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  1. Article ; Online: Catalytic reduction of water pollutants: knowledge gaps, lessons learned, and new opportunities

    Liu, Jinyong / Gao, Jinyu

    Front. Environ. Sci. Eng.. 2023 Feb., v. 17, no. 2 p.26-26

    2023  

    Abstract: In this paper, we discuss the previous advances, current challenges, and future opportunities for the research of catalytic reduction of water pollutants. We present five case studies on the development of palladium-based catalysts for nitrate, chlorate, ...

    Abstract In this paper, we discuss the previous advances, current challenges, and future opportunities for the research of catalytic reduction of water pollutants. We present five case studies on the development of palladium-based catalysts for nitrate, chlorate, and perchlorate reduction with hydrogen gas under ambient conditions. We emphasize the realization of new functionalities through the screening and design of catalytic metal sites, including (i) platinum group metal (PGM) nanoparticles, (ii) the secondary metals for improving the reaction rate and product selectivity of nitrate reduction, (iii) oxygen-atom-transfer metal oxides for chlorate and perchlorate reduction, and (iv) ligand-enhanced coordination complexes for substantial activity enhancement. We also highlight the facile catalyst preparation approach that brought significant convenience to catalyst optimization. Based on our own studies, we then discuss directions of the catalyst research effort that are not immediately necessary or desirable, including (1) systematic study on the downstream aspects of under-developed catalysts, (2) random integration with hot concepts without a clear rationale, and (3) excessive and decorative experiments. We further address some general concerns regarding using H₂ and PGMs in the catalytic system. Finally, we recommend future catalyst development in both “fundamental” and “applied” aspects. The purpose of this perspective is to remove major misconceptions about reductive catalysis research and bring back significant innovations for both scientific advancements and engineering applications to benefit environmental protection.
    Keywords catalysts ; catalytic activity ; chlorates ; environmental protection ; hydrogen ; nanoparticles ; nitrate reduction ; nitrates ; perchlorates ; platinum
    Language English
    Dates of publication 2023-02
    Size p. 26.
    Publishing place Higher Education Press
    Document type Article ; Online
    Note Review
    ZDB-ID 2662203-8
    ISSN 2095-221X ; 2095-2201
    ISSN (online) 2095-221X
    ISSN 2095-2201
    DOI 10.1007/s11783-023-1626-z
    Database NAL-Catalogue (AGRICOLA)

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  2. Article ; Online: Preparation and Synergy of Supported Ru

    Gao, Jinyu / Xie, Shaohua / Liu, Fudong / Liu, Jinyong

    Environmental science & technology

    2023  Volume 57, Issue 9, Page(s) 3962–3970

    Abstract: Chlorate ( ... ...

    Abstract Chlorate (ClO
    MeSH term(s) Palladium ; Chlorates ; Oxidation-Reduction ; Hydrogen-Ion Concentration
    Chemical Substances Palladium (5TWQ1V240M) ; Chlorates
    Language English
    Publishing date 2023-02-21
    Publishing country United States
    Document type Journal Article ; Research Support, Non-U.S. Gov't ; Research Support, U.S. Gov't, Non-P.H.S.
    ISSN 1520-5851
    ISSN (online) 1520-5851
    DOI 10.1021/acs.est.3c00415
    Database MEDical Literature Analysis and Retrieval System OnLINE

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  3. Article ; Online: Electrocatalytic Perchlorate Reduction Using an Oxorhenium Complex Supported on a Ti

    Almassi, Soroush / Ren, Changxu / Liu, Jinyong / Chaplin, Brian P

    Environmental science & technology

    2022  Volume 56, Issue 5, Page(s) 3267–3276

    Abstract: An organometallic rhenium catalyst was deposited on a ... ...

    Abstract An organometallic rhenium catalyst was deposited on a Ti
    MeSH term(s) Chlorides ; Hydrogen ; Kinetics ; Oxidation-Reduction ; Perchlorates ; Rhenium ; Titanium ; Water ; Water Pollutants, Chemical/analysis
    Chemical Substances Chlorides ; Perchlorates ; Water Pollutants, Chemical ; Water (059QF0KO0R) ; perrhenate (14333-24-5) ; Rhenium (7440-15-5) ; Hydrogen (7YNJ3PO35Z) ; Titanium (D1JT611TNE) ; perchlorate (VLA4NZX2P4)
    Language English
    Publishing date 2022-02-17
    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.1c08220
    Database MEDical Literature Analysis and Retrieval System OnLINE

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  4. Article ; Online: Overexpression of miR-133b protects against isoflurane-induced learning and memory impairment.

    Zhang, Yu / Liu, Jinyong / Xie, Cuili / Wu, Pingping

    Experimental and therapeutic medicine

    2021  Volume 22, Issue 5, Page(s) 1207

    Abstract: A number of microRNAs (miRs) have been identified as being involved in the regulation of anesthesia-induced cognitive impairment. The aim of the present study was to investigated the role and potential mechanism of miR-133b in isoflurane-induced learning ...

    Abstract A number of microRNAs (miRs) have been identified as being involved in the regulation of anesthesia-induced cognitive impairment. The aim of the present study was to investigated the role and potential mechanism of miR-133b in isoflurane-induced learning and memory impairment. An animal model of isoflurane exposure was established using neonatal Sprague-Dawley rats. The rats were trained for Morris water maze (MWM) testing to assess their spatial learning and memory ability. Reverse transcription-quantitative polymerase chain reaction was used for the measurement of miR-133b expression in hippocampal tissues and primary hippocampal neuron cultures. Cell viability was assessed using a Cell Counting Kit-8 assay, and flow cytometric analysis was used to determine the rate of apoptosis. The MWM test results indicated that during the training period, the time required to locate the platform was significantly increased for rats exposed to isoflurane, and this increased time was reduced by the overexpression of miR-133b. The results of a probe trial indicated that isoflurane exposure increased escape latency and decreased the time spent in the platform area for isoflurane-treated rats; however, these effects were reversed by the injection of miR-133b agomir. The
    Language English
    Publishing date 2021-08-24
    Publishing country Greece
    Document type Journal Article
    ZDB-ID 2683844-8
    ISSN 1792-1015 ; 1792-0981
    ISSN (online) 1792-1015
    ISSN 1792-0981
    DOI 10.3892/etm.2021.10641
    Database MEDical Literature Analysis and Retrieval System OnLINE

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  5. Article ; Online: Substantial defluorination of polychlorofluorocarboxylic acids triggered by anaerobic microbial hydrolytic dechlorination.

    Jin, Bosen / Liu, Huaqing / Che, Shun / Gao, Jinyu / Yu, Yaochun / Liu, Jinyong / Men, Yujie

    Nature water

    2023  Volume 1, Issue 5, Page(s) 451–461

    Abstract: Chlorinated polyfluorocarboxylic acids (Cl-PFCAs) derived from the widely used chlorotrifluoroethylene (CTFE) polymers and oligomers may enter and influence the aquatic environment. Here, we report significant defluorination of Cl-PFCAs by an anaerobic ... ...

    Abstract Chlorinated polyfluorocarboxylic acids (Cl-PFCAs) derived from the widely used chlorotrifluoroethylene (CTFE) polymers and oligomers may enter and influence the aquatic environment. Here, we report significant defluorination of Cl-PFCAs by an anaerobic microbial community via novel pathways triggered by anaerobic microbial dechlorination. Cl-PFCAs first underwent microbial reductive, hydrolytic, and eliminative dechlorination, and it was the hydrolytic dechlorination that led to significant spontaneous defluorination. Hydrolytic dechlorination was favored with increased Cl-substitutions. An isolated, highly enriched anaerobic defluorinating culture was dominated by two genomes closest to
    Language English
    Publishing date 2023-05-15
    Publishing country England
    Document type Journal Article
    ISSN 2731-6084
    ISSN (online) 2731-6084
    DOI 10.1038/s44221-023-00077-6
    Database MEDical Literature Analysis and Retrieval System OnLINE

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  6. Article ; Online: Oxidative Transformation of Nafion-Related Fluorinated Ether Sulfonates: Comparison with Legacy PFAS Structures and Opportunities of Acidic Persulfate Digestion for PFAS Precursor Analysis.

    Liu, Zekun / Jin, Bosen / Rao, Dandan / Bentel, Michael J / Liu, Tianchi / Gao, Jinyu / Men, Yujie / Liu, Jinyong

    Environmental science & technology

    2024  Volume 58, Issue 14, Page(s) 6415–6424

    Abstract: The total oxidizable precursor (TOP) assay has been extensively used for detecting PFAS pollutants that do not have analytical standards. It uses hydroxyl radicals ( ... ...

    Abstract The total oxidizable precursor (TOP) assay has been extensively used for detecting PFAS pollutants that do not have analytical standards. It uses hydroxyl radicals (HO
    MeSH term(s) Ether ; Fluorocarbons/analysis ; Water Pollutants, Chemical/analysis ; Carboxylic Acids ; Ethers ; Alkanesulfonates ; Ethyl Ethers ; Environmental Pollutants ; Digestion ; Oxidative Stress ; Fluorocarbon Polymers
    Chemical Substances perfluorosulfonic acid (39464-59-0) ; Ether (0F5N573A2Y) ; Fluorocarbons ; Water Pollutants, Chemical ; Carboxylic Acids ; Ethers ; Alkanesulfonates ; Ethyl Ethers ; Environmental Pollutants ; Fluorocarbon Polymers
    Language English
    Publishing date 2024-03-25
    Publishing country United States
    Document type Journal Article
    ISSN 1520-5851
    ISSN (online) 1520-5851
    DOI 10.1021/acs.est.3c06289
    Database MEDical Literature Analysis and Retrieval System OnLINE

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  7. Article ; Online: Electrostatic Field in Contact-Electro-Catalysis Driven C-F Bond Cleavage of Perfluoroalkyl Substances.

    Wang, Yanfeng / Zhang, Jing / Zhang, Wenkai / Yao, Jiaming / Liu, Jinyong / He, Huan / Gu, Cheng / Gao, Guandao / Jin, Xin

    Angewandte Chemie (International ed. in English)

    2024  Volume 63, Issue 19, Page(s) e202402440

    Abstract: Perfluoroalkyl substances (PFASs) are persistent and toxic to human health. It is demanding for high-efficient and green technologies to remove PFASs from water. In this study, a novel PFAS treatment technology was developed, utilizing ... ...

    Abstract Perfluoroalkyl substances (PFASs) are persistent and toxic to human health. It is demanding for high-efficient and green technologies to remove PFASs from water. In this study, a novel PFAS treatment technology was developed, utilizing polytetrafluoroethylene (PTFE) particles (1-5 μm) as the catalyst and a low frequency ultrasound (US, 40 kHz, 0.3 W/cm
    Language English
    Publishing date 2024-03-15
    Publishing country Germany
    Document type Journal Article
    ZDB-ID 2011836-3
    ISSN 1521-3773 ; 1433-7851
    ISSN (online) 1521-3773
    ISSN 1433-7851
    DOI 10.1002/anie.202402440
    Database MEDical Literature Analysis and Retrieval System OnLINE

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  8. Article: Microbial Defluorination of Unsaturated Per- and Polyfluorinated Carboxylic Acids under Anaerobic and Aerobic Conditions: A Structure Specificity Study

    Yu, Yaochun / Che, Shun / Ren, Changxu / Jin, Bosen / Tian, Zhenyu / Liu, Jinyong / Men, Yujie

    Environmental science & technology. 2022 Apr. 04, v. 56, no. 8

    2022  

    Abstract: The recently discovered microbial reductive defluorination of two C₆ branched and unsaturated fluorinated carboxylic acids (FCAs) provided valuable insights into the environmental fate of per- and polyfluoroalkyl substances (PFASs) and potential ... ...

    Abstract The recently discovered microbial reductive defluorination of two C₆ branched and unsaturated fluorinated carboxylic acids (FCAs) provided valuable insights into the environmental fate of per- and polyfluoroalkyl substances (PFASs) and potential bioremediation strategies. However, a systematic investigation is needed to further demonstrate the role of C═C double bonds in the biodegradability of unsaturated PFASs. Here, we examined the structure-biodegradability relationships of 13 FCAs, including nine commercially available unsaturated FCAs and four structurally similar saturated ones, in an anaerobic defluorinating enrichment and an activated sludge community. The anaerobic and aerobic transformation/defluorination pathways were elucidated. The results showed that under anaerobic conditions, the α,β-unsaturation is crucial for FCA biotransformation via reductive defluorination and/or hydrogenation pathways. With sp² C–F bonds being substituted by C–H bonds, the reductive defluorination became less favorable than hydrogenation. Moreover, for the first time, we reported enhanced degradability and defluorination capability of specific unsaturated FCA structures with trifluoromethyl (−CF₃) branches at the α/β-carbon. Such FCA structures can undergo anaerobic abiotic defluorination in the presence of reducing agents and significant aerobic microbial defluorination. Given the diverse applications and emerging concerns of fluorochemicals, this work not only advances the fundamental understanding of the fate of unsaturated PFASs in natural and engineered environments but also may provide insights into the design of readily degradable fluorinated alternatives to existing PFAS compounds.
    Keywords activated sludge ; biodegradability ; bioremediation ; biotransformation ; environmental fate ; hydrogenation
    Language English
    Dates of publication 2022-0404
    Size p. 4894-4904.
    Publishing place American Chemical Society
    Document type Article
    ISSN 1520-5851
    DOI 10.1021/acs.est.1c05509
    Database NAL-Catalogue (AGRICOLA)

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  9. Article: Accelerated Degradation of Perfluorosulfonates and Perfluorocarboxylates by UV/Sulfite + Iodide: Reaction Mechanisms and System Efficiencies

    Liu, Zekun / Chen, Zhanghao / Gao, Jinyu / Yu, Yaochun / Men, Yujie / Gu, Cheng / Liu, Jinyong

    Environmental science & technology. 2022 Feb. 28, v. 56, no. 6

    2022  

    Abstract: The addition of iodide (I–) in the UV/sulfite system (UV/S) significantly accelerated the reductive degradation of perfluorosulfonates (PFSAs, CₙF₂ₙ₊₁SO₃–) and perfluorocarboxylates (PFCAs, CₙF₂ₙ₊₁COO–). Using the highly recalcitrant perfluorobutane ... ...

    Abstract The addition of iodide (I–) in the UV/sulfite system (UV/S) significantly accelerated the reductive degradation of perfluorosulfonates (PFSAs, CₙF₂ₙ₊₁SO₃–) and perfluorocarboxylates (PFCAs, CₙF₂ₙ₊₁COO–). Using the highly recalcitrant perfluorobutane sulfonate (C₄F₉SO₃–) as a probe, we optimized the UV/sulfite + iodide system (UV/S + I) to degrade n = 1–7 PFCAs and n = 4, 6, 8 PFSAs. In general, the kinetics of per- and polyfluoroalkyl substance (PFAS) decay, defluorination, and transformation product formations in UV/S + I were up to three times faster than those in UV/S. Both systems achieve a similar maximum defluorination. The enhanced reaction rates and optimized photoreactor settings lowered the EE/O for PFCA degradation below 1.5 kW h m–³. The relatively high quantum yield of eₐq– from I– made the availability of hydrated electrons (eₐq–) in UV/S + I and UV/I two times greater than that in UV/S. Meanwhile, the rapid scavenging of reactive iodine species by SO₃²– made the lifetime of eₐq– in UV/S + I eight times longer than that in UV/I. The addition of I– also substantially enhanced SO₃²– utilization in treating concentrated PFAS. The optimized UV/S + I system achieved >99.7% removal of most PFSAs and PFCAs and >90% overall defluorination in a synthetic solution of concentrated PFAS mixtures and NaCl. We extended the discussion over molecular transformation mechanisms, development of PFAS degradation technologies, and the fate of iodine species.
    Keywords environmental science ; iodides ; iodine ; perfluorocarbons ; sulfites ; sulfonates ; technology
    Language English
    Dates of publication 2022-0228
    Size p. 3699-3709.
    Publishing place American Chemical Society
    Document type Article
    ISSN 1520-5851
    DOI 10.1021/acs.est.1c07608
    Database NAL-Catalogue (AGRICOLA)

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  10. Article: Electrocatalytic Perchlorate Reduction Using an Oxorhenium Complex Supported on a Ti₄O₇ Reactive Electrochemical Membrane

    Almassi, Soroush / Ren, Changxu / Liu, Jinyong / Chaplin, Brian P.

    Environmental science & technology. 2022 Feb. 17, v. 56, no. 5

    2022  

    Abstract: An organometallic rhenium catalyst was deposited on a Ti₄O₇ reactive electrochemical membrane (Re/REM) for the electrocatalytic reduction of aqueous ClO₄– to Cl–. Results showed increasing ClO₄– reduction upon increasing cathodic potential (i.e., −0.4 to– ...

    Abstract An organometallic rhenium catalyst was deposited on a Ti₄O₇ reactive electrochemical membrane (Re/REM) for the electrocatalytic reduction of aqueous ClO₄– to Cl–. Results showed increasing ClO₄– reduction upon increasing cathodic potential (i.e., −0.4 to–1.7 V/SHE). A 5 mM ClO₄– solution was reduced by ∼21% in a single pass (residence time ∼0.2 s) through the Re/REM at a pH of 7, with >99% Cl– selectivity and a current efficiency of ∼100%. Kinetic analysis indicated that the reaction rate constant increased from 3953 to 7128 L h–¹ gRₑ–¹ at pH values of 9 to 3, respectively, and was mass transport-limited at pH < 5. The rate constants were 2 orders of magnitude greater than reported values for an analogous catalytic system using hydrogen as an electron donor. A continuous flow Re/REM system reduced 1 ppm ClO₄– in a groundwater sample by >99.9% for the first 93.5 h, and concentrations were lower than the EPA ClO₄– guideline (56 ppb) for 374 h of treatment. The fast ClO₄– reduction kinetics and high chloride selectivity without the need for acidic conditions and a continual hydrogen electron donor supply for catalyst regeneration indicate the promising ability of the Re/REM for aqueous electrocatalytic ClO₄– treatment.
    Keywords catalysts ; electrochemistry ; environmental science ; groundwater ; guidelines ; hydrogen ; kinetics ; pH ; perchlorates ; rhenium ; technology
    Language English
    Dates of publication 2022-0217
    Size p. 3267-3276.
    Publishing place American Chemical Society
    Document type Article
    ISSN 1520-5851
    DOI 10.1021/acs.est.1c08220
    Database NAL-Catalogue (AGRICOLA)

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