Manipulating p‐π Resonance through Methoxy Group Engineering in Covalent Organic Frameworks for an Efficient Photocatalytic Hydrogen Evolution DOI
Zhipeng Luo,

Shipeng Zhu,

Haizhou Xue

et al.

Angewandte Chemie, Journal Year: 2024, Volume and Issue: unknown

Published: Dec. 23, 2024

Abstract Kinetic factors frequently emerge as the primary constraints in photocatalysis, exerting a critical influence on efficacy of polymeric photocatalysts. The diverse conjugation systems within covalent organic frameworks (COFs) can significantly impact photon absorption, energy level structures, charge separation and migration kinetics. Consequently, these limitations often manifest unsatisfactory kinetic behavior, which adversely affects photocatalytic activity COFs. To address challenges, we propose methoxy (−OMe) molecular engineering strategy designed to enhance carrier kinetics mitigate mass transfer resistance. Through strategic modulation position quantity −OMe units, effectively manipulate p‐π conjugation, thereby enhancing migration. Moreover, COFs enriched with moieties exhibit enhanced dynamics due hydrophilic nature groups, facilitate diffusion reactants products porous structure. This approach is hypothesized drive an efficient hydrogen evolution reaction.

Language: Английский

Dual–Acceptor Engineering in Pyrene‐Based Covalent Organic Frameworks for Boosting Photocatalytic Hydrogen Evolution DOI

Nengyi Liu,

Shuailei Xie, Yuxing Huang

et al.

Advanced Energy Materials, Journal Year: 2024, Volume and Issue: 14(40)

Published: July 18, 2024

Abstract The integration of electron donor (D) and acceptor (A) units into covalent organic frameworks (COFs) has received increasing interest due to its potential for efficient photocatalytic hydrogen (H 2 ) evolution from water. Nevertheless, the advancement D–A COFs is still constrained by limited investigations on engineering, which enables highly effective charge transfer pathways in deliver photoexcited electrons a preferential orientation enhance performance. Herein, two systems with D–A–A configurations based molecular engineering strategy are proposed construct three distinct COFs. Specifically, TAPPy‐DBTDP‐COF merging one pyrene‐based benzothiadiazole acceptors realized an average H rate 12.7 mmol h −1 g under visible light, among highest ever reported typical D–A‐type COF systems. combination experimental theoretical analysis signifies crucial role dual‐acceptor arrangement promoting exciton dissociation carrier migration. These findings underscore significant structural design, conducive separation holes resulting superior activities.

Language: Английский

Citations

33
Programming Tetrathiafulvalene‐Based Covalent Organic Frameworks for Promoted Photoinduced Molecular Oxygen Activation DOI

Hetao Xu,

Shuling Xia,

Chunlei Li

et al.

Angewandte Chemie International Edition, Journal Year: 2024, Volume and Issue: 63(29)

Published: May 6, 2024

Abstract Despite the pivotal role of molecular oxygen (O 2 ) activation in artificial photosynthesis, efficiency is often restricted by sluggish exciton dissociation and charge transfer kinetics within polymer photocatalysts. Herein, we propose two tetrathiafulvalene (TTF)‐based imine‐linked covalent organic frameworks (COFs) with tailored donor‐acceptor (D–A) structures, TTF‐PDI‐COF TTF‐TFPP‐COF, to promote O activation. Because enhanced electron push‐pull interactions that facilitated separation behavior, exhibited superior photocatalytic activity electron‐induced reactions over TTF‐TFPP‐COF under visible light irradiation, including photosynthesis ( E )‐3‐amino‐2‐thiocyano‐ α , β ‐unsaturated compounds H . These findings highlight significant potential rational design COFs D–A configurations as suitable candidates for advanced applications.

Language: Английский

Citations

24
Covalent organic framework nanomaterials: Syntheses, architectures, and applications DOI
Qing Li, Yuanyuan Zhu,

Tao Pan

et al.

Advances in Colloid and Interface Science, Journal Year: 2025, Volume and Issue: 339, P. 103427 - 103427

Published: Feb. 6, 2025

Language: Английский

Citations

4
Thermally triggered topological polymerization in diacetylene-functionalized covalent organic framework toward enhanced memristive properties DOI
Pan‐Ke Zhou, Yuxing Huang, Ziyue Yu

et al.

Science China Chemistry, Journal Year: 2025, Volume and Issue: unknown

Published: Jan. 3, 2025

Language: Английский

Citations

2
Enhancing the performance of polyoxometalate-based memristors in harsh environments based on hydrogen bonding cooperative π-conjugation interaction DOI
Mingze Meng,

Yiqun Gao,

Yi‐Ping Chen

et al.

Inorganic Chemistry Frontiers, Journal Year: 2025, Volume and Issue: unknown

Published: Jan. 1, 2025

Three water-soluble organic–inorganic hybridized POMs-based memristor are proposed. The introduction of organic ligands improves its performance. mechanism the device during high temperature operation was explored using 2D-COS-IR.

Language: Английский

Citations

1
Electric Eels Inspired Iontronic Artificial Skin with Multimodal Perception and In‐Sensor Reservoir Computing DOI
Haiqing Pei,

Huiqian Hu,

Yu Dong

et al.

Advanced Functional Materials, Journal Year: 2025, Volume and Issue: unknown

Published: April 18, 2025

Abstract As the largest sensory organ, human skin generates ionic signals in response to tactile, thermal, and electrical stimuli, which are then transmitted neurons processed by brain, thereby enabling sensing memory, ultimately promoting conscious perception decision‐making. However, existing artificial skins face significant challenges including inability achieve multimodal memory simultaneously (i.e., stimuli), difficulty detecting ultra‐low currents, limitations rich synaptic behaviors that essential for highly efficient in‐sensor reservoir computing. Inspired electric eels, study here develops an based on iontronic p‐n junctions consisting of PolyAT PolyES bi‐layered structures. This features broad detection ranges temperature (−80 120 °C, well beyond reach hydrogel counterparties), pressure (0.075 Pa 400 kPa, among highest sensitivities ever reported), current (1–200 nA), meanwhile demonstrates functions. Additionally, incorporating a robotic hand can grasp objects with different temperatures weights demand. Further, fully memristive computing is implemented skin, allowing sensing, decoding, learning via stimulation, achieving 91.3% accuracy classifying MNIST handwritten digit images.

Language: Английский

Citations

1
2D photocatalysts for hydrogen peroxide synthesis DOI
Liyong Ding, Zhenhua Pan, Qian Wang

et al.

Chinese Chemical Letters, Journal Year: 2024, Volume and Issue: 35(12), P. 110125 - 110125

Published: June 18, 2024

Language: Английский

Citations

7
Engineering Titanium Dioxide/Titanocene-Polysulfide Interface for Flexible, Optical-Modulated, and Thermal-Tolerant Multilevel Memristor DOI
Pan‐Ke Zhou, Xi Lin,

Yiqun Gao

et al.

Nano Letters, Journal Year: 2025, Volume and Issue: unknown

Published: Feb. 7, 2025

Multifunctional memristors with a high memory density, low power consumption, flexibility, programmability, and environmental robustness are essential for next-generation memories. In this work, titanocene-polysulfide complex (Cp2TiS5) strong S···S interactions hydrogen bonds was synthesized integrated TiO2 to create novel Cu/TiO2/Cp2TiS5/Ag memristor. This device shows bipolar nonvolatile performance remarkable ON/OFF ratio (104.8), switching voltages (VSET, -0.16 V; VRESET, +0.15 V), consumption (2.7 × 10-4 μW). It exhibits multilevel behavior, optical modulation (VSET decreases from -1.35 -0.17 V decreasing irradiation wavelength), thermal tolerance (up 200 °C). The electron-rich Cp2TiS5 layer protects the Ag-CFs, while TiO2's oxygen vacancies unsaturated Ti atoms interact sulfur Cp2TiS5, lowering Schottky barrier facilitating charge transport. work offers promising opportunities in flexible memristive devices neuromorphic computing under extreme conditions.

Language: Английский

Citations

1
Reconfigurable Neuromorphic Computing Using Methyl-Engineered One-Dimensional Covalent Organic Framework Memristors DOI
Pan‐Ke Zhou, Ziyue Yu, Tao Zeng

et al.

Nano Letters, Journal Year: 2025, Volume and Issue: unknown

Published: March 25, 2025

The rapid evolution of neuromorphic devices seeks to bridge biological neural networks and artificial systems, enabling energy-efficient scalable computing for next-generation intelligence. Herein, we introduce methyl-engineered one-dimensional covalent organic framework (1D COF)-based memristors as a transformative platform reconfigurable computing. incorporation methyl groups enhances localized polarization effects within the COF framework, effectively mitigating random Ag+ migration/diffusion stabilizing conductive filament morphology. This strategic modification yields with exceptional multilevel storage capabilities, exhibiting superior stability, linearity, reproducibility. Moreover, highly ordered architecture customizable chemical environment methyl-functionalized 1D allows precise control over resistive switching behaviors, facilitating emulation synaptic functions development network architectures. Demonstrating performance in tasks such high-accuracy image recognition, these showcase significant promise foundation energy-efficient, systems.

Language: Английский

Citations

1
Programming Tetrathiafulvalene‐Based Covalent Organic Frameworks for Promoted Photoinduced Molecular Oxygen Activation DOI

Hetao Xu,

Shuling Xia,

Chunlei Li

et al.

Angewandte Chemie, Journal Year: 2024, Volume and Issue: 136(29)

Published: May 6, 2024

Abstract Despite the pivotal role of molecular oxygen (O 2 ) activation in artificial photosynthesis, efficiency is often restricted by sluggish exciton dissociation and charge transfer kinetics within polymer photocatalysts. Herein, we propose two tetrathiafulvalene (TTF)‐based imine‐linked covalent organic frameworks (COFs) with tailored donor‐acceptor (D–A) structures, TTF‐PDI‐COF TTF‐TFPP‐COF, to promote O activation. Because enhanced electron push‐pull interactions that facilitated separation behavior, exhibited superior photocatalytic activity electron‐induced reactions over TTF‐TFPP‐COF under visible light irradiation, including photosynthesis ( E )‐3‐amino‐2‐thiocyano‐ α , β ‐unsaturated compounds H . These findings highlight significant potential rational design COFs D–A configurations as suitable candidates for advanced applications.

Language: Английский

Citations

5