Alkali and donor–acceptor bridged three-dimensional interpenetrating polymer networks boost photocatalytic performance by efficient electron delocalization and charge transfer

Li, Shuqi; Jin, Zhiquan; Lai, Weishun; Zhang, Haiyan; Da, Wang; Song, Shuang

doi:10.1016/j.apcatb.2021.120153

Cited by 23 publications

(7 citation statements)

References 41 publications

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“…28 Another emerging peak was observed at 2225 cm −1 in CTF-SDs corresponding to the asymmetric stretching of −CN groups, whose intensity gradually increased with increasing dosage of NaBH 4 . 17 These results verified that defect reconstruction, namely, collaborative −CN exposure and B doping, in the configuration of CTF was successfully achieved via thermal decomposition with the NaBH 4 approach.…”

Section: ■ Results and Discussionsupporting

confidence: 66%

“…The peak at 810 cm –1 and absorptions in the region of 1300–1670 cm –1 should be ascribed to the out-of-plane bending vibration of triazine rings and the stretching modes of aromatic C–N heterocycles, respectively, which confirmed the presence of triazine rings. , Compared with the pristine CTF, CTF-SDs displayed new absorption bands at 1180 and 1100 cm –1 , corresponding to the stretching modes of the B–C bond . Another emerging peak was observed at 2225 cm –1 in CTF-SDs corresponding to the asymmetric stretching of −CN groups, whose intensity gradually increased with increasing dosage of NaBH 4 . These results verified that defect reconstruction, namely, collaborative −CN exposure and B doping, in the configuration of CTF was successfully achieved via thermal decomposition with the NaBH 4 approach.…”

Section: Resultsmentioning

confidence: 94%

“…The introduction of structural defects into a conjugated polymer plane has recently been adopted as an efficient strategy for boosting the photocatalytic activity under visible light illumination. Our previous studies found that the incorporation of cyano-based defect sites enlarged the degree of π-delocalization of conjugated CTFs, , leading to not only a modulated band structure but also a redshift of the maximum adsorption wavelength for improved light-harvesting ability. More interestingly, cyano defects in CTFs are expected to serve as artificial defect accumulation sites to withdraw electrons from excitons so as to minimize the exciton binding energy and prompt charge separation, analogous to the action of nicotinamide adenine dinucleotide phosphate (NADPH) or adenosine triphosphate (ATP) in the natural photosynthesis system.…”

Section: Introductionmentioning

confidence: 99%

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Covalent Triazine Frameworks with Defective Accumulation Sites: Exceptionally Modulated Electronic Structure for Solar-Driven Oxidative Activation of Peroxymonosulfate

Zeng

Jin

et al. 2022

Environ. Sci. Technol.

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Precisely tailoring the electronic structure and surface chemistry of metal-free covalent triazine frameworks (CTFs) for efficient photoactivation of oxyanions is environmentally desirable but still challenging. Of interest to us in this work was to construct artificial defective accumulation sites into a CTF network (CTF-SD x ) to synchronously modulate both thermodynamic (e.g., band structure) and kinetic (e.g., charge separation/transfer/utilization and surface adsorption) behaviors and probe how the transformation affected the subsequent activation mechanism of peroxymonosulfate (PMS). With the incorporation of terminal cyano (−CN) groups and boron (B) dopants, the delocalized CTF-SD underwent a narrowed electronic energy gap for increased optical absorption as well as a downshifted valence band position for enhanced oxidation capacity. Moreover, the localized charge accumulation regions induced by the electron-withdrawing −CN groups facilitated the exciton dissociation process, while the adjacent electron-deficient areas enabled strong affinity toward PMS molecules. All of these merits impelled the photoactivation reaction with PMS, and a 15-fold enhancement of bisphenol-A (BPA) removal was found in the CTF-SD2/PMS/vis system compared with the corresponding pristine CTF system. Mechanistic investigations demonstrated that this system decomposed organics primarily through a singlet oxygen-mediated nonradical process, which originated from PMS oxidative activation over photoinduced holes initiated by an electron transfer process, thereby opening a new avenue for designing an efficient PMS activation strategy for the selective oxidation of organic pollutants.

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Section: ■ Results and Discussionsupporting

confidence: 66%

Section: Resultsmentioning

confidence: 94%

Section: Introductionmentioning

confidence: 99%

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Covalent Triazine Frameworks with Defective Accumulation Sites: Exceptionally Modulated Electronic Structure for Solar-Driven Oxidative Activation of Peroxymonosulfate

Zeng

Jin

et al. 2022

Environ. Sci. Technol.

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“…On the other hand, the inclusion of Nb nanoparticles in the structure of the device lowers the contact resistance between the metal and the active layer, resulting in a reduction in the device’s series resistance. By minimizing carrier aggregation in the interface, decreasing the series resistance boosts the current density and power conversion efficiency of the device [ 55 , 56 ].…”

Section: Resultsmentioning

confidence: 99%

Doping with Niobium Nanoparticles as an Approach to Increase the Power Conversion Efficiency of P3HT:PCBM Polymer Solar Cells

et al. 2023

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Metal additive processing in polymer: fullerene bulk heterojunction systems is recognized as a viable way for improving polymer photovoltage performance. In this study, the effect of niobium (Nb) metal nanoparticles at concentrations of 2, 4, 6, and 8 mg/mL on poly(3-hexylthiophene-2,5-diyl) (P3HT)-6,6]-phenyl C61-butyric acid methyl ester (PCBM) blends was analyzed. The effect of Nb volume concentration on polymer crystallinity, optical properties, and surface structure of P3HT and PCBM, as well as the enhancement of the performance of P3HT:PC61BM solar cells, are investigated. Absorption of the P3HT:PC61BM mix is seen to have a high intensity and a red shift at 500 nm. The reduction in PL intensity with increasing Nb doping concentrations indicates an increase in PL quenching, suggesting that the domain size of P3HT or conjugation length increases. With a high Nb concentration, crystallinity, material composition, surface roughness, and phase separation are enhanced. Nb enhances PCBM’s solubility in P3HT and decreases the size of amorphous P3HT domains. Based on the J–V characteristics and the optoelectronic study of the thin films, the improvement results from a decreased recombination current, changes in morphology and crystallinity, and an increase in the effective exciton lifespan. At high doping concentrations of Nb nanoparticles, the development of the short-circuit current (JSC) is associated with alterations in the crystalline structure of P3HT. The highest-performing glass/ITO/PEDOT:PSS/P3HT:PCBM:Nb/MoO3/Au structures have short-circuit current densities (JSC) of 16.86 mA/cm2, open-circuit voltages (VOC) of 466 mV, fill factors (FF) of 65.73%, and power conversion efficiency (µ) of 5.16%.

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“…Moreover, O@CF had less flat band edges as compared to COF and O@C, confirming its enhanced delocalized orbitals. [26] Particularly, O@CF possessed a very close conduction band edge (CBM) and valence band edge (VBM), which further account for its narrow-band gap structure and enhanced electron transfer capability. Additionally, DFT calculations revealed the spatial distributions of photoexcited holes and electrons in O@CF.…”

Section: Resultsmentioning

confidence: 99%

Engineering Carbon Nanotube‐Based Photoactive COF to Synergistically Arm a Multifunctional Antibacterial Hydrogel

Lin,

Zhang,

et al. 2023

Adv Funct Materials

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Enhancing the covalent organic framework (COF)’s photocatalytic ability synergistically with gelling formulations remains an urgent challenge for extended bio‐applications. Herein, COF is homogeneously coated on an oxidized carbon nanotube (OCNT) and coordinated by Fe3+ to obtain tubular nanocomplex OCNT@COF‐Fe (O@CF). The results showed that the photodynamic reactive oxygen species (ROS) generation ability of O@CF is enhanced due to the wrapped OCNT and the coordinated Fe3+, which can respectively serve as intermolecular charge transfer channel and electron acceptors/substrates (O2 and H2O) adsorbent to narrow the energy band gaps, increase the light absorption, and decrease the photogenerated carrier recombination. Synergistically, O@CF exhibited pH‐dependent peroxidase and catalase activities, which further enhanced ROS generation and relieved hypoxia, respectively. Meanwhile, O@CF possessed degradation of COF coatings‐dependent photothermal performances. Then, O@CF is evenly incorporated into Schiff base hydrogel via the COF coating‐participated covalent cross‐linking, to obtain an electroconductive hydrogel OCNT@COF‐Fe@Gel (O@CF@G). This O@CF@G can not only improve the mechanical properties of pure gel but also inherit the multifunction of O@CF. Consequently, it can well adhere to diabetic wounds for imbibition, drug‐resistant biofilm elimination, gram‐positive and negative bacteria killing, hypoxia alleviation, and intercellular electrical signal conduction, thus accelerating wound healing.

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Alkali and donor–acceptor bridged three-dimensional interpenetrating polymer networks boost photocatalytic performance by efficient electron delocalization and charge transfer

Cited by 23 publications

References 41 publications

Covalent Triazine Frameworks with Defective Accumulation Sites: Exceptionally Modulated Electronic Structure for Solar-Driven Oxidative Activation of Peroxymonosulfate

Covalent Triazine Frameworks with Defective Accumulation Sites: Exceptionally Modulated Electronic Structure for Solar-Driven Oxidative Activation of Peroxymonosulfate

Doping with Niobium Nanoparticles as an Approach to Increase the Power Conversion Efficiency of P3HT:PCBM Polymer Solar Cells

Engineering Carbon Nanotube‐Based Photoactive COF to Synergistically Arm a Multifunctional Antibacterial Hydrogel

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