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Cited by 29

The DOI matches its Crossref record; 46 of the 46 references it cites were found in a registry or an index.

An Eco‐Friendly, Tunable and Scalable Method for Producing Porous Functional Nanomaterials Designed Using Molecular Interactions

Manning, Joseph R. H., Yip, Thomas W. S., Centi, Alessia, Jorge, Miguel, Patwardhan, Siddharth V.·2017·ChemSusChem
DOI 10.1002/cssc.201700027PMC PMC5434938
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Abstract

Despite significant improvements in the synthesis of templated silica materials, post‐synthesis purification remains highly expensive and renders the materials industrially unviable. In this study this issue is addressed for porous bioinspired silica by developing a rapid room‐temperature solution method for complete extraction of organic additives. Using elemental analysis and N 2 and CO 2 adsorption, the ability to both purify and controllably tailor the composition, porosity and surface chemistry of bioinspired silica in a single step is demonstrated. For the first time the extraction is modelled using molecular dynamics, revealing that the removal mechanism is dominated by surface‐charge interactions. This is extended to other additive chemistry, leading to a wider applicability of the method to other materials. Finally the environmental benefits of the new method are estimated and compared with previous purification techniques, demonstrating significant improvements in sustainability.

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Crossref · 10.1002/cssc.201700027

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Figures

Figure 1 Graph of additive concentration in silica versus acidification pH value determined by elemental analysis for both PEHA and DETA.
Figure 1 Graph of additive concentration in silica versus acidification pH value determined by elemental analysis for both PEHA and DETA.CC BY · PubMed Central
Figure 2 Total and microporous surface area of silica produced using PEHA as measured by t‐plot (microporous data offset for clarity), with overlay lines at 30 and 300 m2 g−1.
Figure 2 Total and microporous surface area of silica produced using PEHA as measured by t‐plot (microporous data offset for clarity), with overlay lines at 30 and 300 m2 g−1.CC BY · PubMed Central
Figure 3 SEM images of PEHA‐silica before (top) and after (bottom) acid treatment, showing no observable change in morphology. Scale bars are 500 nm.
Figure 3 SEM images of PEHA‐silica before (top) and after (bottom) acid treatment, showing no observable change in morphology. Scale bars are 500 nm.CC BY · PubMed Central
Figure 4 Calculated additive volume removed (squares) and measured micropore volume created from additive removal (circles) against treatment pH value.
Figure 4 Calculated additive volume removed (squares) and measured micropore volume created from additive removal (circles) against treatment pH value.CC BY · PubMed Central
Figure 5 Effect of treatment method on surface area: U=untreated; WR=water reflux; C=calcined; A=acid treated; A+C=acid treated then calcined.
Figure 5 Effect of treatment method on surface area: U=untreated; WR=water reflux; C=calcined; A=acid treated; A+C=acid treated then calcined.CC BY · PubMed Central
Figure 6 MD simulations depicting (a) interaction between one PEHA amine group and a surface siloxide ion at pH≈7, (b) PEHA desorption after surface neutralisation at pH≈2 and (c) continued adsorption of methyl‐substituted PEHA to silica at pH 2 owing to strong hydrophobic interactions.
Figure 6 MD simulations depicting (a) interaction between one PEHA amine group and a surface siloxide ion at pH≈7, (b) PEHA desorption after surface neutralisation at pH≈2 and (c) continued adsorption of methyl‐substituted PEHA to silica at pH 2 owing to strong hydrophobic interactions.CC BY · PubMed Central
Figure 7 Comparison of additive removal effectiveness between poly(ethyleneimine) (PEI) and methyl‐substituted poly(ethyleneimine) (QPEI), showing 25 % decrease in effectiveness when using QPEI.
Figure 7 Comparison of additive removal effectiveness between poly(ethyleneimine) (PEI) and methyl‐substituted poly(ethyleneimine) (QPEI), showing 25 % decrease in effectiveness when using QPEI.CC BY · PubMed Central
Figure 8 Simulated PEHA–siloxide ion interaction strengths, normalised against availability of precursor ions.
Figure 8 Simulated PEHA–siloxide ion interaction strengths, normalised against availability of precursor ions.CC BY · PubMed Central
Figure 9 Proposed distribution of additive molecules (red lines) within secondary particles of bioinspired silica (dotted lines), which are composed of primary particles (grey circles). (a) Untreated silica composites contain additives adsorbed to both the particle surface and inside. (b) After partial treatment to pH 5, only the surface‐adsorbed additive molecules are released. (c) After treatment at pH 2, all additive molecules are released.
Figure 9 Proposed distribution of additive molecules (red lines) within secondary particles of bioinspired silica (dotted lines), which are composed of primary particles (grey circles). (a) Untreated silica composites contain additives adsorbed to both the particle surface and inside. (b) After partial treatment to pH 5, only the surface‐adsorbed additive molecules are released. (c) After treatment at pH 2, all additive molecules are released.CC BY · PubMed Central
Figure 10 (a) Partial uptake curves at 100 mbar CO2 for bioinspired silica treated at different pH values. Data collected prior to pressure stabilisation have been omitted for clarity. (b) Comparison of CO2 adsorption half‐times (circles) and equilibrium adsorbed amount (squares) estimated from kinetic‐modelling results.
Figure 10 (a) Partial uptake curves at 100 mbar CO2 for bioinspired silica treated at different pH values. Data collected prior to pressure stabilisation have been omitted for clarity. (b) Comparison of CO2 adsorption half‐times (circles) and equilibrium adsorbed amount (squares) estimated from kinetic‐modelling results.CC BY · PubMed Central

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Citations

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Research works printed but not linked: 1

  1. 10.1007/978-1-4899-2070-6 · DOI

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Metadata

Authors
Manning, J. R. H., Yip, T. W. S., Centi, A., Jorge, M., & Patwardhan, S. V.
Venue
ChemSusChem
Publisher
Wiley
Published
2017-03-29
Volume
10
Issue
8
Pages
1683-1691
ISSN
  • 1864-5631
  • 1864-564X
DOI
10.1002/cssc.201700027
PMC
PMC5434938
Cited by
29
References
46
Language
en
Licence
creativecommons.org/licenses/by/4.0/ (vor)
Funders
Engineering and Physical Sciences Research Council (EP/L014297/1, EP/L017059/1, EP/J019704/2, EP/K031260/1, EP/K000586/1)

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