ACS ES&T engineering最新文献

{"title":"Surface Complexation and Packed Bed Mass Transport Models Enable Adsorbent Design for Arsenate and Vanadate Removal","authors":"Emily Briese, Ken Niimi, Annika Hjelmstad, Paul Westerhoff","doi":"10.1021/acsestengg.4c00315","DOIUrl":"https://doi.org/10.1021/acsestengg.4c00315","url":null,"abstract":"Co-occurrence of metal oxo-anions (e.g., arsenate) in drinking water poses human health risks. To understand and predict competition and breakthrough for individual or mixtures of oxo-anions in continuous-flow packed bed adsorption systems, we linked equilibrium surface complexation models (SCMs) with a pore surface diffusion model (PSDM). After parametrization, using data for two commercial adsorbents, the SCM and PSDM predicted well the adsorption isotherm data and column breakthrough curves, respectively, for single-solute (arsenate) and bisolute water chemistries (arsenate, vanadate) as well as chromatographic displacement of previously adsorbed arsenate by vanadate. Surface and pore diffusivities for both commercial adsorbents were 3.0 to 3.5 x10^–12 cm²/s and 1.1 to 0.8 x10^–6 cm²/s, respectively. After validation, SCM + PSDM was used in silico to evaluate adsorbent media characteristics, variable water chemistries, and reactor configurations. When contrasting hypothetical crystalline versus amorphous metal (hydr)oxide adsorbents, increasing surface site density resulted in higher Freundlich isotherm capacity (<i>K</i>_F) but did not impact 1/<i>n</i>. Increasing surface binding affinities beneficially impacted both the <i>K</i>_F and 1/<i>n</i> isotherms and would improve the performance of point-of-use (POU) adsorbent system applications. In silico simulation results suggest prioritizing enhancing adsorbent capacity (<i>q</i>) through improved surface reactivity in the design of new POU adsorbent materials rather than focusing on reducing mass transport limitations through intraparticle pore design. For municipal-scale adsorption systems, the PSDM simulation of the mass transfer zone shape was evaluated for hypothetical adsorbent pore designs (i.e., intraparticle porosity (ε_p) and tortuosity) and demonstrated that ε_p control was a key strategy to improve performance.","PeriodicalId":7008,"journal":{"name":"ACS ES&T engineering","volume":null,"pages":null},"PeriodicalIF":7.1,"publicationDate":"2024-08-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142204240","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}

{"title":"Surface Complexation and Packed Bed Mass Transport Models Enable Adsorbent Design for Arsenate and Vanadate Removal","authors":"Emily Briese,&nbsp;Ken Niimi,&nbsp;Annika Hjelmstad and Paul Westerhoff*,&nbsp;","doi":"10.1021/acsestengg.4c0031510.1021/acsestengg.4c00315","DOIUrl":"https://doi.org/10.1021/acsestengg.4c00315https://doi.org/10.1021/acsestengg.4c00315","url":null,"abstract":"<p >Co-occurrence of metal oxo-anions (e.g., arsenate) in drinking water poses human health risks. To understand and predict competition and breakthrough for individual or mixtures of oxo-anions in continuous-flow packed bed adsorption systems, we linked equilibrium surface complexation models (SCMs) with a pore surface diffusion model (PSDM). After parametrization, using data for two commercial adsorbents, the SCM and PSDM predicted well the adsorption isotherm data and column breakthrough curves, respectively, for single-solute (arsenate) and bisolute water chemistries (arsenate, vanadate) as well as chromatographic displacement of previously adsorbed arsenate by vanadate. Surface and pore diffusivities for both commercial adsorbents were 3.0 to 3.5 x10^–12 cm²/s and 1.1 to 0.8 x10^–6 cm²/s, respectively. After validation, SCM + PSDM was used in silico to evaluate adsorbent media characteristics, variable water chemistries, and reactor configurations. When contrasting hypothetical crystalline versus amorphous metal (hydr)oxide adsorbents, increasing surface site density resulted in higher Freundlich isotherm capacity (<i>K</i>_F) but did not impact 1/<i>n</i>. Increasing surface binding affinities beneficially impacted both the <i>K</i>_F and 1/<i>n</i> isotherms and would improve the performance of point-of-use (POU) adsorbent system applications. In silico simulation results suggest prioritizing enhancing adsorbent capacity (<i>q</i>) through improved surface reactivity in the design of new POU adsorbent materials rather than focusing on reducing mass transport limitations through intraparticle pore design. For municipal-scale adsorption systems, the PSDM simulation of the mass transfer zone shape was evaluated for hypothetical adsorbent pore designs (i.e., intraparticle porosity (ε_p) and tortuosity) and demonstrated that ε_p control was a key strategy to improve performance.</p>","PeriodicalId":7008,"journal":{"name":"ACS ES&T engineering","volume":null,"pages":null},"PeriodicalIF":7.4,"publicationDate":"2024-08-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142407707","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}

{"title":"Biological Waste-Derived Dual-Site Catalyst Empowers Electro-Fenton Systems to Sustainably Decontaminate Livestock Wastewater","authors":"Ke-Yu Chen, Yun-Xin Huang, Qian Zhang, Shou-Yan Zhao, Wen-Ting Liu, Qi Wang, Bao-Cheng Huang, Ren-Cun Jin","doi":"10.1021/acsestengg.4c00413","DOIUrl":"https://doi.org/10.1021/acsestengg.4c00413","url":null,"abstract":"Livestock and poultry industries are pivotal for meat production, but produced wastewater with heavy pollution challenges environmental sustainability and public health. The electro-Fenton (EF) process, capable of in situ production and activation of hydrogen peroxide, is promising for decontaminating recalcitrant pollutants, yet fabricating a highly active bifunctional cathode catalyst across a broad pH range remains a bottleneck. Guided by green chemistry principles, we synthesized a dual-site catalyst from biological waste to facilitate hydroxyl radical production. Combined experimental and theoretical investigations unveiled that the Fe₂O₃ sites facilitated H₂O₂ generation via catalyzing the oxygen reduction reaction, whereas Fe₃N sites promoted in situ H₂O₂ activation into hydroxyl radicals. This electrocatalyst, integrated into a gas diffusion electrode, achieved stable, aeration-free mineralization of antibiotic contaminants at neutral pH with a low energy consumption of just 0.94 kWh/g of removed total organic carbon. The further development of a tandem system that coupled the anammox bioprocess with the EF process exhibited exceptional efficiency in both nitrogen removal and tertiary purification of actual livestock wastewater, obviating the need for pH adjustments or Fenton reagent additives. These findings underscore the potential scalability and application of our proposed approach in promoting sustainable wastewater management practices.","PeriodicalId":7008,"journal":{"name":"ACS ES&T engineering","volume":null,"pages":null},"PeriodicalIF":7.1,"publicationDate":"2024-08-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142226152","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}

{"title":"Enhancing Anaerobic Digestion of Food Waste by Combining Carriers and Microaeration: Performance and Potential Mechanisms","authors":"Baocun Wu, Yi Wang, Linyan He, Miao Liu, Jinjing Xiang, Yongdong Chen, Li Gu, Jinze Li, Lin Li, Weiliang Pan, Qiang He","doi":"10.1021/acsestengg.4c00298","DOIUrl":"https://doi.org/10.1021/acsestengg.4c00298","url":null,"abstract":"Enhancing the anaerobic digestion (AD) of organic wastes has been a widely discussed topic. This study aims to enhance AD performance by combining microaeration with conductive or nonconductive carriers, using food waste as the substrate. The use of carriers alone enhanced methane production, and microaeration further improved performance. The conductive carrier showed significant enhancement with microaeration, achieving a daily methane yield of 478 ± 11.3 mL CH₄/g VS, which was 1.1 and 1.3 times higher than that of the nonconductive carrier and the control digester, respectively. Furthermore, the study explored various aspects, including oxidative stress, antioxidant capacity, and microbial community structure during digestion. The results demonstrated that combining microaeration with a conductive carrier improved hydrolytic-acidification efficiency and promoted direct interspecies electron transfer among syntrophic microorganisms. Methanogenic archaea aggregated on the carrier surface and formed consortia with facultative anaerobes, thereby mitigating oxidative stress effects on cells and enhancing total methane production. Moreover, metabolomics analysis showed that combining conductive carriers with microaeration enhanced ATP transport across the bacterial membrane, accelerated nutrient conversion, and caused significant changes in metabolites and intermediates related to glycerophospholipids, amino acids, and signal transduction pathways.","PeriodicalId":7008,"journal":{"name":"ACS ES&T engineering","volume":null,"pages":null},"PeriodicalIF":7.1,"publicationDate":"2024-08-13","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142204242","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}

{"title":"Enhancing Anaerobic Digestion of Food Waste by Combining Carriers and Microaeration: Performance and Potential Mechanisms","authors":"Baocun Wu,&nbsp;Yi Wang,&nbsp;Linyan He,&nbsp;Miao Liu,&nbsp;Jinjing Xiang,&nbsp;Yongdong Chen,&nbsp;Li Gu*,&nbsp;Jinze Li*,&nbsp;Lin Li,&nbsp;Weiliang Pan and Qiang He,&nbsp;","doi":"10.1021/acsestengg.4c0029810.1021/acsestengg.4c00298","DOIUrl":"https://doi.org/10.1021/acsestengg.4c00298https://doi.org/10.1021/acsestengg.4c00298","url":null,"abstract":"<p >Enhancing the anaerobic digestion (AD) of organic wastes has been a widely discussed topic. This study aims to enhance AD performance by combining microaeration with conductive or nonconductive carriers, using food waste as the substrate. The use of carriers alone enhanced methane production, and microaeration further improved performance. The conductive carrier showed significant enhancement with microaeration, achieving a daily methane yield of 478 ± 11.3 mL CH₄/g VS, which was 1.1 and 1.3 times higher than that of the nonconductive carrier and the control digester, respectively. Furthermore, the study explored various aspects, including oxidative stress, antioxidant capacity, and microbial community structure during digestion. The results demonstrated that combining microaeration with a conductive carrier improved hydrolytic-acidification efficiency and promoted direct interspecies electron transfer among syntrophic microorganisms. Methanogenic archaea aggregated on the carrier surface and formed consortia with facultative anaerobes, thereby mitigating oxidative stress effects on cells and enhancing total methane production. Moreover, metabolomics analysis showed that combining conductive carriers with microaeration enhanced ATP transport across the bacterial membrane, accelerated nutrient conversion, and caused significant changes in metabolites and intermediates related to glycerophospholipids, amino acids, and signal transduction pathways.</p>","PeriodicalId":7008,"journal":{"name":"ACS ES&T engineering","volume":null,"pages":null},"PeriodicalIF":7.4,"publicationDate":"2024-08-13","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142436870","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}

{"title":"Nanoconfined Cobalt Ferrite Composite Carbon Nanotube Membrane Oxidation-Filtration System for Water Decontamination","authors":"Huanran Ma,&nbsp;Lijun Zhang,&nbsp;Xiao Zhang,&nbsp;Zonglin Pan*,&nbsp;Ruisong Xu,&nbsp;Guanlong Wang*,&nbsp;Xinfei Fan,&nbsp;Huixia Lu*,&nbsp;Shuaifei Zhao and Chengwen Song,&nbsp;","doi":"10.1021/acsestengg.4c0028210.1021/acsestengg.4c00282","DOIUrl":"https://doi.org/10.1021/acsestengg.4c00282https://doi.org/10.1021/acsestengg.4c00282","url":null,"abstract":"<p >Constructing a membrane-confined peroxymonosulfate (PMS) activation system has emerged as a promising strategy for efficient water decontamination. Herein, a novel cobalt ferrite (CoFe₂O₄)-filled open-end carbon nanotube (OCNT) membrane filtration system was proposed, aiming to integrate dual metal centers and nanoconfinement for enhancing PMS activation (MFPA) toward water decontamination. The optimal CoFe₂O₄@OCNT MFPA process displayed 100% phenol removal within a residence time of 5.7 s, whose <i>k</i> (1.17 s^–1) was 3.0, 5.6, and 3.9 times higher than that of CoO@OCNT, FeO@OCNT, and CoFe₂O₄/CCNT (surface-loaded closed end cap CNT), respectively. Experimental results and theoretical calculations jointly unravel the nonradical-dominated (¹O₂ and electron transfer) oxidation mechanism, leading to the wide-pH adaptation and superior stability in the complex water matrix. Mechanism analysis showed that fast cycling of Co²⁺/Co³⁺ was achieved via synergistic promotion between dual metal centers and the nanoconfinement effect, which coboosted the PMS consumption as well as reactive oxygen species generation (especially ¹O₂). Compared with the single metal center, the dual metal centers of internal CoFe₂O₄ exhibited coenhanced electron cloud density (amount of charge transfer) and adsorption energy for PMS, resulting in O–O cleavage and elongated O–H. Meanwhile, the oxygen vacancy defect (O_def) on CoFe₂O₄ also contributed to the nonradical process, which not only served as the precursor of ¹O₂ generation but also acted as a transfer station for electrons.</p>","PeriodicalId":7008,"journal":{"name":"ACS ES&T engineering","volume":null,"pages":null},"PeriodicalIF":7.4,"publicationDate":"2024-08-12","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142407781","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}

{"title":"Nanoconfined Cobalt Ferrite Composite Carbon Nanotube Membrane Oxidation-Filtration System for Water Decontamination","authors":"Huanran Ma, Lijun Zhang, Xiao Zhang, Zonglin Pan, Ruisong Xu, Guanlong Wang, Xinfei Fan, Huixia Lu, Shuaifei Zhao, Chengwen Song","doi":"10.1021/acsestengg.4c00282","DOIUrl":"https://doi.org/10.1021/acsestengg.4c00282","url":null,"abstract":"Constructing a membrane-confined peroxymonosulfate (PMS) activation system has emerged as a promising strategy for efficient water decontamination. Herein, a novel cobalt ferrite (CoFe₂O₄)-filled open-end carbon nanotube (OCNT) membrane filtration system was proposed, aiming to integrate dual metal centers and nanoconfinement for enhancing PMS activation (MFPA) toward water decontamination. The optimal CoFe₂O₄@OCNT MFPA process displayed 100% phenol removal within a residence time of 5.7 s, whose <i>k</i> (1.17 s^–1) was 3.0, 5.6, and 3.9 times higher than that of CoO@OCNT, FeO@OCNT, and CoFe₂O₄/CCNT (surface-loaded closed end cap CNT), respectively. Experimental results and theoretical calculations jointly unravel the nonradical-dominated (¹O₂ and electron transfer) oxidation mechanism, leading to the wide-pH adaptation and superior stability in the complex water matrix. Mechanism analysis showed that fast cycling of Co²⁺/Co³⁺ was achieved via synergistic promotion between dual metal centers and the nanoconfinement effect, which coboosted the PMS consumption as well as reactive oxygen species generation (especially ¹O₂). Compared with the single metal center, the dual metal centers of internal CoFe₂O₄ exhibited coenhanced electron cloud density (amount of charge transfer) and adsorption energy for PMS, resulting in O–O cleavage and elongated O–H. Meanwhile, the oxygen vacancy defect (O_def) on CoFe₂O₄ also contributed to the nonradical process, which not only served as the precursor of ¹O₂ generation but also acted as a transfer station for electrons.","PeriodicalId":7008,"journal":{"name":"ACS ES&T engineering","volume":null,"pages":null},"PeriodicalIF":7.1,"publicationDate":"2024-08-12","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142204241","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}

{"title":"Vital Threshold and Underlying Mechanism for the Complete Remediation of Oil and Microplastic Co-Contaminated Soil by Fast Pyrolysis","authors":"Zi-Ying Hu,&nbsp; and ,&nbsp;Hong Jiang*,&nbsp;","doi":"10.1021/acsestengg.4c0020410.1021/acsestengg.4c00204","DOIUrl":"https://doi.org/10.1021/acsestengg.4c00204https://doi.org/10.1021/acsestengg.4c00204","url":null,"abstract":"<p >The coexistence of microplastics (MPs) and oil contaminants in soil has led to a new pollution scenario around the oil-production region, yet how to cost-effectively remediate soil with combined pollutants has rarely been explored. Herein, we propose a fast pyrolysis technique to perfectly remediate MP_S-oil copresence soil (MPs-oil-soil). The experimental data showed that pyrolysis at 500 °C for 15 min is a key threshold for the complete removal of MPs and petroleum contaminants from soil. Above this threshold, seed germination and the growth of wheat in the soil increased, and the rhizosphere microbial population decreased with increasing abundance of beneficial microbial flora, such as <i>Proteobacteria, Actinobacteria and</i> Bacteroidetes (which promote the circulation of nutrients and help to strengthen plant resistance). Structural equation modeling revealed that temperature had a more significant positive effect on the remediation effect than did time. Two-dimensional correlation spectroscopy combined with synchronous fluorescence spectroscopy showed that the presence of MPs was the main factor affecting the pyrolysis threshold. Three-dimensional excitation–emission matrix and UV–visible absorption spectroscopy revealed large differences in the aromaticity and relative molecular weight of dissolved organic matter before and after the pyrolysis threshold. These findings shed light on the mechanistic understanding of the pyrolytic remediation of microplastics and oil-contaminated soils.</p>","PeriodicalId":7008,"journal":{"name":"ACS ES&T engineering","volume":null,"pages":null},"PeriodicalIF":7.4,"publicationDate":"2024-08-11","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142228031","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}

{"title":"Vital Threshold and Underlying Mechanism for the Complete Remediation of Oil and Microplastic Co-Contaminated Soil by Fast Pyrolysis","authors":"Zi-Ying Hu, Hong Jiang","doi":"10.1021/acsestengg.4c00204","DOIUrl":"https://doi.org/10.1021/acsestengg.4c00204","url":null,"abstract":"The coexistence of microplastics (MPs) and oil contaminants in soil has led to a new pollution scenario around the oil-production region, yet how to cost-effectively remediate soil with combined pollutants has rarely been explored. Herein, we propose a fast pyrolysis technique to perfectly remediate MP_S-oil copresence soil (MPs-oil-soil). The experimental data showed that pyrolysis at 500 °C for 15 min is a key threshold for the complete removal of MPs and petroleum contaminants from soil. Above this threshold, seed germination and the growth of wheat in the soil increased, and the rhizosphere microbial population decreased with increasing abundance of beneficial microbial flora, such as <i>Proteobacteria, Actinobacteria and</i> Bacteroidetes (which promote the circulation of nutrients and help to strengthen plant resistance). Structural equation modeling revealed that temperature had a more significant positive effect on the remediation effect than did time. Two-dimensional correlation spectroscopy combined with synchronous fluorescence spectroscopy showed that the presence of MPs was the main factor affecting the pyrolysis threshold. Three-dimensional excitation–emission matrix and UV–visible absorption spectroscopy revealed large differences in the aromaticity and relative molecular weight of dissolved organic matter before and after the pyrolysis threshold. These findings shed light on the mechanistic understanding of the pyrolytic remediation of microplastics and oil-contaminated soils.","PeriodicalId":7008,"journal":{"name":"ACS ES&T engineering","volume":null,"pages":null},"PeriodicalIF":7.1,"publicationDate":"2024-08-11","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141948973","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}

{"title":"Dispersed Pr on Nickel Oxide for Efficient Nitrous Oxide Direct Decomposition in Simulated Nitric Acid Exhaust","authors":"Zhuoyi Zhang,&nbsp;Yunshuo Wu,&nbsp;Yuxin Sun,&nbsp;Haiqiang Wang,&nbsp;Zhongbiao Wu and Xuanhao Wu*,&nbsp;","doi":"10.1021/acsestengg.4c0031410.1021/acsestengg.4c00314","DOIUrl":"https://doi.org/10.1021/acsestengg.4c00314https://doi.org/10.1021/acsestengg.4c00314","url":null,"abstract":"<p >Nitrous oxide (N₂O) is a potent greenhouse gas with a high global warming potential. The N₂O direct decomposition (deN₂O) is currently the most widely used technique due to its operational simplicity and lack of secondary pollution. The presence of impurity gases in industrial exhaust increases the challenge of eliminating N₂O, urging the development of highly active and stable catalysts for its degradation. In this study, a series of praseodymium (Pr)-doped nickel oxide (NiO) catalysts were synthesized for N₂O degradation. These catalysts showed higher N₂O decomposition activity (<i>T</i>₁₀₀ = 400–440 °C) than pure NiO (<i>T</i>₁₀₀ = 480 °C) and also demonstrated high resistance to impurity gases in simulated industrial nitric acid tail gas. In the catalyst with a Pr to Ni ratio of 0.002, the highly dispersed Pr on the NiO surface regulated its particle size and increased specific surface area and pore volume. DFT calculations revealed that Pr significantly enhanced the electron-donating ability of Ni²⁺, facilitating the dissociative adsorption of N₂O on the catalyst surface, where O existed in the form of Ni³⁺-O*. Additionally, Pr reduced the desorption energy of O₂, the rate-determining step. During the reaction, Pr³⁺ transferred electrons to Ni³⁺ via f-d electron hopping, stabilizing the active Ni²⁺ sites and enabling an efficient catalytic reaction. These findings demonstrate the practical potential of this catalyst and provide new insights into the degradation of N₂O in industrial exhaust gases, offering a promising avenue for application.</p>","PeriodicalId":7008,"journal":{"name":"ACS ES&T engineering","volume":null,"pages":null},"PeriodicalIF":7.4,"publicationDate":"2024-08-08","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142430597","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}