Overall solar H2O2 generation in water and real seawater by covalent organic frameworks with kgd topology.
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| Title: | Overall solar H2O2 generation in water and real seawater by covalent organic frameworks with kgd topology. |
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| Authors: | Yue, Jie-Yu1 (AUTHOR) yuejieyu@sdnu.edu.cn, Song, Li-Ping1 (AUTHOR), Pan, Zi-Xian1 (AUTHOR), Cheng, Min2 (AUTHOR), Wang, Xuan2 (AUTHOR), Xu, Qing1,3 (AUTHOR) xuqing@sari.ac.cn, Yang, Peng1 (AUTHOR) yangpeng@sdnu.edu.cn |
| Source: | Chemical Engineering Journal. Jan2025, Vol. 504, pN.PAG-N.PAG. 1p. |
| Subjects: | Oxidation-reduction reaction, Escherichia coli, Activation energy, Oxidation of water, Oxygen reduction |
| Abstract: | Two innovative covalent organic frameworks (COFs) with kgd topology are constructed for photocatalytic H 2 O 2 formation for the first time, realizing overall H 2 O 2 generation in water and real seawater with high production rates via the oxygen reduction reaction and the water oxidation reaction among the best COF-based photocatalysts, inspiring the photocatalytic performance modulation by topology design. [Display omitted] • Two novel COFs with kgd topology (TPT-COF and TPB-COF) were constructed for H 2 O 2 generation for the first time. • In pure water and real seawater, TPT-COF and TPB-COF exhibited superior H 2 O 2 generation rates, among the best organic photocatalysts, manifesting a potential sustainable blueprint for making H 2 O 2. • Experimental and theoretical investigations proved that TPT-COF and TPB-COF can drive the overall solar H 2 O 2 generation via O 2 -O 2 −-H 2 O 2 , O 2 -O 2 −-O 2 1-H 2 O 2 , and H 2 O-H 2 O 2 three pathways. • The seawater-produced H 2 O 2 can be utilized for E. coli sterilization, providing a guide for the sustainable use of seawater for high-value chemical production. Applying covalent organic frameworks (COFs) for photosynthesizing H 2 O 2 has garnered significant research interest due to their customizable structures and functions. Nevertheless, there is still much room to tailor the structures of COFs to achieve high H 2 O 2 yields, fulfilling the future industrial requirements for massive and green H 2 O 2 generation. Herein, by topology design, we fabricate two novel COFs with kgd topology for H 2 O 2 production. In pure water and O 2 , the non-sacrificial H 2 O 2 evolution rates of TPT-COF and TPB-COF are 5903 and 7874 μmol g−1h−1 (4006 and 5696 μmol g−1h−1 in real seawater), outperforming their counterparts with hcb topology, ranking ahead of COF-based photocatalysts. Thorough experimental and computational inspections corroborate the indirect 2e− oxygen reduction and direct 2e− water oxidation paths of TPT-COF and TPB-COF for overall H 2 O 2 photogeneration. The boosted charge carrier separation, easier adsorption of O 2 and water, and lower energy barriers of the formation of *OOH and *OH intermediates in TPB-COF make it a superior photocatalyst for producing H 2 O 2 than TPT-COF. This is the first time COFs with kgd topology are constructed towards H 2 O 2 synthesis, inspiring the photocatalytic performance modulation by topology design. Additionally, the seawater-produced H 2 O 2 can be exploited for sterilization, enlightening a blueprint for sustainable utilizing seawater for high-value chemicals. [ABSTRACT FROM AUTHOR] |
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| Database: | Engineering Source |
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