Reduction of nitrogen-oxygen containing compounds (NOCs) by surface-associated Fe(II) and comparison with soluble Fe(II) complexes
Both Fe(II) adsorbed onto mineral surfaces and soluble Fe(II) complexes are important natural reductants; however, no research has directly compared their reaction kinetics and mechanisms. In this work, the reduction kinetics of heterogeneous Fe(II)-goethite versus homogeneous Fe(II)-tiron were comp...
Ausführliche Beschreibung
Autor*in: |
Li, Xiang [verfasserIn] Chen, Yiling [verfasserIn] Zhang, Huichun [verfasserIn] |
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Format: |
E-Artikel |
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Sprache: |
Englisch |
Erschienen: |
2019 |
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Schlagwörter: |
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Übergeordnetes Werk: |
Enthalten in: The chemical engineering journal - Amsterdam : Elsevier, 1997, 370, Seite 782-791 |
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Übergeordnetes Werk: |
volume:370 ; pages:782-791 |
DOI / URN: |
10.1016/j.cej.2019.03.203 |
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Katalog-ID: |
ELV002221179 |
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520 | |a Both Fe(II) adsorbed onto mineral surfaces and soluble Fe(II) complexes are important natural reductants; however, no research has directly compared their reaction kinetics and mechanisms. In this work, the reduction kinetics of heterogeneous Fe(II)-goethite versus homogeneous Fe(II)-tiron were compared for the first time toward thirteen structurally diverse nitrogen-oxygen containing compounds (NOCs). The reduction of NOCs followed pseudo-first-order reaction kinetics in Fe(II)-goethite, with the rate constant k varying over a wide range from 8.56 h−1 to <0.0001 h−1. In electrochemical experiments where NOCs were physically separated from Fe(II)-goethite, k of carbadox was 3.6 times greater than that of a structurally similar compound that cannot complex with surface Fe(II), while such difference in batch reactors was 531 times. Similar differences in the reactivity of NOCs between the two reactors were reported for Fe(II)-tiron. The good linear cross correlations between the reactivity of Fe(II)-goethite and that of Fe(II)-tiron toward NOCs, nitroaromatics, and polyhalogenated compounds (R2 = 0.76–0.94) can be used to predict the reactivity of other structurally related compounds by both reductants. On the basis of the FTIR and UV spectra, surface complexation was further inferred; both the amino functional groups and the pyridine ring were involved in the complexation, with the ring-N more strongly involved than the ring-O. As opposed to the large differences observed in the reactivity of the two Fe(II) reductants, similar reactivity was obtained when an outer-sphere reductant dithionite was employed. Overall, these results show that complexation between certain NOCs and surface-associated Fe(II) existed which facilitated the reduction reaction. | ||
650 | 4 | |a Surface associated Fe(II) | |
650 | 4 | |a Nitrogen-oxygen containing compounds (NOCs) | |
650 | 4 | |a Reduction | |
650 | 4 | |a Surface complexation | |
650 | 4 | |a Soluble Fe(II) complexes | |
650 | 4 | |a Cross correlation | |
700 | 1 | |a Chen, Yiling |e verfasserin |4 aut | |
700 | 1 | |a Zhang, Huichun |e verfasserin |4 aut | |
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10.1016/j.cej.2019.03.203 doi (DE-627)ELV002221179 (ELSEVIER)S1385-8947(19)30678-3 DE-627 ger DE-627 rda eng 660.05 DE-101 660 DE-101 660 DE-600 58.10 bkl Li, Xiang verfasserin aut Reduction of nitrogen-oxygen containing compounds (NOCs) by surface-associated Fe(II) and comparison with soluble Fe(II) complexes 2019 nicht spezifiziert zzz rdacontent Computermedien c rdamedia Online-Ressource cr rdacarrier Both Fe(II) adsorbed onto mineral surfaces and soluble Fe(II) complexes are important natural reductants; however, no research has directly compared their reaction kinetics and mechanisms. In this work, the reduction kinetics of heterogeneous Fe(II)-goethite versus homogeneous Fe(II)-tiron were compared for the first time toward thirteen structurally diverse nitrogen-oxygen containing compounds (NOCs). The reduction of NOCs followed pseudo-first-order reaction kinetics in Fe(II)-goethite, with the rate constant k varying over a wide range from 8.56 h−1 to <0.0001 h−1. In electrochemical experiments where NOCs were physically separated from Fe(II)-goethite, k of carbadox was 3.6 times greater than that of a structurally similar compound that cannot complex with surface Fe(II), while such difference in batch reactors was 531 times. Similar differences in the reactivity of NOCs between the two reactors were reported for Fe(II)-tiron. The good linear cross correlations between the reactivity of Fe(II)-goethite and that of Fe(II)-tiron toward NOCs, nitroaromatics, and polyhalogenated compounds (R2 = 0.76–0.94) can be used to predict the reactivity of other structurally related compounds by both reductants. On the basis of the FTIR and UV spectra, surface complexation was further inferred; both the amino functional groups and the pyridine ring were involved in the complexation, with the ring-N more strongly involved than the ring-O. As opposed to the large differences observed in the reactivity of the two Fe(II) reductants, similar reactivity was obtained when an outer-sphere reductant dithionite was employed. Overall, these results show that complexation between certain NOCs and surface-associated Fe(II) existed which facilitated the reduction reaction. Surface associated Fe(II) Nitrogen-oxygen containing compounds (NOCs) Reduction Surface complexation Soluble Fe(II) complexes Cross correlation Chen, Yiling verfasserin aut Zhang, Huichun verfasserin aut Enthalten in The chemical engineering journal Amsterdam : Elsevier, 1997 370, Seite 782-791 Online-Ressource (DE-627)320500322 (DE-600)2012137-4 (DE-576)098330152 1873-3212 nnns volume:370 pages:782-791 GBV_USEFLAG_U SYSFLAG_U GBV_ELV SSG-OLC-PHA GBV_ILN_20 GBV_ILN_22 GBV_ILN_23 GBV_ILN_24 GBV_ILN_31 GBV_ILN_32 GBV_ILN_40 GBV_ILN_60 GBV_ILN_62 GBV_ILN_63 GBV_ILN_65 GBV_ILN_69 GBV_ILN_70 GBV_ILN_73 GBV_ILN_74 GBV_ILN_90 GBV_ILN_95 GBV_ILN_100 GBV_ILN_105 GBV_ILN_110 GBV_ILN_150 GBV_ILN_151 GBV_ILN_224 GBV_ILN_370 GBV_ILN_602 GBV_ILN_702 GBV_ILN_2003 GBV_ILN_2004 GBV_ILN_2005 GBV_ILN_2011 GBV_ILN_2014 GBV_ILN_2015 GBV_ILN_2020 GBV_ILN_2021 GBV_ILN_2025 GBV_ILN_2027 GBV_ILN_2034 GBV_ILN_2038 GBV_ILN_2044 GBV_ILN_2048 GBV_ILN_2049 GBV_ILN_2050 GBV_ILN_2056 GBV_ILN_2059 GBV_ILN_2061 GBV_ILN_2064 GBV_ILN_2065 GBV_ILN_2068 GBV_ILN_2111 GBV_ILN_2112 GBV_ILN_2113 GBV_ILN_2118 GBV_ILN_2122 GBV_ILN_2129 GBV_ILN_2143 GBV_ILN_2147 GBV_ILN_2148 GBV_ILN_2152 GBV_ILN_2153 GBV_ILN_2190 GBV_ILN_2336 GBV_ILN_2507 GBV_ILN_2522 GBV_ILN_4035 GBV_ILN_4037 GBV_ILN_4112 GBV_ILN_4125 GBV_ILN_4126 GBV_ILN_4242 GBV_ILN_4251 GBV_ILN_4305 GBV_ILN_4313 GBV_ILN_4323 GBV_ILN_4324 GBV_ILN_4325 GBV_ILN_4326 GBV_ILN_4333 GBV_ILN_4334 GBV_ILN_4335 GBV_ILN_4338 GBV_ILN_4393 58.10 Verfahrenstechnik: Allgemeines AR 370 782-791 045F 660.05 |
spelling |
10.1016/j.cej.2019.03.203 doi (DE-627)ELV002221179 (ELSEVIER)S1385-8947(19)30678-3 DE-627 ger DE-627 rda eng 660.05 DE-101 660 DE-101 660 DE-600 58.10 bkl Li, Xiang verfasserin aut Reduction of nitrogen-oxygen containing compounds (NOCs) by surface-associated Fe(II) and comparison with soluble Fe(II) complexes 2019 nicht spezifiziert zzz rdacontent Computermedien c rdamedia Online-Ressource cr rdacarrier Both Fe(II) adsorbed onto mineral surfaces and soluble Fe(II) complexes are important natural reductants; however, no research has directly compared their reaction kinetics and mechanisms. In this work, the reduction kinetics of heterogeneous Fe(II)-goethite versus homogeneous Fe(II)-tiron were compared for the first time toward thirteen structurally diverse nitrogen-oxygen containing compounds (NOCs). The reduction of NOCs followed pseudo-first-order reaction kinetics in Fe(II)-goethite, with the rate constant k varying over a wide range from 8.56 h−1 to <0.0001 h−1. In electrochemical experiments where NOCs were physically separated from Fe(II)-goethite, k of carbadox was 3.6 times greater than that of a structurally similar compound that cannot complex with surface Fe(II), while such difference in batch reactors was 531 times. Similar differences in the reactivity of NOCs between the two reactors were reported for Fe(II)-tiron. The good linear cross correlations between the reactivity of Fe(II)-goethite and that of Fe(II)-tiron toward NOCs, nitroaromatics, and polyhalogenated compounds (R2 = 0.76–0.94) can be used to predict the reactivity of other structurally related compounds by both reductants. On the basis of the FTIR and UV spectra, surface complexation was further inferred; both the amino functional groups and the pyridine ring were involved in the complexation, with the ring-N more strongly involved than the ring-O. As opposed to the large differences observed in the reactivity of the two Fe(II) reductants, similar reactivity was obtained when an outer-sphere reductant dithionite was employed. Overall, these results show that complexation between certain NOCs and surface-associated Fe(II) existed which facilitated the reduction reaction. Surface associated Fe(II) Nitrogen-oxygen containing compounds (NOCs) Reduction Surface complexation Soluble Fe(II) complexes Cross correlation Chen, Yiling verfasserin aut Zhang, Huichun verfasserin aut Enthalten in The chemical engineering journal Amsterdam : Elsevier, 1997 370, Seite 782-791 Online-Ressource (DE-627)320500322 (DE-600)2012137-4 (DE-576)098330152 1873-3212 nnns volume:370 pages:782-791 GBV_USEFLAG_U SYSFLAG_U GBV_ELV SSG-OLC-PHA GBV_ILN_20 GBV_ILN_22 GBV_ILN_23 GBV_ILN_24 GBV_ILN_31 GBV_ILN_32 GBV_ILN_40 GBV_ILN_60 GBV_ILN_62 GBV_ILN_63 GBV_ILN_65 GBV_ILN_69 GBV_ILN_70 GBV_ILN_73 GBV_ILN_74 GBV_ILN_90 GBV_ILN_95 GBV_ILN_100 GBV_ILN_105 GBV_ILN_110 GBV_ILN_150 GBV_ILN_151 GBV_ILN_224 GBV_ILN_370 GBV_ILN_602 GBV_ILN_702 GBV_ILN_2003 GBV_ILN_2004 GBV_ILN_2005 GBV_ILN_2011 GBV_ILN_2014 GBV_ILN_2015 GBV_ILN_2020 GBV_ILN_2021 GBV_ILN_2025 GBV_ILN_2027 GBV_ILN_2034 GBV_ILN_2038 GBV_ILN_2044 GBV_ILN_2048 GBV_ILN_2049 GBV_ILN_2050 GBV_ILN_2056 GBV_ILN_2059 GBV_ILN_2061 GBV_ILN_2064 GBV_ILN_2065 GBV_ILN_2068 GBV_ILN_2111 GBV_ILN_2112 GBV_ILN_2113 GBV_ILN_2118 GBV_ILN_2122 GBV_ILN_2129 GBV_ILN_2143 GBV_ILN_2147 GBV_ILN_2148 GBV_ILN_2152 GBV_ILN_2153 GBV_ILN_2190 GBV_ILN_2336 GBV_ILN_2507 GBV_ILN_2522 GBV_ILN_4035 GBV_ILN_4037 GBV_ILN_4112 GBV_ILN_4125 GBV_ILN_4126 GBV_ILN_4242 GBV_ILN_4251 GBV_ILN_4305 GBV_ILN_4313 GBV_ILN_4323 GBV_ILN_4324 GBV_ILN_4325 GBV_ILN_4326 GBV_ILN_4333 GBV_ILN_4334 GBV_ILN_4335 GBV_ILN_4338 GBV_ILN_4393 58.10 Verfahrenstechnik: Allgemeines AR 370 782-791 045F 660.05 |
allfields_unstemmed |
10.1016/j.cej.2019.03.203 doi (DE-627)ELV002221179 (ELSEVIER)S1385-8947(19)30678-3 DE-627 ger DE-627 rda eng 660.05 DE-101 660 DE-101 660 DE-600 58.10 bkl Li, Xiang verfasserin aut Reduction of nitrogen-oxygen containing compounds (NOCs) by surface-associated Fe(II) and comparison with soluble Fe(II) complexes 2019 nicht spezifiziert zzz rdacontent Computermedien c rdamedia Online-Ressource cr rdacarrier Both Fe(II) adsorbed onto mineral surfaces and soluble Fe(II) complexes are important natural reductants; however, no research has directly compared their reaction kinetics and mechanisms. In this work, the reduction kinetics of heterogeneous Fe(II)-goethite versus homogeneous Fe(II)-tiron were compared for the first time toward thirteen structurally diverse nitrogen-oxygen containing compounds (NOCs). The reduction of NOCs followed pseudo-first-order reaction kinetics in Fe(II)-goethite, with the rate constant k varying over a wide range from 8.56 h−1 to <0.0001 h−1. In electrochemical experiments where NOCs were physically separated from Fe(II)-goethite, k of carbadox was 3.6 times greater than that of a structurally similar compound that cannot complex with surface Fe(II), while such difference in batch reactors was 531 times. Similar differences in the reactivity of NOCs between the two reactors were reported for Fe(II)-tiron. The good linear cross correlations between the reactivity of Fe(II)-goethite and that of Fe(II)-tiron toward NOCs, nitroaromatics, and polyhalogenated compounds (R2 = 0.76–0.94) can be used to predict the reactivity of other structurally related compounds by both reductants. On the basis of the FTIR and UV spectra, surface complexation was further inferred; both the amino functional groups and the pyridine ring were involved in the complexation, with the ring-N more strongly involved than the ring-O. As opposed to the large differences observed in the reactivity of the two Fe(II) reductants, similar reactivity was obtained when an outer-sphere reductant dithionite was employed. Overall, these results show that complexation between certain NOCs and surface-associated Fe(II) existed which facilitated the reduction reaction. Surface associated Fe(II) Nitrogen-oxygen containing compounds (NOCs) Reduction Surface complexation Soluble Fe(II) complexes Cross correlation Chen, Yiling verfasserin aut Zhang, Huichun verfasserin aut Enthalten in The chemical engineering journal Amsterdam : Elsevier, 1997 370, Seite 782-791 Online-Ressource (DE-627)320500322 (DE-600)2012137-4 (DE-576)098330152 1873-3212 nnns volume:370 pages:782-791 GBV_USEFLAG_U SYSFLAG_U GBV_ELV SSG-OLC-PHA GBV_ILN_20 GBV_ILN_22 GBV_ILN_23 GBV_ILN_24 GBV_ILN_31 GBV_ILN_32 GBV_ILN_40 GBV_ILN_60 GBV_ILN_62 GBV_ILN_63 GBV_ILN_65 GBV_ILN_69 GBV_ILN_70 GBV_ILN_73 GBV_ILN_74 GBV_ILN_90 GBV_ILN_95 GBV_ILN_100 GBV_ILN_105 GBV_ILN_110 GBV_ILN_150 GBV_ILN_151 GBV_ILN_224 GBV_ILN_370 GBV_ILN_602 GBV_ILN_702 GBV_ILN_2003 GBV_ILN_2004 GBV_ILN_2005 GBV_ILN_2011 GBV_ILN_2014 GBV_ILN_2015 GBV_ILN_2020 GBV_ILN_2021 GBV_ILN_2025 GBV_ILN_2027 GBV_ILN_2034 GBV_ILN_2038 GBV_ILN_2044 GBV_ILN_2048 GBV_ILN_2049 GBV_ILN_2050 GBV_ILN_2056 GBV_ILN_2059 GBV_ILN_2061 GBV_ILN_2064 GBV_ILN_2065 GBV_ILN_2068 GBV_ILN_2111 GBV_ILN_2112 GBV_ILN_2113 GBV_ILN_2118 GBV_ILN_2122 GBV_ILN_2129 GBV_ILN_2143 GBV_ILN_2147 GBV_ILN_2148 GBV_ILN_2152 GBV_ILN_2153 GBV_ILN_2190 GBV_ILN_2336 GBV_ILN_2507 GBV_ILN_2522 GBV_ILN_4035 GBV_ILN_4037 GBV_ILN_4112 GBV_ILN_4125 GBV_ILN_4126 GBV_ILN_4242 GBV_ILN_4251 GBV_ILN_4305 GBV_ILN_4313 GBV_ILN_4323 GBV_ILN_4324 GBV_ILN_4325 GBV_ILN_4326 GBV_ILN_4333 GBV_ILN_4334 GBV_ILN_4335 GBV_ILN_4338 GBV_ILN_4393 58.10 Verfahrenstechnik: Allgemeines AR 370 782-791 045F 660.05 |
allfieldsGer |
10.1016/j.cej.2019.03.203 doi (DE-627)ELV002221179 (ELSEVIER)S1385-8947(19)30678-3 DE-627 ger DE-627 rda eng 660.05 DE-101 660 DE-101 660 DE-600 58.10 bkl Li, Xiang verfasserin aut Reduction of nitrogen-oxygen containing compounds (NOCs) by surface-associated Fe(II) and comparison with soluble Fe(II) complexes 2019 nicht spezifiziert zzz rdacontent Computermedien c rdamedia Online-Ressource cr rdacarrier Both Fe(II) adsorbed onto mineral surfaces and soluble Fe(II) complexes are important natural reductants; however, no research has directly compared their reaction kinetics and mechanisms. In this work, the reduction kinetics of heterogeneous Fe(II)-goethite versus homogeneous Fe(II)-tiron were compared for the first time toward thirteen structurally diverse nitrogen-oxygen containing compounds (NOCs). The reduction of NOCs followed pseudo-first-order reaction kinetics in Fe(II)-goethite, with the rate constant k varying over a wide range from 8.56 h−1 to <0.0001 h−1. In electrochemical experiments where NOCs were physically separated from Fe(II)-goethite, k of carbadox was 3.6 times greater than that of a structurally similar compound that cannot complex with surface Fe(II), while such difference in batch reactors was 531 times. Similar differences in the reactivity of NOCs between the two reactors were reported for Fe(II)-tiron. The good linear cross correlations between the reactivity of Fe(II)-goethite and that of Fe(II)-tiron toward NOCs, nitroaromatics, and polyhalogenated compounds (R2 = 0.76–0.94) can be used to predict the reactivity of other structurally related compounds by both reductants. On the basis of the FTIR and UV spectra, surface complexation was further inferred; both the amino functional groups and the pyridine ring were involved in the complexation, with the ring-N more strongly involved than the ring-O. As opposed to the large differences observed in the reactivity of the two Fe(II) reductants, similar reactivity was obtained when an outer-sphere reductant dithionite was employed. Overall, these results show that complexation between certain NOCs and surface-associated Fe(II) existed which facilitated the reduction reaction. Surface associated Fe(II) Nitrogen-oxygen containing compounds (NOCs) Reduction Surface complexation Soluble Fe(II) complexes Cross correlation Chen, Yiling verfasserin aut Zhang, Huichun verfasserin aut Enthalten in The chemical engineering journal Amsterdam : Elsevier, 1997 370, Seite 782-791 Online-Ressource (DE-627)320500322 (DE-600)2012137-4 (DE-576)098330152 1873-3212 nnns volume:370 pages:782-791 GBV_USEFLAG_U SYSFLAG_U GBV_ELV SSG-OLC-PHA GBV_ILN_20 GBV_ILN_22 GBV_ILN_23 GBV_ILN_24 GBV_ILN_31 GBV_ILN_32 GBV_ILN_40 GBV_ILN_60 GBV_ILN_62 GBV_ILN_63 GBV_ILN_65 GBV_ILN_69 GBV_ILN_70 GBV_ILN_73 GBV_ILN_74 GBV_ILN_90 GBV_ILN_95 GBV_ILN_100 GBV_ILN_105 GBV_ILN_110 GBV_ILN_150 GBV_ILN_151 GBV_ILN_224 GBV_ILN_370 GBV_ILN_602 GBV_ILN_702 GBV_ILN_2003 GBV_ILN_2004 GBV_ILN_2005 GBV_ILN_2011 GBV_ILN_2014 GBV_ILN_2015 GBV_ILN_2020 GBV_ILN_2021 GBV_ILN_2025 GBV_ILN_2027 GBV_ILN_2034 GBV_ILN_2038 GBV_ILN_2044 GBV_ILN_2048 GBV_ILN_2049 GBV_ILN_2050 GBV_ILN_2056 GBV_ILN_2059 GBV_ILN_2061 GBV_ILN_2064 GBV_ILN_2065 GBV_ILN_2068 GBV_ILN_2111 GBV_ILN_2112 GBV_ILN_2113 GBV_ILN_2118 GBV_ILN_2122 GBV_ILN_2129 GBV_ILN_2143 GBV_ILN_2147 GBV_ILN_2148 GBV_ILN_2152 GBV_ILN_2153 GBV_ILN_2190 GBV_ILN_2336 GBV_ILN_2507 GBV_ILN_2522 GBV_ILN_4035 GBV_ILN_4037 GBV_ILN_4112 GBV_ILN_4125 GBV_ILN_4126 GBV_ILN_4242 GBV_ILN_4251 GBV_ILN_4305 GBV_ILN_4313 GBV_ILN_4323 GBV_ILN_4324 GBV_ILN_4325 GBV_ILN_4326 GBV_ILN_4333 GBV_ILN_4334 GBV_ILN_4335 GBV_ILN_4338 GBV_ILN_4393 58.10 Verfahrenstechnik: Allgemeines AR 370 782-791 045F 660.05 |
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10.1016/j.cej.2019.03.203 doi (DE-627)ELV002221179 (ELSEVIER)S1385-8947(19)30678-3 DE-627 ger DE-627 rda eng 660.05 DE-101 660 DE-101 660 DE-600 58.10 bkl Li, Xiang verfasserin aut Reduction of nitrogen-oxygen containing compounds (NOCs) by surface-associated Fe(II) and comparison with soluble Fe(II) complexes 2019 nicht spezifiziert zzz rdacontent Computermedien c rdamedia Online-Ressource cr rdacarrier Both Fe(II) adsorbed onto mineral surfaces and soluble Fe(II) complexes are important natural reductants; however, no research has directly compared their reaction kinetics and mechanisms. In this work, the reduction kinetics of heterogeneous Fe(II)-goethite versus homogeneous Fe(II)-tiron were compared for the first time toward thirteen structurally diverse nitrogen-oxygen containing compounds (NOCs). The reduction of NOCs followed pseudo-first-order reaction kinetics in Fe(II)-goethite, with the rate constant k varying over a wide range from 8.56 h−1 to <0.0001 h−1. In electrochemical experiments where NOCs were physically separated from Fe(II)-goethite, k of carbadox was 3.6 times greater than that of a structurally similar compound that cannot complex with surface Fe(II), while such difference in batch reactors was 531 times. Similar differences in the reactivity of NOCs between the two reactors were reported for Fe(II)-tiron. The good linear cross correlations between the reactivity of Fe(II)-goethite and that of Fe(II)-tiron toward NOCs, nitroaromatics, and polyhalogenated compounds (R2 = 0.76–0.94) can be used to predict the reactivity of other structurally related compounds by both reductants. On the basis of the FTIR and UV spectra, surface complexation was further inferred; both the amino functional groups and the pyridine ring were involved in the complexation, with the ring-N more strongly involved than the ring-O. As opposed to the large differences observed in the reactivity of the two Fe(II) reductants, similar reactivity was obtained when an outer-sphere reductant dithionite was employed. Overall, these results show that complexation between certain NOCs and surface-associated Fe(II) existed which facilitated the reduction reaction. Surface associated Fe(II) Nitrogen-oxygen containing compounds (NOCs) Reduction Surface complexation Soluble Fe(II) complexes Cross correlation Chen, Yiling verfasserin aut Zhang, Huichun verfasserin aut Enthalten in The chemical engineering journal Amsterdam : Elsevier, 1997 370, Seite 782-791 Online-Ressource (DE-627)320500322 (DE-600)2012137-4 (DE-576)098330152 1873-3212 nnns volume:370 pages:782-791 GBV_USEFLAG_U SYSFLAG_U GBV_ELV SSG-OLC-PHA GBV_ILN_20 GBV_ILN_22 GBV_ILN_23 GBV_ILN_24 GBV_ILN_31 GBV_ILN_32 GBV_ILN_40 GBV_ILN_60 GBV_ILN_62 GBV_ILN_63 GBV_ILN_65 GBV_ILN_69 GBV_ILN_70 GBV_ILN_73 GBV_ILN_74 GBV_ILN_90 GBV_ILN_95 GBV_ILN_100 GBV_ILN_105 GBV_ILN_110 GBV_ILN_150 GBV_ILN_151 GBV_ILN_224 GBV_ILN_370 GBV_ILN_602 GBV_ILN_702 GBV_ILN_2003 GBV_ILN_2004 GBV_ILN_2005 GBV_ILN_2011 GBV_ILN_2014 GBV_ILN_2015 GBV_ILN_2020 GBV_ILN_2021 GBV_ILN_2025 GBV_ILN_2027 GBV_ILN_2034 GBV_ILN_2038 GBV_ILN_2044 GBV_ILN_2048 GBV_ILN_2049 GBV_ILN_2050 GBV_ILN_2056 GBV_ILN_2059 GBV_ILN_2061 GBV_ILN_2064 GBV_ILN_2065 GBV_ILN_2068 GBV_ILN_2111 GBV_ILN_2112 GBV_ILN_2113 GBV_ILN_2118 GBV_ILN_2122 GBV_ILN_2129 GBV_ILN_2143 GBV_ILN_2147 GBV_ILN_2148 GBV_ILN_2152 GBV_ILN_2153 GBV_ILN_2190 GBV_ILN_2336 GBV_ILN_2507 GBV_ILN_2522 GBV_ILN_4035 GBV_ILN_4037 GBV_ILN_4112 GBV_ILN_4125 GBV_ILN_4126 GBV_ILN_4242 GBV_ILN_4251 GBV_ILN_4305 GBV_ILN_4313 GBV_ILN_4323 GBV_ILN_4324 GBV_ILN_4325 GBV_ILN_4326 GBV_ILN_4333 GBV_ILN_4334 GBV_ILN_4335 GBV_ILN_4338 GBV_ILN_4393 58.10 Verfahrenstechnik: Allgemeines AR 370 782-791 045F 660.05 |
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660.05 DE-101 660 DE-101 660 DE-600 58.10 bkl Reduction of nitrogen-oxygen containing compounds (NOCs) by surface-associated Fe(II) and comparison with soluble Fe(II) complexes Surface associated Fe(II) Nitrogen-oxygen containing compounds (NOCs) Reduction Surface complexation Soluble Fe(II) complexes Cross correlation |
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Reduction of nitrogen-oxygen containing compounds (NOCs) by surface-associated Fe(II) and comparison with soluble Fe(II) complexes |
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Reduction of nitrogen-oxygen containing compounds (NOCs) by surface-associated Fe(II) and comparison with soluble Fe(II) complexes |
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Li, Xiang |
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reduction of nitrogen-oxygen containing compounds (nocs) by surface-associated fe(ii) and comparison with soluble fe(ii) complexes |
title_auth |
Reduction of nitrogen-oxygen containing compounds (NOCs) by surface-associated Fe(II) and comparison with soluble Fe(II) complexes |
abstract |
Both Fe(II) adsorbed onto mineral surfaces and soluble Fe(II) complexes are important natural reductants; however, no research has directly compared their reaction kinetics and mechanisms. In this work, the reduction kinetics of heterogeneous Fe(II)-goethite versus homogeneous Fe(II)-tiron were compared for the first time toward thirteen structurally diverse nitrogen-oxygen containing compounds (NOCs). The reduction of NOCs followed pseudo-first-order reaction kinetics in Fe(II)-goethite, with the rate constant k varying over a wide range from 8.56 h−1 to <0.0001 h−1. In electrochemical experiments where NOCs were physically separated from Fe(II)-goethite, k of carbadox was 3.6 times greater than that of a structurally similar compound that cannot complex with surface Fe(II), while such difference in batch reactors was 531 times. Similar differences in the reactivity of NOCs between the two reactors were reported for Fe(II)-tiron. The good linear cross correlations between the reactivity of Fe(II)-goethite and that of Fe(II)-tiron toward NOCs, nitroaromatics, and polyhalogenated compounds (R2 = 0.76–0.94) can be used to predict the reactivity of other structurally related compounds by both reductants. On the basis of the FTIR and UV spectra, surface complexation was further inferred; both the amino functional groups and the pyridine ring were involved in the complexation, with the ring-N more strongly involved than the ring-O. As opposed to the large differences observed in the reactivity of the two Fe(II) reductants, similar reactivity was obtained when an outer-sphere reductant dithionite was employed. Overall, these results show that complexation between certain NOCs and surface-associated Fe(II) existed which facilitated the reduction reaction. |
abstractGer |
Both Fe(II) adsorbed onto mineral surfaces and soluble Fe(II) complexes are important natural reductants; however, no research has directly compared their reaction kinetics and mechanisms. In this work, the reduction kinetics of heterogeneous Fe(II)-goethite versus homogeneous Fe(II)-tiron were compared for the first time toward thirteen structurally diverse nitrogen-oxygen containing compounds (NOCs). The reduction of NOCs followed pseudo-first-order reaction kinetics in Fe(II)-goethite, with the rate constant k varying over a wide range from 8.56 h−1 to <0.0001 h−1. In electrochemical experiments where NOCs were physically separated from Fe(II)-goethite, k of carbadox was 3.6 times greater than that of a structurally similar compound that cannot complex with surface Fe(II), while such difference in batch reactors was 531 times. Similar differences in the reactivity of NOCs between the two reactors were reported for Fe(II)-tiron. The good linear cross correlations between the reactivity of Fe(II)-goethite and that of Fe(II)-tiron toward NOCs, nitroaromatics, and polyhalogenated compounds (R2 = 0.76–0.94) can be used to predict the reactivity of other structurally related compounds by both reductants. On the basis of the FTIR and UV spectra, surface complexation was further inferred; both the amino functional groups and the pyridine ring were involved in the complexation, with the ring-N more strongly involved than the ring-O. As opposed to the large differences observed in the reactivity of the two Fe(II) reductants, similar reactivity was obtained when an outer-sphere reductant dithionite was employed. Overall, these results show that complexation between certain NOCs and surface-associated Fe(II) existed which facilitated the reduction reaction. |
abstract_unstemmed |
Both Fe(II) adsorbed onto mineral surfaces and soluble Fe(II) complexes are important natural reductants; however, no research has directly compared their reaction kinetics and mechanisms. In this work, the reduction kinetics of heterogeneous Fe(II)-goethite versus homogeneous Fe(II)-tiron were compared for the first time toward thirteen structurally diverse nitrogen-oxygen containing compounds (NOCs). The reduction of NOCs followed pseudo-first-order reaction kinetics in Fe(II)-goethite, with the rate constant k varying over a wide range from 8.56 h−1 to <0.0001 h−1. In electrochemical experiments where NOCs were physically separated from Fe(II)-goethite, k of carbadox was 3.6 times greater than that of a structurally similar compound that cannot complex with surface Fe(II), while such difference in batch reactors was 531 times. Similar differences in the reactivity of NOCs between the two reactors were reported for Fe(II)-tiron. The good linear cross correlations between the reactivity of Fe(II)-goethite and that of Fe(II)-tiron toward NOCs, nitroaromatics, and polyhalogenated compounds (R2 = 0.76–0.94) can be used to predict the reactivity of other structurally related compounds by both reductants. On the basis of the FTIR and UV spectra, surface complexation was further inferred; both the amino functional groups and the pyridine ring were involved in the complexation, with the ring-N more strongly involved than the ring-O. As opposed to the large differences observed in the reactivity of the two Fe(II) reductants, similar reactivity was obtained when an outer-sphere reductant dithionite was employed. Overall, these results show that complexation between certain NOCs and surface-associated Fe(II) existed which facilitated the reduction reaction. |
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title_short |
Reduction of nitrogen-oxygen containing compounds (NOCs) by surface-associated Fe(II) and comparison with soluble Fe(II) complexes |
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