Two-Dimensional Covalent Heptazine-Based Framework Enables Highly Photocatalytic Performance for Overall Water Splitting,Advanced Science

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Two-Dimensional Covalent Heptazine-Based Framework Enables Highly Photocatalytic Performance for Overall Water Splitting
Advanced Science ( IF 14.3 ) Pub Date : 2022-08-10 , DOI: 10.1002/advs.202202417
Yingnan Zhao ₁ , Cong Wang ₂ , Xingqi Han ₁ , Zhongling Lang ₃ , Congcong Zhao ₁ , Liying Yin ₁ , Huiying Sun ₁ , Likai Yan ₁ , Hongda Ren ₁ , Huaqiao Tan _{1,

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Affiliation

Screening high-efficiency 2D conjugated polymers toward visible-light-driven overall water splitting (OWS) is one of the most promising but challenging research directions to realize solar-to-hydrogen (STH) energy conversion and storage. “Mystery molecule” heptazine is an intriguing hydrogen evolution reaction (HER) building block. By covalently linking with the electron-rich alkynyl and phenyl oxygen evolution reaction (OER) active units, 10 experimentally feasible 2D covalent heptazine-based frameworks (CHFs) are constructed and screened four promising visible-light-driven OWS photocatalysts, which are linked by p-phenyl (CHF-4), p-phenylenediynyl (CHF-7), m-phenylenediynyl (CHF-8), and phenyltriynyl (CHF-9), respectively. Their HER and OER active sites achieve completely spatially separated, where HER active sites focus on heptazine units and OER active sites located on alkynyl or phenyl units. Their lower overpotentials allow them to spontaneously trigger the surface OWS reaction under their own light-induced bias without using any sacrificial agents and cocatalysts. Among them, CHF-7 shows the best photocatalytic performance with an ideal STH energy conversion efficiency estimated at 12.04%, indicating that it is a promising photocatalyst for industrial OWS. This work not only provides an innovative idea for the exploration of novel polymer photocatalysts for OWS but also supplies a direction for the development of heptazine derivatives.

中文翻译：

二维共价七嗪基框架可实现整体水分解的高光催化性能

筛选用于可见光驱动的整体水分解（OWS）的高效二维共轭聚合物是实现太阳能到氢（STH）能量转换和存储的最有前途但最具挑战性的研究方向之一。 “神秘分子”庚嗪是一种有趣的析氢反应 (HER) 结构单元。通过与富电子的炔基和苯基析氧反应（OER）活性单元共价连接，构建了10个实验上可行的二维共价庚嗪基框架（CHF），并筛选了四种有前途的可见光驱动的OWS光催化剂，它们通过以下方式连接分别为对苯基(CHF-4)、对苯二炔基(CHF-7)、间苯二炔基(CHF-8)和苯基三炔基(CHF-9)。它们的HER和OER活性位点实现了完全空间分离，其中HER活性位点集中在庚嗪单元上，OER活性位点位于炔基或苯基单元上。它们较低的过电势使它们能够在自己的光诱导偏压下自发触发表面 OWS 反应，而无需使用任何牺牲剂和助催化剂。其中，CHF-7表现出最好的光催化性能，理想的STH能量转换效率估计为12.04%，表明它是一种有前途的工业OWS光催化剂。该工作不仅为OWS新型聚合物光催化剂的探索提供了创新思路，也为庚嗪衍生物的开发提供了方向。

更新日期：2022-08-10

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