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研究分野エンジニアリング化学工学電気化学エネルギー貯蔵と変換
高効率の光触媒のための共性有機フレームワークのスタッキング構成の溶媒駆動精密制御

高効率の光触媒のための共性有機フレームワークのスタッキング構成の溶媒駆動精密制御

Yixue Xu ^1,2, Fan Qiu ^1,2, Yubin Fu ^3,4, Shun-Feng Li ³, Xing Su ³, Kunquan Hong ⁵, Mei-Mei Zhang ⁶, Xin Zhao ^3,7, Yuqiao Wang ^1,2, Shun-Qi Xu ³

Yixue Xu ^1,2, Fan Qiu ^1,2, Yubin Fu ^3,4

¹Research Center for Nano Photoelectrochemistry and Devices, School of Chemistry and Chemical Engineering, Southeast University, Nanjing, 211189, China.
²Yangtze River Delta Carbon Neutrality Strategy Development Institute, Southeast University, Nanjing, 210096, China.
³School of Energy and Environment, Southeast University, Nanjing, 211189, China.
⁴Center for Advancing Electronics Dresden (cfaed) & Faculty of Chemistry, Food Chemistry, Technische Universität Dresden, 01062, Dresden, Germany.
⁵School of Physics, Southeast University, Nanjing, 211189, China.
⁶The Institute for Advanced Studies, Wuhan University, Wuhan, 430072, China.
⁷State Key Laboratory of Organometallic Chemistry, Shanghai Institute of Organic Chemistry, Chinese Academy of Sciences, Shanghai, 200032, China.

⁰Research Center for Nano Photoelectrochemistry and Devices, School of Chemistry and Chemical Engineering, Southeast University, Nanjing, 211189, China.

Angewandte Chemie +

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2025年8月30日

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PubMedで要約を見る

まとめ

この要約は機械生成です。

研究者は,よりよい光触媒化のために,2D COF のスタッキングを制御するための新しい方法を開発しました. ABC-スタックされたCOF-TD-ABCはAA-スタックされたCOF-TD-AAよりも水素の進化率が著しく高かった.

科学分野

材料科学
キャタリシス
ナノテクノロジー

背景

二次元共性有機フレームワーク (2D COF) は,表面積と調節性特性により,光触媒として大きな可能性を秘めている.
2D COFにおける層間堆積の制御は,電荷輸送と触媒効率の最適化に不可欠ですが,依然として重要な課題です.

研究の目的

金属組み込み2DCOFのインターレイヤーのスタッキング構成を精密に制御するための溶剤駆動戦略を開発する.
異なるスタッキング構成 (AAが遮蔽され,ABCが散らばる) が,特に水素の進化に対して,光触媒性能に与える影響を調査する.

主な方法

1-ブタノールを使用した溶剤駆動戦略を使用して,協調相互作用を調節し,金属組み込み2DCOFで特定のAA (COF-TD-AA) とABC (COF-TD-ABC) スタッキング構成を達成しました.
COF-TD-AAとCOF-TD-ABCの両方をPt共触媒と組み合わせて,光触媒の水素進化率を測定した.

主要な成果

ABCを積み重ねたCOF-TD-ABCは,COF-TD-AAと比較して,光吸収と優れた電荷移動/分離効率を示した.
COF-TD-ABCは,COF-TD-AA (3.12 mmol g−1 h−1) よりも約3. 5倍高い高い水素進化率を達成しました.

結論

2D COFのインターレイヤーのスタッキングの正確な制御は,その光触媒活性に大きな影響を及ぼします.
開発された溶媒駆動戦略は,充電ダイナミクスを改善するためにスタッキング構成を調整することによって,高性能のCOFベースの光触媒を設計するための経路を提供します.

キーワード:

協和有機フレームワーク光触媒水素進化反応溶剤による合成スタッキング・モジュレーション構造と資産の関係

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関連する概念動画

Thermal and Photochemical Electrocyclic Reactions: Overview

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Electrocyclic reactions are reversible reactions. They involve an intramolecular cyclization or ring-opening of a conjugated polyene. Shown below are two examples of electrocyclic reactions. In the first reaction, the formation of the cyclic product is favored. In contrast, in the second reaction, ring-opening is favored due to the high ring strain associated with cyclobutene formation.

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The absorption of UV–visible light by conjugated systems causes the promotion of an electron from the ground state to the excited state. Consequently, photochemical electrocyclic reactions proceed via the excited-state HOMO rather than the ground-state HOMO. Since the ground- and excited-state HOMOs have different symmetries, the stereochemical outcome of electrocyclic reactions depends on the mode of activation; i.e., thermal or photochemical.
Selection Rules: Photochemical Activation

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