ACS ES&T engineeringPub Date : 2025-02-15DOI: 10.1021/acsestengg.4c0088110.1021/acsestengg.4c00881
Chao Zhang, Qihao Cao, Jing Zhang, Bo Fu, Yan Zhang and He Liu*,
{"title":"Accumulated Acetate Serves as a Driving Force for the Succession of Heterotrophic Microbiome and Acetate Degradation in Microbial Electrosynthesis Systems","authors":"Chao Zhang, Qihao Cao, Jing Zhang, Bo Fu, Yan Zhang and He Liu*, ","doi":"10.1021/acsestengg.4c0088110.1021/acsestengg.4c00881","DOIUrl":"https://doi.org/10.1021/acsestengg.4c00881https://doi.org/10.1021/acsestengg.4c00881","url":null,"abstract":"<p >In microbial electrosynthesis (MES) systems, acetate is an important primary product generated through the reduction of oxidized CO<sub>2</sub>. However, microbes that negatively regulated acetate synthesis through acetate degradation in MES are still unclear. This study used DNA stable isotope probing (SIP) and sequencing techniques to explore the reason for acetate degradation and the taxa and succession patterns of the degrading microbiome. The results showed that with the transition from acetate synthesis to degradation, the relative abundance of unclassified_f_Rhodocyclaceae, which is identified as acetate-degrading bacteria, increased rapidly in suspensions and was significantly higher than its abundance in biofilms. Meanwhile, the quantity of DNA in suspensions is higher than that in biofilms, further demonstrating that the dominant unclassified_f_Rhodocyclaceae in the degrading microbiome were mainly present in suspensions. The results of DNA-SIP-coupled metagenomic sequencing revealed that the primary acetate-degrading species belonged to Rhodocyclaceae including <i>Azonexus hydrophilus</i>, <i>Azonexus fungiphilus</i>, etc. In addition, the potential syntrophic acetate-oxidizing bacteria <i>Mesotoga infera</i> could form a syntrophic relationship with <i>Desulfolutivibrio sulfodismutans</i> to participate in acetate degradation. In situ product removal experiments showed that acetate drove the degrading microbiome growth, and timely acetate removal could effectively inhibit the proliferation of degrading bacteria. This study fills the research gap of acetate degrading microbiome in MES systems.</p>","PeriodicalId":7008,"journal":{"name":"ACS ES&T engineering","volume":"5 5","pages":"1255–1266 1255–1266"},"PeriodicalIF":7.4,"publicationDate":"2025-02-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143921334","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}
ACS ES&T engineeringPub Date : 2025-02-15DOI: 10.1021/acsestengg.4c0079510.1021/acsestengg.4c00795
Jingkun An, Yuyan Tang, Zhihong Ye, Xin Wang, Yujie Feng and Nan Li*,
{"title":"Tuning Three-Electron Oxygen Reduction Pathway for •OH Production from O2: A Critical Review of Fundamental Principles, Catalyst/Electrode Development, and Application","authors":"Jingkun An, Yuyan Tang, Zhihong Ye, Xin Wang, Yujie Feng and Nan Li*, ","doi":"10.1021/acsestengg.4c0079510.1021/acsestengg.4c00795","DOIUrl":"https://doi.org/10.1021/acsestengg.4c00795https://doi.org/10.1021/acsestengg.4c00795","url":null,"abstract":"<p >The oxygen reduction reaction (ORR) has been widely studied and applied in various fields. Traditionally, the ORR could be classified into a two-electron pathway with hydrogen peroxide (H<sub>2</sub>O<sub>2</sub>) as the product and a four-electron pathway with water (H<sub>2</sub>O) as the product. Recently, a three-electron pathway, namely, catalyzing O<sub>2</sub> directly into a hydroxyl radical (•OH), has attracted growing attention. Given the development prospects of this emerging reaction, this review focuses on the fundamental principles, catalytic material developments, and applications of the three-electron ORR-based Fenton (like) process. New insight into two/three/four-electron ORR based on proton/electron flow is illustrated, and the required features as well as electrode design strategy are summarized. Extensive discussions on the development and application of monometallic, polymetallic, and metal-free three-electron ORR electrodes are provided. The catalytic mechanisms involved in reactive oxygen species (ROSs) formation, structure–function relationship, and key active site transformation are presented. Finally, the challenges and future prospects of the three-electron ORR are discussed.</p>","PeriodicalId":7008,"journal":{"name":"ACS ES&T engineering","volume":"5 3","pages":"584–606 584–606"},"PeriodicalIF":7.4,"publicationDate":"2025-02-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143609005","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}
ACS ES&T engineeringPub Date : 2025-02-15DOI: 10.1021/acsestengg.4c0076810.1021/acsestengg.4c00768
Wm. Vincent Anderson, Hendrik Verweij and Linda K. Weavers*,
{"title":"Energy Analysis of Electrofiltration in a Homogeneous Macroporous α-Al2O3 Membrane","authors":"Wm. Vincent Anderson, Hendrik Verweij and Linda K. Weavers*, ","doi":"10.1021/acsestengg.4c0076810.1021/acsestengg.4c00768","DOIUrl":"https://doi.org/10.1021/acsestengg.4c00768https://doi.org/10.1021/acsestengg.4c00768","url":null,"abstract":"<p >Membrane filtration offers high-quality permeate at the cost of energy-intensive mechanical pumping. Electrofiltration, or electric field-assisted water permeation, has shown promise in reducing energy expenses, eliminating mechanical components, and providing instantaneous flow reversal for membrane defouling. However, fundamental analysis of the energy consumption, energy efficiency, defined as the specific energy consumption, SEC, and standardized nomenclature hinders development. Using a sintered random loose packing of monodisperse α-Al<sub>2</sub>O<sub>3</sub> spheres to create a well-defined geometry, microstructure, and composition, we investigated electroosmotic flow through the membrane to evaluate the SEC of components within an electrofiltration membrane. At minimal transmembrane pressure and compared to no electric field, application of an electrical potential, ΔΦ, of 10 V (pressure difference of 1.2 kPa, pH 3.8, and 22 °C) increased the membrane flux 15-fold from the initial 2–31 LMH. The observed energy consumption with the well-defined physical membrane properties and net electroosmotic flow (EOF) of 29 LMH resulted in SEC<sub>EOF</sub> = 0.31 kWh/m<sup>3</sup>. A fundamental determination of the theoretical minimum SEC, SEC<sub>EOF</sub><sup>min</sup>, is estimated to be 0.006 kWh/m<sup>3</sup>. While the SEC<sub>EOF</sub> determined is efficient for traditional membrane filtration and literature reported SEC<sub>EOF</sub>, the SEC<sub>EOF</sub> in this study is ascribed almost entirely to electrode losses and ionic transport resistance. These energy losses indicate significant opportunities to improve energy efficiency of electric field-assisted filtrations. This quantitative evaluation identifies electrofiltration performance and reasons for energy loss within an EOF system, which may be further studied to improve the energy efficiency of electric field-assisted filtration.</p>","PeriodicalId":7008,"journal":{"name":"ACS ES&T engineering","volume":"5 4","pages":"1003–1010 1003–1010"},"PeriodicalIF":7.4,"publicationDate":"2025-02-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143814428","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}
ACS ES&T engineeringPub Date : 2025-02-12DOI: 10.1021/acsestengg.4c0089510.1021/acsestengg.4c00895
Yusra S. Khalid, S. M. Mohaiminul Islam, Shafigh Mehraeen and Brian P. Chaplin*,
{"title":"Reactive-Transport Modeling of Oxidation Pathways of Insensitive High Munitions in Porous Flow-Through Electrodes","authors":"Yusra S. Khalid, S. M. Mohaiminul Islam, Shafigh Mehraeen and Brian P. Chaplin*, ","doi":"10.1021/acsestengg.4c0089510.1021/acsestengg.4c00895","DOIUrl":"https://doi.org/10.1021/acsestengg.4c00895https://doi.org/10.1021/acsestengg.4c00895","url":null,"abstract":"<p >A mathematical reactive-transport model was developed to investigate the electrochemical oxidation pathways of 2,4-dinitroanisole (DNAN), nitroguanidine (NQ), and 3-nitro-1,2,4-triazol-5-one (NTO), which are insensitive high explosives (IHEs) produced by the Department of Defense. Proposed electrochemical oxidation pathways for DNAN, NQ, and NTO were validated using reactive-transport modeling, density functional theory (DFT) simulations, and experimental data. The reactive-transport model was calibrated to experimental data collected with and without NaCl to evaluate the effects of hydroxyl radicals (OH<sup>•</sup>) and the chlorine evolution reaction (CER) on IHE oxidation pathways. DFT simulations provided further insight into the reactions between IHE and reactive chlorine species (RCSs). The findings revealed that the initial electrochemical oxidation step of DNAN and NTO was primarily by direct electron transfer, with minimal contribution from reactions with OH<sup>•</sup>. In contrast, NQ exhibited electrode surface blocking due to electrochemical polymerization in the absence of NaCl. However, the presence of NaCl generated RCSs that reacted with NQ, reducing electrode surface blocking. The model also accounted for solvent decomposition and background species reactions, providing a comprehensive understanding of the electrochemical oxidation processes for DNAN, NQ, and NTO. The model can be applied to guide electrochemical treatment of IHEs at Department of Defense sites.</p>","PeriodicalId":7008,"journal":{"name":"ACS ES&T engineering","volume":"5 5","pages":"1267–1278 1267–1278"},"PeriodicalIF":7.4,"publicationDate":"2025-02-12","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143921331","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}
ACS ES&T engineeringPub Date : 2025-02-12DOI: 10.1021/acsestengg.4c0082410.1021/acsestengg.4c00824
Patrícia Pereira, Willem Slear, Peter M. Guirguis, Phillip E. Savage* and Christian W. Pester*,
{"title":"Influence of Metal Salts on the Hydrolysis of Postconsumer Poly(ethylene Terephthalate)","authors":"Patrícia Pereira, Willem Slear, Peter M. Guirguis, Phillip E. Savage* and Christian W. Pester*, ","doi":"10.1021/acsestengg.4c0082410.1021/acsestengg.4c00824","DOIUrl":"https://doi.org/10.1021/acsestengg.4c00824https://doi.org/10.1021/acsestengg.4c00824","url":null,"abstract":"<p >This study reveals the effects of 23 metal salts on the hydrolysis of postconsumer poly(ethylene terephthalate) (PET). Isothermal reactions were conducted at 200 °C for 2 h and with a 1/10 (w/w) loading of PET and water. Terephthalic acid (TPA) yields of at least 80% were obtained with indium and ytterbium triflates, zinc iodide, potassium and sodium carbonates, potassium phosphate, and sodium bicarbonate. Without additives, the TPA yield was less than 10%, suggesting that these salts are potential candidates to improve the chemical recycling of PET. We expect complete catalytic depolymerization of PET to be available at longer times or higher temperatures. Reuse of zinc acetate solution for sequential hydrolysis experiments consistently gave high TPA yields for six cycles. We used experimental dataset and machine learning to determine that TPA yields and PET conversion were primarily influenced by the mass ratio of metal salt to PET, Lewis acidity, solution ionic strength, and pH. The catalytic effect of some metal triflates first increased with increasing Lewis acidity but peaked and declined as the Lewis acidity increased further. This suggests that higher Lewis acidity not only increases the intrinsic rate of hydrolysis but also increases the strength of the solvation shell around the catalyst, thereby hindering its access to the ester bonds in PET.</p>","PeriodicalId":7008,"journal":{"name":"ACS ES&T engineering","volume":"5 5","pages":"1140–1148 1140–1148"},"PeriodicalIF":7.4,"publicationDate":"2025-02-12","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143921332","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}
ACS ES&T engineeringPub Date : 2025-02-12DOI: 10.1021/acsestengg.4c0081710.1021/acsestengg.4c00817
Ao Zhong, Kehan Li, Zeyu Duan, Haiqiang Wang* and Zhongbiao Wu,
{"title":"Efficient Degradation of Trimethylamine via Vacuum Ultraviolet Irradiation with Morphology-Tuned CeO2","authors":"Ao Zhong, Kehan Li, Zeyu Duan, Haiqiang Wang* and Zhongbiao Wu, ","doi":"10.1021/acsestengg.4c0081710.1021/acsestengg.4c00817","DOIUrl":"https://doi.org/10.1021/acsestengg.4c00817https://doi.org/10.1021/acsestengg.4c00817","url":null,"abstract":"<p >Trimethylamine (TMA) is a common malodorous compound that poses serious environmental and health risks. Four different structures of cerium oxide (CeO<sub>2</sub>), namely, cubes, hollow spheres, octahedrons, and spindles, were successfully synthesized via a hydrothermal method and then used for TMA degradation in a vacuum ultraviolet photocatalytic oxidation system. All the synthesized catalysts exhibited enhanced activity compared with commercial CeO<sub>2</sub>. The hollow-sphere CeO<sub>2</sub> demonstrated high catalytic performance, achieving 75.9% mineralization of TMA within 90 min and substantially reduced ozone generation (stable 0 ppm in outlet). Additionally, the total outlet concentration of secondary nitrogenous pollutants (NO<sub><i>x</i></sub> and NH<sub>3</sub>) remained below 2.5 ppm. In situ infrared spectroscopy was employed to elucidate the degradation pathway of TMA under vacuum ultraviolet irradiation, comparing sphere CeO<sub>2</sub> with commercial CeO<sub>2</sub>. The superior TMA degradation performance of the hollow-sphere CeO<sub>2</sub> was attributed to its higher Ce<sup>3+</sup> ratio as well as increased oxygen, increased charge separation efficiency, and radical generation. This study provides new insights into the optimization of CeO<sub>2</sub>-based photocatalysts to efficiently degrade TMA and offers promising solutions for odor control and environmental protection.</p>","PeriodicalId":7008,"journal":{"name":"ACS ES&T engineering","volume":"5 5","pages":"1111–1121 1111–1121"},"PeriodicalIF":7.4,"publicationDate":"2025-02-12","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143921333","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}
ACS ES&T engineeringPub Date : 2025-02-11DOI: 10.1021/acsestengg.5c0011110.1021/acsestengg.5c00111
Brian P. Chaplin*,
{"title":"Advanced Electrochemical Technologies for Water Treatment, Resource Recovery, and Sustainable Energy","authors":"Brian P. Chaplin*, ","doi":"10.1021/acsestengg.5c0011110.1021/acsestengg.5c00111","DOIUrl":"https://doi.org/10.1021/acsestengg.5c00111https://doi.org/10.1021/acsestengg.5c00111","url":null,"abstract":"","PeriodicalId":7008,"journal":{"name":"ACS ES&T engineering","volume":"5 3","pages":"566–568 566–568"},"PeriodicalIF":7.4,"publicationDate":"2025-02-11","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143608927","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}
ACS ES&T engineeringPub Date : 2025-02-09DOI: 10.1021/acsestengg.4c0086110.1021/acsestengg.4c00861
Lianghui Xia, Yujie Liu, Kang Hui Lim, Qiyuan Liu, Meizan Jing*, Yanfei Jian, Jingjing Wang, He Xu, Mudi Ma*, Shouning Chai, Reem Albilali and Chi He*,
{"title":"Stretched Pd-CoOx Interfaces-Induced Oxygen Vacancy Consecutive Activation Realizes Light Alkane Efficacious Destruction","authors":"Lianghui Xia, Yujie Liu, Kang Hui Lim, Qiyuan Liu, Meizan Jing*, Yanfei Jian, Jingjing Wang, He Xu, Mudi Ma*, Shouning Chai, Reem Albilali and Chi He*, ","doi":"10.1021/acsestengg.4c0086110.1021/acsestengg.4c00861","DOIUrl":"https://doi.org/10.1021/acsestengg.4c00861https://doi.org/10.1021/acsestengg.4c00861","url":null,"abstract":"<p >The introduction of oxygen vacancies (O<sub>v</sub>) into catalyst structures has proven to be an effective strategy for enhancing their activity. To maintain their catalytic performance, however, the efficacious replenishing of the continuously depleted O<sub>v</sub> during reactions is pivotal and still a great challenge. To address this, a Pd-CoO<sub>x</sub>/CeO<sub>2</sub> catalyst (Pd-Ens) with highly exposed Pd-CoO<sub><i>x</i></sub> interfaces was rationally crafted, over which remarkable propane degradation activity, stability, and SO<sub>2</sub> resistance can be obtained owing to high Pd<sup>2+</sup> ratio and significant O<sub>v</sub> content. The exposed Pd–CoO<sub><i>x</i></sub> interfaces stretched the lattice of Pd–Ens catalyst, which boosts the redox capacity and charge transfer ability, facilitating the activation of lattice oxygen (O<sub>lat</sub>) for O<sub>v</sub> generation and subsequently stabilizing the Pd species. Continuous O<sub>lat</sub> activation and abundant O<sub>v</sub> promote the adsorption and activation of propane and oxygen over Pd–Ens, accelerating the formation of the acetone intermediate while expediting subsequent deep oxidation. Moreover, the adsorption of SO<sub>2</sub> impurity is well limited over Pd–Ens surface attributing to the existence of Pd–CoO<sub><i>x</i></sub> interfaces. In comparison, the Pd–Sup2 counterpart with internal PdO/Co<sub>3</sub>O<sub>4</sub> interfaces exhibits inferior propane catalytic performance and SO<sub>2</sub> resistance due to the irreversible O<sub>v</sub> depletion, extensive Pd species oxidation, and strong SO<sub>2</sub> adsorption. Besides, the weak mineralization ability makes Pd–Sup2 yield more harmful byproducts. These findings offer crucial guidance for developing efficient and practicable catalysts for light alkane degradation as well as other heterogeneous oxidation reactions.</p>","PeriodicalId":7008,"journal":{"name":"ACS ES&T engineering","volume":"5 5","pages":"1226–1241 1226–1241"},"PeriodicalIF":7.4,"publicationDate":"2025-02-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143921287","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}
ACS ES&T engineeringPub Date : 2025-02-07DOI: 10.1021/acsestengg.4c0066610.1021/acsestengg.4c00666
Jaemin Choi, Dahye Min, Kali Rigby, Eun-Tae Yun, Jaesung Kim, Yae-Eun Kim, Yong-Yoon Ahn, Yunho Lee, Changha Lee, Eun-Ju Kim, Pedro J. J. Alvarez, Jae-Hong Kim and Jaesang Lee*,
{"title":"Encapsulating Co and Pd Nanoparticles as Spatially Separated Dual Active Sites for Heterogeneous Persulfate Activation: Synergistic Catalysis and Switching of the Primary Reaction Pathway","authors":"Jaemin Choi, Dahye Min, Kali Rigby, Eun-Tae Yun, Jaesung Kim, Yae-Eun Kim, Yong-Yoon Ahn, Yunho Lee, Changha Lee, Eun-Ju Kim, Pedro J. J. Alvarez, Jae-Hong Kim and Jaesang Lee*, ","doi":"10.1021/acsestengg.4c0066610.1021/acsestengg.4c00666","DOIUrl":"https://doi.org/10.1021/acsestengg.4c00666https://doi.org/10.1021/acsestengg.4c00666","url":null,"abstract":"<p >This study demonstrates that the carbon encapsulation of Pd and Co as spatially isolated redox-active sites can synergistically enhance the activation of peroxymonosulfate (PMS) and peroxydisulfate (PDS) and enable persulfate precursor-sensitive degradation routes. The superiority of bimetal–carbon composites (i.e., Pd/Co@NC) was confirmed based on a higher efficiency of Pd/Co@NC with varying Pd/Co ratios for persulfate activation than the sum of efficiencies of single metal-component catalysts applied at corresponding dosages. Treatment performances of Pd/Co@NC with different metal compositions aligned with the dependence of electrical conductivity and binding affinity of Pd/Co@NC on the relative metal content. Reflecting differential reactivity of monometallic components toward persulfate, the primary degradation pathway was switched, depending on the persulfate type. Pd/Co@NC caused radical-induced oxidation upon PMS addition while initiating nonradical PDS activation through electron-transfer mediation, based on retarding effects of radical scavengers, reactivity toward multiple organics, Koutecký–Levich plots, electron paramagnetic spectral features, and product distribution. The fabrication strategy to enable the separate carbon encapsulation of two metallic sites with different catalytic reactivity created metal–carbon composites that retained the advantages of radical and nonradical persulfate activation under realistic treatment conditions; i.e., treatability of a wide spectrum of organics and minimal interference of background compounds in complex water matrices.</p>","PeriodicalId":7008,"journal":{"name":"ACS ES&T engineering","volume":"5 3","pages":"756–771 756–771"},"PeriodicalIF":7.4,"publicationDate":"2025-02-07","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143608942","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}
ACS ES&T engineeringPub Date : 2025-02-05DOI: 10.1021/acsestengg.4c0078210.1021/acsestengg.4c00782
Jian Lu, Huan He, Tianyang Zhang, Qi Fu, Renjie Pan, Chao Zeng*, Yanbo Zhou and Bin Xu*,
{"title":"Fe(II)/Sulfite Process with Rapid Fe(II) Oxidation Enhances p-Arsanilic Acid Oxidation and Simultaneous Arsenic Adsorption","authors":"Jian Lu, Huan He, Tianyang Zhang, Qi Fu, Renjie Pan, Chao Zeng*, Yanbo Zhou and Bin Xu*, ","doi":"10.1021/acsestengg.4c0078210.1021/acsestengg.4c00782","DOIUrl":"https://doi.org/10.1021/acsestengg.4c00782https://doi.org/10.1021/acsestengg.4c00782","url":null,"abstract":"<p >Most studies focus on the oxidation capability of the Fe(II)/sulfite (Fe(II)/S(IV)) process for organic pollutants but overlook the phenomenon of rapid iron particle formation. The coupling of oxidation and <i>in situ</i> adsorption by iron particulates holds great potential for the deep removal of organometallic compounds. Herein, the removal of an organoarsenic compound of <i>p</i>-arsanilic acid (<i>p</i>-ASA) by Fe(II)/S(IV) was investigated. This process demonstrated efficient and rapid <i>p</i>-ASA degradation, achieving 95% <i>p</i>-ASA removal (10 μM) within 3 min, which is comparable to those of the Fe(II)/PDS and Fe(II)/PMS processes. Various evidence indicated that SO<sub>5</sub><sup>•–</sup> was the primary radical driving <i>p</i>-ASA degradation, selectively attacking the amino group with As(V) as the ultimate byproduct. Ultrafast Fe(II) oxidation and iron particle formation were observed, with over 90% of Fe(II) ions converted into insoluble iron particles within 30 s. However, the Fe(II)/PDS and Fe(II)/PMS processes generated very few iron particles. It was found that S(IV)’s proton-taking feature increased the pH, significantly promoting Fe(II) oxidation, hydrolysis, and precipitation. The formed iron particles were amorphous ferric(oxyhydr)oxides, and showed great efficiency for As(V) adsorption during their formation. As a result, the Fe(II)/S(IV) process showed superior efficiency for total arsenic removal. In addition, the process remained effective under real water matrices. Overall, this study offers theoretical and data-driven guidance for applying this promising one-step procedure for effectively treating organic arsenic in water.</p>","PeriodicalId":7008,"journal":{"name":"ACS ES&T engineering","volume":"5 4","pages":"1011–1022 1011–1022"},"PeriodicalIF":7.4,"publicationDate":"2025-02-05","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143814440","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}