Photocatalytic proton reduction by a computationally identified, molecular hydrogen-bonded framework
We show that a hydrogen-bonded framework, TBAP -α, with extended π-stacked pyrene columns has a sacrificial photocatalytic hydrogen production rate of up to 3108 μmol g −1 h −1 . This is the highest activity reported for a molecular organic crystal. By comparison, a chemically-identical but amorphou...
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| Published in | Journal of materials chemistry. A, Materials for energy and sustainability Vol. 8; no. 15; pp. 7158 - 717 |
|---|---|
| Main Authors | , , , , , , , , , , , , , |
| Format | Journal Article |
| Language | English |
| Published |
Cambridge
Royal Society of Chemistry
2020
|
| Subjects | |
| Online Access | Get full text |
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| Abstract | We show that a hydrogen-bonded framework,
TBAP
-α, with extended π-stacked pyrene columns has a sacrificial photocatalytic hydrogen production rate of up to 3108 μmol g
−1
h
−1
. This is the highest activity reported for a molecular organic crystal. By comparison, a chemically-identical but amorphous sample of
TBAP
was 20-200 times less active, depending on the reaction conditions, showing unambiguously that crystal packing in molecular crystals can dictate photocatalytic activity. Crystal structure prediction (CSP) was used to predict the solid-state structure of
TBAP
and other functionalised, conformationally-flexible pyrene derivatives. Specifically, we show that energy-structure-function (ESF) maps can be used to identify molecules such as
TBAP
that are likely to form extended π-stacked columns in the solid state. This opens up a methodology for the
a priori
computational design of molecular organic photocatalysts and other energy-relevant materials, such as organic electronics.
A hydrogen-bonded organic framework is an effective photocatalyst for producing hydrogen from water. Its crystal structure is key to its activity; a chemically identical, amorphous version is almost inactive, as rationalized by crystal structure prediction. |
|---|---|
| AbstractList | We show that a hydrogen-bonded framework, TBAP-α, with extended π-stacked pyrene columns has a sacrificial photocatalytic hydrogen production rate of up to 3108 μmol g−1 h−1. This is the highest activity reported for a molecular organic crystal. By comparison, a chemically-identical but amorphous sample of TBAP was 20–200 times less active, depending on the reaction conditions, showing unambiguously that crystal packing in molecular crystals can dictate photocatalytic activity. Crystal structure prediction (CSP) was used to predict the solid-state structure of TBAP and other functionalised, conformationally-flexible pyrene derivatives. Specifically, we show that energy–structure–function (ESF) maps can be used to identify molecules such as TBAP that are likely to form extended π-stacked columns in the solid state. This opens up a methodology for the a priori computational design of molecular organic photocatalysts and other energy-relevant materials, such as organic electronics. We show that a hydrogen-bonded framework, TBAP-α, with extended π-stacked pyrene columns has a sacrificial photocatalytic hydrogen production rate of up to 3108 μmol g⁻¹ h⁻¹. This is the highest activity reported for a molecular organic crystal. By comparison, a chemically-identical but amorphous sample of TBAP was 20–200 times less active, depending on the reaction conditions, showing unambiguously that crystal packing in molecular crystals can dictate photocatalytic activity. Crystal structure prediction (CSP) was used to predict the solid-state structure of TBAP and other functionalised, conformationally-flexible pyrene derivatives. Specifically, we show that energy–structure–function (ESF) maps can be used to identify molecules such as TBAP that are likely to form extended π-stacked columns in the solid state. This opens up a methodology for the a priori computational design of molecular organic photocatalysts and other energy-relevant materials, such as organic electronics. We show that a hydrogen-bonded framework, TBAP -α, with extended π-stacked pyrene columns has a sacrificial photocatalytic hydrogen production rate of up to 3108 μmol g −1 h −1 . This is the highest activity reported for a molecular organic crystal. By comparison, a chemically-identical but amorphous sample of TBAP was 20-200 times less active, depending on the reaction conditions, showing unambiguously that crystal packing in molecular crystals can dictate photocatalytic activity. Crystal structure prediction (CSP) was used to predict the solid-state structure of TBAP and other functionalised, conformationally-flexible pyrene derivatives. Specifically, we show that energy-structure-function (ESF) maps can be used to identify molecules such as TBAP that are likely to form extended π-stacked columns in the solid state. This opens up a methodology for the a priori computational design of molecular organic photocatalysts and other energy-relevant materials, such as organic electronics. A hydrogen-bonded organic framework is an effective photocatalyst for producing hydrogen from water. Its crystal structure is key to its activity; a chemically identical, amorphous version is almost inactive, as rationalized by crystal structure prediction. We show that a hydrogen-bonded framework, TBAP -α, with extended π-stacked pyrene columns has a sacrificial photocatalytic hydrogen production rate of up to 3108 μmol g −1 h −1 . This is the highest activity reported for a molecular organic crystal. By comparison, a chemically-identical but amorphous sample of TBAP was 20–200 times less active, depending on the reaction conditions, showing unambiguously that crystal packing in molecular crystals can dictate photocatalytic activity. Crystal structure prediction (CSP) was used to predict the solid-state structure of TBAP and other functionalised, conformationally-flexible pyrene derivatives. Specifically, we show that energy–structure–function (ESF) maps can be used to identify molecules such as TBAP that are likely to form extended π-stacked columns in the solid state. This opens up a methodology for the a priori computational design of molecular organic photocatalysts and other energy-relevant materials, such as organic electronics. |
| Author | Day, Graeme M Pulido, Angeles Wilbraham, Liam Sprick, Reiner Sebastian Spackman, Peter R McMahon, David P Little, Marc A Aitchison, Catherine M Clowes, Rob Zwijnenburg, Martijn A Cooper, Andrew I Kane, Christopher M Wang, Xiaoyan Chen, Linjiang |
| AuthorAffiliation | University of Liverpool Department of Chemistry Leverhulme Research Centre for Functional Materials Design University of Southampton Department of Chemistry and Materials Innovation Factory Computational Systems Chemistry University College London School of Chemistry |
| AuthorAffiliation_xml | – name: Department of Chemistry and Materials Innovation Factory – name: University of Liverpool – name: University of Southampton – name: Computational Systems Chemistry – name: Department of Chemistry – name: Leverhulme Research Centre for Functional Materials Design – name: School of Chemistry – name: University College London |
| Author_xml | – sequence: 1 givenname: Catherine M surname: Aitchison fullname: Aitchison, Catherine M – sequence: 2 givenname: Christopher M surname: Kane fullname: Kane, Christopher M – sequence: 3 givenname: David P surname: McMahon fullname: McMahon, David P – sequence: 4 givenname: Peter R surname: Spackman fullname: Spackman, Peter R – sequence: 5 givenname: Angeles surname: Pulido fullname: Pulido, Angeles – sequence: 6 givenname: Xiaoyan surname: Wang fullname: Wang, Xiaoyan – sequence: 7 givenname: Liam surname: Wilbraham fullname: Wilbraham, Liam – sequence: 8 givenname: Linjiang surname: Chen fullname: Chen, Linjiang – sequence: 9 givenname: Rob surname: Clowes fullname: Clowes, Rob – sequence: 10 givenname: Martijn A surname: Zwijnenburg fullname: Zwijnenburg, Martijn A – sequence: 11 givenname: Reiner Sebastian surname: Sprick fullname: Sprick, Reiner Sebastian – sequence: 12 givenname: Marc A surname: Little fullname: Little, Marc A – sequence: 13 givenname: Graeme M surname: Day fullname: Day, Graeme M – sequence: 14 givenname: Andrew I surname: Cooper fullname: Cooper, Andrew I |
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| Copyright | Copyright Royal Society of Chemistry 2020 |
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| Snippet | We show that a hydrogen-bonded framework,
TBAP
-α, with extended π-stacked pyrene columns has a sacrificial photocatalytic hydrogen production rate of up to... We show that a hydrogen-bonded framework, TBAP-α, with extended π-stacked pyrene columns has a sacrificial photocatalytic hydrogen production rate of up to... |
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| SubjectTerms | Catalytic activity Chemical bonds Computer applications Crystal structure Crystallography Crystals electronics Hydrogen Hydrogen bonding Hydrogen production Organic crystals Photocatalysis photocatalysts prediction Pyrene Solid state Structure-function relationships |
| Title | Photocatalytic proton reduction by a computationally identified, molecular hydrogen-bonded framework |
| URI | https://www.proquest.com/docview/2389266989 https://www.proquest.com/docview/2439434877 https://urn.kb.se/resolve?urn=urn:nbn:se:liu:diva-209146 |
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