首页 > 最新文献

Environmental science. Advances最新文献

英文 中文
Impacts of biochar and slag on carbon sequestration potential and sustainability assessment of MgO-stabilized marine soils: insights from MIP analysis† 生物炭和矿渣对氧化镁稳定的海洋土壤固碳潜力和可持续性评估的影响:MIP 分析的启示
IF 3.5 Q3 ENGINEERING, ENVIRONMENTAL Pub Date : 2024-09-02 DOI: 10.1039/D4VA00095A
Chikezie Chimere Onyekwena, Qi Li, Yong Wang, Ishrat Hameed Alvi, Yunlu Hou, Chima Finnian Ukaomah and Theogene Hakuzweyezu

Mineral carbonation is a promising strategy for mitigating carbon emissions and combating climate change. This study investigates the efficacy and sustainability of MgO-based stabilization techniques for soft marine soils, incorporating supplementary cementitious materials (SCMs) such as biochar and slag. A combination of laboratory experiments and rigorous analyses was utilized to elucidate the complex interplay between the additives and their impacts on soil hydraulic characteristics, carbon sequestration potential, embodied energy, and economic viability. Mercury intrusion porosimetry (MIP) was employed to characterize pore structure changes induced by carbonation, while X-ray diffraction (XRD) and scanning electron microscopy (SEM) were used to correlate mineral formations. The results indicate that MgO–biochar-treated soils exhibit enhanced soil air content, pore connectivity, and carbon sequestration efficiency compared to MgO–slag-treated soils, exhibiting reduced pore volumes and limited CO2 diffusion. Integrating biochar with MgO enhanced brucite and nesquehonite precipitation due to biochar's porous structure and functionalized surface area, facilitating gas diffusion and nucleation for mineral formation. Sustainability assessments highlight the environmental and economic trade-offs, positioning MgO–biochar and MgO–slag combinations as cost-effective and environmentally friendly alternatives. This research provides theoretical guidance for sustainable soil stabilization and efficient CO2 mineralization, offering valuable insights for researchers, practitioners, and policymakers addressing climate change challenges.

矿物碳化是减少碳排放和应对气候变化的一项有前途的战略。本研究调查了以氧化镁为基础的软质海洋土壤稳定技术的有效性和可持续性,并结合了生物炭和矿渣等补充胶凝材料(SCMs)。研究结合实验室实验和严格的分析,阐明了添加剂之间复杂的相互作用及其对土壤水力特性、固碳潜力、体现能源和经济可行性的影响。采用汞渗入孔隙测定法(MIP)来描述碳化引起的孔隙结构变化,同时采用 X 射线衍射(XRD)和扫描电子显微镜(SEM)来关联矿物形态。结果表明,与氧化镁-矿渣处理过的土壤相比,氧化镁-生物炭处理过的土壤空气含量、孔隙连通性和固碳效率都有所提高,但孔隙体积减少,二氧化碳扩散受限。由于生物炭的多孔结构和功能化表面积,将生物炭与氧化镁结合可提高青金石和内沸石的沉淀,促进气体扩散和矿物形成的成核。可持续性评估强调了环境和经济的权衡,将氧化镁-生物炭和氧化镁-矿渣组合定位为具有成本效益和环境友好的替代品。这项研究为可持续的土壤稳定化和高效的二氧化碳矿化提供了理论指导,为应对气候变化挑战的研究人员、从业人员和决策者提供了宝贵的见解。
{"title":"Impacts of biochar and slag on carbon sequestration potential and sustainability assessment of MgO-stabilized marine soils: insights from MIP analysis†","authors":"Chikezie Chimere Onyekwena, Qi Li, Yong Wang, Ishrat Hameed Alvi, Yunlu Hou, Chima Finnian Ukaomah and Theogene Hakuzweyezu","doi":"10.1039/D4VA00095A","DOIUrl":"10.1039/D4VA00095A","url":null,"abstract":"<p >Mineral carbonation is a promising strategy for mitigating carbon emissions and combating climate change. This study investigates the efficacy and sustainability of MgO-based stabilization techniques for soft marine soils, incorporating supplementary cementitious materials (SCMs) such as biochar and slag. A combination of laboratory experiments and rigorous analyses was utilized to elucidate the complex interplay between the additives and their impacts on soil hydraulic characteristics, carbon sequestration potential, embodied energy, and economic viability. Mercury intrusion porosimetry (MIP) was employed to characterize pore structure changes induced by carbonation, while X-ray diffraction (XRD) and scanning electron microscopy (SEM) were used to correlate mineral formations. The results indicate that MgO–biochar-treated soils exhibit enhanced soil air content, pore connectivity, and carbon sequestration efficiency compared to MgO–slag-treated soils, exhibiting reduced pore volumes and limited CO<small><sub>2</sub></small> diffusion. Integrating biochar with MgO enhanced brucite and nesquehonite precipitation due to biochar's porous structure and functionalized surface area, facilitating gas diffusion and nucleation for mineral formation. Sustainability assessments highlight the environmental and economic trade-offs, positioning MgO–biochar and MgO–slag combinations as cost-effective and environmentally friendly alternatives. This research provides theoretical guidance for sustainable soil stabilization and efficient CO<small><sub>2</sub></small> mineralization, offering valuable insights for researchers, practitioners, and policymakers addressing climate change challenges.</p>","PeriodicalId":72941,"journal":{"name":"Environmental science. Advances","volume":" 11","pages":" 1564-1577"},"PeriodicalIF":3.5,"publicationDate":"2024-09-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.rsc.org/en/content/articlepdf/2024/va/d4va00095a?page=search","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142208599","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
Naked eye detection of arsenite, arsenate, and H2S by a Schiff base naphthaldehyde conjugate using a single paper strip, based on a deprotonation mechanism† 基于去质子化机理,使用单纸条的席夫碱萘醛共轭物裸眼检测亚砷酸盐、砷酸盐和 H2S
IF 3.5 Q3 ENGINEERING, ENVIRONMENTAL Pub Date : 2024-08-27 DOI: 10.1039/D4VA00213J
Diptiman De, Priyotosh Ghosh, Sriman De and Prithidipa Sahoo

Considering the significant toxicity of arsenite (AsO2), arsenate (AsO43−), and hydrogen sulphide (H2S), the early detection of these ions and gas using simple methods like naked-eye chemosensing could have substantial implications for environmental and industrial applications. With these factors in mind, we have developed a novel and straightforward colorimetric chemosensor called NADNP (2-hydroxy naphthaldehyde conjugated 2,4-dinitrophenyl hydrazine) for swift paper-based colorimetric detection of arsenite, arsenate, and H2S, based on a deprotonation mechanism. NADNP exhibits strong binding affinity towards sulfide, arsenite, and arsenate, with very lower detection limits (LOD) of 0.17 μM, 0.15 μM and 0.15 μM respectively, and the binding stoichiometry between these detected ions and NADNP is determined to be 1 : 1 through Job's plot analysis. Structural elucidation and electronic properties calculation have been conducted via DFT (Density Functional Theory) studies for correlation with the spectroscopic analyses. The ‘three-in-one’ paper strip-based chemosensor could be considered a promising colorimetric tool for rapid, cost-effective, selective, and sensitive “on-spot” sensing and monitoring of arsenite, arsenate, and sulfide in environmental samples.

考虑到亚砷酸盐(AsO2-)、砷酸盐(AsO43-)和硫化氢(H2S)的剧毒性,使用肉眼化学传感等简单方法对这些离子和气体进行早期检测可能会对环境和工业应用产生重大影响。考虑到这些因素,我们基于去质子化机理,开发了一种新颖、简单的比色化学传感器 NADNP(2-羟基萘醛共轭 2,4-二硝基苯肼),用于基于纸张的亚砷酸盐、砷酸盐和 H2S 的快速比色检测。NADNP 对硫化物、亚砷酸盐和砷酸盐具有很强的结合亲和力,检测限(LOD)非常低,分别为 0.17 μM、0.15 μM 和 0.15 μM:通过约伯图分析,确定这些检测到的离子与 NADNP 的结合比例为 1:1。通过密度泛函理论(DFT)研究进行了结构阐释和电子特性计算,以便与光谱分析相关联。这种 "三合一 "纸条式化学传感器是一种很有前途的比色工具,可用于快速、经济、选择性和灵敏地 "现场 "感应和监测环境样品中的亚砷酸盐、砷酸盐和硫化物。
{"title":"Naked eye detection of arsenite, arsenate, and H2S by a Schiff base naphthaldehyde conjugate using a single paper strip, based on a deprotonation mechanism†","authors":"Diptiman De, Priyotosh Ghosh, Sriman De and Prithidipa Sahoo","doi":"10.1039/D4VA00213J","DOIUrl":"10.1039/D4VA00213J","url":null,"abstract":"<p >Considering the significant toxicity of arsenite (AsO<small><sub>2</sub></small><small><sup>−</sup></small>), arsenate (AsO<small><sub>4</sub></small><small><sup>3−</sup></small>), and hydrogen sulphide (H<small><sub>2</sub></small>S), the early detection of these ions and gas using simple methods like naked-eye chemosensing could have substantial implications for environmental and industrial applications. With these factors in mind, we have developed a novel and straightforward colorimetric chemosensor called NADNP (2-hydroxy naphthaldehyde conjugated 2,4-dinitrophenyl hydrazine) for swift paper-based colorimetric detection of arsenite, arsenate, and H<small><sub>2</sub></small>S, based on a deprotonation mechanism. NADNP exhibits strong binding affinity towards sulfide, arsenite, and arsenate, with very lower detection limits (LOD) of 0.17 μM, 0.15 μM and 0.15 μM respectively, and the binding stoichiometry between these detected ions and NADNP is determined to be 1 : 1 through Job's plot analysis. Structural elucidation and electronic properties calculation have been conducted <em>via</em> DFT (Density Functional Theory) studies for correlation with the spectroscopic analyses. The ‘three-in-one’ paper strip-based chemosensor could be considered a promising colorimetric tool for rapid, cost-effective, selective, and sensitive “on-spot” sensing and monitoring of arsenite, arsenate, and sulfide in environmental samples.</p>","PeriodicalId":72941,"journal":{"name":"Environmental science. Advances","volume":" 11","pages":" 1578-1585"},"PeriodicalIF":3.5,"publicationDate":"2024-08-27","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.rsc.org/en/content/articlepdf/2024/va/d4va00213j?page=search","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142208624","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
Life cycle assessment methods for investigating novel food packaging systems 研究新型食品包装系统的生命周期评估方法
IF 3.5 Q3 ENGINEERING, ENVIRONMENTAL Pub Date : 2024-08-26 DOI: 10.1039/D3VA00380A
Ina Bremenkamp and Maria J. Sousa Gallagher

The high volume of plastic waste generated and its potential harm to wildlife and ecosystems are negative consequences of poor end-of-life food packaging management. An essential part of designing food packaging is minimizing its environmental impact, which is a significant challenge for the industry. The aim of this study was to examine existing life cycle assessment (LCA) approaches for investigating the environmental advantages of novel food packaging systems in the field of ready-to-eat fish and meat products. The scope of studies differed, with some including food products and others focusing on the direct and/or indirect environmental impacts of packaging. The reviewed LCA performances showed how different focuses could be used as sequential steps in obtaining a comprehensive understanding of the environmental impact of a food-packaging system. By considering a holistic LCA approach and evaluating the environmental performance of different packagings, industry stakeholders can make informed decisions. Therefore, playing an active role that balances necessity and wastefulness and creates efficient and sustainable packaging solutions.

产生的大量塑料垃圾及其对野生动物和生态系统的潜在危害是报废食品包装管理不善的负面后果。设计食品包装的一个重要部分是最大限度地减少其对环境的影响,这对该行业来说是一项重大挑战。本研究旨在考察现有的生命周期评估(LCA)方法,以调查即食鱼类和肉类产品领域新型食品包装系统的环境优势。研究范围各不相同,有的包括食品,有的则侧重于包装对环境的直接和/或间接影响。经审查的生命周期评估结果表明,在全面了解食品包装系统对环境的影响时,可以将不同的重点作为连续的步骤。通过考虑整体生命周期评估方法和评估不同包装的环境绩效,行业利益相关者可以做出明智的决策。因此,在平衡必要性和浪费之间发挥积极作用,创造高效和可持续的包装解决方案。
{"title":"Life cycle assessment methods for investigating novel food packaging systems","authors":"Ina Bremenkamp and Maria J. Sousa Gallagher","doi":"10.1039/D3VA00380A","DOIUrl":"10.1039/D3VA00380A","url":null,"abstract":"<p >The high volume of plastic waste generated and its potential harm to wildlife and ecosystems are negative consequences of poor end-of-life food packaging management. An essential part of designing food packaging is minimizing its environmental impact, which is a significant challenge for the industry. The aim of this study was to examine existing life cycle assessment (LCA) approaches for investigating the environmental advantages of novel food packaging systems in the field of ready-to-eat fish and meat products. The scope of studies differed, with some including food products and others focusing on the direct and/or indirect environmental impacts of packaging. The reviewed LCA performances showed how different focuses could be used as sequential steps in obtaining a comprehensive understanding of the environmental impact of a food-packaging system. By considering a holistic LCA approach and evaluating the environmental performance of different packagings, industry stakeholders can make informed decisions. Therefore, playing an active role that balances necessity and wastefulness and creates efficient and sustainable packaging solutions.</p>","PeriodicalId":72941,"journal":{"name":"Environmental science. Advances","volume":" 10","pages":" 1337-1350"},"PeriodicalIF":3.5,"publicationDate":"2024-08-26","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.rsc.org/en/content/articlepdf/2024/va/d3va00380a?page=search","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142208623","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
The financial market wants to believe in European sustainability. Time trends and persistence analysis of green vs. brown bond yields 金融市场希望相信欧洲的可持续性。绿色债券与棕色债券收益率的时间趋势和持续性分析
IF 3.5 Q3 ENGINEERING, ENVIRONMENTAL Pub Date : 2024-08-23 DOI: 10.1039/D4VA00193A
Manuel Monge

Green bonds are becoming a popular investment option as a result of growing investor awareness of social and environmental issues. Green bonds are financial securities used to fund initiatives aimed at mitigating the effects of global industrialization on the environment and climate change, as well as initiatives that make use of cutting-edge technology. For the SDGs to be achieved, this kind of financial product must be successfully promoted. Therefore, the objective of this research work is to statistically analyze the characteristics of green and brown bond yields. In addition, to ascertain how the two yields relate to one another and how they change over time.

由于投资者对社会和环境问题的认识不断提高,绿色债券正成为一种流行的投资选择。绿色债券是一种金融证券,用于资助旨在减轻全球工业化对环境和气候变化影响的倡议,以及利用尖端技术的倡议。要实现可持续发展目标,就必须成功推广此类金融产品。因此,本研究工作的目标是统计分析绿色债券和棕色债券收益率的特点。此外,还要弄清这两种收益率之间的关系以及它们随时间的变化情况。
{"title":"The financial market wants to believe in European sustainability. Time trends and persistence analysis of green vs. brown bond yields","authors":"Manuel Monge","doi":"10.1039/D4VA00193A","DOIUrl":"10.1039/D4VA00193A","url":null,"abstract":"<p >Green bonds are becoming a popular investment option as a result of growing investor awareness of social and environmental issues. Green bonds are financial securities used to fund initiatives aimed at mitigating the effects of global industrialization on the environment and climate change, as well as initiatives that make use of cutting-edge technology. For the SDGs to be achieved, this kind of financial product must be successfully promoted. Therefore, the objective of this research work is to statistically analyze the characteristics of green and brown bond yields. In addition, to ascertain how the two yields relate to one another and how they change over time.</p>","PeriodicalId":72941,"journal":{"name":"Environmental science. Advances","volume":" 10","pages":" 1452-1463"},"PeriodicalIF":3.5,"publicationDate":"2024-08-23","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.rsc.org/en/content/articlepdf/2024/va/d4va00193a?page=search","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142208626","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
Dioxins in the Arctic: local sources vs. long-range transport† 北极的二恶英:本地来源与远距离迁移
IF 3.5 Q3 ENGINEERING, ENVIRONMENTAL Pub Date : 2024-08-22 DOI: 10.1039/D4VA00202D
Ling Gou, Shijie Song, Tao Huang, Zaili Ling, Kaijie Chen, Jiayi Xin, Enze Geng, Jiaxin Wang, Yuan Zhao, Hong Gao and Jianmin Ma

With a unique geographical location and a fragile ecological environment, the Arctic has been a major concern of contamination by persistent organic pollutants (POPs), such as dioxins, also termed polychlorinated dibenzo-p-dioxins and dibenzofurans (PCDD/Fs) due to their high toxicity. Under the influence of global warming, increasing wildfires have occurred in northern territories of the Northern Hemisphere (NH) in the recent decade. Given the proximity of these natural sources, the Arctic is likely subject to growing risks of local and nearby wildfire emissions of POPs. By implementing an updated global PCDD/Fs atmospheric emission inventory from 2011 to 2020 into an atmospheric transport model, we quantitatively assessed the PCDD/Fs pollution in the Arctic atmosphere. We explored the impact of wildfire combustion on PCDD/Fs pollution in the Arctic atmosphere and evaluated the relative significance of local and remote emissions from wildfire and anthropogenic sources. The results revealed that PCDD/Fs emissions from wildfire sources played an increasingly important role in PCDD/Fs pollution in the Arctic, contributing to about 70% of PCDD/Fs concentrations in Arctic air in 2020. Within the Arctic circle, wildfire emissions have also exceeded anthropogenic emissions since the late 2010s. This study provides data support for further assessment of wildfires' impact on the Arctic region's ecological environment and valuable information for assessing the effectiveness of PCDD/Fs (and other POPs) emission control.

北极地理位置独特,生态环境脆弱,一直是持久性有机污染物(POPs)污染的主要关注点,如二恶英,由于其毒性较高,也被称为多氯二苯并对二恶英和多氯二苯并呋喃(PCDD/Fs)。受全球变暖的影响,近十年来,北半球北部地区的野火越来越多。由于靠近这些自然污染源,北极地区可能会面临越来越大的本地和附近野火排放持久性有机污染物的风险。通过将 2011 年至 2020 年更新的全球多氯二苯并对二恶英和多氯二苯并呋喃大气排放清单应用到大气传输模型中,我们对北极大气中的多氯二苯并对二恶英和多氯二苯并呋喃污染进行了定量评估。我们探讨了野火燃烧对北极大气中多氯二苯并对二恶英和多氯二苯并呋喃污染的影响,并评估了野火和人为来源的本地和远程排放的相对重要性。结果表明,野火源的多氯二苯并对二恶英和多氯二苯并呋喃排放在北极多氯二苯并对二恶英和多氯二苯并呋喃污染中扮演着越来越重要的角色,到2020年,约占北极空气中多氯二苯并对二恶英和多氯二苯并呋喃浓度的70%。在北极圈内,自 2010 年代末以来,野火排放也超过了人为排放。这项研究为进一步评估野火对北极地区生态环境的影响提供了数据支持,也为评估多氯二苯并对二恶英和多氯二苯并呋喃(及其他持久性有机污染物)排放控制的有效性提供了宝贵信息。
{"title":"Dioxins in the Arctic: local sources vs. long-range transport†","authors":"Ling Gou, Shijie Song, Tao Huang, Zaili Ling, Kaijie Chen, Jiayi Xin, Enze Geng, Jiaxin Wang, Yuan Zhao, Hong Gao and Jianmin Ma","doi":"10.1039/D4VA00202D","DOIUrl":"10.1039/D4VA00202D","url":null,"abstract":"<p >With a unique geographical location and a fragile ecological environment, the Arctic has been a major concern of contamination by persistent organic pollutants (POPs), such as dioxins, also termed polychlorinated dibenzo-<em>p</em>-dioxins and dibenzofurans (PCDD/Fs) due to their high toxicity. Under the influence of global warming, increasing wildfires have occurred in northern territories of the Northern Hemisphere (NH) in the recent decade. Given the proximity of these natural sources, the Arctic is likely subject to growing risks of local and nearby wildfire emissions of POPs. By implementing an updated global PCDD/Fs atmospheric emission inventory from 2011 to 2020 into an atmospheric transport model, we quantitatively assessed the PCDD/Fs pollution in the Arctic atmosphere. We explored the impact of wildfire combustion on PCDD/Fs pollution in the Arctic atmosphere and evaluated the relative significance of local and remote emissions from wildfire and anthropogenic sources. The results revealed that PCDD/Fs emissions from wildfire sources played an increasingly important role in PCDD/Fs pollution in the Arctic, contributing to about 70% of PCDD/Fs concentrations in Arctic air in 2020. Within the Arctic circle, wildfire emissions have also exceeded anthropogenic emissions since the late 2010s. This study provides data support for further assessment of wildfires' impact on the Arctic region's ecological environment and valuable information for assessing the effectiveness of PCDD/Fs (and other POPs) emission control.</p>","PeriodicalId":72941,"journal":{"name":"Environmental science. Advances","volume":" 11","pages":" 1552-1563"},"PeriodicalIF":3.5,"publicationDate":"2024-08-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.rsc.org/en/content/articlepdf/2024/va/d4va00202d?page=search","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142208628","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
Soil greenhouse gas fluxes in corn systems with varying agricultural practices and pesticide levels† 不同农业实践和农药水平下玉米种植系统的土壤温室气体通量
IF 3.5 Q3 ENGINEERING, ENVIRONMENTAL Pub Date : 2024-08-22 DOI: 10.1039/D4VA00105B
Eri Saikawa, Alexander Avramov, Nicholas Basinger, Jerzi Hood, Nandita Gaur, Aaron Thompson, Angela Moore, Douglas Wolf and Yaoxing Wu

Pesticides are biologically active compounds and their application may alter soil microbial communities and thus could possibly impact greenhouse gas (GHG) emissions. However, this aspect of agricultural production is rarely studied at the field scale. To address this knowledge gap, we conducted a 2 year field study growing maize (corn) under three pesticide application levels (none, medium, and high) in two agricultural practices: bare soil (conventional) and using cereal rye as a cover crop. In plots with no pesticide inputs, weeds were managed through hand removal weekly. We quantified GHG emissions, changes in soil labile carbon (C), nitrogen (N), and other typical growth parameters in the Iron Horse Farm, Georgia. Corn grain yields were within 93% of the estimated site yield potential, with yield significantly higher in 2021 than in 2022. Using a linear mixed model, including the data in both 2021 and 2022 for soil nutrients, soil temperature, soil moisture, agricultural practice, and pesticide levels as fixed effects and date and plot as random effects, soil surface carbon dioxide (CO2) fluxes were statistically significantly associated with soil temperature and soil moisture. Soil nitrous oxide (N2O) emissions were only associated with soil moisture. Soils in general served as a sink for methane (CH4) in all the agricultural practices and soil CH4 fluxes were also only associated with soil moisture. Three plots with a high soil C/N ratio with a visible presence of biochar resulted in several high CH4 flux events during the growing season. Soils from all plots were net sources of GHG and there were no significant differences in the amount of soil C sequestered between the plots. Our study shows that none of the variables we analyzed – yield, individual/net GHG emissions or the amount of C sequestered – in the two years of our experiment were impacted by the magnitude of pesticide application. However, this may change in a long-term experiment. Further research is also warranted to understand the underlying mechanism for high CH4 pulses, whether reactive oxygen species from the application of biochar might be the cause of large negative consequences on climate, depending on conditions.

农药是具有生物活性的化合物,施用农药可能会改变土壤微生物群落,从而可能影响温室气体(GHG)的排放。然而,人们很少在田间规模上对农业生产的这一方面进行研究。为了填补这一知识空白,我们进行了一项为期两年的田间研究,在裸土(常规)和使用黑麦作为覆盖作物的两种农业生产方式中,玉米在三种农药施用水平(无、中、高)下生长。在不施用农药的地块中,每周通过人工清除杂草。我们量化了佐治亚州铁马农场的温室气体排放量、土壤可变碳(C)、氮(N)的变化以及其他典型的生长参数。玉米谷物产量在估计的现场产量潜力的 93% 范围内,2021 年的产量明显高于 2022 年。采用线性混合模型,将 2021 年和 2022 年的土壤养分、土壤温度、土壤湿度、农业实践和农药水平数据作为固定效应,将日期和地块作为随机效应,结果表明,土壤表面二氧化碳 (CO2) 通量与土壤温度和土壤湿度有显著的统计学关联。土壤一氧化二氮排放量只与土壤湿度有关。在所有农业实践中,土壤一般都是甲烷的吸收汇,土壤甲烷通量也只与土壤湿度有关。三个土壤碳氮比较高的地块明显含有生物炭,在生长季节产生了几次较高的甲烷通量。所有地块的土壤都是温室气体的净来源,不同地块的土壤固碳量没有显著差异。我们的研究表明,在两年的实验中,我们分析的变量--产量、单个/净温室气体排放量或固碳量--都没有受到农药施用量的影响。不过,这种情况在长期实验中可能会发生变化。进一步的研究对于了解高 C/N 比玉米田高 CH4 量的内在机理至关重要,因为生物炭的积极影响可能与对气候的巨大负面影响同时存在,这取决于具体条件。
{"title":"Soil greenhouse gas fluxes in corn systems with varying agricultural practices and pesticide levels†","authors":"Eri Saikawa, Alexander Avramov, Nicholas Basinger, Jerzi Hood, Nandita Gaur, Aaron Thompson, Angela Moore, Douglas Wolf and Yaoxing Wu","doi":"10.1039/D4VA00105B","DOIUrl":"10.1039/D4VA00105B","url":null,"abstract":"<p >Pesticides are biologically active compounds and their application may alter soil microbial communities and thus could possibly impact greenhouse gas (GHG) emissions. However, this aspect of agricultural production is rarely studied at the field scale. To address this knowledge gap, we conducted a 2 year field study growing maize (corn) under three pesticide application levels (none, medium, and high) in two agricultural practices: bare soil (conventional) and using cereal rye as a cover crop. In plots with no pesticide inputs, weeds were managed through hand removal weekly. We quantified GHG emissions, changes in soil labile carbon (C), nitrogen (N), and other typical growth parameters in the Iron Horse Farm, Georgia. Corn grain yields were within 93% of the estimated site yield potential, with yield significantly higher in 2021 than in 2022. Using a linear mixed model, including the data in both 2021 and 2022 for soil nutrients, soil temperature, soil moisture, agricultural practice, and pesticide levels as fixed effects and date and plot as random effects, soil surface carbon dioxide (CO<small><sub>2</sub></small>) fluxes were statistically significantly associated with soil temperature and soil moisture. Soil nitrous oxide (N<small><sub>2</sub></small>O) emissions were only associated with soil moisture. Soils in general served as a sink for methane (CH<small><sub>4</sub></small>) in all the agricultural practices and soil CH<small><sub>4</sub></small> fluxes were also only associated with soil moisture. Three plots with a high soil C/N ratio with a visible presence of biochar resulted in several high CH<small><sub>4</sub></small> flux events during the growing season. Soils from all plots were net sources of GHG and there were no significant differences in the amount of soil C sequestered between the plots. Our study shows that none of the variables we analyzed – yield, individual/net GHG emissions or the amount of C sequestered – in the two years of our experiment were impacted by the magnitude of pesticide application. However, this may change in a long-term experiment. Further research is also warranted to understand the underlying mechanism for high CH<small><sub>4</sub></small> pulses, whether reactive oxygen species from the application of biochar might be the cause of large negative consequences on climate, depending on conditions.</p>","PeriodicalId":72941,"journal":{"name":"Environmental science. Advances","volume":" 12","pages":" 1760-1774"},"PeriodicalIF":3.5,"publicationDate":"2024-08-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.rsc.org/en/content/articlepdf/2024/va/d4va00105b?page=search","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142208625","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
Investigations on particle emissions of large-bore engines powered by natural gas and hydrogen† 以天然气和氢气为动力的大排量发动机的颗粒排放调查
IF 3.5 Q3 ENGINEERING, ENVIRONMENTAL Pub Date : 2024-08-19 DOI: 10.1039/D4VA00200H
Felina Armbruster, Alexander Gelner, Andreas Zepf, Maximilian Prager, Martin Härtl and Malte Jaensch

In an effort to mitigate the impact of climate change, e.g., by reducing the emission of greenhouse gases, hydrogen is becoming an increasingly attractive alternative energy source, replacing conventional long-chain hydrocarbon fuels in the energy and transport sector. While there is a shift in individual transport towards battery-electric applications, the maritime and energy production sectors rely on a high energy density and time- and location-independent availability of the energy carrier. Therefore, large-bore engines powered by renewable fuels have the potential to shift the industry towards a climate-neutral operation. Besides the emission of greenhouse gases, internal combustion engines are known for emitting pollutant emissions, harming human health and the environment. Research on particle emissions of natural gas and hydrogen engines has mainly focused on automotive and heavy-duty applications. Hence, this study investigates particle emissions of a large-bore single-cylinder research engine powered by hydrogen, compared to natural gas, for the first time. Investigations on particles with a diameter as low as 10 nm showed particle numbers of 104 to 105 # cm−3, unexpectedly achieving slightly higher particle numbers in hydrogen than in natural gas operations. This is due to particles from lubricant oil and a stronger fuel interaction with the liner oil film in hydrogen operation, demonstrated within a 3D-CFD simulation. The concentrations are still lower by several orders of magnitude than in long-chain hydrocarbon fuel operations of identical engines. An extended emissions analysis based on the gaseous components THC, CO, and CO2 shows the negligible carbonaceous emissions induced by these oil-based particles.

为了减轻气候变化的影响,例如减少温室气体的排放,氢气正在成为一种越来越有吸引力的替代能源,在能源和运输领域取代传统的长链碳氢化合物燃料。虽然个体运输业正在向电池电力应用转变,但海运和能源生产部门则依赖于高能量密度以及不受时间和地点限制的能源载体。因此,以可再生燃料为动力的大口径发动机有可能使该行业转向气候中和运行。除了排放温室气体外,内燃机还排放污染物,危害人类健康和环境。有关天然气和氢气发动机颗粒物排放的研究主要集中在汽车和重型应用领域。因此,本研究首次对以氢气为动力的大口径单缸研究型发动机的颗粒物排放进行了调查,并与天然气进行了比较。对直径小至 10 纳米的颗粒进行的调查显示,颗粒数为 104 至 105 # cm-3,氢气中的颗粒数意外地略高于天然气运行中的颗粒数。这是因为在氢气运行中,润滑油中的颗粒和燃料与衬垫油膜的相互作用更强,这在 3D-CFD 模拟中得到了证实。与使用长链碳氢化合物燃料的相同发动机相比,其浓度仍然低几个数量级。基于气体成分 THC、CO 和 CO2 的扩展排放分析表明,这些油基颗粒引起的碳排放可以忽略不计。
{"title":"Investigations on particle emissions of large-bore engines powered by natural gas and hydrogen†","authors":"Felina Armbruster, Alexander Gelner, Andreas Zepf, Maximilian Prager, Martin Härtl and Malte Jaensch","doi":"10.1039/D4VA00200H","DOIUrl":"10.1039/D4VA00200H","url":null,"abstract":"<p >In an effort to mitigate the impact of climate change, <em>e.g.</em>, by reducing the emission of greenhouse gases, hydrogen is becoming an increasingly attractive alternative energy source, replacing conventional long-chain hydrocarbon fuels in the energy and transport sector. While there is a shift in individual transport towards battery-electric applications, the maritime and energy production sectors rely on a high energy density and time- and location-independent availability of the energy carrier. Therefore, large-bore engines powered by renewable fuels have the potential to shift the industry towards a climate-neutral operation. Besides the emission of greenhouse gases, internal combustion engines are known for emitting pollutant emissions, harming human health and the environment. Research on particle emissions of natural gas and hydrogen engines has mainly focused on automotive and heavy-duty applications. Hence, this study investigates particle emissions of a large-bore single-cylinder research engine powered by hydrogen, compared to natural gas, for the first time. Investigations on particles with a diameter as low as 10 nm showed particle numbers of 10<small><sup>4</sup></small> to 10<small><sup>5</sup></small> # cm<small><sup>−3</sup></small>, unexpectedly achieving slightly higher particle numbers in hydrogen than in natural gas operations. This is due to particles from lubricant oil and a stronger fuel interaction with the liner oil film in hydrogen operation, demonstrated within a 3D-CFD simulation. The concentrations are still lower by several orders of magnitude than in long-chain hydrocarbon fuel operations of identical engines. An extended emissions analysis based on the gaseous components THC, CO, and CO<small><sub>2</sub></small> shows the negligible carbonaceous emissions induced by these oil-based particles.</p>","PeriodicalId":72941,"journal":{"name":"Environmental science. Advances","volume":" 11","pages":" 1524-1536"},"PeriodicalIF":3.5,"publicationDate":"2024-08-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.rsc.org/en/content/articlepdf/2024/va/d4va00200h?page=search","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142208629","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
Investigating Thermomyces lanuginosus and Purpureocillium lilacinum to produce advanced myco-materials through selective fungal decellularization 研究通过选择性真菌脱细胞作用生产高级真菌材料的兰氏热酵母菌和紫胶酵母菌
IF 3.5 Q3 ENGINEERING, ENVIRONMENTAL Pub Date : 2024-08-15 DOI: 10.1039/D3VA00217A
Nikita Verma, Satya Eswari Jujjavarapu and Chinmaya Mahapatra

In healthcare and human life, and with the growing need for environmentally friendly materials to replace synthetic ones, biomaterials are essential. Desirable biomaterials may now be created using a wide range of extracted natural polymers. Mycelium-based biomaterials are being developed into more adaptable, inexpensive, and self-replicating products. Some fungal species, like Pleurotus ostreatus and Ganoderma lucidum, have been recognised as excellent sources of biomaterials with unique morphological, mechanical, and hydrodynamical characteristics. Thermomyces lanuginosus and Purpureocillium lilacinum are two fungal strains that may be used to create biomaterials. This article seeks to introduce these strains and use experimentation to identify their distinctive characteristics. The fungus was cultivated in a lab, and the growth kinetics of the fungus were estimated. The strains of P. lilacinum and T. lanuginosus had maximum specific growth rates (μmax) of 1.34 ± 0.024 and 3.09 ± 0.019 L−1 d−1, respectively. Decellularization of the fungal biomass was performed using 0.1% SDS solution, after which the scaffolds were created by drying the biomass in plastic moulds. Following that, analysis using scanning electron microscopy (SEM), energy dispersive X-ray spectroscopy (EDS), and Fourier transform infrared spectroscopy (FT-IR) was carried out. The porosity and swelling ratio were also determined and hydrodynamic characterization was performed for the samples. The results show that mycelia have the potential to serve as inexpensive, all-natural bio-scaffolds and T. lanuginosus-prepared materials have a larger swelling ratio and increased porosity, which makes them better myco-materials than those formed from P. lilacinum.

在医疗保健和人类生活中,人们越来越需要环保材料来替代合成材料,因此生物材料是必不可少的。现在,人们可以利用各种提取的天然聚合物制造出理想的生物材料。以菌丝体为基础的生物材料正被开发成适应性更强、成本更低和可自我复制的产品。一些真菌物种,如 Pleurotus ostreatus 和 Ganoderma lucidum,已被认为是具有独特形态、机械和流体力学特性的生物材料的极佳来源。热酵母菌(Thermomyces lanuginosus)和紫云英真菌(Purpureocillium lilacinum)是两种可用于制造生物材料的真菌菌株。本文旨在介绍这两种菌株,并通过实验确定它们的独特特性。在实验室中培养真菌,并估算真菌的生长动力学。P. lilacinum 和 T. lanuginosus 菌株的最大特定生长率(μmax)分别为 1.34 ± 0.024 和 3.09 ± 0.019 L-1 d-1。使用 0.1% SDS 溶液对真菌生物质进行脱细胞处理,然后在塑料模具中干燥生物质,制成支架。随后,使用扫描电子显微镜(SEM)、能量色散 X 射线光谱(EDS)和傅立叶变换红外光谱(FT-IR)进行了分析。此外,还测定了样品的孔隙率和膨胀率,并进行了流体力学表征。研究结果表明,菌丝体具有作为廉价、全天然生物支架的潜力,而蓝藻菌丝体制备的材料具有更大的膨胀率和更高的孔隙率,这使其成为比丝兰菌丝体更好的生物材料。
{"title":"Investigating Thermomyces lanuginosus and Purpureocillium lilacinum to produce advanced myco-materials through selective fungal decellularization","authors":"Nikita Verma, Satya Eswari Jujjavarapu and Chinmaya Mahapatra","doi":"10.1039/D3VA00217A","DOIUrl":"10.1039/D3VA00217A","url":null,"abstract":"<p >In healthcare and human life, and with the growing need for environmentally friendly materials to replace synthetic ones, biomaterials are essential. Desirable biomaterials may now be created using a wide range of extracted natural polymers. Mycelium-based biomaterials are being developed into more adaptable, inexpensive, and self-replicating products. Some fungal species, like <em>Pleurotus ostreatus</em> and <em>Ganoderma lucidum</em>, have been recognised as excellent sources of biomaterials with unique morphological, mechanical, and hydrodynamical characteristics. <em>Thermomyces lanuginosus</em> and <em>Purpureocillium lilacinum</em> are two fungal strains that may be used to create biomaterials. This article seeks to introduce these strains and use experimentation to identify their distinctive characteristics. The fungus was cultivated in a lab, and the growth kinetics of the fungus were estimated. The strains of <em>P. lilacinum</em> and <em>T. lanuginosus</em> had maximum specific growth rates (<em>μ</em><small><sub>max</sub></small>) of 1.34 ± 0.024 and 3.09 ± 0.019 L<small><sup>−1</sup></small> d<small><sup>−1</sup></small>, respectively. Decellularization of the fungal biomass was performed using 0.1% SDS solution, after which the scaffolds were created by drying the biomass in plastic moulds. Following that, analysis using scanning electron microscopy (SEM), energy dispersive X-ray spectroscopy (EDS), and Fourier transform infrared spectroscopy (FT-IR) was carried out. The porosity and swelling ratio were also determined and hydrodynamic characterization was performed for the samples. The results show that mycelia have the potential to serve as inexpensive, all-natural bio-scaffolds and <em>T. lanuginosus</em>-prepared materials have a larger swelling ratio and increased porosity, which makes them better myco-materials than those formed from <em>P. lilacinum.</em></p>","PeriodicalId":72941,"journal":{"name":"Environmental science. Advances","volume":" 10","pages":" 1413-1425"},"PeriodicalIF":3.5,"publicationDate":"2024-08-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.rsc.org/en/content/articlepdf/2024/va/d3va00217a?page=search","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142208647","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
Surfactant-enhanced coagulation and flocculation improves the removal of perfluoroalkyl substances from surface water† 表面活性剂强化混凝和絮凝可提高地表水中全氟烷基物质的去除率
IF 3.5 Q3 ENGINEERING, ENVIRONMENTAL Pub Date : 2024-08-13 DOI: 10.1039/D4VA00093E
Amith Sadananda Maroli, Yi Zhang, Jonathan Lubiantoro and Arjun K. Venkatesan

Coagulation/flocculation is a widely used water and wastewater treatment process due to its low cost, simplicity, and effectiveness. However, the process is not effective in the treatment of per- and polyfluoroalkyl substances (PFAS), the presence and treatment of which is an ongoing challenge for water providers. Here, we explore cationic surfactant-enhanced coagulation as a process modification to target the removal of PFAS in existing coagulation/flocculation systems. Batch experiments, in jar testing apparatus, were performed to assess the removal of two short-chain and two long-chain PFAS at an initial concentration of 10 μg L−1 with the addition of cetyltrimethylammonium chloride (CTAC) as the coagulant-aid. Our findings suggest that elevated coagulant dose (60 mg L−1 of alum or 100 mg L−1 of FeCl3) coupled with the addition of a cationic surfactant (1 mg L−1 of CTAC) significantly enhanced the removal of both short-chain (perfluorobutane sulfonate: PFBS removal to >40%) and long-chain PFAS (perfluorooctanoic acid: PFOA and perfluorooctane sulfonate: PFOS removal to >80%), with FeCl3 showing better performance than alum. Sulfonates (PFBS, PFOS) were shown to be removed more efficiently compared to carboxylates (PFBA, PFOA), presumably due to their higher hydrophobicity leading to better interactions with the flocs. Furthermore, CTAC in combination with traditionally used additives such as powdered activated carbon (PAC), served as a better aid for PFAS treatment and improved the removal of PFBS, PFOA, and PFOS to >98%. This study highlights that introducing a cost-effective pre-treatment with a cationic surfactant to existing conventional treatment systems can improve the performance efficiency in treating PFAS-contaminated waters.

混凝/絮凝因其成本低、操作简单、效果显著而被广泛应用于水和废水处理工艺中。然而,该工艺在处理全氟烷基和多氟烷基物质(PFAS)方面效果不佳,这些物质的存在和处理一直是供水企业面临的挑战。在此,我们探讨了阳离子表面活性剂增强混凝作为一种工艺改造,以去除现有混凝/絮凝系统中的 PFAS。我们在罐式测试设备中进行了批量实验,以评估在添加十六烷基三甲基氯化铵(CTAC)作为助凝剂的情况下,初始浓度为 10 μg L-1 的两种短链和两种长链 PFAS 的去除情况。我们的研究结果表明,提高混凝剂剂量(60 毫克/升-1 的明矾或 100 毫克/升-1 的氯化铁)并添加阳离子表面活性剂(1 毫克/升-1 的十六烷基三甲基氯化铵)可显著提高短链(全氟丁烷磺酸:PFBS 的去除率为 40%)和长链 PFAS(全氟辛酸、全氟辛烷磺酸和全氟辛基铵)的去除率:全氟辛酸和全氟辛烷磺酸)和长链 PFAS(全氟辛酸和全氟辛烷磺酸):全氟辛酸和全氟辛烷磺酸的去除率可达 80%),其中氯化铁的性能优于明矾。与羧酸盐(PFBA、PFOA)相比,磺酸盐(PFBS、PFOS)的去除效率更高,这可能是由于磺酸盐的疏水性更高,能更好地与絮凝物相互作用。此外,CTAC 与粉末活性炭 (PAC) 等传统添加剂结合使用,可以更好地辅助全氟辛烷磺酸的处理,并将全氟辛烷磺酸、全氟辛酸和全氟辛烷磺酸的去除率提高到 98%。这项研究表明,在现有的传统处理系统中引入一种具有成本效益的阳离子表面活性剂进行预处理,可以提高处理受 PFAS 污染水体的性能效率。
{"title":"Surfactant-enhanced coagulation and flocculation improves the removal of perfluoroalkyl substances from surface water†","authors":"Amith Sadananda Maroli, Yi Zhang, Jonathan Lubiantoro and Arjun K. Venkatesan","doi":"10.1039/D4VA00093E","DOIUrl":"10.1039/D4VA00093E","url":null,"abstract":"<p >Coagulation/flocculation is a widely used water and wastewater treatment process due to its low cost, simplicity, and effectiveness. However, the process is not effective in the treatment of per- and polyfluoroalkyl substances (PFAS), the presence and treatment of which is an ongoing challenge for water providers. Here, we explore cationic surfactant-enhanced coagulation as a process modification to target the removal of PFAS in existing coagulation/flocculation systems. Batch experiments, in jar testing apparatus, were performed to assess the removal of two short-chain and two long-chain PFAS at an initial concentration of 10 μg L<small><sup>−1</sup></small> with the addition of cetyltrimethylammonium chloride (CTAC) as the coagulant-aid. Our findings suggest that elevated coagulant dose (60 mg L<small><sup>−1</sup></small> of alum or 100 mg L<small><sup>−1</sup></small> of FeCl<small><sub>3</sub></small>) coupled with the addition of a cationic surfactant (1 mg L<small><sup>−1</sup></small> of CTAC) significantly enhanced the removal of both short-chain (perfluorobutane sulfonate: PFBS removal to &gt;40%) and long-chain PFAS (perfluorooctanoic acid: PFOA and perfluorooctane sulfonate: PFOS removal to &gt;80%), with FeCl<small><sub>3</sub></small> showing better performance than alum. Sulfonates (PFBS, PFOS) were shown to be removed more efficiently compared to carboxylates (PFBA, PFOA), presumably due to their higher hydrophobicity leading to better interactions with the flocs. Furthermore, CTAC in combination with traditionally used additives such as powdered activated carbon (PAC), served as a better aid for PFAS treatment and improved the removal of PFBS, PFOA, and PFOS to &gt;98%. This study highlights that introducing a cost-effective pre-treatment with a cationic surfactant to existing conventional treatment systems can improve the performance efficiency in treating PFAS-contaminated waters.</p>","PeriodicalId":72941,"journal":{"name":"Environmental science. Advances","volume":" 12","pages":" 1714-1721"},"PeriodicalIF":3.5,"publicationDate":"2024-08-13","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.rsc.org/en/content/articlepdf/2024/va/d4va00093e?page=search","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142208555","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
Accurate modeling of the potential energy surface of atmospheric molecular clusters boosted by neural networks† 利用神经网络对大气分子簇的势能面进行精确建模。
IF 3.5 Q3 ENGINEERING, ENVIRONMENTAL Pub Date : 2024-08-13 DOI: 10.1039/D4VA00255E
Jakub Kubečka, Daniel Ayoubi, Zeyuan Tang, Yosef Knattrup, Morten Engsvang, Haide Wu and Jonas Elm

The computational cost of accurate quantum chemistry (QC) calculations of large molecular systems can often be unbearably high. Machine learning offers a lower computational cost compared to QC methods while maintaining their accuracy. In this study, we employ the polarizable atom interaction neural network (PaiNN) architecture to train and model the potential energy surface of molecular clusters relevant to atmospheric new particle formation, such as sulfuric acid–ammonia clusters. We compare the differences between PaiNN and previous kernel ridge regression modeling for the Clusteromics I–V data sets. We showcase three models capable of predicting electronic binding energies and interatomic forces with mean absolute errors of <0.3 kcal mol−1 and <0.2 kcal mol−1 Å−1, respectively. Furthermore, we demonstrate that the error of the modeled properties remains below the chemical accuracy of 1 kcal mol−1 even for clusters vastly larger than those in the training database (up to (H2SO4)15(NH3)15 clusters, containing 30 molecules). Consequently, we emphasize the potential applications of these models for faster and more thorough configurational sampling and for boosting molecular dynamics studies of large atmospheric molecular clusters.

对大型分子系统进行精确量子化学(QC)计算的计算成本往往高得难以承受。与 QC 方法相比,机器学习在保持其准确性的同时,还能降低计算成本。在本研究中,我们采用可极化原子相互作用神经网络(PaiNN)架构来训练和模拟与大气新粒子形成相关的分子簇(如硫酸-氨簇)的势能面。我们比较了 PaiNN 与之前针对 Clusteromics I-V 数据集的核岭回归建模之间的差异。我们展示了三种能够预测电子结合能和原子间作用力的模型,其平均绝对误差分别为-1 和-1 Å-1。此外,我们还证明了建模属性的误差仍低于 1 kcal mol-1 的化学精度,即使是比训练数据库中的集群大得多的集群(多达 (H2SO4)15(NH3)15 集群,包含 30 个分子)也是如此。因此,我们强调这些模型在更快、更彻底的构型采样以及促进大型大气分子簇的分子动力学研究方面的潜在应用。
{"title":"Accurate modeling of the potential energy surface of atmospheric molecular clusters boosted by neural networks†","authors":"Jakub Kubečka, Daniel Ayoubi, Zeyuan Tang, Yosef Knattrup, Morten Engsvang, Haide Wu and Jonas Elm","doi":"10.1039/D4VA00255E","DOIUrl":"10.1039/D4VA00255E","url":null,"abstract":"<p >The computational cost of accurate quantum chemistry (QC) calculations of large molecular systems can often be unbearably high. Machine learning offers a lower computational cost compared to QC methods while maintaining their accuracy. In this study, we employ the polarizable atom interaction neural network (PaiNN) architecture to train and model the potential energy surface of molecular clusters relevant to atmospheric new particle formation, such as sulfuric acid–ammonia clusters. We compare the differences between PaiNN and previous kernel ridge regression modeling for the Clusteromics I–V data sets. We showcase three models capable of predicting electronic binding energies and interatomic forces with mean absolute errors of &lt;0.3 kcal mol<small><sup>−1</sup></small> and &lt;0.2 kcal mol<small><sup>−1</sup></small> Å<small><sup>−1</sup></small>, respectively. Furthermore, we demonstrate that the error of the modeled properties remains below the chemical accuracy of 1 kcal mol<small><sup>−1</sup></small> even for clusters vastly larger than those in the training database (up to (H<small><sub>2</sub></small>SO<small><sub>4</sub></small>)<small><sub>15</sub></small>(NH<small><sub>3</sub></small>)<small><sub>15</sub></small> clusters, containing 30 molecules). Consequently, we emphasize the potential applications of these models for faster and more thorough configurational sampling and for boosting molecular dynamics studies of large atmospheric molecular clusters.</p>","PeriodicalId":72941,"journal":{"name":"Environmental science. Advances","volume":" 10","pages":" 1438-1451"},"PeriodicalIF":3.5,"publicationDate":"2024-08-13","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.ncbi.nlm.nih.gov/pmc/articles/PMC11334116/pdf/","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142037920","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
期刊
Environmental science. Advances
全部 Acc. Chem. Res. ACS Applied Bio Materials ACS Appl. Electron. Mater. ACS Appl. Energy Mater. ACS Appl. Mater. Interfaces ACS Appl. Nano Mater. ACS Appl. Polym. Mater. ACS BIOMATER-SCI ENG ACS Catal. ACS Cent. Sci. ACS Chem. Biol. ACS Chemical Health & Safety ACS Chem. Neurosci. ACS Comb. Sci. ACS Earth Space Chem. ACS Energy Lett. ACS Infect. Dis. ACS Macro Lett. ACS Mater. Lett. ACS Med. Chem. Lett. ACS Nano ACS Omega ACS Photonics ACS Sens. ACS Sustainable Chem. Eng. ACS Synth. Biol. Anal. Chem. BIOCHEMISTRY-US Bioconjugate Chem. BIOMACROMOLECULES Chem. Res. Toxicol. Chem. Rev. Chem. Mater. CRYST GROWTH DES ENERG FUEL Environ. Sci. Technol. Environ. Sci. Technol. Lett. Eur. J. Inorg. Chem. IND ENG CHEM RES Inorg. Chem. J. Agric. Food. Chem. J. Chem. Eng. Data J. Chem. Educ. J. Chem. Inf. Model. J. Chem. Theory Comput. J. Med. Chem. J. Nat. Prod. J PROTEOME RES J. Am. Chem. Soc. LANGMUIR MACROMOLECULES Mol. Pharmaceutics Nano Lett. Org. Lett. ORG PROCESS RES DEV ORGANOMETALLICS J. Org. Chem. J. Phys. Chem. J. Phys. Chem. A J. Phys. Chem. B J. Phys. Chem. C J. Phys. Chem. Lett. Analyst Anal. Methods Biomater. Sci. Catal. Sci. Technol. Chem. Commun. Chem. Soc. Rev. CHEM EDUC RES PRACT CRYSTENGCOMM Dalton Trans. Energy Environ. Sci. ENVIRON SCI-NANO ENVIRON SCI-PROC IMP ENVIRON SCI-WAT RES Faraday Discuss. Food Funct. Green Chem. Inorg. Chem. Front. Integr. Biol. J. Anal. At. Spectrom. J. Mater. Chem. A J. Mater. Chem. B J. Mater. Chem. C Lab Chip Mater. Chem. Front. Mater. Horiz. MEDCHEMCOMM Metallomics Mol. Biosyst. Mol. Syst. Des. Eng. Nanoscale Nanoscale Horiz. Nat. Prod. Rep. New J. Chem. Org. Biomol. Chem. Org. Chem. Front. PHOTOCH PHOTOBIO SCI PCCP Polym. Chem.
×
引用
GB/T 7714-2015
复制
MLA
复制
APA
复制
导出至
BibTeX EndNote RefMan NoteFirst NoteExpress
×
0
微信
客服QQ
Book学术公众号 扫码关注我们
反馈
×
意见反馈
请填写您的意见或建议
请填写您的手机或邮箱
×
提示
您的信息不完整,为了账户安全,请先补充。
现在去补充
×
提示
您因"违规操作"
具体请查看互助需知
我知道了
×
提示
现在去查看 取消
×
提示
确定
Book学术官方微信
Book学术文献互助
Book学术文献互助群
群 号:481959085
Book学术
文献互助 智能选刊 最新文献 互助须知 联系我们:info@booksci.cn
Book学术提供免费学术资源搜索服务,方便国内外学者检索中英文文献。致力于提供最便捷和优质的服务体验。
Copyright © 2023 Book学术 All rights reserved.
ghs 京公网安备 11010802042870号 京ICP备2023020795号-1