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  1. Article: Role of Ferryl Ion Intermediates in Fast Fenton Chemistry on Aqueous Microdroplets

    Gu, Alan Y. / Musgrave, Charles / Goddard, William A. / Hoffmann, Michael R. / Colussi, Agustín J.

    Environmental science & technology. 2021 July 02, v. 55, no. 21

    2021  

    Abstract: In the aqueous environment, Feᴵᴵ ions enhance the oxidative potential of ozone and hydrogen peroxide by generating the reactive oxoiron species (ferryl ion, FeᴵⱽO²⁺) and hydroxyl radical (·OH) via Fenton chemistry. Herein, we investigate factors that ... ...

    Abstract In the aqueous environment, Feᴵᴵ ions enhance the oxidative potential of ozone and hydrogen peroxide by generating the reactive oxoiron species (ferryl ion, FeᴵⱽO²⁺) and hydroxyl radical (·OH) via Fenton chemistry. Herein, we investigate factors that control the pathways of these reactive intermediates in the oxidation of dimethyl sulfoxide (Me₂SO) in Feᴵᴵ solutions reacting with O₃ in both bulk-phase water and on the surfaces of aqueous microdroplets. Electrospray ionization mass spectrometry is used to quantify the formation of dimethyl sulfone (Me₂SO₂, from FeᴵⱽO²⁺ + Me₂SO) and methanesulfonate (MeSO₃–, from ·OH + Me₂SO) over a wide range of Feᴵᴵ and O₃ concentrations and pH. In addition, the role of environmentally relevant organic ligands on the reaction kinetics was also explored. The experimental results show that Fenton chemistry proceeds at a rate ∼10⁴ times faster on microdroplets than that in bulk-phase water. Since the production of MeSO₃– is initiated by ·OH radicals at diffusion-controlled rates, experimental ratios of Me₂SO₂/MeSO₃– > 10² suggest that FeᴵⱽO²⁺ is the dominant intermediate under all conditions. Me₂SO₂ yields in the presence of ligands, L, vary as volcano-plot functions of E⁰(LFeᴵⱽO²⁺+ O₂/LFe²⁺ + O₃) reduction potentials calculated by DFT with a maximum achieved in the case of L≡oxalate. Our findings underscore the key role of ferryl FeᴵⱽO²⁺ intermediates in Fenton chemistry taking place on aqueous microdroplets.
    Keywords dimethyl sulfoxide ; electrospray ionization mass spectrometry ; environmental science ; hydrogen peroxide ; hydroxyl radicals ; ligands ; oxidation ; ozone ; pH ; reaction kinetics ; technology
    Language English
    Dates of publication 2021-0702
    Size p. 14370-14377.
    Publishing place American Chemical Society
    Document type Article
    ISSN 1520-5851
    DOI 10.1021/acs.est.1c01962
    Database NAL-Catalogue (AGRICOLA)

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  2. Article ; Online: Role of Ferryl Ion Intermediates in Fast Fenton Chemistry on Aqueous Microdroplets.

    Gu, Alan Y / Musgrave, Charles / Goddard, William A / Hoffmann, Michael R / Colussi, Agustín J

    Environmental science & technology

    2021  Volume 55, Issue 21, Page(s) 14370–14377

    Abstract: In the aqueous environment, ... ...

    Abstract In the aqueous environment, Fe
    MeSH term(s) Hydrogen Peroxide ; Hydroxyl Radical ; Iron ; Oxidation-Reduction ; Water
    Chemical Substances Water (059QF0KO0R) ; ferryl iron (14127-53-8) ; Hydroxyl Radical (3352-57-6) ; Hydrogen Peroxide (BBX060AN9V) ; Iron (E1UOL152H7)
    Language English
    Publishing date 2021-07-02
    Publishing country United States
    Document type Journal Article ; Research Support, U.S. Gov't, Non-P.H.S.
    ISSN 1520-5851
    ISSN (online) 1520-5851
    DOI 10.1021/acs.est.1c01962
    Database MEDical Literature Analysis and Retrieval System OnLINE

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  3. Article ; Online: Tacrolimus time-in-therapeutic range is associated with freedom from acute rejection and graft failure following intestinal transplantation.

    Santeusanio, Andrew D / Gu, Alan / Weinberg, Alan D / Moon, Jang / Iyer, Kishore R

    Clinical transplantation

    2021  Volume 35, Issue 6, Page(s) e14291

    Abstract: Background: Trough-adjusted tacrolimus is commonly prescribed following intestinal transplantation to prevent allograft rejection. Despite established practice, there remains limited direct evidence linking tacrolimus levels with improved clinical ... ...

    Abstract Background: Trough-adjusted tacrolimus is commonly prescribed following intestinal transplantation to prevent allograft rejection. Despite established practice, there remains limited direct evidence linking tacrolimus levels with improved clinical outcomes.
    Methods: This was a single-center review of all adult non-liver containing intestinal allograft recipients from 2011 to 2018. Patients received lymphocyte depleting induction and maintenance immunosuppression consisting of tacrolimus and a corticosteroid taper. Tacrolimus time-in-therapeutic range (TAC-TTR) was calculated for all patients from the date of transplant until 1-year post-transplant using Rosendaal's method. Cox-Proportional hazards modeling was utilized to assess freedom from acute rejection and graft failure stratified by TAC-TTR quartile.
    Results: 47 patients were included in the review. Mean TAC-TTR for the cohort was 30.2% ± 11.4. Fifteen episodes of acute rejection were observed, 8 of which were severe. Patients in the highest TAC-TTR quartile >36% had a lower incidence of acute rejection and graft failure relative to patients with a TAC-TTR <20%. Cox-Proportional hazards modeling found a 10% decrease in TAC-TTR was associated with an increased hazard for acute rejection (2.03), severe acute rejection (2.19), and graft loss (3.33).
    Conclusion: The results of this study suggest that decreasing TAC-TTR is a risk factor for both acute rejection as well as intestinal allograft failure.
    MeSH term(s) Adult ; Freedom ; Graft Rejection/drug therapy ; Graft Rejection/etiology ; Graft Survival ; Humans ; Immunosuppressive Agents/therapeutic use ; Kidney Transplantation ; Tacrolimus/therapeutic use
    Chemical Substances Immunosuppressive Agents ; Tacrolimus (WM0HAQ4WNM)
    Language English
    Publishing date 2021-04-03
    Publishing country Denmark
    Document type Journal Article
    ZDB-ID 639001-8
    ISSN 1399-0012 ; 0902-0063
    ISSN (online) 1399-0012
    ISSN 0902-0063
    DOI 10.1111/ctr.14291
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  4. Article: Membrane-Based In-Gel Loop-Mediated Isothermal Amplification (mgLAMP) System for SARS-CoV-2 Quantification in Environmental Waters

    Zhu, Yanzhe / Wu, Xunyi / Gu, Alan / Dobelle, Leopold / Cid, Clément A. / Li, Jing / Hoffmann, Michael R.

    Environmental science & technology. 2021 Dec. 30, v. 56, no. 2

    2021  

    Abstract: Since the COVID-19 pandemic is expected to become endemic, quantification of severe acute respiratory syndrome coronavirus-2 (SARS-CoV-2) in ambient waters is critical for environmental surveillance and for early detection of outbreaks. Herein, we report ...

    Abstract Since the COVID-19 pandemic is expected to become endemic, quantification of severe acute respiratory syndrome coronavirus-2 (SARS-CoV-2) in ambient waters is critical for environmental surveillance and for early detection of outbreaks. Herein, we report the development of a membrane-based in-gel loop-mediated isothermal amplification (mgLAMP) system that is designed for the rapid point-of-use quantification of SARS-CoV-2 particles in environmental waters. The mgLAMP system integrates the viral concentration, in-assay viral lysis, and on-membrane hydrogel-based RT-LAMP quantification using enhanced fluorescence detection with a target-specific probe. With a sample-to-result time of less than 1 h, mgLAMP successfully detected SARS-CoV-2 below 0.96 copies/mL in Milli-Q water. In surface water, the lowest detected SARS-CoV-2 concentration was 93 copies/mL for mgLAMP, while the reverse transcription quantitative polymerase chain reaction (RT-qPCR) with optimal pretreatment was inhibited at 930 copies/mL. A 3D-printed portable device is designed to integrate heated incubation and fluorescence illumination for the simultaneous analysis of nine mgLAMP assays. Smartphone-based imaging and machine learning-based image processing are used for the interpretation of results. In this report, we demonstrate that mgLAMP is a promising method for large-scale environmental surveillance of SARS-CoV-2 without the need for specialized equipment, highly trained personnel, and labor-intensive procedures.
    Keywords COVID-19 infection ; Severe acute respiratory syndrome coronavirus 2 ; environmental monitoring ; fluorescence ; human resources ; lighting ; portable equipment ; quantitative polymerase chain reaction ; reverse transcription ; reverse transcription loop-mediated isothermal amplification ; surface water
    Language English
    Dates of publication 2021-1230
    Size p. 862-873.
    Publishing place American Chemical Society
    Document type Article
    ISSN 1520-5851
    DOI 10.1021/acs.est.1c04623
    Database NAL-Catalogue (AGRICOLA)

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  5. Article ; Online: Membrane-Based In-Gel Loop-Mediated Isothermal Amplification (mgLAMP) System for SARS-CoV-2 Quantification in Environmental Waters.

    Zhu, Yanzhe / Wu, Xunyi / Gu, Alan / Dobelle, Leopold / Cid, Clément A / Li, Jing / Hoffmann, Michael R

    Environmental science & technology

    2021  Volume 56, Issue 2, Page(s) 862–873

    Abstract: Since the COVID-19 pandemic is expected to become endemic, quantification of severe acute respiratory syndrome coronavirus-2 (SARS-CoV-2) in ambient waters is critical for environmental surveillance and for early detection of outbreaks. Herein, we report ...

    Abstract Since the COVID-19 pandemic is expected to become endemic, quantification of severe acute respiratory syndrome coronavirus-2 (SARS-CoV-2) in ambient waters is critical for environmental surveillance and for early detection of outbreaks. Herein, we report the development of a membrane-based in-gel loop-mediated isothermal amplification (mgLAMP) system that is designed for the rapid point-of-use quantification of SARS-CoV-2 particles in environmental waters. The mgLAMP system integrates the viral concentration, in-assay viral lysis, and on-membrane hydrogel-based RT-LAMP quantification using enhanced fluorescence detection with a target-specific probe. With a sample-to-result time of less than 1 h, mgLAMP successfully detected SARS-CoV-2 below 0.96 copies/mL in Milli-Q water. In surface water, the lowest detected SARS-CoV-2 concentration was 93 copies/mL for mgLAMP, while the reverse transcription quantitative polymerase chain reaction (RT-qPCR) with optimal pretreatment was inhibited at 930 copies/mL. A 3D-printed portable device is designed to integrate heated incubation and fluorescence illumination for the simultaneous analysis of nine mgLAMP assays. Smartphone-based imaging and machine learning-based image processing are used for the interpretation of results. In this report, we demonstrate that mgLAMP is a promising method for large-scale environmental surveillance of SARS-CoV-2 without the need for specialized equipment, highly trained personnel, and labor-intensive procedures.
    MeSH term(s) COVID-19 ; Humans ; Molecular Diagnostic Techniques ; Nucleic Acid Amplification Techniques ; Pandemics ; RNA, Viral ; SARS-CoV-2 ; Sensitivity and Specificity
    Chemical Substances RNA, Viral
    Language English
    Publishing date 2021-12-30
    Publishing country United States
    Document type Journal Article ; Research Support, Non-U.S. Gov't
    ISSN 1520-5851
    ISSN (online) 1520-5851
    DOI 10.1021/acs.est.1c04623
    Database MEDical Literature Analysis and Retrieval System OnLINE

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  6. Article ; Online: Solar Urea: Towards a Sustainable Fertilizer Industry.

    Xia, Meikun / Mao, Chengliang / Gu, Alan / Tountas, Athanasios A / Qiu, Chenyue / Wood, Thomas E / Li, Young Feng / Ulmer, Ulrich / Xu, Yangfan / Viasus, Camilo J / Ye, Jessica / Qian, Chenxi / Ozin, Geoffrey

    Angewandte Chemie (International ed. in English)

    2021  Volume 61, Issue 1, Page(s) e202110158

    Abstract: Urea, an agricultural fertilizer, nourishes humanity. The century-old Bosch-Meiser process provides the world's urea. It is multi-step, consumes enormous amounts of non-renewable energy, and has a large ... ...

    Abstract Urea, an agricultural fertilizer, nourishes humanity. The century-old Bosch-Meiser process provides the world's urea. It is multi-step, consumes enormous amounts of non-renewable energy, and has a large CO
    Language English
    Publishing date 2021-11-23
    Publishing country Germany
    Document type Journal Article ; Research Support, Non-U.S. Gov't
    ZDB-ID 2011836-3
    ISSN 1521-3773 ; 1433-7851
    ISSN (online) 1521-3773
    ISSN 1433-7851
    DOI 10.1002/anie.202110158
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  7. Article: Photothermal Catalyst Engineering: Hydrogenation of Gaseous CO

    Jia, Jia / Wang, Hong / Lu, Zhuole / O'Brien, Paul G / Ghoussoub, Mireille / Duchesne, Paul / Zheng, Ziqi / Li, Peicheng / Qiao, Qiao / Wang, Lu / Gu, Alan / Jelle, Abdinoor A / Dong, Yuchan / Wang, Qiang / Ghuman, Kulbir Kaur / Wood, Thomas / Qian, Chenxi / Shao, Yue / Qiu, Chenyue /
    Ye, Miaomiao / Zhu, Yimei / Lu, Zheng-Hong / Zhang, Peng / Helmy, Amr S / Singh, Chandra Veer / Kherani, Nazir P / Perovic, Doug D / Ozin, Geoffrey A

    Advanced science (Weinheim, Baden-Wurttemberg, Germany)

    2017  Volume 4, Issue 10, Page(s) 1700252

    Abstract: This study has designed and implemented a library of hetero-nanostructured catalysts, denoted as Pd@ ... ...

    Abstract This study has designed and implemented a library of hetero-nanostructured catalysts, denoted as Pd@Nb
    Language English
    Publishing date 2017-07-25
    Publishing country Germany
    Document type Journal Article
    ZDB-ID 2808093-2
    ISSN 2198-3844
    ISSN 2198-3844
    DOI 10.1002/advs.201700252
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