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Constructive Feedback 建设性反馈
IF 9.028 1区 环境科学与生态学 Q1 ENGINEERING, ENVIRONMENTAL Pub Date : 2024-11-26 DOI: 10.1021/acs.est.4c11755
Julie B. Zimmerman, Pedro Alvarez, Jordi Dachs, Gregory Lowry, Susan Richardson, Fernando Rosario-Ortiz, Daniel Schlenk, David Waite, Peng Wang
Constructive feedback is the essence of advancing the scientific enterprise. It goes beyond mere critique and criticism, instead generously providing guidance for refining, for deepening, for strengthening, for improving. This type of input requires a generous reviewer, one who views critique as an opportunity for improvement rather than denigration. It is reflective of an individual who is willing to share their knowledge and expertise to help make the science─and the scientists─better. This type of feedback can offer a blueprint for enhancement, helping authors to elevate their research and enhance its impact. Constructive feedback begins with a mindset, one that sees potential in every submission and each review as an opportunity for growth and collaboration. In honoring the Peer Review Award winners, we celebrate individuals who embody this ideal, providing feedback that is as supportive as it is rigorous. They demonstrate an exceptional ability to identify strengths and weaknesses in submissions, all while providing authors with actionable guidance to improve their work. In this way, they play a critical role in advancing the quality of academic literature and fostering a culture of intellectual growth. This approach is crucial not just for individual papers but also for the scientific community as a whole to sustain and enhance public trust in our scientific contributions. A reviewer’s insightful critique can help shape the direction of future research, spark a new idea, and enable innovation. Constructive feedback fosters an environment in which knowledge evolves collaboratively, benefiting from the collective wisdom of the community. Ultimately, the Peer Review Award winners remind us that constructive feedback is not about finding faults; it is not just about evaluating, but rather enhancing. Constructive feedback is about building the knowledge basis, in building trust in science, in building the next generation of scholars. In recognizing their efforts, we celebrate these reviewers for building our community. <b>Super Reviewer Award</b> Bin Chen, <i>Beijing Normal University</i> Razi Epsztein, <i>Technion Israel Institute of Technology</i> Mingliang Fang, <i>Nanyang Technological University</i> Peter Herzsprung, <i>Helmholtz Centre for Environmental Research - UFZ</i> Carrie McDonough, <i>Carnegie Mellon University</i> Daisuke Minakata, <i>Michigan Technological University</i> Carsten Prasse, <i>Johns Hopkins University</i> Wenhui Qiu, <i>South University of Science and Technology</i> Collin Ward, <i>Woods Hole Oceanographic Institution</i> Han-Chao Zhang, <i>University of Science and Technology of China</i> Bingsheng Zhou, <i>Institute of Hydrobiology, Chinese Academy of Sciences</i> Shulin Zhuang, <i>Zhejiang University</i> <b>Excellence in Review</b> Qiqing Chen, <i>East China Normal University</i> Xinyi Cui, <i>Nanjing University</i> Jeseth Delgado Vela, <i>Duke University</i> Miriam Diamond, <i>University of Toronto</i> Lin Du, <i
建设性反馈是推进科学事业的精髓。它超越了单纯的批评和批判,而是慷慨地为完善、深化、加强和改进提供指导。这种类型的意见建议要求评论者慷慨大方,将批评视为改进的机会,而不是诋毁。它反映了一个人愿意分享自己的知识和专长,以帮助科学--和科学家--变得更好。这种类型的反馈可以提供一个改进蓝图,帮助作者提升研究水平,扩大研究影响。建设性的反馈始于一种心态,一种将每一份投稿和每一次审稿都视为成长与合作机会的心态。在表彰同行评审奖获得者的过程中,我们表彰那些体现了这一理想的个人,他们提供的反馈既支持又严格。他们表现出了卓越的能力,能够发现稿件中的优点和不足,同时为作者提供可行的指导,以改进他们的工作。通过这种方式,他们在提高学术文献质量和培养知识成长文化方面发挥着至关重要的作用。这种方法不仅对单篇论文至关重要,而且对整个科学界来说,也是维持和提高公众对我们科学贡献的信任的关键。审稿人富有洞察力的评论有助于确定未来研究的方向,激发新的想法,促进创新。建设性的反馈意见营造了一种环境,在这种环境中,知识可以协同发展,并从社区的集体智慧中获益。归根结底,同行评审奖的获奖者提醒我们,建设性反馈不是找茬,也不仅仅是评价,而是提升。建设性反馈关乎知识基础的建设,关乎科学信任的建立,关乎下一代学者的培养。为表彰这些审稿人的努力,我们为他们建设我们的社区而喝彩。超级审稿人奖 陈斌,北京师范大学 Razi Epsztein,以色列理工学院 方明亮,南洋理工大学 Peter Herzsprung,亥姆霍兹环境研究中心-UFZ Carrie McDonough,卡内基梅隆大学 Daisuke Minakata、密歇根理工大学 Carsten Prasse,约翰霍普金斯大学 邱文辉,南方科技大学 Collin Ward,伍兹霍尔海洋研究所 张汉超,中国科学技术大学 周炳生,中国科学院水生生物研究所 庄树林、浙江大学优秀评论员 华东师范大学 陈其庆 南京大学 崔欣怡 杜克大学 Jeseth Delgado Vela 多伦多大学 Miriam Diamond 山东大学 Lin Du 多伦多大学 Elizabeth Edwards 多伦多大学 Satoshi Endo、国立环境研究所 Aleksandar Goranov,老多米尼克大学 Atsuko Ikeda,北海道大学 Sai Liang,广东工业大学 Fudong Liu,加州大学河滨分校 Runzeng Liu,山东大学 Jinxing Ma,广东工业大学 Garrett McKay,德克萨斯 A&;M 大学 Andrew Meharg,贝尔法斯特女王大学 Bingcai Pan,南京大学 Corinne Scown,劳伦斯伯克利国家实验室 Wenpo Shan,中国科学院城市环境研究所 Virender Sharma,德克萨斯 A&;M University Elsie Sunderland, Harvard University Tiezheng Tong, Colorado State University Jason White, Connecticut Agricultural Experiment Station Lingtian Xie, South China Normal University Xin Yang, Sun Yat-Sen University Zhe Yang, The University of Queensland Ran Yin, Nanjing University Bo Yuan, Norwegian University of Science and Technology Songhu Yuan, China University of Geosciences Bofan Zhang, Tokyo Metropolitan University Hao Zhu, Tulane University 本文尚未被其他出版物引用。
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引用次数: 0
Effect of 60Co Irradiation on Boehmite Dissolution in Caustic Solutions 60Co 辐照对苛性钠溶液中沸石溶解的影响
IF 9.028 1区 环境科学与生态学 Q1 ENGINEERING, ENVIRONMENTAL Pub Date : 2024-11-26 DOI: 10.1021/acs.est.4c07544
Yatong Zhao, Ping Chen, Xiang Wang, Hanna Hlushko, Jay A. LaVerne, Lili Liu, Carolyn I. Pearce, Zheming Wang, Kevin M. Rosso, Xin Zhang
Here, we examine how radiation impacts the dissolution behavior of boehmite by subjecting dry nanoparticles of different sizes to 60Co γ radiation and subsequently analyzing their dissolution behavior in caustic solutions as a function of temperature. The measured kinetics show that irradiation with an amount 228.24 Mrad significantly slows the dissolution rate, particularly for smaller sizes at lower temperatures. Specifically, the temperature-dependent dissolution rates of irradiated 20 nm boehmite versus pristine material in 3 M NaOH solutions were several times lower (e.g., rate constant of 0.026 vs 0.075 h–1 at 60 °C), with an apparent activation energy 40 kJ mol–1 higher. Although various imaging techniques and X-ray diffraction measurements consistently revealed no obvious differences between pristine and irradiated samples, after irradiation significant binding energy shifts were detected in the X-ray photoelectron Spectroscopy peaks of Al 2p and O 1s, and a change in their relative intensities indicated a lower O/Al ratio. This suggests that γ-irradiation may stabilize boehmite particle surfaces by driving their chemistry and structure toward more stable aluminum oxide forms. This finding may help explain slower dissolution rates of boehmite in nuclear waste and may be useful for the development of more robust predictive models and effective strategies for waste processing.
在这里,我们将不同尺寸的干纳米颗粒置于 60Co γ 辐射下,然后分析它们在苛性碱溶液中的溶解行为与温度的函数关系,从而研究辐射如何影响沸石的溶解行为。测量的动力学结果表明,辐照量为 228.24 Mrad 的辐照会显著降低溶解速率,尤其是在较低温度下对较小尺寸的纳米颗粒而言。具体地说,在 3 M NaOH 溶液中,经辐照的 20 纳米玻镁石的溶解速率比原始材料低几倍(例如,60 °C 时的速率常数为 0.026 h-1 与 0.075 h-1),表观活化能高出 40 kJ mol-1。虽然各种成像技术和 X 射线衍射测量始终显示原始样品和辐照样品之间没有明显差异,但在辐照后,在 Al 2p 和 O 1s 的 X 射线光电子能谱峰中检测到明显的结合能移动,其相对强度的变化表明 O/Al 比率降低。这表明,γ-辐照可能会使沸石颗粒表面的化学和结构趋向于更稳定的氧化铝形式,从而使其更加稳定。这一发现可能有助于解释核废料中沸石溶解速度较慢的原因,并有助于开发更可靠的预测模型和制定有效的废料处理策略。
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引用次数: 0
MoS2 Nanosheets at Low Doses Induced Cardiotoxicity in Developing Zebrafish via Ferroptosis: Influence of Lateral Size and Surface Modification 低剂量 MoS2 纳米片通过铁突变诱发发育中斑马鱼的心脏毒性:横向尺寸和表面改性的影响
IF 9.028 1区 环境科学与生态学 Q1 ENGINEERING, ENVIRONMENTAL Pub Date : 2024-11-26 DOI: 10.1021/acs.est.4c08685
Wei Zou, Yishuang Chang, Xingli Zhang, Xinyu Li, Caixia Jin, Guoqing Zhang, Zhiguo Cao, Qixing Zhou
The widespread applications of molybdenum disulfide (MoS2) nanosheets inevitably result in their release into aquatic environments, necessitating an exploration of their potential toxic effects on aquatic organisms. This study analyzes the cardiac responses of zebrafish larvae exposed to MoS2, with a focus on the influence of size and surface modifications. At higher concentrations (1 and 5 mg/L), MoS2 nanosheets hampered larval growth without influencing cardiomyogenesis. At lower doses (0.5–100 μg/L), small-sized MoS2 (ssMoS2, 187.2 nm) significantly impaired cardiac development, as proved by morphology abnormality, decreased heartbeat, stroke volume, and cardiac output, whereas these undesirable changes were not observed in the cysteine-modified form. Large-sized nanosheets (1.638 μm) did not localize to the heart, barely showing a cardiac disorder. Transcriptomics, biochemical analysis, and computational simulation validated that ssMoS2 aggravated Fe2+ overload through excessive ferritinophagy and ferroportin-1 inhibition, accompanied by down-regulation of glutathione peroxidase 4 and activation of PUFAs esterification, leading to ferroptosis. Significant associations between ferroptosis signals and cardiac indices, along with the ferrostatin-1 inhibition test, confirmed the ferroptosis-mediated cardiotoxicity of ssMoS2. Our study provides a key understanding of molecular events underlying MoS2-induced cardiotoxicity and highlights the importance of size and surface characteristics, which are significant for risk assessment and the safe design of nanoproducts.
二硫化钼(MoS2)纳米片的广泛应用不可避免地会将其释放到水生环境中,因此有必要探讨其对水生生物的潜在毒性影响。本研究分析了暴露于 MoS2 的斑马鱼幼虫的心脏反应,重点关注尺寸和表面修饰的影响。在较高浓度(1 毫克/升和 5 毫克/升)下,MoS2 纳米片会阻碍幼体生长,但不会影响心肌生成。在较低剂量(0.5-100 μg/L)下,小尺寸的 MoS2(ssMoS2,187.2 nm)会显著影响心脏的发育,表现为形态异常、心跳次数减少、搏出量减少和心输出量减少,而半胱氨酸修饰型则不会出现这些不良变化。大尺寸纳米片(1.638 μm)没有定位到心脏,几乎没有显示出心脏功能紊乱。转录组学、生化分析和计算模拟验证了ssMoS2通过过度吞噬铁蛋白和抑制铁蛋白-1来加重Fe2+过载,并伴随着谷胱甘肽过氧化物酶4的下调和PUFAs酯化的激活,从而导致铁变态反应。铁蛋白沉积信号与心脏指标之间的显著关联以及铁前列素-1抑制试验证实了ssMoS2介导的铁蛋白沉积对心脏的毒性。我们的研究为了解 MoS2 诱导心脏毒性的分子事件提供了关键信息,并强调了尺寸和表面特征的重要性,这对风险评估和纳米产品的安全设计具有重要意义。
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引用次数: 0
Retrofitting Coal Power Units with Biomass and Coal Cofiring Intensifies Air Pollution and Health Risks 用生物质和燃煤技术改造煤电机组加剧了空气污染和健康风险
IF 9.028 1区 环境科学与生态学 Q1 ENGINEERING, ENVIRONMENTAL Pub Date : 2024-11-26 DOI: 10.1021/acs.est.4c04122
Bo Wang, Shuling Xu, Zhaohua Wang, Yuli Shan, Bin Zhang, Hao Li, Nana Deng, Han Shi
Retrofitting coal power units with biomass and coal cofiring technology provides a promising pathway toward low-carbon transition. However, such a retrofitting approach may also pose potential environmental and health risks, even aggravating regional disparities. Here, we propose a comprehensive framework to evaluate the associated risks of Biomass and Coal Cofiring Retrofit (BCCR) in China. We find that air pollutants such as SO2, PM2.5, and NOx will increase by an average of 27.9, 38.04, and 42.79% respectively compared to the scenario with no BCCR. The national-wide PM2.5 concentration-related premature mortalities in scenarios with BCCR are projected to increase by 23.53% on average in 2030. Moreover, the Highest-20% of provinces with higher health risks (also health vulnerable groups such as the elderly and children concentrated area) are 19 times greater than that in the Lowest-20% group. Results suggest that implementing a Targeted Pollution Control strategy for areas with higher health risks would be an economical and effective way to reduce the total pollutants emissions and mitigate the regional disparities in health risks. Our research proposes stringent pollution control measures on biomass and coal cofiring retrofit in advance in regions with the utmost necessity to facilitate a fair transition toward clean energy.
利用生物质和煤炭联合燃烧技术改造煤电机组为实现低碳转型提供了一条大有可为的途径。然而,这种改造方法也可能带来潜在的环境和健康风险,甚至加剧地区差异。在此,我们提出了一个综合框架来评估中国生物质和煤炭燃烧改造(BCCR)的相关风险。我们发现,与不进行生物质和煤炭燃烧改造的情景相比,二氧化硫、PM2.5 和氮氧化物等空气污染物将分别平均增加 27.9%、38.04% 和 42.79%。预计到 2030 年,在采用《生物多样性公约》的情景下,全国范围内与 PM2.5 浓度相关的过早死亡人数将平均增加 23.53%。此外,健康风险最高的 20% 省份(也包括老年人和儿童集中区等健康弱势群体)是健康风险最低的 20% 省份的 19 倍。研究结果表明,对健康风险较高的地区实施有针对性的污染控制策略,是减少污染物排放总量、缓解健康风险地区差异的经济而有效的方法。我们的研究建议在最有必要的地区提前对生物质和煤炭联合燃烧改造采取严格的污染控制措施,以促进向清洁能源的公平过渡。
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引用次数: 0
Transforming Aviation's Impact on the Climate: Rethinking the Research Strategy. 改变航空对气候的影响:重新思考研究战略。
IF 10.8 1区 环境科学与生态学 Q1 ENGINEERING, ENVIRONMENTAL Pub Date : 2024-11-26 Epub Date: 2024-11-15 DOI: 10.1021/acs.est.4c08470
Steffen Kallbekken, Marianne T Lund, David G Victor

Aviation is under tremendous pressure to mitigate its impacts on the climate, but the best response strategies are unknown today due to deep uncertainties. How low-emission fuels will scale to levels relevant for the industry, along with the best strategies for managing contrails and other non-CO2 effects, are unknowable today with unknown cost and disruption. A conventional risk-based approach that involves investment across a known set of options is unworkable; instead, we argue that an experimentalist approach is needed that addresses deep uncertainties head on. This hinges on four key factors: a critical mass of actors facing strong incentives to identify solutions, a wide search for alternatives through experiments, periodic assessments, and adjustment of goals and strategies. Present strategies do not give enough attention to higher-risk alternatives with disruptive potential, because those approaches have few political and organizational supporters. Small groups of highly motivated actors─such as the nascent coalition of first movers on clean aviation already forming in Europe and the U.S.─could initiate an experimentalist program. The challenges of the aviation sector mirror other hard-to-abate sectors, making this framework potentially applicable to a wider set of sectors where technological, business, and investment choices are shrouded in deep uncertainty.

航空业面临着减轻其对气候影响的巨大压力,但由于存在严重的不确定性,目前尚不清楚最佳的应对策略。如何将低排放燃料推广到与航空业相关的水平,以及管理烟雾和其他非二氧化碳影响的最佳策略,如今都是未知数,其成本和破坏性也是未知数。传统的基于风险的方法,即投资于一系列已知的选择方案是行不通的;相反,我们认为需要一种实验主义的方法,直接解决深层次的不确定性。这取决于四个关键因素:有足够多的行动者面临着寻找解决方案的强烈动机、通过实验广泛寻找替代方案、定期评估以及调整目标和战略。目前的战略没有足够重视具有破坏潜力的高风险替代方案,因为这些方案的政治和组织支持者很少。一些积极性很高的小团体--如欧洲和美国已经形成的清洁航空先行者联盟--可以启动一项实验计划。航空业所面临的挑战与其他难以消弭的行业如出一辙,这使得本框架有可能适用于更广泛的行业,在这些行业中,技术、商业和投资选择都被深深的不确定性所笼罩。
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引用次数: 0
Transcriptomic and Methylomic Analyses Show Significant Shifts in Biosynthetic Processes and Reduced Intrapopulation Gene Expression Variance in PAH-Adapted Atlantic Killifish. 转录组和甲基组分析表明,适应多环芳烃的大西洋鳉鱼的生物合成过程发生了显著变化,种群内基因表达变异减少。
IF 10.8 1区 环境科学与生态学 Q1 ENGINEERING, ENVIRONMENTAL Pub Date : 2024-11-26 Epub Date: 2024-11-17 DOI: 10.1021/acs.est.4c06845
Akila Harishchandra, Richard T Di Giulio, Nishad Jayasundara

Environmental contaminants pose a significant selection pressure across taxa, potentiating evolved resistance to chemicals. However, rapid evolution may alter molecular and physiological homeostasis leading to trade-offs. To elucidate molecular underpinnings of evolved chemical resistance, we compared liver gene expression and methylation profiles in polycyclic aromatic hydrocarbon (PAH)-adapted Atlantic killifish (Fundulus heteroclitus) in the Republic site (RP), Elizabeth River, Virginia with PAH-sensitive Kings Creek (KC) fish. We found 1607 differentially expressed and 2252 alternatively spliced genes between RP and KC, with highly enriched genes involving lipid and amino acid metabolism, respectively. While 308 genes had differentially methylated regions, only 13 of these genes were differentially expressed. The aryl hydrocarbon receptor 2b gene (ahr2b) was differentially methylated and expressed, as well as alternatively spliced signifying its critical role in mediating PAH tolerance. Notably, the intrapopulation coefficient of variation (CoV) was lower in 82% of 17,566 expressed genes in RP fish compared to KC fish. Among other pathways, these genes with low CoV were highly enriched in bioenergetic processes inferring reduced metabolic physiological variation as a population in RP fish. Altered metabolic gene expression and overall reduced gene expression variance in RP fish warrant further studies on fitness trade-offs including altered susceptibility to other stressors associated with rapid adaptation to anthropogenic pressures.

环境污染物对不同类群造成了巨大的选择压力,增强了进化过程中对化学品的抵抗力。然而,快速进化可能会改变分子和生理平衡,从而导致权衡。为了阐明进化的耐化学性的分子基础,我们比较了弗吉尼亚州伊丽莎白河共和国遗址(RP)中适应多环芳烃(PAH)的大西洋鳉鱼(Fundulus heteroclitus)与对多环芳烃敏感的国王溪(KC)鱼的肝脏基因表达和甲基化图谱。我们在 RP 和 KC 之间发现了 1607 个差异表达基因和 2252 个替代剪接基因,其中涉及脂质和氨基酸代谢的基因高度富集。虽然有 308 个基因有不同的甲基化区域,但其中只有 13 个基因有不同的表达。芳基碳氢化合物受体 2b 基因(ahr2b)的甲基化和表达存在差异,而且还存在交替剪接,这表明该基因在介导多环芳烃耐受性方面起着关键作用。值得注意的是,与 KC 鱼类相比,RP 鱼类 17,566 个表达基因中有 82% 的种群内变异系数(CoV)较低。在其他途径中,这些变异系数较低的基因在生物能过程中高度富集,推断出 RP 鱼群体中代谢生理变异减少。RP 鱼代谢基因表达的改变和基因表达变异的总体降低,值得进一步研究其适应性权衡问题,包括与快速适应人为压力相关的对其他压力因素的易感性的改变。
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引用次数: 0
Climate Policy Reduces Racial Disparities in Air Pollution from Transportation and Power Generation. 气候政策减少了交通和发电造成的空气污染中的种族差异。
IF 10.8 1区 环境科学与生态学 Q1 ENGINEERING, ENVIRONMENTAL Pub Date : 2024-11-26 DOI: 10.1021/acs.est.4c03719
Katherine H Jordan, Luke R Dennin, Peter J Adams, Paulina Jaramillo, Nicholas Z Muller

Energy system optimization models facilitate analyses on a national or regional scale. However, understanding the impacts of climate policy on specific populations requires a much higher spatial resolution. Here, we link an energy system optimization model to an integrated assessment model via an emission downscaling algorithm, translating air pollution emissions from nine U.S. regions to U.S. counties. We simulate the impacts of six distinct policy scenarios, including a current policy and a 2050 net-zero target, on NOx, SO2, and PM2.5 emissions from on-road transportation and electricity generation. We compare different policies based on their ability to reduce emission exposure and exposure disparity across racial groups, allowing decision-makers to assess the air pollution impacts of various policy instruments more holistically. Modeled policies include a clean electricity standard, an on-road ICE vehicle ban, a carbon tax, and a scenario that reaches net-zero GHG emissions by 2050. While exposure and disparities decrease in all scenarios, our results reveal persistent disparities until at least 2040, particularly for Black non-Hispanic Americans. Our estimates of avoided deaths due to air pollution emphasize the importance of policy timing, showing that thousands of lives can be saved by taking action in the near-term.

能源系统优化模型有助于在国家或地区范围内进行分析。然而,了解气候政策对特定人群的影响需要更高的空间分辨率。在这里,我们通过排放降尺度算法将能源系统优化模型与综合评估模型联系起来,将美国九个地区的空气污染排放转化为美国各县的空气污染排放。我们模拟了六种不同政策情景(包括现行政策和 2050 年净零目标)对公路运输和发电产生的氮氧化物、二氧化硫和 PM2.5 排放的影响。我们根据不同政策减少排放的能力以及不同种族群体之间的排放差异对其进行了比较,从而使决策者能够更全面地评估各种政策工具对空气污染的影响。模拟的政策包括清洁电力标准、道路内燃机汽车禁令、碳税以及到 2050 年实现温室气体净零排放的方案。虽然在所有方案中暴露和差距都会减少,但我们的结果显示至少在 2040 年之前差距会持续存在,尤其是对非西班牙裔美国黑人而言。我们对避免空气污染导致的死亡人数的估计强调了政策时机的重要性,表明在短期内采取行动可以挽救成千上万人的生命。
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引用次数: 0
Computational Study on the Octahedral Surfaces of Magnetite Nanoparticles and Their Solvent Interaction. 磁铁矿纳米颗粒八面体表面及其溶剂相互作用的计算研究
IF 10.8 1区 环境科学与生态学 Q1 ENGINEERING, ENVIRONMENTAL Pub Date : 2024-11-26 Epub Date: 2024-11-14 DOI: 10.1021/acs.est.4c06531
Anita S Katheras, Konstantinos Karalis, Matthias Krack, Andreas C Scheinost, Sergey V Churakov

Magnetite nanoparticles (MNPs) play an important role in geological and environmental systems because of their redox reactivity and ability to sequester a wide range of metals and metalloids. X-ray absorption spectroscopy conducted at metal and metalloid edges has suggested that the magnetite {111} faces of octahedrally shaped nanoparticles play a dominant role in the redox and sorption processes of these elements. However, studies directly probing the magnetite surfaces, especially in their fully solvated state, are scarce. Therefore, we investigated the speciation and stability over a wide Eh/pH range of octahedrally shaped MNPs of 2 nm size by means of Kohn-Sham density functional theory with Hubbard correction (DFT+U). By altering the protonation state of the crystals, a redox-sensitive response of the octahedrally coordinated Fe could be achieved. Furthermore, the preferential H distribution could be identified, highlighting the difference between the edges, vertices, and facets of the nanocrystals. Subsequently, the interactions of the MNPs with a solvent of pure water or a 0.5 M NaCl solution were studied by classical molecular dynamics (MD) simulations. Finally, a comparison of the corresponding macroscopic magnetite (111) surface to the investigated MNPs was conducted.

磁铁矿纳米颗粒(MNPs)因其氧化还原反应性和对多种金属和类金属的吸附能力而在地质和环境系统中发挥着重要作用。在金属和类金属边缘进行的 X 射线吸收光谱分析表明,八面体纳米粒子的磁铁矿 {111} 面在这些元素的氧化还原和吸附过程中起着主导作用。然而,直接探测磁铁矿表面,尤其是其完全溶解状态的研究却很少。因此,我们采用带有哈伯德校正(DFT+U)的 Kohn-Sham 密度泛函理论,研究了尺寸为 2 纳米的八面体 MNPs 在较宽 Eh/pH 范围内的标示和稳定性。通过改变晶体的质子化状态,可以实现八面体配位铁的氧化还原敏感响应。此外,还能确定 H 的优先分布,突出了纳米晶体边缘、顶点和切面之间的差异。随后,通过经典分子动力学(MD)模拟研究了 MNPs 与纯水或 0.5 M NaCl 溶液溶剂的相互作用。最后,将相应的宏观磁铁矿 (111) 表面与所研究的 MNPs 进行了比较。
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引用次数: 0
Freeze-Thaw Cycle Events Enable the Deep Disintegration of Biochar: Release of Dissolved Black Carbon and Its Structural-Dependent Carbon Sequestration Capacity. 冻融循环事件使生物炭深度解体:溶解黑碳的释放及其结构决定的碳封存能力。
IF 10.8 1区 环境科学与生态学 Q1 ENGINEERING, ENVIRONMENTAL Pub Date : 2024-11-26 Epub Date: 2024-11-14 DOI: 10.1021/acs.est.4c07262
Lang Zhu, Na Chen, Xianglei Zhang, Luyao Ren, Rui Zou, Jia Xie, Zhiqiang Wang, Huiqiang Yang, Zelin Hao, Jianjun Qin, Hanzhong Jia

Biochar is widely regarded as a recalcitrant carbon pool. However, the impact of freeze-thaw cycle events on its storage capacity, particularly on the release of dissolved black carbon (DBC), has remained poorly investigated. This study investigated the release behavior of DBC from biochar pyrolyzed at 300-700 °C during freeze-thaw cycles and their retention capacity in soil. Freeze-thaw cycles dramatically promoted DBC release (33.08-230.74 mg C L-1), exhibiting an order of magnitude higher than those without freeze-thaw process. The release kinetics of freeze-thaw-induced DBC varied depending on the pyrolysis temperature of biochar due to the different disintegration mechanisms. Interestingly, the retention capacity of freeze-thaw-induced DBC in soil showed a reduction ranging from 7.7 to 29.5% compared to DBC without the freeze-thaw process. This reduction can be attributed to numerous hydrophilic low-molecular-weight compounds (16.97-75.31%) in freeze-thaw-induced DBC, as evidenced by the results of size exclusion chromatography, fluorescence excitation/emission matrix, Fourier transform infrared spectroscopy, and nuclear magnetic resonance. These compounds tend to concentrate in the aqueous phase rather than being retained in the soil, potentially exacerbating the outflow of dissolved organic carbon. These findings clarify the release behavior of DBC during freeze-thaw cycles and reveal their contribution to the attenuation of carbon pools in cold regions.

生物炭被广泛认为是一种难降解的碳库。然而,关于冻融循环事件对其储存能力的影响,特别是对溶解黑碳(DBC)释放的影响,研究仍然很少。本研究调查了在 300-700 °C 下热解的生物炭在冻融循环期间的 DBC 释放行为及其在土壤中的保留能力。冻融循环极大地促进了 DBC 的释放(33.08-230.74 毫克 C L-1),比无冻融过程的释放量高出一个数量级。由于分解机制不同,冻融诱导的 DBC 释放动力学随生物炭的热解温度而变化。有趣的是,与未经冻融处理的 DBC 相比,冻融诱导的 DBC 在土壤中的保留能力降低了 7.7% 至 29.5%。从尺寸排阻色谱、荧光激发/发射矩阵、傅立叶变换红外光谱和核磁共振的结果来看,冻融诱导的 DBC 中含有大量亲水性低分子量化合物(16.97%-75.31%)。这些化合物往往集中在水相中,而不是保留在土壤中,这可能会加剧溶解有机碳的外流。这些发现澄清了冻融循环期间 DBC 的释放行为,并揭示了它们对寒冷地区碳库衰减的贡献。
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引用次数: 0
Constructive Feedback 建设性反馈
IF 10.8 1区 环境科学与生态学 Q1 ENGINEERING, ENVIRONMENTAL Pub Date : 2024-11-26 DOI: 10.1021/acs.est.4c1175510.1021/acs.est.4c11755
Julie B. Zimmerman*, Pedro Alvarez, Jordi Dachs, Gregory Lowry, Susan Richardson, Fernando Rosario-Ortiz, Daniel Schlenk, David Waite and Peng Wang, 
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引用次数: 0
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