Atomically Asymmetrical Ir–O–Co Sites Enable Efficient Chloride‐mediated Ethylene Electrooxidation in Neutral Seawater DOI
Linke Cai, Yao Liu, Ying Gao

et al.

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

Published: Oct. 25, 2024

Abstract The chloride‐mediated ethylene oxidation reaction (EOR) of chlorohydrin (ECH) via electrocatalysis is practically attractive because its sustainability and mild conditions. However, the chlorine (COR), which essential for above process, commonly catalyzed by dimensionally stable anodes (DSAs) with high contents precious Ru and/or Ir. development highly efficient COR electrocatalysts composed nonprecious metals or decreased amounts desirable. Herein, we report a modified Co 3 O 4 single‐atom Ir substitution (Ir 1 /Co ) as electrocatalyst EOR to ECH in neutral seawater. achieves Faradaic efficiency (FE) up 94.8 % generation remarkable stability. Combining experimental results density functional theory (DFT) calculations, unique atomically asymmetrical Ir−O−Co configuration strong electron coupling effect Ir1/Co can accelerate transfer increase kinetics maintain structural stability during COR. Moreover, system integrating anodic cathodic H 2 ‐mediated show total FE ~170 paired electrosynthesis glycol (EG) using raw material. technoeconomic analysis highlights promising application prospects this system.

Language: Английский

Isolated Metal Centers Activate Small Molecule Electrooxidation: Mechanisms and Applications DOI Open Access
Yanmin Hu,

Tingting Chao,

Yuhai Dou

et al.

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

Published: Jan. 26, 2025

Abstract Electrochemical oxidation of small molecules shows great promise to substitute oxygen evolution reaction (OER) or hydrogen (HOR) enhance kinetics and reduce energy consumption, as well produce high‐valued chemicals serve fuels. For these reactions, high‐valence metal sites generated at oxidative potentials are typically considered active trigger the process molecules. Isolated atom site catalysts (IASCs) have been developed an ideal system precisely regulate state coordination environment single‐metal centers, thus optimize their catalytic property. The isolated in IASCs inherently possess a positive state, can be more readily homogeneous under than nanoparticle counterparts. Meanwhile, merely centers but lack ensemble sites, which alter adsorption configurations compared with counterparts, induce various pathways mechanisms change product selectivity. More importantly, construction is discovered limit d‐electron back donation CO 2p * orbital overly strong on resolve poisoning problems most electro‐oxidation reactions improve stability. Based advantages fields electrochemical molecules, this review summarizes recent developments advancements focusing anodic HOR fuel cells OER electrolytic alternative such formic acid/methanol/ethanol/glycerol/urea/5‐hydroxymethylfurfural (HMF) key reactions. merits different decoding structure–activity relationships specifically discussed guide precise design structural regulation from perspective comprehensive mechanism. Finally, future prospects challenges put forward, aiming motivate application possibilities for diverse functional IASCs.

Language: Английский

Citations

1
Direct Electrooxidation of Ethylene to Ethylene Glycol over 90% Faradaic Efficiency Enabled by Cl– Modification of the Pd Surface DOI

An-Zhen Li,

Xiongbo Wang,

Shuwei Li

et al.

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

Published: March 14, 2025

Direct electrochemical ethylene-to-ethylene glycol (C2H4-to-EG) conversion can potentially reduce the consumption of fossil fuels and emission carbon dioxide (CO2) compared with traditional thermo-catalytic approach. Palladium (Pd) prepared by electrodeposition is represented as a promising electrocatalyst; however, it exhibits low Ethylene (EG) current density (<4 mA cm-2), Faradaic efficiency (<60%), productivity (<10 μmol h-1), hindering practical applications. Herein, we report nanodendrite palladium catalyst supported on large-area gas diffusion electrode. This gives high EG (12 cm-2) (227 h-1) but (65%). With further Cl- ions modification, increased to record-high value 92%, (18 (∼340 were also promoted. Experimental data suggest that strong electron-withdrawing feature reduces oxidation ability in situ generated Pd-OH species, inhibiting overoxidation aldehyde. Meanwhile, alters adsorption configuration─from parallel dual-site coordination vertical single-site coordination─over Pd surface, thus preventing C-C bond cleavage CO2. In addition, facilitates generation active species improve catalytic activity. work demonstrates great potential surface ion modification for improving activity selectivity direct C2H4-to-EG conversion, which may have implications diverse value-added chemicals electrosynthesis.

Language: Английский

Citations

1
Pathway-Dependent Ion Effects for Electrocatalytic Olefin Epoxidation DOI

Shuangshuang Cha,

Yizhou Yang, Yujia Liu

et al.

ACS Sustainable Chemistry & Engineering, Journal Year: 2025, Volume and Issue: unknown

Published: April 3, 2025

Language: Английский

Citations

0
Insight into Carbon Hybrid and Interfacial Modulation for High-Performance Electrosynthesis of Ethylene Glycol DOI
Xiaoqiang Li, Guo‐Yi Duan, Yue Pan

et al.

ACS Catalysis, Journal Year: 2025, Volume and Issue: unknown, P. 6572 - 6580

Published: April 7, 2025

Language: Английский

Citations

0
Electrocatalytic organic transformation reactions in green chemistry: Exploring nanocrystals and single atom catalysts DOI
Ziwei Deng, Yuexin Guo,

Zhiyi Sun

et al.

Nano Research, Journal Year: 2024, Volume and Issue: 17(11), P. 9326 - 9344

Published: Aug. 9, 2024

Language: Английский

Citations

2
Upgrading ethylene via renewable energy-driven electrocatalysis DOI

Hanyu Wang,

Dunfeng Gao,

Guoxiong Wang

et al.

Science China Chemistry, Journal Year: 2024, Volume and Issue: 67(12), P. 3944 - 3951

Published: Aug. 23, 2024

Language: Английский

Citations

2
Atomically Asymmetrical Ir–O–Co Sites Enable Efficient Chloride‐mediated Ethylene Electrooxidation in Neutral Seawater DOI
Linke Cai, Yao Liu, Ying Gao

et al.

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

Published: Oct. 25, 2024

The chloride-mediated ethylene oxidation reaction (EOR) of chlorohydrin (ECH) via electrocatalysis is practically attractive because its sustainability and mild conditions. However, the chlorine (COR), which essential for above process, commonly catalyzed by dimensionally stable anodes (DSAs) with high contents precious Ru and/or Ir. development highly efficient COR electrocatalysts composed nonprecious metals or decreased amounts desirable. Herein, we report a modified Co

Language: Английский

Citations

2
Atomically Asymmetrical Ir–O–Co Sites Enable Efficient Chloride‐mediated Ethylene Electrooxidation in Neutral Seawater DOI
Linke Cai, Yao Liu, Ying Gao

et al.

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

Published: Oct. 25, 2024

Abstract The chloride‐mediated ethylene oxidation reaction (EOR) of chlorohydrin (ECH) via electrocatalysis is practically attractive because its sustainability and mild conditions. However, the chlorine (COR), which essential for above process, commonly catalyzed by dimensionally stable anodes (DSAs) with high contents precious Ru and/or Ir. development highly efficient COR electrocatalysts composed nonprecious metals or decreased amounts desirable. Herein, we report a modified Co 3 O 4 single‐atom Ir substitution (Ir 1 /Co ) as electrocatalyst EOR to ECH in neutral seawater. achieves Faradaic efficiency (FE) up 94.8 % generation remarkable stability. Combining experimental results density functional theory (DFT) calculations, unique atomically asymmetrical Ir−O−Co configuration strong electron coupling effect Ir1/Co can accelerate transfer increase kinetics maintain structural stability during COR. Moreover, system integrating anodic cathodic H 2 ‐mediated show total FE ~170 paired electrosynthesis glycol (EG) using raw material. technoeconomic analysis highlights promising application prospects this system.

Language: Английский

Citations

0