Organogel Polymer Electrocatalysts for Two‐Electron Oxygen Reduction DOI Open Access
Lili Li, Binbin Wang,

Hongni Chen

et al.

Small, Journal Year: 2024, Volume and Issue: unknown

Published: Dec. 20, 2024

Polymer gels, renowned for unparalleled chemical stability and self-sustaining properties, have garnered significant attention in electrocatalysis. Notably, organic polymer gels that exhibit temperature sensitivity incorporate suitable polar nonvolatile liquids, enhance electronic conductivity, impart distinct morphological features, but remain largely unexplored as electrocatalysts oxygen reduction reaction (ORR). To address this issue, an innovative strategy is proposed synergistic modulation of the rigidity mainchain molecular skeleton length alkyl sidechains, enabling development organogel polymers with a sol-gel temperature-sensitive phase transition promises high selectivity enhanced activity electrocatalytic processes. shortening sidechain can significantly affect gelation behavior internal microstructure catalyst, which modifies electron state, ultimately impacting catalytic gel catalysts. In particular, phenyl-containing Ph-FL1 short sidechains demonstrates outstanding 2e

Language: Английский

Host-guest-induced electronic state triggers two-electron oxygen reduction electrocatalysis DOI Creative Commons

Hongni Chen,

Chao Wang,

Han Wu

et al.

Nature Communications, Journal Year: 2024, Volume and Issue: 15(1)

Published: Oct. 25, 2024

Supramolecular polymers possess great potential in catalysis owing to their distinctive molecular recognition and dynamic crosslinking features. However, investigating supramolecular electrocatalysts with high efficiency oxygen reduction reaction hydrogen peroxide (ORHP) remains an unexplored frontier. Herein, we present organic for ORHP by introducing cyclodextrin-containing noncovalent building blocks, affording these supramolecules abundant bonds. The electronic states kinetics are further well-modulated via a host-guest strategy, resulting appropriate regional electron binding force controllable chemical activity. Notably, integrating units into phenyl group-containing model covalent polymer achieves production rate of 9.14 mol g

Language: Английский

Citations

17
Covalent organic frameworks as advanced materials for adsorption and analysis of contaminants in environmental, biological and food matrices DOI

Yanmin Liang,

Yan Qi,

Nannan Zhong

et al.

Coordination Chemistry Reviews, Journal Year: 2025, Volume and Issue: 533, P. 216507 - 216507

Published: Feb. 21, 2025

Language: Английский

Citations

1
Insights into the Formation of Covalent Organic Frameworks by Probing Interfacial Water Structure using Vibrational Sum Frequency Generation Spectroscopy DOI Creative Commons
Ravindra Pandey,

Yogesh Kumar,

Srinivasa Rao Varanasi

et al.

Research Square (Research Square), Journal Year: 2025, Volume and Issue: unknown

Published: Jan. 20, 2025

Abstract Covalent organic frameworks (COFs) are an emerging class of porous materials with diverse applications across multiple fields. Most the ongoing research related to COFs predominantly focuses on developing new through novel linkers and innovative reactions, as well exploring their applications. A detailed molecular-level understanding COF synthesis is essential for advanced materials. The water structure adjacent can significantly influence design highly efficient heterogeneous catalysis, photocatalytic splitting, purification, aid in charge storage mechanism COF-based electrodes at electrode/electrolyte interfaces. To address this issue, we synthesized a 2D thin film via photon-assisted imine condensation water-air interface investigated process using vibrational sum frequency generation (VSFG) spectroscopy. We examined role catalyst, light, interfacial molecules COF. VSFG spectroscopy utilized successfully distinguish between amorphous crystalline films surface. Moreover, it was found that exhibits increased ordering stronger hydrogen bonding proximity

Language: Английский

Citations

0
Precisely Tuning the Electronic Structure of Organic Polymer Electrocatalysts via Thiophene-Based Moieties for Enhanced Oxygen Reduction Reaction DOI Creative Commons
Dongye Li, Binbin Wang,

Kunpeng Zheng

et al.

iScience, Journal Year: 2025, Volume and Issue: 28(3), P. 112007 - 112007

Published: Feb. 12, 2025

Optimizing molecular structures in oxygen reduction reaction (ORR) is crucial for enhancing catalytic efficiency and stability, particularly with respect to the effective adsorption conversion of intermediates. Sulfur-containing heterocyclic compound thiophene can precisely modulate electronic states local charge densities, thereby fine-tuning reactivity microporous polymers, yet, it remains a largely unexplored area. Herein, thiophene-based building blocks featuring diversified linkers into phenyl-containing model Ph-CMP are developed, affording thiophene-fused BPT-CMP thiophene-linked BCT-CMP. The electron density capacity frameworks well regulated through condensation connecting modification, showing excellent half-wave potentials compared reversible hydrogen electrode, surpassing even most metal-free polymer electrocatalysts. Through theoretical calculations experimental results, we have validated that skeleton (BPT-CMP) triggers activation units, exposed pentatomic carbon atom (site-3) serving as active site.

Language: Английский

Citations

0
Regulating the Isomerization Geometry and Energy State of Covalent Organic Frameworks for Enhanced Oxygen Reduction Activity DOI Open Access

Hongni Chen,

Daohao Li,

Min Lin

et al.

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

Published: Feb. 19, 2025

Abstract Embedding isomer entities onto crystalline frameworks with precisely defined spatial distributions represents a promising approach to enhancing the efficiency of oxygen reduction reaction (ORR) in fuel cells. However, accurately constructing covalent organic (COFs) regulate energy state effectively remains significant challenge. Herein, an innovative geometric isomerization strategy aimed at minimizing rotational barrier (ΔE), average local ionization (ALIE), and Gibbs free (ΔG) for ORR within COFs is proposed. Based on this strategy, isomeric Py‐COF‐αα 2,2‐substitution, Py‐COF‐ββ 3,3‐substitution, Py‐COF‐αβ 2,3‐substitution mainchain have been obtained. The electronic states intermediate adsorption capabilities are finely tuned through modification, yielding controllable chemical activity. Notably, lower ΔE between thiophenes achieves remarkable performance, evidenced by half‐wave potential 0.77 V vs reversible hydrogen electrode (RHE), surpassing most reported metal‐free electrocatalysts. Combined theoretical prediction situ Raman spectra, it revealed that increased dipole moment non‐uniform charge distribution caused endows pentacyclic‐carbon (thiophene β‐position) far from sulfur atoms efficient catalytic This work has opened up novel paradigm underscores pivotal role regulation facilitating catalysis.

Language: Английский

Citations

0
Morphology Regulation Is Achieved by Volatile Solid Additives in Halogen-Free Solvents to Fabricate Efficient Polymer Solar Cells DOI
Yanglong Hou,

Qiao Wang,

Yifan Yang

et al.

ACS Applied Materials & Interfaces, Journal Year: 2025, Volume and Issue: unknown

Published: Feb. 26, 2025

The meticulous control of micromorphology in high power conversion efficiency (PCE) polymer solar cells (PSCs) typically relies on halogenated solvents, which pose serious threats to both environmental sustainability and human health. In this work, a green efficient method for fabricating PCE PSCs with halogen-free solvents is developed. By introducing volatile solid additives 1-bromo-2,6-dichlorobenzene (DIB) 1-bromo-2,3,5-trichlorobenzene (TIB) into toluene the aggregation behaviors PM6:L8-BO were meticulously regulated, forming distinct fibrous morphology; detail, vertical direction exhibited pattern acceptor enrichment at top donor bottom, leads enhanced exciton dissociation efficiency, improved charge transport performance, significantly reducing recombination, finally PCEs, as maximum PCEs 18.56 17.67%, respectively, are notably higher than those devices without additives. Furthermore, since can be completely removed from active layer, additive-treated exhibit superior morphology photovoltaic stability. This therefore, unveils straightforward environmentally friendly preparing PSCs, instrumental facilitating large-scale commercialization PSC technology.

Language: Английский

Citations

0
Highly Ordered Conductive Metal‐Organic Frameworks with Chemically Confined Polyoxometalate Clusters: A Dual‐Functional Electrocatalyst for Efficient H2O2 Synthesis and Biomass Valorization DOI

Tong Bao,

You Wu, Chencheng Tang

et al.

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

Published: March 18, 2025

Abstract The design of bifunctional and high‐performance electrocatalysts that can be used as both cathodes anodes for the two‐electron oxygen reduction reaction (2e − ORR) biomass valorization is attracting increasing attention. Herein, a conserved ligand replacement strategy developed synthesis highly ordered conductive metal‐organic frameworks (Ni‐HITP, HITP = 2, 3, 6, 7, 10, 11‐hexaiminotriphenylene) with chemically confined phosphotungstic acid (PW 12 ) nanoclusters in nanopores. newly formed Ni−O−W bonds resultant Ni‐HITP/PW modulate electronic structures Ni W sites, which are favorable cathodic 2e ORR to H 2 O production anodic 5‐hydroxymethylfurfural oxidation (HMFOR) 5‐furandicarboxylic (FDCA), respectively. In combination deliberately retained pores, dual‐functional composites enable rate 9.51 mol g cat −1 h an FDCA yield 96.8% at current density 100 mA cm −2 /cell voltage 1.38 V integrated ORR/HMFOR system, significantly improved than traditional ORR/oxygen evolution system. This work has provided new insights into rational advanced electrocatalytic systems green valuable chemicals.

Language: Английский

Citations

0
Electron‐Deficient Organic Molecules Based on B←N Unit: A N‐Type Room‐Temperature Chemiresistive Sensors with Moisture Resistance DOI Creative Commons
Binbin Wang,

Yali Xing,

Kewei Zhang

et al.

Advanced Science, Journal Year: 2024, Volume and Issue: unknown

Published: Nov. 14, 2024

Organic molecules with tailorable chemical structures, high stability, and solution processability have great potential in the sensing field. Compared p-type organic small (OSMs), electron-dominated n-type analogs show superior conductivity when exposed to reducing gases, which can achieve outstanding sensor signal-to-noise ratios. However, inadequate humidity resistance at room temperature hinders development of such molecules. Herein, an A-D-π-D-A molecular design strategy is proposed based on electron-deficient B←N units, results effective intramolecular charge transport sensitive responses by extending π-conjugation bridge. As a result, ST-2BP configuration shows prominent sensitivity 787 (R

Language: Английский

Citations

2
Construction of a Pore-Confined Catalyst in a Vinylene-Linked Covalent Organic Framework for the Oxygen Reduction Reaction DOI
Xuewen Li, Shuai Yang, Xiubei Yang

et al.

ACS Catalysis, Journal Year: 2024, Volume and Issue: unknown, P. 17862 - 17870

Published: Nov. 19, 2024

Two-dimensional metal-containing covalent organic frameworks (COFs) have been employed as electrocatalysts. However, the metal sites were stacked within layers with strong interactions, which hindered mass transport to them in catalytic process. Herein, we constructed a pore-confined catalyst vinylene-linked COF for oxygen reduction reaction (ORR) via Katritzky reaction. By anchoring along pore walls bonds, units well-exposed during process and retained crystallinity porosity, facilitating access sites. In addition, electron/charge transported from framework modulated electronic states, thus improving activity. The exhibited half-wave potential of 0.85 V activity 109.7 A g–1, are better than those other reported COFs. Theoretical calculations revealed that interaction between contributed easy formation OOH* OH*, resulting high This work provides insights into designing COFs based on C═C linkages.

Language: Английский

Citations

2
Modulating Oxygen Reduction Activity in Chalcogenophene‐Incorporated Organic Electrocatalysts through Main‐Group Element Engineering DOI Open Access
Shuqi Cheng, Binbin Wang,

Hongni Chen

et al.

Small, Journal Year: 2024, Volume and Issue: unknown

Published: Dec. 23, 2024

Abstract Organic small molecules (OSMs) with well‐defined structures are crucial integral components of cathode catalysts for fuel cells. Despite the acknowledged potential heteroatom doping to enhance catalytic performance metal‐free carbon‐based catalysts, there exists a notable gap in conducting molecular structure and activity, particularly under premise maintaining constant skeleton clear structure. Herein, charge distribution is modulated by introducing different chalcogens into same through main‐group engineering. Among these OSMs, Se‐containing molecule OSM‐Se combined carbonized calcium alginate exhibits quasi‐four‐electron‐transfer oxygen reduction reaction pathway, displaying superior half‐wave ( E 1/2 ) 0.73 V, accompanied outstanding electrochemical stability. Density functional theory calculations demonstrate that can capabilities adsorbing dissociating molecules, contribute reducing barrier reaction. This study presents straightforward yet highly effective approach OSM electrocatalysts.

Language: Английский

Citations

1