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Support work-function dependent Fenton-like catalytic activity of Co single atoms for selective cobalt(IV)=O generation

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Science Bulletin 2024年第24期69卷 3867-3875页

作者： Xue Li Xiangcheng Zhang junyu Lang Baoxue Zhou pedro j.j.alvarez Lizhi Zhang Mingce Long School of Environmental Science and Engineering Shanghai Jiao Tong UniversityShanghai 200240China School of Physical Science and Technology ShanghaiTech UniversityShanghai 201210China Department of Civil and Environmental Engineering Rice UniversityHoustonTX 77005USA

In Fenton-like reactions,high-valent cobalt-oxo(Co^(IV)=O)has attracted increasing interests due to high redox potential,long lifetime,and anti-interference properties,but its generation is hindered by the electron repulsion between the electron rich oxo-and cobalt ***,we demonstrate Co^(IV)=O generation from peroxymonosulfate(PMS)activation over cobalt single-atom catalysts(Co-SACs)using in-situ Co K-edge X-ray absorption spectra,and discern that Co^(IV)=O generation is dependent on the support work-function(WF)due to the strong electronic metal-support interaction(EMSI).Supports with a high WF value like anatase-TiO_(2)facilitate the binding of PMS-terminal oxo-ligand to Co sites by extracting Cod electrons,thus decreasing the generation barrier for the critical intermediate(Co-OOSO_(3)^(2-)).The Co atoms anchored on anatase-TiO_(2)(Co-TiO_(2))exhibited enhanced Co^(IV)=O generation and superior activity for sulfamethoxazole(SMX)degradation during PMS *** normalized steady-state concentration of Co^(IV)=O in Co-TiO_(2)/PMS system was three orders of magnitude higher than that of free radicals,and 1.3-to 11-fold higher than that generated in other Co-SACs/PMS ***-TiO_(2)/PMS sustained efficient removal of SMX with minimal Co^(2+)leaching under continuous flow operation,suggesting its attractive water purification ***,these results underscore the significance of support selection for enhanced generation of high-valent metal-oxo species and efficient PMS activation in supported metal SACs.

关键词： Peroxymonosulfate activation Electronic metal-support interaction Single-atom catalysts High-valent cobalt-oxo Work-function

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Molecular signature of soil organic matter under different land uses in the Lake Chaohu Basin

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Eco-Environment & Health 2022年第4期1卷 212-218页

作者： Han Gao Huixin Li Chen Lin pedro j.j.alvarez Caroline A.Masiello Dongqiang Zhu Ao Kong Xiaolei Qu State Key Laboratory of Pollution Control and Resource Reuse School of the EnvironmentNanjing UniversityNanjing 210023China School of Finance Nanjing University of Finance and EconomicsNanjing 210023China Key Laboratory of Watershed Geographic Sciences Institute of Geography and LimnologyChinese Academy of SciencesNanjing 210008China State Environmental Protection Key Laboratory of Soil Environmental Management and Pollution Control Nanjing Institute of Environmental SciencesMinistry of Ecology and Environment of ChinaNanjing 210042China Department of Civil and Environmental Engineering Rice UniversityHouston TX 77005USA Department of Earth Environmental and Planetary SciencesRice UniversityHouston TX 77005USA School of Urban and Environmental Sciences Peking UniversityBeijing 100871China

The concentration and molecular composition of soil organic matter(SOM)are important factors in mitigation against climate change as well as providing other ecosystem *** quantitative understanding of how land use influences SOM molecular composition and associated turnover dynamics is limited,which underscores the need for high-throughput analytical approaches and molecular marker signatures to clarify this *** a high-throughput untargeted mass spectrometry screening and molecular markers,we show that forest,farmland and urban land uses result in distinct molecular signatures of SOM in the Lake Chaohu *** markers indicate that forest SOM has abundant carbon contents from vegetation and condensed organic carbon,leading to high soil organic carbon(SOC)*** SOM has moderate carbon contents from vegetation,and limited content of condensed organic carbon,with SOC significantly lower than that of forest *** SOM has high abundance of condensed organic carbon markers due to anthropogenic activities but relatively low in markers from ***,urban soils have the highest black carbon/SOC ratio among these land ***,our results suggested that the molecular signature of SOM varies significantly with land use in the Lake Chaohu Basin,influencing carbon *** strategy of molecular fingerprinting and marker discovery is expected to enlighten further research on SOM molecular signatures and cycling dynamics.

关键词： High-throughput untargeted mass spectrometry screening Mass spectrum processing algorithm Soil organic matter Molecular signature Land use

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Unintended Consequences of Silver Nanoparticle Releases: Mechanistic Insights from Microbiology

Unintended Consequences of Silver Nanoparticle Releases: Mec...

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全国环境纳米技术及生物效应学术研讨会

作者： pedro j.j.alvarez Dept.of Civil ＆ Environmental Engineering Rice University

As a broad-spectrum antimicrobial agent, silver nanoparticles（AgNPs） are by far the most widely commercialized nanomaterial;about one-quarter of about 1500 nanotechnology-enhanced commercial products contain AgNPs. Thus, it is important to consider the unintended consequences of accidental and incidental releases of AgNPs to the environment and to sewage treatment plants. This presentation will address how AgNPs may affect ecosystem productivity and critical microbial ecosystem services, including biological treatment processes. We will also discern whether AgNPs exert direct "particle-specific" effects beyond the known antimicrobial activity of released silver ions（Ag+）, which is critical to understand how water chemistry affects nanoparticle bioavailability, reactivity and toxicity. Differential effects of AgNPs on bacterial gene expression and activities associated with the nitrogen cycle will also be discussed in the context of water quality. Counterintuitive effects of sub-lethal exposure to AgNPs on microbial viability and biofilm formation will also be presented. Finally, the results will be integrated to infer on how to steward safer and eco-responsible nanotechnology.

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Co单原子类芬顿催化中CoIV=O生成选择性与载体功函相关（英文）

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Science Bulletin 2024年第24期 3867-3875页

作者：李雪张向成郎峻宇周保学 pedro j.j.alvarez 张礼知龙明策 School of Environmental Science and Engineering Shanghai Jiao Tong University School of Physical Science and Technology ShanghaiTech University Department of Civil and Environmental Engineering Rice University

In Fenton-like reactions,high-valent cobalt-oxo (CoIV=O) has attracted increasing interests due to high redox potential,long lifetime,and anti-interference properties,but its generation is hindered by the electron repulsion between the electron rich oxo-and cobalt ***,we demonstrate CoIV=O generation from peroxymonosulfate （PMS） activation over cobalt single-atom catalysts （Co-SACs） using in-situ Co K-edge X-ray absorption spectra,and discern that CoIV=O generation is dependent on the support work-function （WF） due to the strong electronic metal-support interaction （EMSI）.Supports with a high WFvalue like anatase-TiO2facilitate the binding of PMS-terminal oxo-ligand to Co sites by extracting Cod electrons,thus decreasing the generation barrier for the critical intermediate (Co-OOSO32-).The Co atoms anchored on anatase-TiO2（Co-TiO2） exhibited enhanced CoIV=O generation and superior activity for sulfamethoxazole （SMX） degradation during PMS *** normalized steady-state concentration of CoIV=O in Co-TiO2/PMS system was three orders of magnitude higher than that of free radicals,and 1.3- to 11-fold higher than that generated in other Co-SACs/PMS ***-TiO2/PMS sustained efficient removal of SMX with minimal Co2+leaching under continuous flow operation,suggesting its attractive water purification ***,these results underscore the significance of support selection for enhanced generation of high-valent metal-oxo species and efficient PMS activation in supported metal SACs.

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Touristic urbanization and greening of coastal dune fields:A long-term assessment of a temperate sandy barrier of Argentina

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journal of Geographical Sciences 2025年第1期35卷 206-230页

作者： GARZO pedro Andrés DADON joséRoberto ISLA Federico Ignacio Instituto de Investigaciones Marinas y Costeras(IIMyC-CONICET/UNMDP) Av.Juan B.Justo 2550Mar del Plata7600Buenos AiresArgentina Instituto de Geología de Costas y del Cuaternario Dr.Enrique j.Schnack(IGCC-CIC/UNMDP) Funes 3350Mar del Plata7600Buenos AiresArgentina Facultad de Arquitectura Diseño y UrbanismoCentro de Investigaciones Gestión de Espacios Costeros(GEC-FADU/UBA)Universidad de Buenos AiresIntendente Güiraldes 2160Pabellón ⅢPiso 4Ciudad Autónoma de Buenos Aires1428Argentina Consejo Nacional de Investigaciones Científicas y Técnicas(CONICET) Buenos AiresArgentina

Dune barrier systems represent highly sought-after coastal landscapes for tourism and urban development around the ***,a century ago,they were considered hazardous environments due to their great dynamic *** a result,stabilization practices were considered *** systematic introduction of fast-growing exotic trees helped stabilize the sand,making it easier for tourism urbanization to take place,but also leading to erosion *** paper aims to assess long-term changes in vegetation cover over a large temperate barrier in *** complex region includes urban resorts,afforestation zones,and protected areas.A GIS-based geospatial analysis was conducted using a large satellite database(>350 images),and the future evolution of the vegetation was *** results revealed two primary spatiotemporal patterns associated with a gradual expansion of vegetation cover,accompanied by a concurrent reduction in sandy *** 1986,the dune area comprised 75%more surface than vegetation,whereas in 2021,it represented 60%less than ***,the 2050 scenario suggests a potential 40%reduction of dunes in certain *** is necessary to enhance management actions aimed at maintaining dune mobility and ensuring local and regional sediment ***-term management strategies must focus on restoring native plant communities and controlling invasive species,and avoiding new dune fixation initiatives based on the introduction of exotic species.

关键词： nature reserves afforestation sediment balance dune management NDVI

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Kinetics of the reaction of OH radical with ethylfluoroacetate,ethyl 4,4,4-trifluorobutyrate,and butylfluoroacetate

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journal of Environmental Sciences 2025年第5期151卷 273-283页

作者： pedro L.Lugo Vianni Straccia Mariano A.Teruel María B.Blanco Laboratorio Universitario de Química y Contaminación del Aire(L.U.Q.C.A) Institute for Research in Physical Chemistry of Córdoba(I.N.F.I.Q.C.)Department of Physical ChemistryFaculty of Chemical SciencesNational University of CórdobaUniversity CityCórdoba 5000Argentina Institute for Atmospheric and Environmental Research University of WuppertalWuppertal DE-42097Germany

Kinetics of the gas-phase reactions of•OH radicals with a series of fluoroesters were studied for the first time at 298±3 K and atmospheric *** rate coefficients were determined by in situ FTIR spectroscopy in nitrogen and GC-FID in air to monitor the decay of reactants and *** following coefficient values(in 10^(−12)cm^(3)/(molecule•sec))were obtained for ethyl fluoroacetate(EFA),ethyl 4,4,4-trifluorobutyrate(ETB),and butyl fluoroacetate(BFA),respectively:k_(1)(EFA+OH)=1.15±0.25 by FTIR and 1.34±0.23 by GC-FID;k_(2)(ETB+OH)=1.61±0.36 by FTIR and 2.02±0.30 by GC-FID;k_(3)(BFA+OH)=2.24±0.37 by *** trends were developed and correlated with the number of CH_(3)and F substituents in the fluoroester,and structure-activity relationships(SARs)calculations were *** addition,the tropospheric lifetimes of EFA,ETB,and BFA upon degradation by OH radicals were calculated to be 9,6,and 5 days,respectively,indicating that these fluorinated compounds could have a possible regional effect from the emission *** small photochemical ozone creation potentials of 9,7,and 19 were estimated for EFA,ETB,and BFA,*** GlobalWarming Potentials(GWPs)for EFA,ETB,and BFA were calculated for different time *** a 20-year time horizon,the GWPs were 1.393,0.063,and 0.062,*** the case of a 100-year time horizon,the GWPs were 0.379,0.017,and 0.017,and for a 500-year time horizon,the GWPs were 0.108,0.005,and 0.005 for EFA,ETB,and BFA.

关键词： CFC replacements sinks in situ FTIR SAR Acidification potentials Greenhouse gases

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Atmospheric chemistry of trifluorodicarbonyls initiated by Cl atoms:Reactivity trends,mechanism,and acid formation yields

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journal of Environmental Sciences 2025年第5期151卷 12-25页

作者： pedro L.Lugo Vianni G.Straccia Cynthia B.Rivela Mariano A.Teruel María B.Blanco Laboratorio Universitario de Química y Contaminación del Aire(L.U.Q.C.A) Instituto de Investigaciones en Fisicoquímica de Córdoba(I.N.F.I.Q.C.)Dpto.de Fisicoquímica.Facultad de Ciencias QuímicasUniversidad Nacional de Córdoba.Ciudad Universitaria5000 CórdobaArgentina Institute for Atmospheric and Environmental Research University of WuppertalDE-42097 WuppertalGermany

Rate coefficients of the gas-phase reactions of Cl atoms with a series of fluorinated diketones(FDKs):CF_(3)C(O)CH_(2)C(O)CH_(3)(TFP),CF_(3)C(O)CH_(2)C(O)CH_(2)CH_(3)(TFH)and CF_(3)C(O)CH_(2)C(O)CH(CH_(3))2(TFMH),have been measured at(298±2)K and under atmospheric *** experiments were performed using the relative-rate method with a GC-FID detection *** different determinations and references used,the following rate coefficients were obtained(in cm3/(molecule·sec)):k_(4)(TFP+Cl)=(1.75±0.21)×10^(−10),k_(5)(TFH+Cl)=(2.05±0.23)×10^(−10),k_(6)(TFMH+Cl)=(2.71±0.34)×10^(−10).Reactivity trends of FDKs were discussed and Free Energy Relationships analysis was *** expression lgkOH=1.68 lgkCl+5.71 was obtained for the reactivity of the studied FDKs together with similar unsaturated VOCs with Cl and OH radicals Additionally,acetic acid(CH_(3)C(O)OH)and trifluoroacetic acid(CF_(3)C(O)OH)were positively identified and quantified as degradation products using in situ FTIR *** to the identified products,atmospheric chemical mechanisms were *** atmospheric implications of the studied reactions were assessed by the estimation of the tropospheric lifetimes of TFP,TFH,and TFMH concerning their reaction with Cl atoms to be 48,41,and 31 hours,*** relatively short residence in the atmosphere of the fluorocarbons studied will have a local/regional impact with restricted *** warming potential(GWP(20 yr))calculated for the studied fluoro diketones were 0.014,0.003 and 0.001 for TFP,TFH and TFMH,respectively with a negligible contribution to the greenhouse effect.

关键词： Fluorinated diketones Kinetics SPME-GC-FID FTIR in situ SAR Free energy relationships

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SARS-CoV-2 proteins show great binding affinity to resin composite monomers and polymerized chains

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World journal of Experimental Medicine 2025年第1期15卷 96-103页

作者： pedro Henrique Sette-de-Souza Moan jéfter Fernandes Costa Boniek Castillo Dutra Borges Faculdade de Odontologia Universidade de Pernambuco-campus ArcoverdeArcoverde 56503-146PernambucoBrazil Programa de Pós-Graduação em Saúde e Desenvolvimento Socioambiental Universidade de Pernambuco-campus GaranhunsGaranhuns 55294-902PernambucoBrazil Programa de Pós-Graduação em Biologia Celular e Molecular Aplicada Universidade de Pernambuco-campus Santo AmaroRecife 50100-130PernambucoBrazil Department of Odontologia Universidade Federal do Rio Grande do NorteNatal 59056-000Rio Grande do NorteBrazil Programa de Pós-Graduação em Ciências Odontológicas Universidade Federal do Rio Grande do NorteNatal 59056-000Rio Grande do NorteBrazil

BACKGROUND Due to saliva and salivary glands are reservoir to severe acute respiratory syndrome-coronavirus 2(SARS-CoV-2),aerosols and saliva droplets are primary sources of cross-infection and are responsible for the high human–human transmission of ***,there is no evidence about how SARSCoV-2 interacts with oral structures,particularly resin *** To evaluate the interaction of SARS-CoV-2 proteins with monomers present in resin composites using in silico *** Four SARS-CoV-2 proteins[*** protease,3C-like protease,papain-like protease(PLpro),and glycoprotein spike]were selected along with salivary amylase as the positive control,and their binding affinity with bisphenol-A glycol dimethacrylate,bisphenol-A ethoxylated dimethacrylate,triethylene glycol dimethacrylate,and urethane dimethacrylate was *** docking was performed using AutoDock Vina and visualised in Chimera UCSF *** best ligand–protein model was identified based on the binding energy(ΔG–kcal/moL).RESULTS Values for the binding energies ranged from-3.6 kcal/moL to-7.3 kcal/*** 3-monomer chain had the lowest binding energy(*** affinity)to PLpro and the glycoprotein ***-polymerised monomers and polymerised chains interacted with SARS-CoV-2 proteins via hydrogen bonds and hydrophobic *** findings suggest an interaction between SARS-CoV-2 proteins and resin *** SARS-CoV-2 proteins show affinity to non-polymerised and polymerised resin composite chains.

关键词： Composite resins COVID-19 SARS-CoV-2 Dental restorations Molecular docking simulation Dentistry

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Merits and limitations of TiO2-based photocatalytic pretreatment of soils impacted by crude oil for expediting bioremediation

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Frontiers of Chemical Science and Engineering 2017年第3期11卷 387-394页

作者： Yu Yang Hassan javed Danning Zhang Deyi Li Roopa Kamath Kevin McVey Kanwartej Sra pedro j.j. alvarez Department of Civil and Environmental Engineering Rice University Houston TX 77005 USA Department of Chemistry Rice University Houston TX 77005 USA Department of Civil and Environmental Engineering Tongji University Shanghai 200092 China Chevron Energy Technology Company Houston TX 77002 USA

Heavy hydrocarbons （HHCs） in soils impacted by crude oil spills are generally recalcitrant to biodegrada- tion due to their low bioavailability and complex chemical structure. In this study, soils were pretreated with varying concentrations of ultraviolet radiation A （UVA） or ultraviolet radiation C （UVC） activated titanium dioxide （TiO2）（1%-5%） under varying moisture conditions （0%- 300% water holding capacity （WHC）） to enhance biodegradation of HCCs and shorten remediation time- frames. We demonstrate that pretreatment of impacted soils with UVC-activated TiO2 in soil slurries could enhance bioremediation of HHCs. Total petroleum hydrocarbon （TPH） removal after 24 h exposure to UVC （254 nm and 4.8 mW/cm2） was （19.15：1.6）% in slurries with 300% WHC and 5 wt-% TiO2. TPH removal was non-selective in the C15-C36 range and increased with moisture content and TiO2 concentration. In a 10-d bioremediation test, TPH removal in treated soil increased to （26.05：0.9）%, compared to （15.45：0.8）% for controls without photo- catalytic pre-treatment. Enhanced biodegradation was also confirmed by respirometry. This suggests that addition of UVC-activated TiO2 to soil slurries can transform recalcitrant hydrocarbons into more bioavailable and biodegradable byproducts and increase the rate of subsequent biodegradation. However, similar results were not observed for soils pretreated with UVA activated TiO2. This suggests that activation of TiO2 by sunlight and direct addition of TiO2 to unsaturated soils within landfarming setting may not be a feasible approach. Nevertheless, less than 1% of UVA （7.5 mW/cm2） or UVC （1.4 mW/cm2） penetrated beyond 0.3 cm soil depth, indicating that limited light penetration through soil would hinder the ability of TiO2 to enhance soil bioremediation under land farming conditions.

关键词： ZiO2 pretreatment bioremediation total petroleum hydrocarbons ultraviolet

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Integrated Groups and Smooth Distribution Groups

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Acta Mathematica Sinica,English Series 2007年第1期23卷 57-64页

作者： pedro j.MIANA Departamento de Matemáticas Universidad de Zaragoza50009Spain

In this paper, we prove directly that α-times integrated groups define algebra homomorphisms. We also give a theorem of equivalence between smooth distribution groups and α-times integrated groups.

关键词： integrated groups distribution groups Weyl fractional calculus

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