Dissolution, Adsorption, and Redox Reaction in Ternary Mixtures of Goethite, Aluminum Oxides, and Hydroquinone

Huichun Zhang; Kowsalya Devi Rasamani; Shifa Zhong; Saru Taujale; Laura R. Baratta; Zijie Yang

doi:10.1021/acs.jpcc.8b12217

Dissolution, Adsorption, and Redox Reaction in Ternary Mixtures of Goethite, Aluminum Oxides, and Hydroquinone

Huichun Zhang^*
, Kowsalya Devi Rasamani
, Shifa Zhong
, Saru Taujale
, Laura R. Baratta
, Zijie Yang

^*Corresponding author for this work

Case Western Reserve University
Temple University

Research output: Contribution to journal › Article › peer-review

6 Scopus citations

Abstract

To better understand the oxidative reactivity of iron oxides in the fate of contaminants in acidic environments, we examined the reactivity of goethite in binary mixtures with Al ₂ O ₃ by carrying out oxidation experiments of hydroquinone (HQ) in the presence of goethite and/or Al ₂ O ₃ at pH 3. Kinetic results revealed inhibiting effects of 0.2-20 g/L of three different types of Al ₂ O ₃ on the oxidative reactivity of goethite. Surprisingly, soluble Al ions of 0.18-18 mM had a negligible impact on the reactivity. It turned out that the Fe ³⁺ dissolved from goethite partly contributed to the observed HQ oxidation and the Al ₂ O ₃ adsorbed the Fe ³⁺ to lead to the slower HQ oxidation. The observed pseudo-first-order rate constants in HQ oxidation had a strong linear correlation with Fe ³⁺ concentration in various goethite and Al ₂ O ₃ mixtures. Separate experiments confirmed the reactivity of Fe ³⁺ toward HQ and the linear correlation between [Fe ³⁺ ] and HQ oxidation reactivity. Finally, sedimentation experiments showed negligible heteroaggregation between goethite and AluC-Al ₂ O ₃ or nAl ₂ O ₃ but intensive heteroaggregation between goethite and Alu 65-Al ₂ O ₃ , which explained the observed highest inhibition effect of Alu 65. Overall, oxide mixtures are very complex whose reactivity is determined by many factors such as oxide dissolution.

Original language	English
Pages (from-to)	4371-4379
Number of pages	9
Journal	Journal of Physical Chemistry C
Volume	123
Issue number	7
DOIs	https://doi.org/10.1021/acs.jpcc.8b12217
State	Published - 21 Feb 2019
Externally published	Yes

Access to Document

10.1021/acs.jpcc.8b12217

Cite this

@article{d580fb68f4cc416e8fcb0fe6331b8468,

title = "Dissolution, Adsorption, and Redox Reaction in Ternary Mixtures of Goethite, Aluminum Oxides, and Hydroquinone",

abstract = " To better understand the oxidative reactivity of iron oxides in the fate of contaminants in acidic environments, we examined the reactivity of goethite in binary mixtures with Al 2 O 3 by carrying out oxidation experiments of hydroquinone (HQ) in the presence of goethite and/or Al 2 O 3 at pH 3. Kinetic results revealed inhibiting effects of 0.2-20 g/L of three different types of Al 2 O 3 on the oxidative reactivity of goethite. Surprisingly, soluble Al ions of 0.18-18 mM had a negligible impact on the reactivity. It turned out that the Fe 3+ dissolved from goethite partly contributed to the observed HQ oxidation and the Al 2 O 3 adsorbed the Fe 3+ to lead to the slower HQ oxidation. The observed pseudo-first-order rate constants in HQ oxidation had a strong linear correlation with Fe 3+ concentration in various goethite and Al 2 O 3 mixtures. Separate experiments confirmed the reactivity of Fe 3+ toward HQ and the linear correlation between [Fe 3+ ] and HQ oxidation reactivity. Finally, sedimentation experiments showed negligible heteroaggregation between goethite and AluC-Al 2 O 3 or nAl 2 O 3 but intensive heteroaggregation between goethite and Alu 65-Al 2 O 3 , which explained the observed highest inhibition effect of Alu 65. Overall, oxide mixtures are very complex whose reactivity is determined by many factors such as oxide dissolution.",

author = "Huichun Zhang and Rasamani, \{Kowsalya Devi\} and Shifa Zhong and Saru Taujale and Baratta, \{Laura R.\} and Zijie Yang",

year = "2019",

month = feb,

day = "21",

doi = "10.1021/acs.jpcc.8b12217",

language = "英语",

volume = "123",

pages = "4371--4379",

journal = "Journal of Physical Chemistry C",

issn = "1932-7447",

publisher = "American Chemical Society",

number = "7",

}

TY - JOUR

T1 - Dissolution, Adsorption, and Redox Reaction in Ternary Mixtures of Goethite, Aluminum Oxides, and Hydroquinone

AU - Zhang, Huichun

AU - Rasamani, Kowsalya Devi

AU - Zhong, Shifa

AU - Taujale, Saru

AU - Baratta, Laura R.

AU - Yang, Zijie

PY - 2019/2/21

Y1 - 2019/2/21

N2 - To better understand the oxidative reactivity of iron oxides in the fate of contaminants in acidic environments, we examined the reactivity of goethite in binary mixtures with Al 2 O 3 by carrying out oxidation experiments of hydroquinone (HQ) in the presence of goethite and/or Al 2 O 3 at pH 3. Kinetic results revealed inhibiting effects of 0.2-20 g/L of three different types of Al 2 O 3 on the oxidative reactivity of goethite. Surprisingly, soluble Al ions of 0.18-18 mM had a negligible impact on the reactivity. It turned out that the Fe 3+ dissolved from goethite partly contributed to the observed HQ oxidation and the Al 2 O 3 adsorbed the Fe 3+ to lead to the slower HQ oxidation. The observed pseudo-first-order rate constants in HQ oxidation had a strong linear correlation with Fe 3+ concentration in various goethite and Al 2 O 3 mixtures. Separate experiments confirmed the reactivity of Fe 3+ toward HQ and the linear correlation between [Fe 3+ ] and HQ oxidation reactivity. Finally, sedimentation experiments showed negligible heteroaggregation between goethite and AluC-Al 2 O 3 or nAl 2 O 3 but intensive heteroaggregation between goethite and Alu 65-Al 2 O 3 , which explained the observed highest inhibition effect of Alu 65. Overall, oxide mixtures are very complex whose reactivity is determined by many factors such as oxide dissolution.

AB - To better understand the oxidative reactivity of iron oxides in the fate of contaminants in acidic environments, we examined the reactivity of goethite in binary mixtures with Al 2 O 3 by carrying out oxidation experiments of hydroquinone (HQ) in the presence of goethite and/or Al 2 O 3 at pH 3. Kinetic results revealed inhibiting effects of 0.2-20 g/L of three different types of Al 2 O 3 on the oxidative reactivity of goethite. Surprisingly, soluble Al ions of 0.18-18 mM had a negligible impact on the reactivity. It turned out that the Fe 3+ dissolved from goethite partly contributed to the observed HQ oxidation and the Al 2 O 3 adsorbed the Fe 3+ to lead to the slower HQ oxidation. The observed pseudo-first-order rate constants in HQ oxidation had a strong linear correlation with Fe 3+ concentration in various goethite and Al 2 O 3 mixtures. Separate experiments confirmed the reactivity of Fe 3+ toward HQ and the linear correlation between [Fe 3+ ] and HQ oxidation reactivity. Finally, sedimentation experiments showed negligible heteroaggregation between goethite and AluC-Al 2 O 3 or nAl 2 O 3 but intensive heteroaggregation between goethite and Alu 65-Al 2 O 3 , which explained the observed highest inhibition effect of Alu 65. Overall, oxide mixtures are very complex whose reactivity is determined by many factors such as oxide dissolution.

UR - https://www.scopus.com/pages/publications/85062211539

U2 - 10.1021/acs.jpcc.8b12217

DO - 10.1021/acs.jpcc.8b12217

M3 - 文章

AN - SCOPUS:85062211539

SN - 1932-7447

VL - 123

SP - 4371

EP - 4379

JO - Journal of Physical Chemistry C

JF - Journal of Physical Chemistry C

IS - 7

ER -

Dissolution, Adsorption, and Redox Reaction in Ternary Mixtures of Goethite, Aluminum Oxides, and Hydroquinone

Abstract

Access to Document

Other files and links

Fingerprint

Cite this