ACS ES&T engineering最新文献

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Optimal Management Strategy for Salt Adsorption Capacity in Machine Learning-Based Flow-Electrode Capacitive Deionization Process 基于机器学习的流电极电容式去离子工艺中盐吸附容量的优化管理策略
IF 7.4
ACS ES&T engineering Pub Date : 2024-07-17 DOI: 10.1021/acsestengg.4c0014210.1021/acsestengg.4c00142
Sung Il Yu, Junbeom Jeon, Yong-Uk Shin* and Hyokwan Bae*, 
{"title":"Optimal Management Strategy for Salt Adsorption Capacity in Machine Learning-Based Flow-Electrode Capacitive Deionization Process","authors":"Sung Il Yu,&nbsp;Junbeom Jeon,&nbsp;Yong-Uk Shin* and Hyokwan Bae*,&nbsp;","doi":"10.1021/acsestengg.4c0014210.1021/acsestengg.4c00142","DOIUrl":"https://doi.org/10.1021/acsestengg.4c00142https://doi.org/10.1021/acsestengg.4c00142","url":null,"abstract":"<p >Flow-electrode capacitive deionization (FCDI) has created a breakthrough toward a more stable desalination performance by adopting a flow-electrode compared to existing capacitive deionization and membrane capacitive deionization as a promising electrochemical water treatment technology. However, the FCDI technology requires investigation of various mechanisms pertaining to flow-electrode materials to achieve system optimization. Further, studies on applying machine learning to the FCDI technology have been scarcely reported. Our study aims to explore optimal algorithms via machine learning for predicting the salt adsorption capacity of FCDI processes and evaluate the feasibility of optimization applications. Concurrently, a comparative analysis was conducted through the performance model indicators of mean absolute error (MAE), mean squared error, and <i>R</i><sup>2</sup> for support vector machine, random forest, and artificial neural network (ANN) algorithms. Herein, we demonstrated that the optimal ANN-based model exhibited the highest predictive performance, achieving <i>R</i><sup>2</sup> and MAE values of 0.996 and 0.21 mg/g, respectively. Additionally, the Shapley additive explanations (SHAP) confirmed a trend in the contribution of influent concentration, aligning closely with the results of statistical analysis. Specifically, the change in voltage of the FCDI process serves as a key factor in determining salt adsorption efficiency. Moreover, a parallel comparison of the Pearson correlation coefficient and SHAP analyses suggests that the impact of voltage entails a nonlinear contribution within the realm of machine learning. Finally, to deploy a machine learning-driven ANN model system, we present multiple factors (e.g., weight of flow-electrodes, influent concentration, and voltages) as a reinforcement learning model for decision-making. This offers valuable insights and guidance for future operations of the FCDI process.</p>","PeriodicalId":7008,"journal":{"name":"ACS ES&T engineering","volume":null,"pages":null},"PeriodicalIF":7.4,"publicationDate":"2024-07-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141955524","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Smooth Vetch (Vicia villosa var.) Coupled with Ball-Milled Composite Mineral Derived from Shell Powder and Phosphate Rock for Remediation of Cadmium-Polluted Farmland: Insights into Synergetic Mechanisms 平滑茄(Vicia villosa var.)与从贝壳粉和磷酸盐岩中提取的球磨复合矿物质用于镉污染农田的修复:对协同机制的见解
IF 7.1
ACS ES&T engineering Pub Date : 2024-07-16 DOI: 10.1021/acsestengg.4c00177
Jianhua Qu, Yuhui Li, Fuxuan Bi, Xiaoyang Liu, Zonghao Dong, Hongli Fan, Mei Yin, Libo Fu, Weidong Cao, Ying Zhang
{"title":"Smooth Vetch (Vicia villosa var.) Coupled with Ball-Milled Composite Mineral Derived from Shell Powder and Phosphate Rock for Remediation of Cadmium-Polluted Farmland: Insights into Synergetic Mechanisms","authors":"Jianhua Qu, Yuhui Li, Fuxuan Bi, Xiaoyang Liu, Zonghao Dong, Hongli Fan, Mei Yin, Libo Fu, Weidong Cao, Ying Zhang","doi":"10.1021/acsestengg.4c00177","DOIUrl":"https://doi.org/10.1021/acsestengg.4c00177","url":null,"abstract":"Herein, a ball-milled composite mineral derived from shell powder and phosphate rock (BSPR) was innovatively coupled with smooth vetch (SV) planting to remediate Cd-polluted soil. The results showed that BSPR coupled with SV could reduce the bioavailability of Cd in soil by 68.1%, which was 2.2 and 3.4 times those of BSPR (31.1%) and SV (20.0%) alone, respectively. The outstanding passivation performance was confirmed to be due to the synergistic effect of BSPR and SV. Specifically, the employment of BSPR not only increased the biomass of SV but also promoted its decomposition, which directly led to the conversion of SV into more humic acid (HA). Under the action of HA, more calcium and phosphorus were released by BSPR and combined with Cd to form stable compounds (e.g., Cd<sub>3</sub>(PO<sub>4</sub>)<sub>2</sub>, Cd<sub>5</sub>(PO<sub>4</sub>)<sub>3</sub>Cl, and Cd<sub><i>n</i></sub>Ca<sub>5–<i>n</i></sub>(PO<sub>4</sub>)<sub>3</sub>OH). Amazingly, due to the excellent performance of synergetic BSPR and SV on Cd passivation and soil improvement, the Cd content in pepper fruit decreased by 38.2% (6.3 times that of SV), and the fresh weight and Ca content of pepper fruit were enhanced by 28.2% and 43.4% (6.7 and 22.8 times that of SV, respectively). Overall, this study provided a novel strategy, i.e., green manure coupled with mineral, for simultaneous remediation of Cd-contaminated farmland and enhancement of pepper’s yield and quality, thus achieving “killing three birds with one stone”.","PeriodicalId":7008,"journal":{"name":"ACS ES&T engineering","volume":null,"pages":null},"PeriodicalIF":7.1,"publicationDate":"2024-07-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141745685","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Smooth Vetch (Vicia villosa var.) Coupled with Ball-Milled Composite Mineral Derived from Shell Powder and Phosphate Rock for Remediation of Cadmium-Polluted Farmland: Insights into Synergetic Mechanisms 平滑茄(Vicia villosa var.)与从贝壳粉和磷酸盐岩中提取的球磨复合矿物质用于镉污染农田的修复:对协同机制的见解
IF 7.4
ACS ES&T engineering Pub Date : 2024-07-16 DOI: 10.1021/acsestengg.4c0017710.1021/acsestengg.4c00177
Jianhua Qu, Yuhui Li, Fuxuan Bi, Xiaoyang Liu, Zonghao Dong, Hongli Fan, Mei Yin, Libo Fu, Weidong Cao and Ying Zhang*, 
{"title":"Smooth Vetch (Vicia villosa var.) Coupled with Ball-Milled Composite Mineral Derived from Shell Powder and Phosphate Rock for Remediation of Cadmium-Polluted Farmland: Insights into Synergetic Mechanisms","authors":"Jianhua Qu,&nbsp;Yuhui Li,&nbsp;Fuxuan Bi,&nbsp;Xiaoyang Liu,&nbsp;Zonghao Dong,&nbsp;Hongli Fan,&nbsp;Mei Yin,&nbsp;Libo Fu,&nbsp;Weidong Cao and Ying Zhang*,&nbsp;","doi":"10.1021/acsestengg.4c0017710.1021/acsestengg.4c00177","DOIUrl":"https://doi.org/10.1021/acsestengg.4c00177https://doi.org/10.1021/acsestengg.4c00177","url":null,"abstract":"<p >Herein, a ball-milled composite mineral derived from shell powder and phosphate rock (BSPR) was innovatively coupled with smooth vetch (SV) planting to remediate Cd-polluted soil. The results showed that BSPR coupled with SV could reduce the bioavailability of Cd in soil by 68.1%, which was 2.2 and 3.4 times those of BSPR (31.1%) and SV (20.0%) alone, respectively. The outstanding passivation performance was confirmed to be due to the synergistic effect of BSPR and SV. Specifically, the employment of BSPR not only increased the biomass of SV but also promoted its decomposition, which directly led to the conversion of SV into more humic acid (HA). Under the action of HA, more calcium and phosphorus were released by BSPR and combined with Cd to form stable compounds (e.g., Cd<sub>3</sub>(PO<sub>4</sub>)<sub>2</sub>, Cd<sub>5</sub>(PO<sub>4</sub>)<sub>3</sub>Cl, and Cd<sub><i>n</i></sub>Ca<sub>5–<i>n</i></sub>(PO<sub>4</sub>)<sub>3</sub>OH). Amazingly, due to the excellent performance of synergetic BSPR and SV on Cd passivation and soil improvement, the Cd content in pepper fruit decreased by 38.2% (6.3 times that of SV), and the fresh weight and Ca content of pepper fruit were enhanced by 28.2% and 43.4% (6.7 and 22.8 times that of SV, respectively). Overall, this study provided a novel strategy, i.e., green manure coupled with mineral, for simultaneous remediation of Cd-contaminated farmland and enhancement of pepper’s yield and quality, thus achieving “killing three birds with one stone”.</p>","PeriodicalId":7008,"journal":{"name":"ACS ES&T engineering","volume":null,"pages":null},"PeriodicalIF":7.4,"publicationDate":"2024-07-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141954871","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Impact of Biochar Addition Levels on Remediation of Uranium-Stressed Soil: Evidence from 16S rDNA and Metabolomics 生物炭添加量对铀胁迫土壤修复的影响:来自 16S rDNA 和代谢组学的证据
IF 7.4
ACS ES&T engineering Pub Date : 2024-07-13 DOI: 10.1021/acsestengg.4c0011510.1021/acsestengg.4c00115
Huachuan Feng, Yilin Wang, Xiaofeng Wang, Nan Li, Qiuyang Li, Jin Li, Xiaoming Chen, Qing Wang* and Wenkun Zhu*, 
{"title":"Impact of Biochar Addition Levels on Remediation of Uranium-Stressed Soil: Evidence from 16S rDNA and Metabolomics","authors":"Huachuan Feng,&nbsp;Yilin Wang,&nbsp;Xiaofeng Wang,&nbsp;Nan Li,&nbsp;Qiuyang Li,&nbsp;Jin Li,&nbsp;Xiaoming Chen,&nbsp;Qing Wang* and Wenkun Zhu*,&nbsp;","doi":"10.1021/acsestengg.4c0011510.1021/acsestengg.4c00115","DOIUrl":"https://doi.org/10.1021/acsestengg.4c00115https://doi.org/10.1021/acsestengg.4c00115","url":null,"abstract":"<p >The addition of soil amendments to facilitate plant-based remediation of soil contaminated with radioactive nuclides is considered a promising approach. Here, we tested different levels of biochar to help clean uranium-contaminated soil in the potted plants. Adding 1% biochar had the best results in deactivating uranium, increasing soil enzyme activity, and promoting ryegrass growth. Microbiological and metabolomic analysis further revealed that 1 wt % biochar significantly enhanced the abundance of microorganisms such as Actinobacteriota and Myxococcota and accelerated the production of differential metabolites such as lipids and lipid-like molecules, organic acids and derivatives, and organic oxygen compounds. The analysis of biological and nonbiological interaction networks indicates that the coordinated interaction between bacteria, enzymes, and metabolites significantly improves the expression level of the ABC transporter’s metabolic pathway. This enhances the resistance of living cells to uranium and maintains system homeostasis under uranium stress. This study provides an example of the application of biochar-assisted phytoremediation and offers theoretical guidance for the remediation of soil contaminated with radioactive nuclides.</p>","PeriodicalId":7008,"journal":{"name":"ACS ES&T engineering","volume":null,"pages":null},"PeriodicalIF":7.4,"publicationDate":"2024-07-13","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141954854","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Impact of Biochar Addition Levels on Remediation of Uranium-Stressed Soil: Evidence from 16S rDNA and Metabolomics 生物炭添加量对铀胁迫土壤修复的影响:来自 16S rDNA 和代谢组学的证据
IF 7.1
ACS ES&T engineering Pub Date : 2024-07-13 DOI: 10.1021/acsestengg.4c00115
Huachuan Feng, Yilin Wang, Xiaofeng Wang, Nan Li, Qiuyang Li, Jin Li, Xiaoming Chen, Qing Wang, Wenkun Zhu
{"title":"Impact of Biochar Addition Levels on Remediation of Uranium-Stressed Soil: Evidence from 16S rDNA and Metabolomics","authors":"Huachuan Feng, Yilin Wang, Xiaofeng Wang, Nan Li, Qiuyang Li, Jin Li, Xiaoming Chen, Qing Wang, Wenkun Zhu","doi":"10.1021/acsestengg.4c00115","DOIUrl":"https://doi.org/10.1021/acsestengg.4c00115","url":null,"abstract":"The addition of soil amendments to facilitate plant-based remediation of soil contaminated with radioactive nuclides is considered a promising approach. Here, we tested different levels of biochar to help clean uranium-contaminated soil in the potted plants. Adding 1% biochar had the best results in deactivating uranium, increasing soil enzyme activity, and promoting ryegrass growth. Microbiological and metabolomic analysis further revealed that 1 wt % biochar significantly enhanced the abundance of microorganisms such as Actinobacteriota and Myxococcota and accelerated the production of differential metabolites such as lipids and lipid-like molecules, organic acids and derivatives, and organic oxygen compounds. The analysis of biological and nonbiological interaction networks indicates that the coordinated interaction between bacteria, enzymes, and metabolites significantly improves the expression level of the ABC transporter’s metabolic pathway. This enhances the resistance of living cells to uranium and maintains system homeostasis under uranium stress. This study provides an example of the application of biochar-assisted phytoremediation and offers theoretical guidance for the remediation of soil contaminated with radioactive nuclides.","PeriodicalId":7008,"journal":{"name":"ACS ES&T engineering","volume":null,"pages":null},"PeriodicalIF":7.1,"publicationDate":"2024-07-13","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141608585","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Prochiral Selectivity in Enzymatic Polyethylene Terephthalate Depolymerization Revealed by Computational Modeling 通过计算建模揭示酶促聚对苯二甲酸乙二醇酯解聚过程中的手性选择性
IF 7.1
ACS ES&T engineering Pub Date : 2024-07-09 DOI: 10.1021/acsestengg.4c00253
Mingna Zheng, Xiaomin Zhu, Yanwei Li, Qingzhu Zhang, Weiliang Dong, Wenxing Wang
{"title":"Prochiral Selectivity in Enzymatic Polyethylene Terephthalate Depolymerization Revealed by Computational Modeling","authors":"Mingna Zheng, Xiaomin Zhu, Yanwei Li, Qingzhu Zhang, Weiliang Dong, Wenxing Wang","doi":"10.1021/acsestengg.4c00253","DOIUrl":"https://doi.org/10.1021/acsestengg.4c00253","url":null,"abstract":"Enzyme catalysis has shown its great power in dealing with global poly(ethylene terephthalate) (PET) waste. However, it is still challenging to design a super enzyme that can treat the sheer volume of worldwide PET waste. Without a complete understanding of the catalytic mechanism, it will be difficult to reach this important goal. Here, we systematically study the PET depolymerization mechanism catalyzed by structurally different hydrolases. The role of fleeting chiral intermediates was proved to be crucial. We observed different prochiral selectivities among these PET hydrolases. While most hydrolases favor <i>Si</i>-face binding, a few hydrolases (e.g., <i>Humicola insolens</i> cutinase) mainly adapt <i>Re</i>-face binding. Interestingly, we found that <i>Si</i>-face binding leads to higher activity than <i>Re</i>-face binding in all of the studied hydrolases. This <i>Si</i>-face selectivity originates from the difficulty of proton transfer from catalytic histidine residue to the substrate and the less stability of the oxyanion hole. Since the <i>Si</i>-face binding ratio ranges from 0 to 95%, we infer that all these hydrolases are not perfectly evolved to degrade PET. Our in silico results highlight that enlarging binding site residues (e.g., Leu66 and Asn69) will enhance enzymatic depolymerization, which was further confirmed by our in vitro experiments where both Leu66Phe and Asn69Phe show significantly increased PET hydrolysis activity. Hopefully, this work will aid the future rational design of super enzymes to fight PET pollution.","PeriodicalId":7008,"journal":{"name":"ACS ES&T engineering","volume":null,"pages":null},"PeriodicalIF":7.1,"publicationDate":"2024-07-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141567481","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Prochiral Selectivity in Enzymatic Polyethylene Terephthalate Depolymerization Revealed by Computational Modeling 通过计算建模揭示酶促聚对苯二甲酸乙二醇酯解聚过程中的手性选择性
IF 7.4
ACS ES&T engineering Pub Date : 2024-07-09 DOI: 10.1021/acsestengg.4c0025310.1021/acsestengg.4c00253
Mingna Zheng, Xiaomin Zhu, Yanwei Li*, Qingzhu Zhang, Weiliang Dong* and Wenxing Wang, 
{"title":"Prochiral Selectivity in Enzymatic Polyethylene Terephthalate Depolymerization Revealed by Computational Modeling","authors":"Mingna Zheng,&nbsp;Xiaomin Zhu,&nbsp;Yanwei Li*,&nbsp;Qingzhu Zhang,&nbsp;Weiliang Dong* and Wenxing Wang,&nbsp;","doi":"10.1021/acsestengg.4c0025310.1021/acsestengg.4c00253","DOIUrl":"https://doi.org/10.1021/acsestengg.4c00253https://doi.org/10.1021/acsestengg.4c00253","url":null,"abstract":"<p >Enzyme catalysis has shown its great power in dealing with global poly(ethylene terephthalate) (PET) waste. However, it is still challenging to design a super enzyme that can treat the sheer volume of worldwide PET waste. Without a complete understanding of the catalytic mechanism, it will be difficult to reach this important goal. Here, we systematically study the PET depolymerization mechanism catalyzed by structurally different hydrolases. The role of fleeting chiral intermediates was proved to be crucial. We observed different prochiral selectivities among these PET hydrolases. While most hydrolases favor <i>Si</i>-face binding, a few hydrolases (e.g., <i>Humicola insolens</i> cutinase) mainly adapt <i>Re</i>-face binding. Interestingly, we found that <i>Si</i>-face binding leads to higher activity than <i>Re</i>-face binding in all of the studied hydrolases. This <i>Si</i>-face selectivity originates from the difficulty of proton transfer from catalytic histidine residue to the substrate and the less stability of the oxyanion hole. Since the <i>Si</i>-face binding ratio ranges from 0 to 95%, we infer that all these hydrolases are not perfectly evolved to degrade PET. Our in silico results highlight that enlarging binding site residues (e.g., Leu66 and Asn69) will enhance enzymatic depolymerization, which was further confirmed by our in vitro experiments where both Leu66Phe and Asn69Phe show significantly increased PET hydrolysis activity. Hopefully, this work will aid the future rational design of super enzymes to fight PET pollution.</p>","PeriodicalId":7008,"journal":{"name":"ACS ES&T engineering","volume":null,"pages":null},"PeriodicalIF":7.4,"publicationDate":"2024-07-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142228136","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Unveiling the Mechanistic Role of Surface Nitrogen and Sulfur in Boosting the Dechlorination Performance of Zero-Valent Iron 揭示表面氮和硫在提高零价铁脱氯性能中的机理作用
IF 7.1
ACS ES&T engineering Pub Date : 2024-07-01 DOI: 10.1021/acsestengg.4c00241
Li Gong, Jingting Chen, Lei Shen, Zaizhi Zhang, Chenyun Xia, Fei Wu, Yancai Yao, Chengshuai Liu, Liyuan Liang, Feng He
{"title":"Unveiling the Mechanistic Role of Surface Nitrogen and Sulfur in Boosting the Dechlorination Performance of Zero-Valent Iron","authors":"Li Gong, Jingting Chen, Lei Shen, Zaizhi Zhang, Chenyun Xia, Fei Wu, Yancai Yao, Chengshuai Liu, Liyuan Liang, Feng He","doi":"10.1021/acsestengg.4c00241","DOIUrl":"https://doi.org/10.1021/acsestengg.4c00241","url":null,"abstract":"Nitridated zero-valent iron (N-ZVI) and its sulfidated counterpart (S–N-ZVI) are promising materials for groundwater remediation. The dechlorination performance of N-ZVI and S–N-ZVI is intricately linked to the specific N and S surface speciation, yet their roles in tuning the physicochemical characteristics, dechlorination reactivity, and electron selectivity of both particles remain unclear. In this study, we synthesized ZVIs using varied N and S agents, leading to the formation of different surface N species (iron nitrides (Fe<sub><i>x</i></sub>N<sub><i>y</i></sub>), pyridinic, and graphitic nitrogen) and sulfur species (FeS and FeS<sub>2</sub>). The trichloroethylene (TCE) dechlorination rate showed a linear correlation with Fe<sub><i>x</i></sub>N<sub><i>y</i></sub> content, indicating Fe<sub><i>x</i></sub>N<sub><i>y</i></sub>-mediated ZVI dechlorination. Hydrogen production capacity was, however, linearly correlated with pyridinic N. Electron paramagnetic resonance (EPR) analysis revealed that pyridinic N enhanced proton transfer processes, thereby facilitating atomic hydrogen generation. This was further supported by the reduced H/D kinetic isotope effects (KIEs) in N-ZVI (2.07) and S–N-ZVI (∼1) compared to unmodified ZVI (3.06) and noticeable mitigation of surface passivation in N-ZVI and S–N-ZVI at pH 9. FeS and FeS<sub>2</sub> species minimized the hydrogen evolution reaction and removed the proton transfer limitation in TCE dechlorination. This magnifies the effect of Fe<sub><i>x</i></sub>N<sub><i>y</i></sub> and contributes to a synergistic interplay between nitridation and sulfidation in enhancing the dechlorination kinetics.","PeriodicalId":7008,"journal":{"name":"ACS ES&T engineering","volume":null,"pages":null},"PeriodicalIF":7.1,"publicationDate":"2024-07-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141549701","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Unveiling the Mechanistic Role of Surface Nitrogen and Sulfur in Boosting the Dechlorination Performance of Zero-Valent Iron 揭示表面氮和硫在提高零价铁脱氯性能中的机理作用
IF 7.4
ACS ES&T engineering Pub Date : 2024-07-01 DOI: 10.1021/acsestengg.4c0024110.1021/acsestengg.4c00241
Li Gong, Jingting Chen, Lei Shen, Zaizhi Zhang, Chenyun Xia, Fei Wu, Yancai Yao, Chengshuai Liu, Liyuan Liang and Feng He*, 
{"title":"Unveiling the Mechanistic Role of Surface Nitrogen and Sulfur in Boosting the Dechlorination Performance of Zero-Valent Iron","authors":"Li Gong,&nbsp;Jingting Chen,&nbsp;Lei Shen,&nbsp;Zaizhi Zhang,&nbsp;Chenyun Xia,&nbsp;Fei Wu,&nbsp;Yancai Yao,&nbsp;Chengshuai Liu,&nbsp;Liyuan Liang and Feng He*,&nbsp;","doi":"10.1021/acsestengg.4c0024110.1021/acsestengg.4c00241","DOIUrl":"https://doi.org/10.1021/acsestengg.4c00241https://doi.org/10.1021/acsestengg.4c00241","url":null,"abstract":"<p >Nitridated zero-valent iron (N-ZVI) and its sulfidated counterpart (S–N-ZVI) are promising materials for groundwater remediation. The dechlorination performance of N-ZVI and S–N-ZVI is intricately linked to the specific N and S surface speciation, yet their roles in tuning the physicochemical characteristics, dechlorination reactivity, and electron selectivity of both particles remain unclear. In this study, we synthesized ZVIs using varied N and S agents, leading to the formation of different surface N species (iron nitrides (Fe<sub><i>x</i></sub>N<sub><i>y</i></sub>), pyridinic, and graphitic nitrogen) and sulfur species (FeS and FeS<sub>2</sub>). The trichloroethylene (TCE) dechlorination rate showed a linear correlation with Fe<sub><i>x</i></sub>N<sub><i>y</i></sub> content, indicating Fe<sub><i>x</i></sub>N<sub><i>y</i></sub>-mediated ZVI dechlorination. Hydrogen production capacity was, however, linearly correlated with pyridinic N. Electron paramagnetic resonance (EPR) analysis revealed that pyridinic N enhanced proton transfer processes, thereby facilitating atomic hydrogen generation. This was further supported by the reduced H/D kinetic isotope effects (KIEs) in N-ZVI (2.07) and S–N-ZVI (∼1) compared to unmodified ZVI (3.06) and noticeable mitigation of surface passivation in N-ZVI and S–N-ZVI at pH 9. FeS and FeS<sub>2</sub> species minimized the hydrogen evolution reaction and removed the proton transfer limitation in TCE dechlorination. This magnifies the effect of Fe<sub><i>x</i></sub>N<sub><i>y</i></sub> and contributes to a synergistic interplay between nitridation and sulfidation in enhancing the dechlorination kinetics.</p>","PeriodicalId":7008,"journal":{"name":"ACS ES&T engineering","volume":null,"pages":null},"PeriodicalIF":7.4,"publicationDate":"2024-07-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142228015","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Distinct Mechanisms between Free Iron Species and Magnetite Addition in Anaerobic Digestion on Alleviating Ammonia Inhibition 厌氧消化中的游离铁物种和磁铁矿添加物在缓解氨抑制作用方面的不同机制
IF 7.1
ACS ES&T engineering Pub Date : 2024-06-28 DOI: 10.1021/acsestengg.4c00171
Xiao-Feng Dai, Yanru Bai, Shu-Juan Lian, Xue-Jiao Qi, Kai Feng, Shan-Fei Fu, Rong-Bo Guo
{"title":"Distinct Mechanisms between Free Iron Species and Magnetite Addition in Anaerobic Digestion on Alleviating Ammonia Inhibition","authors":"Xiao-Feng Dai, Yanru Bai, Shu-Juan Lian, Xue-Jiao Qi, Kai Feng, Shan-Fei Fu, Rong-Bo Guo","doi":"10.1021/acsestengg.4c00171","DOIUrl":"https://doi.org/10.1021/acsestengg.4c00171","url":null,"abstract":"Ammonia inhibition often occurs during anaerobic digestion (AD) of the protein-rich substrate. Iron-containing substances were proved to be efficient in alleviating the ammonia stress. However, the mechanisms behind, especially the distinct impacts of different forms of iron materials, are not fully revealed. Here, the alleviating performances of FeCl<sub>3</sub> and Fe<sub>3</sub>O<sub>4</sub> on AD systems under ammonia stress were investigated. Moreover, the mechanisms behind these were revealed and compared at the transcriptional level. Results showed that FeCl<sub>3</sub> and Fe<sub>3</sub>O<sub>4</sub> additions with an equal amount of iron element content (1.29 mM) led to the increased cumulative biogas and methane yields under an ammonia concentration of 3 g/L. Furthermore, the addition of iron-containing substances alleviated the accumulation of volatile fatty acids (VFAs) and extracellular polymeric substances (soluble carbohydrates and protein) caused by ammonia stress, which also had an obvious positive effect on the electron transfer capability. Microbial analysis demonstrated that the microbes (e.g., orders <i>Methanosarcinales</i>, <i>Clostridiales</i>, and <i>Syntrophobacterales</i>) associated with direct interspecies electron transfer (DIET), syntrophic acetate oxidization, and degradation of organic compounds were enriched. Metatranscriptomic analysis showed that ammonia inhibited the AD process by disrupting cellular redox homeostasis, infecting the ATPase activity, affecting cellular energy supply, inhibiting methane-producing enzyme activity, and suppressing the expression of cell conductive structure genes. Meanwhile, the addition of FeCl<sub>3</sub> and Fe<sub>3</sub>O<sub>4</sub> enhanced the cellular basal metabolism and energy supply, as well as microbial electron transfer and enzymic activities on methanogenesis. Metatranscriptomic analysis indicated that the addition of free iron species (FeCl<sub>3</sub>) can relieve the ammonia stress on syntrophic propionate and acetate oxidizing bacteria, enhance DIET by stimulating the synthesis of c-type cytochrome, and thus promote methane production. Meanwhile, Fe<sub>3</sub>O<sub>4</sub> may promote methane production by stimulating the expression of related genes and facilitating electron transfer in the AD system as a capacitor. Overall, the results demonstrated that ferric chloride and magnetite can alleviate the ammonia inhibition in the AD process of high-nitrogen waste through different mechanisms.","PeriodicalId":7008,"journal":{"name":"ACS ES&T engineering","volume":null,"pages":null},"PeriodicalIF":7.1,"publicationDate":"2024-06-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141507799","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
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