Mechanosynthesis of a Structurally Characterized, Well‐Defined Graphitic Phosphorus‐Linked Carbon Nitride (g‐PCN) with Water Splitting Activity
Abstract Graphitic phosphorus‐linked triazine networks (g‐PCNs) are an emergent class of carbon nitride materials that have attracted attention for their potential role in developing metal‐free water splitting photocatalysts, but remain difficult to access due to complicated synthetic procedures bas...
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| Format: | Article |
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Wiley-VCH
2022-12-01
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| Series: | Advanced Materials Interfaces |
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| Online Access: | https://doi.org/10.1002/admi.202201555 |
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| author | Blaine G. Fiss Georgia Douglas Michael Ferguson Jorge Becerra Jesus Valdez Trong‐On Do Tomislav Friščić Audrey Moores |
| author_facet | Blaine G. Fiss Georgia Douglas Michael Ferguson Jorge Becerra Jesus Valdez Trong‐On Do Tomislav Friščić Audrey Moores |
| author_sort | Blaine G. Fiss |
| collection | DOAJ |
| description | Abstract Graphitic phosphorus‐linked triazine networks (g‐PCNs) are an emergent class of carbon nitride materials that have attracted attention for their potential role in developing metal‐free water splitting photocatalysts, but remain difficult to access due to complicated synthetic procedures based on long reaction times, high‐temperature annealing (above 500 °C), and poor structural understanding. Here, a mild, lower temperature approach for the synthesis of catalytically active g‐PCN through combining a room‐temperature mechanochemical reaction of sodium phosphide and cyanuric chloride with only 1 h annealing at 300 °C is presented. Notably, this mechanosynthesized material is sufficiently ordered to permit unprecedented structural characterization of a g‐PCN layered solid by combining solid‐state magic angle spinning, nuclear magnetic resonance spectroscopy, X‐ray photoelectron spectroscopy, powder X‐ray diffraction (PXRD), and transmission electron microscopy, supported by dispersion‐corrected density functional theory modeling. The excellent match of experimental 31P MAS NMR and PXRD data with modeling of the structure based on phosphorus‐linked triazine network layers makes the herein described mechanochemically synthesized material the first example of a photocatalytically active, as well as structurally characterized, g‐PCN. |
| format | Article |
| id | doaj-art-a8a0669aa85847dbb7af3e754a6e1a31 |
| institution | Matheson Library |
| issn | 2196-7350 |
| language | English |
| publishDate | 2022-12-01 |
| publisher | Wiley-VCH |
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| series | Advanced Materials Interfaces |
| spelling | doaj-art-a8a0669aa85847dbb7af3e754a6e1a312025-07-04T08:30:18ZengWiley-VCHAdvanced Materials Interfaces2196-73502022-12-01935n/an/a10.1002/admi.202201555Mechanosynthesis of a Structurally Characterized, Well‐Defined Graphitic Phosphorus‐Linked Carbon Nitride (g‐PCN) with Water Splitting ActivityBlaine G. Fiss0Georgia Douglas1Michael Ferguson2Jorge Becerra3Jesus Valdez4Trong‐On Do5Tomislav Friščić6Audrey Moores7Centre in Green Chemistry and Catalysis Department of Chemistry McGill University 801 Sherbrooke Street West Montréal Québec H3A 0B8 CanadaCentre in Green Chemistry and Catalysis Department of Chemistry McGill University 801 Sherbrooke Street West Montréal Québec H3A 0B8 CanadaCentre in Green Chemistry and Catalysis Department of Chemistry McGill University 801 Sherbrooke Street West Montréal Québec H3A 0B8 CanadaDepartment of Chemical Engineering Laval University Québec City Québec G1V 0A6 CanadaFacility for Electron Microscopy Research (FEMR) McGill University Montréal Montréal Québec H3A 0C7 CanadaDepartment of Chemical Engineering Laval University Québec City Québec G1V 0A6 CanadaCentre in Green Chemistry and Catalysis Department of Chemistry McGill University 801 Sherbrooke Street West Montréal Québec H3A 0B8 CanadaCentre in Green Chemistry and Catalysis Department of Chemistry McGill University 801 Sherbrooke Street West Montréal Québec H3A 0B8 CanadaAbstract Graphitic phosphorus‐linked triazine networks (g‐PCNs) are an emergent class of carbon nitride materials that have attracted attention for their potential role in developing metal‐free water splitting photocatalysts, but remain difficult to access due to complicated synthetic procedures based on long reaction times, high‐temperature annealing (above 500 °C), and poor structural understanding. Here, a mild, lower temperature approach for the synthesis of catalytically active g‐PCN through combining a room‐temperature mechanochemical reaction of sodium phosphide and cyanuric chloride with only 1 h annealing at 300 °C is presented. Notably, this mechanosynthesized material is sufficiently ordered to permit unprecedented structural characterization of a g‐PCN layered solid by combining solid‐state magic angle spinning, nuclear magnetic resonance spectroscopy, X‐ray photoelectron spectroscopy, powder X‐ray diffraction (PXRD), and transmission electron microscopy, supported by dispersion‐corrected density functional theory modeling. The excellent match of experimental 31P MAS NMR and PXRD data with modeling of the structure based on phosphorus‐linked triazine network layers makes the herein described mechanochemically synthesized material the first example of a photocatalytically active, as well as structurally characterized, g‐PCN.https://doi.org/10.1002/admi.202201555carbon nitridedensity functional theoryhydrogen evolutionmechanochemistryphosphorus |
| spellingShingle | Blaine G. Fiss Georgia Douglas Michael Ferguson Jorge Becerra Jesus Valdez Trong‐On Do Tomislav Friščić Audrey Moores Mechanosynthesis of a Structurally Characterized, Well‐Defined Graphitic Phosphorus‐Linked Carbon Nitride (g‐PCN) with Water Splitting Activity Advanced Materials Interfaces carbon nitride density functional theory hydrogen evolution mechanochemistry phosphorus |
| title | Mechanosynthesis of a Structurally Characterized, Well‐Defined Graphitic Phosphorus‐Linked Carbon Nitride (g‐PCN) with Water Splitting Activity |
| title_full | Mechanosynthesis of a Structurally Characterized, Well‐Defined Graphitic Phosphorus‐Linked Carbon Nitride (g‐PCN) with Water Splitting Activity |
| title_fullStr | Mechanosynthesis of a Structurally Characterized, Well‐Defined Graphitic Phosphorus‐Linked Carbon Nitride (g‐PCN) with Water Splitting Activity |
| title_full_unstemmed | Mechanosynthesis of a Structurally Characterized, Well‐Defined Graphitic Phosphorus‐Linked Carbon Nitride (g‐PCN) with Water Splitting Activity |
| title_short | Mechanosynthesis of a Structurally Characterized, Well‐Defined Graphitic Phosphorus‐Linked Carbon Nitride (g‐PCN) with Water Splitting Activity |
| title_sort | mechanosynthesis of a structurally characterized well defined graphitic phosphorus linked carbon nitride g pcn with water splitting activity |
| topic | carbon nitride density functional theory hydrogen evolution mechanochemistry phosphorus |
| url | https://doi.org/10.1002/admi.202201555 |
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