Electrolyte Effect on Electrocatalytic CO2 Reduction DOI Creative Commons

Jiandong Zhang,

Ziliang Zhang,

Tian‐Ye Chen

et al.

Nanomaterials, Journal Year: 2025, Volume and Issue: 15(9), P. 648 - 648

Published: April 25, 2025

Electrocatalytic CO2 reduction reaction shows great potential for converting into high-value chemicals and fuels at normal temperature pressure, combating climate change achieving carbon neutrality goals. However, the complex pathways involve transfer of multiple electrons protons, resulting in poor product selectivity, existence competitive hydrogen evolution reactions further increases associated difficulties. This review illustrates research progress on micro mechanism electrocatalytic electrolyte environment recent years. The products, pH effects, cation effects anion were systematically summarized. Additionally, challenges difficulties also pointed out. Thus, this provides a theoretical basis future direction improving efficiency selectivity reaction.

Language: Английский

Challenges and Opportunities for Single‐Atom Electrocatalysts: From Lab‐Scale Research to Potential Industry‐Level Applications DOI Creative Commons
Chen Jia, Qian Sun, Ruirui Liu

et al.

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

Published: June 13, 2024

Single-atom electrocatalysts (SACs) are a class of promising materials for driving electrochemical energy conversion reactions due to their intrinsic advantages, including maximum metal utilization, well-defined active structures, and strong interface effects. However, SACs have not reached full commercialization broad industrial applications. This review summarizes recent research achievements in the design crucial electrocatalytic on sites, coordination, substrates, as well synthesis methods. The key challenges facing activity, selectivity, stability, scalability, highlighted. Furthermore, it is pointed out new strategies address these increasing activity enhancing utilization improving optimizing local environment, developing fabrication techniques, leveraging insights from theoretical studies, expanding potential Finally, views offered future direction single-atom electrocatalysis toward commercialization.

Language: Английский

Citations

28
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
Tailoring CO2 Adsorption Configuration with Spatial Confinement Switches Electroreduction Product from Formate to Acetate DOI

Hua‐Qin Wang,

Heyu Sui,

Ya-Long Ding

et al.

Journal of the American Chemical Society, Journal Year: 2025, Volume and Issue: unknown

Published: Feb. 5, 2025

Multi-proton-coupled electron transfer, multitudinous intermediates, and unavoidable competing hydrogen evolution reaction during CO2 electroreduction make it tricky to control high selectivity for specific products. Here, we present spatial confinement of Fe single atoms (FeN2S2) by adjacent FeS clusters (Fe4S4) orientate the transition adsorption configuration from C,O-side O-end, which triggers a shift activated first-step protonation C–C coupling, thus switching target product HCOOH in Faraday efficiency (FE: 90.6%) on FeN2S2 CH3COOH 82.3%) Fe4S4/FeN2S2. The strength *OCHO upon solitary site is linearly related coordination number Fe–S, with predominantly produced over single-atom (ortho-substituted S atoms). Fe4S4 cluster functions as switch reduction product, can not only optimize electronic structure neighboring but also impel complete hydrocarbon intermediate *CH3, followed coupling CO2* *CH3 via synergistic catalysis This strategy provides new avenue modulate reactant model desirable pathways, potential applications diverse multistep electrochemical processes controlled selectivity.

Language: Английский

Citations

6
Modulating the Electronic Properties of Single Ni Atom Catalyst via First‐Shell Coordination Engineering to Boost Electrocatalytic Flue Gas CO2 Reduction DOI Open Access
Zhiyuan Wang, Zhen Chen, Xin Du

et al.

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

Published: Jan. 10, 2025

Abstract Electrochemical converting CO 2 to via single atom catalyst is an effective strategy for reducing concentration in the atmosphere and achieving a carbon‐neutral cycle. However, relatively low industrial processes large energy barriers activating severely obstruct actual application. Reasonably modulating coordination shell of active center enhance activity catalysts. Herein, well‐designed single‐atom electrocatalyst Ni‐N 3 S 1 developed large‐scale synthesis strategy. The constructed S‐C exhibits superior catalytic than 4 ‐C conversion H‐type cells, industrial‐level current density with excellent durability at wide pH range can be achieved gas‐diffusion flow cells. Experimental results functional theory (DFT) calculation demonstrate that introducing electronegative significantly regulate electronic structure site, promoting adsorption capacity decreasing barrier *COOH formation, thus larger size flexibility sulfur mitigate nickel agglomeration stability catalyst. This work provides designing highly catalysts electrocatalysis reactive sites.

Language: Английский

Citations

2
An acid-tolerant metal-organic framework for industrial CO2 electrolysis using a proton exchange membrane DOI Creative Commons
Kang Yang, Ming Li, Tianqi Gao

et al.

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

Published: Aug. 16, 2024

Industrial CO

Language: Английский

Citations

13
Sub‐Nanometer Mono‐Layered Metal–Organic Frameworks Nanosheets for Simulated Flue Gas Photoreduction DOI
Dong He, Qian Wang,

Yan Rong

et al.

Advanced Materials, Journal Year: 2024, Volume and Issue: 36(27)

Published: April 18, 2024

Abstract The dilemma between the thickness and accessible active site triggers design of porous crystalline materials with mono‐layered structure for advanced photo‐catalysis applications. Here, a kind sub‐nanometer nanosheets (Co‐MOF MNSs) through exfoliation specifically designed Co 3 cluster‐based metal–organic frameworks (MOFs) is reported. inherent light‐sensitivity endow Co‐MOF MNSs fully exposed Janus sites that can selectively photo‐reduce CO 2 into formic acid under simulated flue gas. Notably, production efficiency by (0.85 mmol g −1 h ) ≈13 times higher than bulk counterpart (0.065 gas atmosphere, which highest in reported works up to date. Theoretical calculations prove simultaneously available possess activity when compared single site, validating importance nanosheet morphology. These results may facilitate development functional photo‐reduction potential treatment.

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
Electrochemical CO2 Reduction on SnO: Insights into C1 Product Dynamic Distribution and Reaction Mechanisms DOI Creative Commons
Zhongyuan Guo, Tianyi Wang,

Heng Liu

et al.

ACS Catalysis, Journal Year: 2025, Volume and Issue: unknown, P. 3173 - 3183

Published: Feb. 6, 2025

The precise synthesis of desirable products from the electrochemical CO2 reduction reaction (CO2RR) remains challenging, primarily due to unclear structure–activity relationships under in situ conditions. Recognized by their cost-effectiveness and nontoxic nature, Sn-based materials are extensively utilized CO2RR produce valuable chemicals. Notably, our large-scale data mining experimental literature reveals a significant trend: SnO2-based electrocatalysts generate HCOOH, while SnO-based counterparts demonstrate ability both HCOOH CO comparable quantities. Furthermore, findings indicate that SnO underexplored terms its surface speciation for compared materials. Addressing these issues is crucial field electrocatalysis, as understanding them will not only clarify why uniquely influences distribution C1 but also provide insights into how precisely control electrocatalytic processes targeted product synthesis. Herein, we employed constant-potential method combined with coverage reconstruction analyses simulate energetics intermediates elucidate dynamic on resting typical Our analysis effectively identifies active involved CO2RR. comparative simulations between pristine reconstructed surfaces reveal electrochemistry-induced oxygen vacancies direct distribution. By addressing critical issues, aim advance electrocatalysis contribute chemical production CO2, stimulating future exploration conditions other systems.

Language: Английский

Citations

1
Adjustable Selectivity for CO2 Electroreduction to Ethylene or Ethanol by Regulating Interphases Between Copper and Tin Oxides DOI Open Access
Huan Liu, Cheng‐Han Yang,

Tong Bian

et al.

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

Published: Feb. 10, 2025

Abstract Enhancing the selectivity of C 2 products and revealing reaction mechanisms in CO electroreduction (CO RR) remain challenging. Regulating interphases catalysts is one most promising pathways. Herein, between copper (Cu) tin (Sn) oxides are regulated by controlling degree reduction during self‐assembly process, which exhibits obvious different to ethylene ethanol, respectively. The interphase Cu‐SnO ethanol as high 74.6%, while Cu O‐SnO shows 71.4% at –0.6 V versus RHE. In situ Fourier‐transform infrared spectroscopy measurements density functional theory calculations demonstrate that strong electron interaction, preferentially forming key *COH intermediates for asymmetrical C─C coupling produce ethanol. contrast, possesses oxygen vacancies both sites, thus enriching *CO symmetrical interphase. findings this work offer an advanced strategy regulating adjust RR.

Language: Английский

Citations

1
Electrochemical CO2 Reduction in Acidic Media: A Perspective DOI
N. C. Dutta, Sebastian C. Peter

Journal of the American Chemical Society, Journal Year: 2025, Volume and Issue: unknown

Published: March 4, 2025

The electrochemical CO2 reduction reaction (eCO2RR) is a promising approach for converting to useful chemicals and, hence, achieving carbon neutrality. Though high selectivity and activity of products have been achieved recently, all are reported in neutral or alkaline electrolytes. Although these electrolyte media give activity, they face the major challenge low utilization because carbonate formation, which lowers overall efficiency process. Conducting eCO2RR acidic can help overcome issue formation hence increase efficiency. However, there many challenges associated with eCO2RR. Two concerns highly competitive hydrogen evolution salt precipitation issues. This Perspective focuses on fundamentals eCO2RR, recent catalyst development strategies, relevant problems that need be addressed future. In end, we provide future outlook will an idea about focus field

Language: Английский

Citations

1