Fulvic Acid-Mediated Interfacial Reactions on Exposed Hematite Facets during Dissimilatory Iron Reduction

Hu, Shiwen; Wu, Yundang; Li, Fangbai; Shi, Zhenqing; Ma, Chao

doi:10.1021/acs.langmuir.1c00124

Cited by 21 publications

(19 citation statements)

References 75 publications

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“…For example, Gardea-Torresdey and coworkers have studied the impacts of metal oxide nanoparticles on plant health and nutritional value. − Optimizing nanoparticles for adsorption , or dissolution , reactions requires knowledge of the interfacial chemistry at each face of the particle as well as control of the synthesis of nanoparticle habits during nucleation . Hence, improving our molecular-level information about complex nanoparticulate surface-solution chemistries will enable improving agricultural productivity by optimal time-release of nutrients and soil resilience by increasing retention of soil organic carbon.…”

Section: Introductionmentioning

confidence: 99%

Oxide– and Silicate–Water Interfaces and Their Roles in Technology and the Environment

et al. 2023

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Interfacial reactions drive all elemental cycling on Earth and play pivotal roles in human activities such as agriculture, water purification, energy production and storage, environmental contaminant remediation, and nuclear waste repository management. The onset of the 21st century marked the beginning of a more detailed understanding of mineral aqueous interfaces enabled by advances in techniques that use tunable high-flux focused ultrafast laser and X-ray sources to provide near-atomic measurement resolution, as well as by nanofabrication approaches that enable transmission electron microscopy in a liquid cell. This leap into atomic-and nanometer-scale measurements has uncovered scale-dependent phenomena whose reaction thermodynamics, kinetics, and pathways deviate from previous observations made on larger systems. A second key advance is new experimental evidence for what scientists hypothesized but could not test previously, namely, interfacial chemical reactions are frequently driven by "anomalies" or "non-idealities" such as defects, nanoconfinement, and other nontypical chemical structures. Third, progress in computational chemistry has yielded new insights that allow a move beyond simple schematics, leading to a molecular model of these complex interfaces. In combination with surfacesensitive measurements, we have gained knowledge of the interfacial structure and dynamics, including the underlying solid surface and the immediately adjacent water and aqueous ions, enabling a better definition of what constitutes the oxide− and silicate−water interfaces. This critical review discusses how science progresses from understanding ideal solid−water interfaces to more realistic systems, focusing on accomplishments in the last 20 years and identifying challenges and future opportunities for the community to address. We anticipate that the next 20 years will focus on understanding and predicting dynamic transient and reactive structures over greater spatial and temporal ranges as well as systems of greater structural and chemical complexity. Closer collaborations of theoretical and experimental experts across disciplines will continue to be critical to achieving this great aspiration.

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Section: Introductionmentioning

confidence: 99%

Oxide– and Silicate–Water Interfaces and Their Roles in Technology and the Environment

et al. 2023

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“…Additionally, the spectra of dry goethite samples revealed how dehydration altered the molecular scale speciation of coexisting PA and silicate species. These observations are not only directly relevant to soils undergoing wet−dry cycling but also add further insight into the ever-growing literature 42,26,[43][44][45][46][47][48][49]27 on molecular-scale phenomena driving carboxylate-bearing organic ligand adsorption to mineral surfaces.…”

Section: Introductionmentioning

confidence: 59%

“…Of note, the relative importance of these species is affected by pH (MB at low and HB/OS at high pH), ionic strength (MB at high and HB/OS at low ionic strength), as well as the interplay of mineral surface and ligand structures. Fundamental surface science studies on low molecular weight carboxylic acids, which are the focus of this work, have been particularly beneficial along this front. − …”

Section: Introductionmentioning

confidence: 99%

Competitive Carboxylate–Silicate Binding at Iron Oxyhydroxide Surfaces

et al. 2021

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Dissolved silicate ions in wet and dry soils can determine the fate of organic contaminants via competitive binding. While fundamental surface science studies have advanced knowledge of binding in competitive systems, little is still known about the ranges of solution conditions, the time dependence, and the molecular processes controlling competitive silicate–organic binding on minerals. Here we address these issues by describing the competitive adsorption of dissolved silicate and of phthalic acid (PA), a model carboxylate-bearing organic contaminant, onto goethite, a representative natural iron oxyhydroxide nanomineral. Using surface complexation thermodynamic modeling of batch adsorption data and chemometric analyses of vibrational spectra, we find that silicate concentrations representative of natural waters (50–1000 μM) can displace PA bound at goethite surfaces. Below pH ∼8, where PA binds, every bound Si atom removes ∼0.3 PA molecule by competing with reactive singly coordinated hydroxo groups (−OH) on goethite. Long-term (30 days) reaction time and a high silicate concentration (1000 μM) favored silicate polymer formation, and increased silicate while decreasing PA loadings. The multisite complexation model predicted PA and silicate binding in terms of the competition for −OH groups without involving PA/silicate interactions, and in terms of a lowering of outer-Helmholtz potentials of the goethite surface by these anions. The model predicted that silicate binding lowered loadings of PA species, and whose two carboxylate groups are hydrogen- (HB) and metal-bonded (MB) with goethite. Vibrational spectra of dried samples revealed that the loss of water favored greater proportions of MB over HB species, and these coexisted with predominantly monomeric silicate species. These findings underscored the need to develop models for a wider range of organic contaminants in soils exposed to silicate species and undergoing wet–dry cycles.

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“…The physicochemical properties of metal sulfides, such as size, 28 surface defects, 29 and exposed facets, 30 are important factors affecting their surface reactions. Recent studies found that the facet-dependent interactions of biogenic or natural NPs, including dissolution, 29,30 crystallization, 31,32 redoxreaction, 33 fractionation, 34 and microbial transformation, 35 played an important role in various biogeochemical processes. In the anaerobic environment, microbes mediated the formation of CdS, and these CdS particles synthesized by different microorganisms consistently showed nano-size and spherical morphology.…”

Section: Environmental Significancementioning

confidence: 99%

Facet-specific cation exchange and heterogeneous transformation of cadmium sulfide nanoparticles induced by Cu(ii)

Huang

Liu

Cui

et al. 2023

Environ. Sci.: Nano

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Fulvic Acid-Mediated Interfacial Reactions on Exposed Hematite Facets during Dissimilatory Iron Reduction

Cited by 21 publications

References 75 publications

Oxide– and Silicate–Water Interfaces and Their Roles in Technology and the Environment

Oxide– and Silicate–Water Interfaces and Their Roles in Technology and the Environment

Competitive Carboxylate–Silicate Binding at Iron Oxyhydroxide Surfaces

Facet-specific cation exchange and heterogeneous transformation of cadmium sulfide nanoparticles induced by Cu(ii)

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