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Keto-enamine-based covalent organic framework with controllable anthraquinone moieties for superior H2O2 photosynthesis from O2 and water
Chemical Engineering Journal ( IF 13.3 ) Pub Date : 2023-04-23 , DOI: 10.1016/j.cej.2023.143085
Xiangcheng Zhang , Jingzhen Zhang , Jie Miao , Xue Wen , Chao Chen , Baoxue Zhou , Mingce Long
Chemical Engineering Journal ( IF 13.3 ) Pub Date : 2023-04-23 , DOI: 10.1016/j.cej.2023.143085
Xiangcheng Zhang , Jingzhen Zhang , Jie Miao , Xue Wen , Chao Chen , Baoxue Zhou , Mingce Long
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Photocatalytic HO production is a promising strategy for decentralized applications, but to realize efficient HO production in the ambient conditions and absence of organic sacrifice remains challengeable. Herein, anthraquinone functionalized covalent organic frameworks (TpAQ-COFs) were fabricated by β-ketoenamines links of 2,6-diaminoanthraquinone (AQ) and 2, 4, 6-triformylphloroglucinol (Tp), and the structures and compositions were tuned by controlling the condensation time. The increase of time favors the assembly of TpAQ-COFs into more ordered lamellar stacking structure, and induces the increase of enol-imine form. The critical role of anthraquinone moieties as the active sites for oxygen reduction was proved, that is, facilitating charge separation and enhancing the activity and selectivity of HO production. Upon visible light irradiation, the TpAQ-COF synthesized after 12 h reaction has the highest content of anthraquinone moieties and the best performance for HO production (420 μmol h g) in the absence of organic sacrificial agents. These findings bring insights to incorporate anthraquinone chemistry into photocatalysts at molecular levels for efficient HO production.
中文翻译:
具有可控蒽醌部分的基于酮烯胺的共价有机框架,可实现 O2 和水的卓越 H2O2 光合作用
光催化 H2O 生产对于分散式应用来说是一种有前途的策略,但在环境条件下实现高效 H2O 生产且不存在有机牺牲仍然具有挑战性。在此,通过2,6-二氨基蒽醌(AQ)和2,4,6-三甲酰基间苯三酚(Tp)的β-酮烯胺连接制备了蒽醌功能化共价有机骨架(TpAQ-COFs),并通过控制凝结时间。时间的增加有利于TpAQ-COFs组装成更有序的层状堆叠结构,并诱导烯醇亚胺形式的增加。蒽醌部分作为氧还原活性位点的关键作用被证明,即促进电荷分离并提高 H2O 生产的活性和选择性。在可见光照射下,反应12小时后合成的TpAQ-COF在没有有机牺牲剂的情况下具有最高的蒽醌部分含量和最佳的H2O生产性能(420 μmol hg)。这些发现为将蒽醌化学成分在分子水平上融入光催化剂中以高效生产 H2O 提供了见解。
更新日期:2023-04-23
中文翻译:
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具有可控蒽醌部分的基于酮烯胺的共价有机框架,可实现 O2 和水的卓越 H2O2 光合作用
光催化 H2O 生产对于分散式应用来说是一种有前途的策略,但在环境条件下实现高效 H2O 生产且不存在有机牺牲仍然具有挑战性。在此,通过2,6-二氨基蒽醌(AQ)和2,4,6-三甲酰基间苯三酚(Tp)的β-酮烯胺连接制备了蒽醌功能化共价有机骨架(TpAQ-COFs),并通过控制凝结时间。时间的增加有利于TpAQ-COFs组装成更有序的层状堆叠结构,并诱导烯醇亚胺形式的增加。蒽醌部分作为氧还原活性位点的关键作用被证明,即促进电荷分离并提高 H2O 生产的活性和选择性。在可见光照射下,反应12小时后合成的TpAQ-COF在没有有机牺牲剂的情况下具有最高的蒽醌部分含量和最佳的H2O生产性能(420 μmol hg)。这些发现为将蒽醌化学成分在分子水平上融入光催化剂中以高效生产 H2O 提供了见解。