ACS Central Science最新文献_第10页

Correction to “O-GlcNAcylation Facilitates the Interaction between Keratin 18 and Isocitrate Dehydrogenases and Potentially Influencing Cholangiocarcinoma Progression” 更正 "O-GlcNAcylation 促进角蛋白 18 与异柠檬酸脱氢酶之间的相互作用，并可能影响胆管癌的进展"

IF 12.7 1区化学

ACS Central Science Pub Date : 2024-10-21 DOI: 10.1021/acscentsci.4c0130210.1021/acscentsci.4c01302

Xiangfeng Meng, Yue Zhou, Lei Xu, Limu Hu, Changjiang Wang, Xiao Tian, Xiang Zhang, Yi Hao, Bo Cheng, Jing Ma*, Lei Wang*, Jialin Liu* and Ran Xie*,

引用次数: 0

Chemical Fingerprinting of PM2.5 via Sequential Speciation Analysis Using Electrochemical Mass Spectrometry 利用电化学质谱法进行序贯标样分析，对 PM2.5 进行化学指纹识别

IF 10.8 1区化学

ACS Central Science Pub Date : 2024-10-21 DOI: 10.1021/acs.est.4c0168210.1021/acs.est.4c01682

Lili Song, Luyao Zhong, Ting Li, Yufei Chen, Xinglei Zhang, Konstantin Chingin, Ni Zhang, Hui Li, Liyun Hu, Dongfa Guo, Huanwen Chen, Rui Su* and Jiaquan Xu*,

{"title":"Chemical Fingerprinting of PM2.5 via Sequential Speciation Analysis Using Electrochemical Mass Spectrometry","authors":"Lili Song, Luyao Zhong, Ting Li, Yufei Chen, Xinglei Zhang, Konstantin Chingin, Ni Zhang, Hui Li, Liyun Hu, Dongfa Guo, Huanwen Chen, Rui Su* and Jiaquan Xu*, ","doi":"10.1021/acs.est.4c0168210.1021/acs.est.4c01682","DOIUrl":"https://doi.org/10.1021/acs.est.4c01682https://doi.org/10.1021/acs.est.4c01682","url":null,"abstract":"Chemical fingerprinting to characterize the occurrence state and abundance of organic and inorganic constituents within fine particulate matter (PM2.5) is useful in evaluating the associated health risks and tracing pollution sources. Herein, an analytical strategy for the rapid analysis of metal and organic constituents in PM2.5 was developed employing a combination of sequential chemical extraction coupled with mass spectrometry detection. H2O, CH3OH, EDTA-2Na, electrochemical oxidation, and electrochemical reduction were sequentially utilized to extract the chemical constituents in PM2.5 samples on a homemade device employing simultaneous online detection using two linear trap quadrupole mass spectrometers (LTQ-MS) with electrospray ionization (ESI) in positive and negative modes. After a single analytical procedure, dozens of metals (e.g., Pb, Cr, and Cu), organic compounds (e.g., amines, polycyclic aromatic hydrocarbons, and aliphatic acids), and negative ions (e.g., NO3–, NO2–, and Cl–) were comprehensively detected in the water-soluble, liposoluble, insoluble, oxidizable, and reducible fractions of PM2.5 samples, and their physical and chemical relationships were established.","PeriodicalId":10,"journal":{"name":"ACS Central Science","volume":"58 43","pages":"19362–19371 19362–19371"},"PeriodicalIF":10.8,"publicationDate":"2024-10-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142550209","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Coupling Effect of Elemental Carbon and Organic Carbon on the Changes of Optical Properties and Oxidative Potential of Soot Particles under Visible Light 元素碳和有机碳对可见光下烟尘颗粒光学特性和氧化电位变化的耦合效应

IF 10.8 1区化学

ACS Central Science Pub Date : 2024-10-21 DOI: 10.1021/acs.est.4c0921710.1021/acs.est.4c09217

Rui Tang, Jiong Cao, Jing Shang*, Yu Kuang, Hong Geng and Xinghua Qiu,

{"title":"Coupling Effect of Elemental Carbon and Organic Carbon on the Changes of Optical Properties and Oxidative Potential of Soot Particles under Visible Light","authors":"Rui Tang, Jiong Cao, Jing Shang*, Yu Kuang, Hong Geng and Xinghua Qiu, ","doi":"10.1021/acs.est.4c0921710.1021/acs.est.4c09217","DOIUrl":"https://doi.org/10.1021/acs.est.4c09217https://doi.org/10.1021/acs.est.4c09217","url":null,"abstract":"Soot particles, coming from the incomplete combustion of fossil or biomass fuels, feature a core–shell structure with inner elemental carbon (EC) and outer organic carbon (OC). Both EC and OC are known to be photoactive under solar radiation. However, research on their coupling effect during photochemical aging remains limited. This study examines how the optical properties and oxidative potential (OP) of wood, coal, and diesel soot particles with varying EC and OC levels are affected by exposure to visible light. Wood soot, which has the highest OC content, showed the most significant changes in both optical properties and OP, indicating its highest sensitivity to visible light aging. Molecular composition analysis revealed that the reduction of polycyclic aromatic hydrocarbons (PAHs) and methyl-PAHs primarily affects the optical properties, while oxygenated PAHs play a major role in OP. Combined with the results from reactive oxygen species detection, it is suggested that EC initiates photoreactions by generating superoxide anions, while OC undergoes compositional changes that result in subsequent atmospheric effects. These findings enhance our understanding of the photochemical aging process of soot particles and their implications for climate and health.","PeriodicalId":10,"journal":{"name":"ACS Central Science","volume":"58 44","pages":"19832–19842 19832–19842"},"PeriodicalIF":10.8,"publicationDate":"2024-10-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142577717","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

How the Most Neglected Residual Species in MOF-Based Catalysts Involved in Catalytic Reactions to Form Toxic Byproducts 基于 MOF 的催化剂中最容易被忽视的残留物如何参与催化反应并形成有毒副产品

IF 10.8 1区化学

ACS Central Science Pub Date : 2024-10-21 DOI: 10.1021/acs.est.4c0635110.1021/acs.est.4c06351

Fukun Bi, Jiafeng Wei, Bin Gao, Shuting Ma, Ning Liu*, Jingcheng Xu*, Baolin Liu, Yuandong Huang and Xiaodong Zhang*,

{"title":"How the Most Neglected Residual Species in MOF-Based Catalysts Involved in Catalytic Reactions to Form Toxic Byproducts","authors":"Fukun Bi, Jiafeng Wei, Bin Gao, Shuting Ma, Ning Liu*, Jingcheng Xu*, Baolin Liu, Yuandong Huang and Xiaodong Zhang*, ","doi":"10.1021/acs.est.4c0635110.1021/acs.est.4c06351","DOIUrl":"https://doi.org/10.1021/acs.est.4c06351https://doi.org/10.1021/acs.est.4c06351","url":null,"abstract":"In recent years, multifarious new materials have been developed for environmental governance. Thereinto, metal organic framework (MOF)-based catalysts have been widely employed for heterogeneous catalysis because of their high porosity to confine noble metal particles faraway from aggregation. However, the potential reactions between residual species from the material synthesis process and target pollutants, which could form highly toxic byproducts, are often neglected. Herein, we took the widely used Zr-MOF, UiO-66, with highly thermal stability supported Pd catalysts as the example to investigate how the residual species in catalysts are involved in aromatic volatile organic compounds (VOCs) degradation reaction. The results showed that residual Cl species originated from the ZrCl4 metal precursor participated in the VOC degradation reaction, leading to the production of various chlorine-containing byproducts, even the hypertoxicity dioxin precursor, dichlorobenzene. Meanwhile, the chlorination mechanism for the formation of chlorine-containing byproducts was revealed by density functional theory calculation. Furthermore, the highly efficient residual Cl removal approaches are proposed. Importantly, the migration and transformation of residual Cl during the degradation of five benzene series VOCs are comprehensively studied and elucidated. We anticipate that these findings will raise alarm about the neglected issue of residual species in MOF-based catalysts for heterogeneous catalysis, especially environmentally friendly catalysis.","PeriodicalId":10,"journal":{"name":"ACS Central Science","volume":"58 44","pages":"19797–19806 19797–19806"},"PeriodicalIF":10.8,"publicationDate":"2024-10-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142577721","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Enhanced Rock Weathering as a Source of Metals to Promote Methanogenesis and Counteract CO2 Sequestration 强化岩石风化作为促进甲烷生成和抵消二氧化碳封存的金属来源

IF 10.8 1区化学

ACS Central Science Pub Date : 2024-10-21 DOI: 10.1021/acs.est.4c0475110.1021/acs.est.4c04751

Donglei Zhang, Qiang Zeng*, Hongyu Chen, Dongyi Guo, Gaoyuan Li and Hailiang Dong*,

{"title":"Enhanced Rock Weathering as a Source of Metals to Promote Methanogenesis and Counteract CO2 Sequestration","authors":"Donglei Zhang, Qiang Zeng*, Hongyu Chen, Dongyi Guo, Gaoyuan Li and Hailiang Dong*, ","doi":"10.1021/acs.est.4c0475110.1021/acs.est.4c04751","DOIUrl":"https://doi.org/10.1021/acs.est.4c04751https://doi.org/10.1021/acs.est.4c04751","url":null,"abstract":"Enhanced weathering of (ultra)mafic rocks has been proposed as a promising approach to sequester atmospheric CO2 and mitigate climate change. However, these silicate rocks contain varying amounts of trace metals, which are essential cofactors of metallaenzymes in methanogens. We found that weathering of crushed peridotite and basalt significantly promoted the growth and methanogenesis of a model methanogen─Methanosarcina acetivorans C2A under the condition of excess substrate. The released trace metals from peridotite and basalt, especially Fe, Ni, and Co, accounted for the promotion effect. Observation at different spatial scales showed a close association between the rocks and cells. Proteomic analysis revealed that rock amendment significantly enhanced the expression of core metalloenzymes in the methylotrophic methanogenesis pathway. Our study uncovers a previously unrecognized but important negative effect of enhanced rock weathering on methane production, which may counteract the carbon sequestration effort.","PeriodicalId":10,"journal":{"name":"ACS Central Science","volume":"58 44","pages":"19679–19689 19679–19689"},"PeriodicalIF":10.8,"publicationDate":"2024-10-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142577629","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Hydromechanical Modulation of Enzymatic Kinetics Using Microfluidically Configurable Nanoconfinement Arrays.

IF 12.7 1区化学

ACS Central Science Pub Date : 2024-10-21 eCollection Date: 2024-11-27 DOI: 10.1021/acscentsci.4c01094

Yunjie Wen, Yutao Li, Henry C W Chu, Shibo Cheng, Yong Zeng

{"title":"Hydromechanical Modulation of Enzymatic Kinetics Using Microfluidically Configurable Nanoconfinement Arrays.","authors":"Yunjie Wen, Yutao Li, Henry C W Chu, Shibo Cheng, Yong Zeng","doi":"10.1021/acscentsci.4c01094","DOIUrl":"10.1021/acscentsci.4c01094","url":null,"abstract":"Confinement of molecules occurs ubiquitously in nature and fundamentally affects their properties and reactions. Developing synthetic confinement systems capable of precise modulation of chemical reactions is critical to understanding the underlying mechanisms and to promoting numerous applications including biosensing. However, current nanoconfinement systems often require sophisticated fabrication and operation. Here we report a simplified nanoconfinement approach termed Configurable Hydromechanical Enzyme Modulation by Nanoconfinement Landscaping of Chemical Kinetics (CHEMNLOCK). This approach exploits a simple micropost device to generate an array of nanogaps with tunable geometries, enabling flexible spatial modulation of the kinetics of surface-bound enzymatic reactions and substantial enhancement of single-molecule reactions. We envision that the CHEMNLOCK concept could pave a new way for developing scalable and practical nanoconfinement systems with profound impacts on biosensing and clinical diagnostics.","PeriodicalId":10,"journal":{"name":"ACS Central Science","volume":"10 11","pages":"2059-2071"},"PeriodicalIF":12.7,"publicationDate":"2024-10-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.ncbi.nlm.nih.gov/pmc/articles/PMC11613295/pdf/","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142778797","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Correction to "O-GlcNAcylation Facilitates the Interaction between Keratin 18 and Isocitrate Dehydrogenases and Potentially Influencing Cholangiocarcinoma Progression".

IF 12.7 1区化学

ACS Central Science Pub Date : 2024-10-21 eCollection Date: 2024-11-27 DOI: 10.1021/acscentsci.4c01302

Xiangfeng Meng, Yue Zhou, Lei Xu, Limu Hu, Changjiang Wang, Xiao Tian, Xiang Zhang, Yi Hao, Bo Cheng, Jing Ma, Lei Wang, Jialin Liu, Ran Xie

引用次数: 0

Hydromechanical Modulation of Enzymatic Kinetics Using Microfluidically Configurable Nanoconfinement Arrays 利用微流体可配置纳米推力阵列对酶动力学进行水力学调控

IF 12.7 1区化学

ACS Central Science Pub Date : 2024-10-21 DOI: 10.1021/acscentsci.4c0109410.1021/acscentsci.4c01094

Yunjie Wen, Yutao Li, Henry C. W. Chu, Shibo Cheng and Yong Zeng*,

{"title":"Hydromechanical Modulation of Enzymatic Kinetics Using Microfluidically Configurable Nanoconfinement Arrays","authors":"Yunjie Wen, Yutao Li, Henry C. W. Chu, Shibo Cheng and Yong Zeng*, ","doi":"10.1021/acscentsci.4c0109410.1021/acscentsci.4c01094","DOIUrl":"https://doi.org/10.1021/acscentsci.4c01094https://doi.org/10.1021/acscentsci.4c01094","url":null,"abstract":"Confinement of molecules occurs ubiquitously in nature and fundamentally affects their properties and reactions. Developing synthetic confinement systems capable of precise modulation of chemical reactions is critical to understanding the underlying mechanisms and to promoting numerous applications including biosensing. However, current nanoconfinement systems often require sophisticated fabrication and operation. Here we report a simplified nanoconfinement approach termed Configurable Hydromechanical Enzyme Modulation by Nanoconfinement Landscaping of Chemical Kinetics (CHEMNLOCK). This approach exploits a simple micropost device to generate an array of nanogaps with tunable geometries, enabling flexible spatial modulation of the kinetics of surface-bound enzymatic reactions and substantial enhancement of single-molecule reactions. We envision that the CHEMNLOCK concept could pave a new way for developing scalable and practical nanoconfinement systems with profound impacts on biosensing and clinical diagnostics.A configurable nanoconfinement system was built upon pneumatically actuatable microfluidic devices to enable hydromechanical modulation and patterning of surface enzymatic reactions.","PeriodicalId":10,"journal":{"name":"ACS Central Science","volume":"10 11","pages":"2059–2071 2059–2071"},"PeriodicalIF":12.7,"publicationDate":"2024-10-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.acs.org/doi/epdf/10.1021/acscentsci.4c01094","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142719573","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Mitigating Grand Challenges in Life Cycle Inventory Modeling through the Applications of Large Language Models 通过应用大型语言模型缓解生命周期库存建模的巨大挑战

IF 10.8 1区化学

ACS Central Science Pub Date : 2024-10-21 DOI: 10.1021/acs.est.4c0763410.1021/acs.est.4c07634

Qingshi Tu*, Jing Guo, Nan Li, Jianchuan Qi and Ming Xu,

{"title":"Mitigating Grand Challenges in Life Cycle Inventory Modeling through the Applications of Large Language Models","authors":"Qingshi Tu*, Jing Guo, Nan Li, Jianchuan Qi and Ming Xu, ","doi":"10.1021/acs.est.4c0763410.1021/acs.est.4c07634","DOIUrl":"https://doi.org/10.1021/acs.est.4c07634https://doi.org/10.1021/acs.est.4c07634","url":null,"abstract":"The accuracy of life cycle assessment (LCA) studies is often questioned due to the two grand challenges of life cycle inventory (LCI) modeling: (1) missing foreground flow data and (2) inconsistency in background data matching. Traditional mechanistic methods (e.g., process simulation) and existing machine learning (ML) methods (e.g., similarity-based selection methods) are inadequate due to their limitations in scalability and generalizability. The large language models (LLMs) are well-positioned to address these challenges, given the massive and diverse knowledge learned through the pretraining step. Incorporating LLMs into LCI modeling can lead to the automation of inventory data curation from diverse data sources and to the implementation of a multimodal analytical capacity. In this article, we delineated the mechanisms and advantages of LLMs to addressing these two grand challenges. We also discussed the future research to enhance the use of LLMs for LCI modeling, which includes the key areas such as improving retrieval augmented generation (RAG), integration with knowledge graphs, developing prompt engineering strategies, and fine-tuning pretrained LLMs for LCI-specific tasks. The findings from our study serve as a foundation for future research on scalable and automated LCI modeling methods that can provide more appropriate data for LCA calculations.","PeriodicalId":10,"journal":{"name":"ACS Central Science","volume":"58 44","pages":"19595–19603 19595–19603"},"PeriodicalIF":10.8,"publicationDate":"2024-10-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142577660","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Effect, Fate and Remediation of Pharmaceuticals and Personal Care Products (PPCPs) during Anaerobic Sludge Treatment: A Review 厌氧污泥处理过程中药物和个人护理产品 (PPCPs) 的影响、归宿和补救：综述

IF 10.8 1区化学

ACS Central Science Pub Date : 2024-10-20 DOI: 10.1021/acs.est.4c0676010.1021/acs.est.4c06760

Xiaomin Wang, Yufen Wang*, Zixin Zhang, Lixin Tian, Tingting Zhu, Yingxin Zhao, Yindong Tong, Yongkui Yang, Peizhe Sun and Yiwen Liu*,

{"title":"Effect, Fate and Remediation of Pharmaceuticals and Personal Care Products (PPCPs) during Anaerobic Sludge Treatment: A Review","authors":"Xiaomin Wang, Yufen Wang*, Zixin Zhang, Lixin Tian, Tingting Zhu, Yingxin Zhao, Yindong Tong, Yongkui Yang, Peizhe Sun and Yiwen Liu*, ","doi":"10.1021/acs.est.4c0676010.1021/acs.est.4c06760","DOIUrl":"https://doi.org/10.1021/acs.est.4c06760https://doi.org/10.1021/acs.est.4c06760","url":null,"abstract":"Biomass energy recovery from sewage sludge through anaerobic treatment is vital for environmental sustainability and a circular economy. However, large amounts of pharmaceutical and personal care products (PPCPs) remain in sludge, and their interactions with microbes and enzymes would affect resource recovery. This article reviews the effects and mechanisms of PPCPs on anaerobic sludge treatment. Most PPCPs posed adverse impacts on methane production, while certain low-toxicity PPCPs could stimulate volatile fatty acids and biohydrogen accumulation. Changes in the microbial community structure and functional enzyme bioactivities were also summarized with PPCPs exposure. Notably, PPCPs such as carbamazepine could bind with the active sites of the enzyme and induce microbial stress responses. The fate of various PPCPs during anaerobic sludge treatment indicated that PPCPs featuring electron-donating groups (e.g., ·–NH2 and ·–OH), hydrophilicity, and low molecular weight were more susceptible to microbial utilization. Key biodegrading enzymes (e.g., cytochrome P450 and amidase) were crucial for PPCP degradation, although several PPCPs remain refractory to biotransformation. Therefore, remediation technologies including physical pretreatment, chemicals, bioaugmentation, and their combinations for enhancing PPCPs degradation were outlined. Among these strategies, advanced oxidation processes and combined strategies effectively removed complex and refractory PPCPs mainly by generating free radicals, providing recommendations for improving sludge detoxification.","PeriodicalId":10,"journal":{"name":"ACS Central Science","volume":"58 43","pages":"19095–19114 19095–19114"},"PeriodicalIF":10.8,"publicationDate":"2024-10-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142550198","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0