polymers (SGPs) play a fundamental role in the plastics economy, contributing significantly to various facets of our daily life, their end-of-life management remains inadequately addressed. Chemical recycling of SGP wastes, involving depolymerization followed by repolymerization, emerges as a promising solution toward achieving a circular plastics economy. The depolymerization of SGPs is usually in dynamic equilibrium with their polymerization reactions, thus falling under a system amenable to Le Chatelier’s principle. This perspective endeavors to elucidate the interplay between Le Chatelier’s principle and the chemical recycling of SGPs with a particular emphasis on the guidance provided by the principle in the latter process. To this end, we have selected five conventional SGPs, namely, poly(ethylene terephthalate), polyamides, polycarbonates, polyurethanes, and polyureas, as representatives to elucidate how alterations in temperature, pressure, concentrations of products or reactants, and catalysts influence the depolymerization process of SGPs. Additionally, the perspective proposes several potential strategies for achieving the chemical recycling of SGPs by applying Le Chatelier’s principle.</p>","PeriodicalId":29804,"journal":{"name":"ACS Engineering Au","volume":null,"pages":null},"PeriodicalIF":4.3,"publicationDate":"2024-07-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.acs.org/doi/epdf/10.1021/acsengineeringau.4c00015","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142436723","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
Synergistic Removal of Cr(VI) with Stable Nanozerovalent Iron Particles and Ultrasound Assistance in the Presence of Organic Additives 在有机添加剂存在的情况下,利用稳定的纳米泽戊酸铁颗粒和超声波辅助技术协同去除六价铬
ACS Engineering Au Pub Date : 2024-06-05 DOI: 10.1021/acsengineeringau.4c00011
Lucia Cancelada, J. M. Meichtry, Hugo Destaillats, M. Litter
{"title":"Synergistic Removal of Cr(VI) with Stable Nanozerovalent Iron Particles and Ultrasound Assistance in the Presence of Organic Additives","authors":"Lucia Cancelada, J. M. Meichtry, Hugo Destaillats, M. Litter","doi":"10.1021/acsengineeringau.4c00011","DOIUrl":"https://doi.org/10.1021/acsengineeringau.4c00011","url":null,"abstract":"","PeriodicalId":29804,"journal":{"name":"ACS Engineering Au","volume":null,"pages":null},"PeriodicalIF":0.0,"publicationDate":"2024-06-05","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141382968","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Synergistic Removal of Cr(VI) with Stable Nanozerovalent Iron Particles and Ultrasound Assistance in the Presence of Organic Additives 在有机添加剂存在的情况下,利用稳定的纳米泽戊酸铁粒子和超声波辅助技术协同去除六价铬
IF 4.3
ACS Engineering Au Pub Date : 2024-06-05 DOI: 10.1021/acsengineeringau.4c0001110.1021/acsengineeringau.4c00011
Lucia Cancelada, Jorge M. Meichtry, Hugo Destaillats and Marta I. Litter*, 
{"title":"Synergistic Removal of Cr(VI) with Stable Nanozerovalent Iron Particles and Ultrasound Assistance in the Presence of Organic Additives","authors":"Lucia Cancelada,&nbsp;Jorge M. Meichtry,&nbsp;Hugo Destaillats and Marta I. Litter*,&nbsp;","doi":"10.1021/acsengineeringau.4c0001110.1021/acsengineeringau.4c00011","DOIUrl":"https://doi.org/10.1021/acsengineeringau.4c00011https://doi.org/10.1021/acsengineeringau.4c00011","url":null,"abstract":"<p >Commercial stable zerovalent iron nanoparticles (nZVI) (NSTAR, not activated) combined with ultrasound (US) were tested for Cr(VI) reductive removal (0.3 mM, pH 3, Fe/Cr molar ratio of 3:1) in the presence of the carboxylic acids (CAs) ethylenediaminetetraacetic acid (EDTA, 1 mM) or citric acid (Cit, 2 mM), in a system open to the air. No Cr(VI) decay up to 180 min was observed under US when only NSTAR nanoparticles were used, while other previously tested commercial nZVI (N25) showed about 40% decay in a few minutes but without further Cr(VI) removal. The addition of EDTA and Cit enabled Cr(VI) removal with NSTAR in the absence of US without prior activation of the particles. A pseudo zero-order kinetics was followed, yielding 32 and 49% removal with EDTA and Cit, respectively. When US was applied, these values almost doubled, reaching 59 and 88% for EDTA and Cit, respectively. A mechanism for Cr(VI) decay was proposed. The present results indicate that the simultaneous use of US and CAs allows for a synergistic Cr(VI) removal by NSTAR avoiding the need of an activation step of the nanoparticles, with a more effective result of Cit compared with EDTA.</p>","PeriodicalId":29804,"journal":{"name":"ACS Engineering Au","volume":null,"pages":null},"PeriodicalIF":4.3,"publicationDate":"2024-06-05","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.acs.org/doi/epdf/10.1021/acsengineeringau.4c00011","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142436542","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
Effect of SO2 and SO3 Exposure to Cu-CHA on Surface Nitrate and N2O Formation for NH3–SCR 二氧化硫和二氧化硫暴露于 Cu-CHA 对 NH3-SCR 表面硝酸盐和 N2O 生成的影响
IF 4.3
ACS Engineering Au Pub Date : 2024-05-31 DOI: 10.1021/acsengineeringau.4c0000410.1021/acsengineeringau.4c00004
Joonsoo Han*, Joachim D. Bjerregaard, Henrik Grönbeck, Derek Creaser and Louise Olsson*, 
{"title":"Effect of SO2 and SO3 Exposure to Cu-CHA on Surface Nitrate and N2O Formation for NH3–SCR","authors":"Joonsoo Han*,&nbsp;Joachim D. Bjerregaard,&nbsp;Henrik Grönbeck,&nbsp;Derek Creaser and Louise Olsson*,&nbsp;","doi":"10.1021/acsengineeringau.4c0000410.1021/acsengineeringau.4c00004","DOIUrl":"https://doi.org/10.1021/acsengineeringau.4c00004https://doi.org/10.1021/acsengineeringau.4c00004","url":null,"abstract":"<p >We report effects of SO<sub>2</sub> and SO<sub>3</sub> exposure on ammonium nitrate (AN) and N<sub>2</sub>O formation in Cu-CHA used for NH<sub>3</sub>–SCR. First-principles calculations and several characterizations (ICP, BET, XRD, UV–vis–DRS) were applied to characterize the Cu-CHA material and speciation of sulfur species. The first-principles calculations demonstrate that the SO<sub>2</sub> exposure results in both (bi)sulfite and (bi)sulfate whereas the SO<sub>3</sub> exposure yields only (bi)sulfate. Furthermore, SOx adsorption on framework-bound dicopper species is shown to be favored with respect to adsorption onto framework-bound monocopper species. Temperature-programmed reduction with H<sub>2</sub> shows two clear reduction states and larger sulfur uptake for the SO<sub>3</sub>-exposed Cu-CHA compared to the SO<sub>2</sub>-exposed counterpart. Temperature-programmed desorption of formed ammonium nitrate (AN) highlights a significant decrease in nitrate storage due to sulfur species interacting with copper sites in the form of ammonium/copper (bi)bisulfite/sulfate. Especially, highly stable sulfur species from SO<sub>3</sub> exposure influence the NO<sub>2</sub>–SCR chemistry by decreasing the N<sub>2</sub>O selectivity during NH<sub>3</sub>–SCR whereas an increased N<sub>2</sub>O selectivity was observed for the SO<sub>2</sub>-exposed Cu-CHA sample. This study provides fundamental insights into how SO<sub>2</sub> and SO<sub>3</sub> affect the N<sub>2</sub>O formation during ammonium nitrate decomposition in NH<sub>3</sub>–SCR applications, which is a very important topic for practical applications.</p>","PeriodicalId":29804,"journal":{"name":"ACS Engineering Au","volume":null,"pages":null},"PeriodicalIF":4.3,"publicationDate":"2024-05-31","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.acs.org/doi/epdf/10.1021/acsengineeringau.4c00004","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142010400","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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