Rapidly Constructing Meter‐Scale Single‐Molecule Integrated Catalytic Electrode with Hydrophobic Microenvironment for pH‐Universal CO2 Electroreduction DOI Open Access
Yajing Li,

Shu‐Guo Han,

Wenbo Wei

et al.

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

Published: March 21, 2025

Abstract The massive production of cost‐effective and highly‐efficient electrode materials is crucial for industrial CO 2 electroconversion. Herein, this work breaks away from conventional approaches by directly constructing an integrated single‐molecule catalytic (7F‐CoPc@GF) at the meter scale, through integration π‐extended macrocyclic structures into commercial carbon‐based collectors with strong interfacial interactions. This innovative method reshapes traditional design using a liquid‐phase self‐adaptive anchoring strategy, eliminating need conductive adducts binders. In addition, introducing perfluoroalkyl chain, built‐in hydrophobic microenvironment in heterogenized macrocycles optimizes electron migration water interaction around active sites, suppressing hydrogen evolution reaction thereby enhancing pH‐universal electroreduction across broad potential range. Significantly, mechanistic study reveals that not only enhances effective collisions between sites reactants but also facilitates immediate removal products surface. Further development dual value‐added electrolysis systems, incorporating waste gas treatment, highlights versatility extensibility meter‐scale material. These findings offer promising methodology rational stable, binder‐free, large‐size electrodes, advancing sustainable scale.

Language: Английский

Reaction Environment Regulation for Electrocatalytic CO2 Reduction in Acids DOI
Min Zeng,

Wensheng Fang,

Yiren Cen

et al.

Angewandte Chemie International Edition, Journal Year: 2024, Volume and Issue: 63(26)

Published: April 19, 2024

The electrocatalytic CO

Language: Английский

Citations

49

Addressing the Carbonate Issue: Electrocatalysts for Acidic CO2 Reduction Reaction DOI Creative Commons
Weixing Wu, Liangpang Xu, Qian Lü

et al.

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

Published: May 9, 2024

Abstract Electrochemical CO 2 reduction reaction (CO RR) powered by renewable energy provides a promising route to conversion and utilization. However, the widely used neutral/alkaline electrolyte consumes large amount of produce (bi)carbonate byproducts, leading significant challenges at device level, thereby impeding further deployment this reaction. Conducting RR in acidic electrolytes offers solution address “carbonate issue”; however, it presents inherent difficulties due competitive hydrogen evolution reaction, necessitating concerted efforts toward advanced catalyst electrode designs achieve high selectivity activity. This review encompasses recent developments RR, from mechanism elucidation design engineering. begins discussing mechanistic understanding pathway, laying foundation for RR. Subsequently, an in‐depth analysis advancements catalysts is provided, highlighting heterogeneous catalysts, surface immobilized molecular enhancement. Furthermore, progress made device‐level applications summarized, aiming develop high‐performance systems. Finally, existing future directions are outlined, emphasizing need improved selectivity, activity, stability, scalability.

Language: Английский

Citations

23

Advancements in electrochemical CO2 reduction reaction: A review on CO2 mass transport enhancement strategies DOI
Yuan Zhou, Ke Wang, Shaojie Zheng

et al.

Chemical Engineering Journal, Journal Year: 2024, Volume and Issue: 486, P. 150169 - 150169

Published: March 4, 2024

Language: Английский

Citations

17

Efficient acidic CO2 electroreduction to formic acid by modulating electrode structure at industrial-level current DOI
Zhenhui Wang, Hongdong Li, Tian Dong

et al.

Chemical Engineering Journal, Journal Year: 2024, Volume and Issue: 489, P. 151238 - 151238

Published: April 14, 2024

Language: Английский

Citations

14

Pulse Electrolysis Turns on CO2 Methanation through N‐Confused Cupric Porphyrin DOI
Wei Hua,

Tingting Liu,

Zhangyi Zheng

et al.

Angewandte Chemie International Edition, Journal Year: 2024, Volume and Issue: 63(12)

Published: Jan. 30, 2024

Breaking the D

Language: Английский

Citations

13

Dimensionality Engineering toward Carbon Materials for Electrochemical CO2 Reduction: Progress and Prospect DOI

Yadong Du,

Xiangtong Meng, Yangjun Ma

et al.

Advanced Functional Materials, Journal Year: 2024, Volume and Issue: 34(46)

Published: Aug. 9, 2024

Abstract Carbon materials are of great significance in state‐of‐the‐art electrochemical CO 2 reduction (ECR) as key components such electrocatalysts, gas diffusion electrodes, and current collectors. Notably, dimensionalities carbons related manipulations play vital roles boosting ECR performance, e.g., mass/charge transfer dynamics, exposure active sites, reaction space, product's Faradaic efficiency/selectivity, durability. Here, recent endeavors dimensionality engineering toward advanced carbon‐based for is first summarized, including pure (e.g., carbon nanotube graphene) composites, highlight the dimensionality‐dependent properties performance. Various strategies referring to modulation integration have been top‐down, bottom‐up, soft chemical approaches. Design principles dimensionality‐varied elaborated, impacts surface chemistry functional group, wettability, electronic structure) on kinetics product‐targeted mechanisms also scrutinized. Some insights into how manipulation elevates performance acceleration, kinetics, product selectivity provided. At last, a perspective challenges future development discussed. This review aims at providing guidance customizable construction with dependence green energy‐saving electrosynthesis systems.

Language: Английский

Citations

10

Structure regulated CuSn alloy catalyst for selective electrochemical CO2-to-formate conversion at higher current densities DOI
Da Li, Siwei Xie,

Liang Jing-bo

et al.

Separation and Purification Technology, Journal Year: 2024, Volume and Issue: 340, P. 126545 - 126545

Published: Feb. 2, 2024

Language: Английский

Citations

9

Highly Selective Acidic CO2 Electroreduction with Large Current on Polypyrrole‐Modified Ag Catalyst by Local Microenvironment Modulation DOI Open Access
Zhenhui Wang, Weizhou Wang, Qin Yang

et al.

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

Published: Feb. 2, 2025

Abstract Electrocatalytic carbon dioxide reduction (CO 2 RR) holds great promise for capture and utilization. In acidic media, CO RR enables efficient conversion, but with low selectivity due to the competitive hydrogen evolution reaction (HER) catalyst corrosion. Herein, conductive polymer polypyrrole (PPy) coated Ag nanoparticles (NPs) catalysts (Ag@PPy) different thicknesses are designed synthesized, which could create a hydrophobic environment that reduces accessibility of H O NPs thereby inhibiting HER. The coating PPy layer also protects from corrosion improves stability system. Among them, Ag@PPy‐2 appropriate thickness showed up 91.7% electrocatalytic high durability in electrolyte at −300 mA cm −2 . Density functional theory (DFT) calculation shows not only inhibit HER, reduce energy barrier, improve efficiency CO. This study may provide some new ideas design advanced selective by local microenvironmental engineering.

Language: Английский

Citations

1

All-Fiber Volatile Organics-Perceptive Actuators DOI
Shuang Wang, Hao Liu, Yufan Zhang

et al.

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

Published: Feb. 26, 2025

Soft robots with real-time volatile organic compound (VOC) perceptivity are promising for dynamic hazard detection. However, reconciling VOC-responsive actuation an autonomous perception remains challenging. Inspired by Victoria amazonica, which blooms and closes synchronous color change under environmental stimulations, we developed a solvatophore-induced solvatochromic-piezoelectric material synthesizing solvatochromic molecule-modified palygorskite-enhanced polyvinylidene difluoride realized all-fiber actuator piezoelectric properties cooperative visual electrical of organics. Under VOCs, the exhibits bidirectional bending, obvious stable change, characteristic output, allowing identification type concentration VOC. The demonstrates large bending curvature 4.63 cm-1, ultrafast response speed up to 4.36 cm-1 s-1, excellent stability 1500 cycles without fatigue, VOC-induced output reflecting conditions. sensing, manipulation, were demonstrated as applications. VOC-triggered soft robot motion capable autonomously perceiving responding This work presents widely applicable interactive visual-electronic VOC detection strategy safety, health, protection, could also inspire exploitation high-performance responsive fiber materials.

Language: Английский

Citations

1

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