Topology Control of Covalent Organic Frameworks with Interlaced Unsaturated 2D and Saturated 3D Units for Boosting Electrocatalytic Hydrogen Peroxide Production DOI

Han Wu,

Lili Li,

Hongni Chen

et al.

Angewandte Chemie, Journal Year: 2024, Volume and Issue: 136(40)

Published: June 29, 2024

Abstract Modulating the electronic state of multicomponent covalent organic framework (COF) electrocatalysts is crucial for enhancing catalytic activity. However, effect dimensionality on their physicochemical functionalities still lacking. Herein, we report an interlaced unsaturated 2D and saturated 3D strategy to develop multicomponent‐regulated COFs with tunable gradient high selectivity activity electrocatalysis. Compared two‐component model COFs, 2D/3D locally irregular dimensions structures are more practical in optimizing intrinsic electrode surface reaction mass transfer. Remarkably, 2D‐inserted TAE‐COF regulates adsorption mode OOH* species supply a favorable dynamic pathway H 2 O process, thereby achieving excellent production rate 8.50 mol g cat −1 h . Moreover, utilizing theoretical calculation situ ATR‐FTIR experiment, found that central carbon atom tetraphenyl‐based unit (site‐1 site‐6) potential active sites. This operating ability reactants dimensionality‐interconnected building blocks provides idea designing durable efficient electrocatalysts.

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
Topology Control of Covalent Organic Frameworks with Interlaced Unsaturated 2D and Saturated 3D Units for Boosting Electrocatalytic Hydrogen Peroxide Production DOI

Han Wu,

Lili Li,

Hongni Chen

et al.

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

Published: Aug. 13, 2024

Abstract Modulating the electronic state of multicomponent covalent organic framework (COF) electrocatalysts is crucial for enhancing catalytic activity. However, effect dimensionality on their physicochemical functionalities still lacking. Herein, we report an interlaced unsaturated 2D and saturated 3D strategy to develop multicomponent‐regulated COFs with tunable gradient high selectivity activity electrocatalysis. Compared two‐component model COFs, 2D/3D locally irregular dimensions structures are more practical in optimizing intrinsic electrode surface reaction mass transfer. Remarkably, 2D‐inserted TAE‐COF regulates adsorption mode OOH* species supply a favorable dynamic pathway H 2 O process, thereby achieving excellent production rate 8.50 mol g cat −1 h . Moreover, utilizing theoretical calculation situ ATR‐FTIR experiment, found that central carbon atom tetraphenyl‐based unit (site‐1 site‐6) potential active sites. This operating ability reactants dimensionality‐interconnected building blocks provides idea designing durable efficient electrocatalysts.

Language: Английский

Citations

13
Construction of dangling and staggered stacking aldehyde in covalent organic frameworks for 2e− oxygen reduction reaction DOI Creative Commons
Shuang Zheng, Zhaofeng Ouyang, Minghao Liu

et al.

Carbon Neutralization, Journal Year: 2024, Volume and Issue: 3(3), P. 415 - 422

Published: March 26, 2024

Abstract Covalent organic frameworks (COFs) have been utilized as the ideal candidates to preciously construct electrocatalysts. However, highly ordered degree of COFs renders catalytic centers closely stacked, which limits utilization efficiency sites. Herein, we first constructed dangling and staggered‐stacking aldehyde (–CHO) from [4 + 3] for 2e − oxygen reduction reaction (ORR). The new unreacted ‐CHO out COFs' planes, are more easily exposed in electrolytes than sites frameworks. More importantly, these –CHO adopt staggered stacking models, thus provide larger space mass transport those with eclipsed models. In addition, by tuning triratopic linkers COFs, properties well modulated. optimized COF shows high selectivity activity ORR, H 2 O 91%, 12.2 A g −1 , respectively. theoretical calculation further reveals higher pyridine‐contained B18C6‐PTTA‐COF due promoted binding ability intermediate OOH* at carbon –CHO. This work provides us a insight into designing electrocatalysts based on COFs.

Language: Английский

Citations

11
Construction of imide‐linked covalent organic frameworks with palladium nanoparticles for oxygen reduction reaction DOI Creative Commons

Zhuangyan Guo,

Shuai Yang, Minghao Liu

et al.

EcoEnergy, Journal Year: 2024, Volume and Issue: 2(1), P. 192 - 201

Published: March 1, 2024

Abstract Covalent organic frameworks (COFs) have been widely employed as electrocatalysts for oxygen reduction reaction (ORR) due to their diverse and tunable skeletons pores. However, electrocatalytic activity was limited the lack of highly active catalytic sites. In this work, we first immobilized palladium nanoparticles (NPs) into crystal, porous, stable imide‐linked COF ORR. The newly designed had pyridine linkers with imide‐linkages in serving binding sites anchor Pd sites, high surface area open pore channels provide fast mass transport pathway which contributed performance And catalyst delivered onset potential half‐wave COF‐Pd 0.97 0.83 V, a current density 6.1 mA cm −2 , respectively. This work provides us insights developing crystalline COFs metal NPs systems.

Language: Английский

Citations

11
Low-Cost, Facile, and Scalable Manufacturing of Single-Molecule-Integrated Catalytic Electrodes DOI

Shu‐Guo Han,

San-Mei Wang,

Mengke Hu

et al.

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

Published: March 12, 2025

To surmount the shortcomings of powder-based catalysts and small electrode sizes, development meter-scale integrated materials is essential for practical electrocatalytic applications, which requires fine control over effective surface grafting catalytic active sites on large-size electrodes as well addressing challenge balancing cost-effective large-scale manufacturing with highly stable operation. Herein, we report a low-cost, facile, scalable method directly constructing single-molecule-integrated using commercially available, flexible, size-tailored conductive carbon textiles (e.g., graphite felt) well-defined planar conjugated molecules metallophthalocyanines) via heterostacking steered cross-scale heterointerfacial assembly. This universal unlocks limitations traditional approaches that involve integrating catalysts, particles, binders Nafion), supported paper) through multiple processing steps typically result in centimeter-level electrodes. Meaningfully, our enables precise size, composition, microenvironment, structure to match various environments. As proof concept, an thiophene-gilded cobalt phthalocyanine demonstrates outstanding activity stability CO2 electroconversion alkaline, neutral, acidic media under industrially relevant current densities, even flowing paired-electrolysis system. study provides comprehensive scientific data engineering guidance systematic design scalable, binder-free electrodes, thereby promising drive sustainable energy-efficient electrolysis industrial scene.

Language: Английский

Citations

1
Pyrimidine-containing covalent organic frameworks for efficient photosynthesis of hydrogen peroxide via one-step two electron oxygen reduction process DOI
Hongyu Chen, Hao Zhang, Kai Chi

et al.

Nano Research, Journal Year: 2024, Volume and Issue: 17(11), P. 9498 - 9506

Published: Aug. 17, 2024

Language: Английский

Citations

8
High‐Performance Room Temperature Ammonia Sensors Based on Pure Organic Molecules Featuring B‐N Covalent Bond DOI Creative Commons
Qian Wang,

Meilong Wang,

Kunpeng Zheng

et al.

Advanced Science, Journal Year: 2024, Volume and Issue: 11(19)

Published: March 14, 2024

Exploring organic semiconductor gas sensors with high sensitivity and selectivity is crucial for the development of sensor technology. Herein, first time, a promising chemiresistive polymer P-BNT based on novel π-conjugated triarylboron building block reported, showcasing an excellent responsivity over 30 000 (Ra/Rg) against 40 ppm NH

Language: Английский

Citations

4
Low-Cost Aqueous Electrolyte with MBA Additives for Uniform and Stable Zinc Deposition DOI
Wenyan Chen,

Zhibo Xie,

Haichao Chen

et al.

ACS Applied Materials & Interfaces, Journal Year: 2024, Volume and Issue: 16(23), P. 30580 - 30588

Published: June 1, 2024

Aqueous zinc ion batteries (AZIBs) are attracting increasing research interest due to their intrinsic safety, low cost, and scalability. However, the issues including hydrogen evolution, interface corrosion, dendrites at anodes have seriously limited development of aqueous batteries. Here, N,N-methylenebis(acrylamide) (MBA) additives with −CONH- groups introduced form bonds water suppress H2O activity, inhibiting occurrence evolution corrosion reactions interface. In situ optical microscopy demonstrates that MBA additive promotes uniform deposition Zn2+ then suppresses dendrite growth on anode. Therefore, Zn//Ti asymmetric demonstrate a high plating/stripping efficiency 99.5%, while Zn//Zn symmetric display an excellent cycle stability for more than 1000 h. The Zn//MnO2 full cells exhibit remarkable cycling 700 cycles in electrolytes additives. engineering via achieved dendrite-free Zn stable batteries, which is favorable advanced AZIBs practical applications.

Language: Английский

Citations

4
Thiophene and Acetylene Functionalized Conjugated Organic Polymers with Hollow Nanotube Structure toward High-Performance Photocatalytic H2O2 Production DOI
Yuntong Li, Banghan Ding, Yan Sui

et al.

Journal of environmental chemical engineering, Journal Year: 2025, Volume and Issue: 13(1), P. 115319 - 115319

Published: Jan. 5, 2025

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