Amine-Functionalized Copper Catalysts: Hydrogen Bonding Mediated Electrochemical CO<sub>2</sub> Reduction to C<sub>2</sub> Products and Superior Rechargeable Zn-CO<sub>2</sub> Battery Performance DOI Open Access
Dong Xiang,

Kunzhen Li,

Kanghua Miao

et al.

Acta Physico-Chimica Sinica, Journal Year: 2023, Volume and Issue: 0(0), P. 2308027 - 2308027

Published: Jan. 1, 2023

The electrochemical carbon dioxide reduction reaction (eCO2RR) can convert CO2 into valuable chemicals, achieving a cycle.Copper-based catalysts have demonstrated unique ability to produce C2+ products in eCO2RR, which is often limited by the scaling relationship of intermediates, complex mechanism and competitive H2 evolution.Organic functionalization promising strategy for regulating activity selectivity eCO2RR toward products.However, behind such regulation especially at molecular level, remains elusive.In this study, Cu nanoparticles were prepared functionalized with set amine derivatives, including hexadecylamine (HDA), N-methylhexadecylamine (N-MHDA), hexadecyldimethylamine (HDDMA), palmitamide (PMM).The impact structure surfactants on was systematically explored through both experiments theoretical calculations.X-ray photoelectron spectroscopy density functional theory calculations revealed that HDA catalyst surface resulted negative charge transfer from molecules Cu. ECO2RR examined 1.0 mol•L -1 KOH aqueous electrolyte.HDA achieved highest Faradaic efficiency (FE) 73.5% C2 46.4% C2H4, respectively.It also provided partial current 131.4 mA•cm -2 -0.9 V vs. reversible hydrogen electrode (RHE) among these derivatives catalysts.In contrast, FE pristine only 27.0% 50.5 , respectively.Theoretical studies bonding interactions intermediates enriched CO2, CO, other lowered kinetic energy barrier CO-CHO coupling thereby promoted products.Replacing H atoms group methyl groups N-MHDA HDDMA dominant evolution (HER) eCO2RR.PMM Cu-O bond, instead Cu-N as HDA, HDDMA, preferred ethanol production.In situ Raman indicated CO adsorption atop sites HDA-capped catalysts, bridge site clean surfaces, possibly due former case.HDA increased local pH relative catalysts.The Cu-HDA-based rechargeable Zn-CO2 battery exhibited superior maximum power 6.48 mW•cm discharge 16 remarkable durability 60 h, outperforming most reported literature.This work enhances CO2-C2 conversion tuning Cu-based materials, unravels provides new insights promoting organic molecules.

Language: Английский

Regulation of intermediate microenvironment for efficient C–C coupling in electrochemical CO2 reduction DOI
Hao Mei, Qingfeng Hua,

Lina Su

et al.

Journal of Materials Chemistry A, Journal Year: 2024, Volume and Issue: 12(32), P. 20507 - 20526

Published: Jan. 1, 2024

This review summarizes the recent progress in regulation of local reaction intermediates and protons near active sites discusses how their microenvironment affects C–C coupling efficiency electrocatalytic CO 2 RR.

Language: Английский

Citations

1
Fluorine-regulated Cu catalyst boosts electrochemical reduction of CO2 towards ethylene production DOI

Dan Hu,

Jingbo Wen,

Zhibin Pei

et al.

Electrochimica Acta, Journal Year: 2024, Volume and Issue: 509, P. 145317 - 145317

Published: Nov. 5, 2024

Language: Английский

Citations

1
IrPdCuFeNiCoMo Based Core‐Shell Icosahedron Nanocrystals and Nanocages for Efficient and RobustAcidic Oxygen Evolution DOI

Mairui Long,

Siyuan Lai,

Kanghua Miao

et al.

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

Published: Dec. 5, 2024

Abstract Facets engineering of high entropy alloy (HEA) nanocrystals might be achieved via shape‐controlled synthesis, which is promising but remains challenging in designing Ir‐based catalysts towards efficient and robust oxygen evolution reaction (OER) acidic medium. Herein, icosahedra featured with PdCu core IrPdCuFeNiCoMo shell were prepared by wet‐chemical reduction one‐pot, ascribing to the initial formation subsequent deposition diffusion HEA shell. Sequential selective chemical etching results nanocages, delivering an overpotential 235 mV at 10 mA cm −2 , 51.0 dec −1 1624 A g Ir 1.50 V vs reversible hydrogen electrode a conventional three cell. In proton exchange membrane water electrolyzer, it delivers low cell voltage 1.65 1.77 current density 1.0 2.0 respectively, maintains stable over 900 h 500 . Theoretical calculations attribute enhanced intrinsic activity broad distribution binding energy for OER intermediates on HEA, breaks linear scaling relationship accelerates process.

Language: Английский

Citations

1
Effects of metal oxide promoters on Cu-ZnO-Al2O3 for one step DME conversion to ethanol by carbonylation and successive hydrogenation DOI
Hyun Seung Jung, Jong Wook Bae

Catalysis Today, Journal Year: 2023, Volume and Issue: 424, P. 114302 - 114302

Published: July 28, 2023

Language: Английский

Citations

2
Amine-Functionalized Copper Catalysts: Hydrogen Bonding Mediated Electrochemical CO<sub>2</sub> Reduction to C<sub>2</sub> Products and Superior Rechargeable Zn-CO<sub>2</sub> Battery Performance DOI Open Access
Dong Xiang,

Kunzhen Li,

Kanghua Miao

et al.

Acta Physico-Chimica Sinica, Journal Year: 2023, Volume and Issue: 0(0), P. 2308027 - 2308027

Published: Jan. 1, 2023

The electrochemical carbon dioxide reduction reaction (eCO2RR) can convert CO2 into valuable chemicals, achieving a cycle.Copper-based catalysts have demonstrated unique ability to produce C2+ products in eCO2RR, which is often limited by the scaling relationship of intermediates, complex mechanism and competitive H2 evolution.Organic functionalization promising strategy for regulating activity selectivity eCO2RR toward products.However, behind such regulation especially at molecular level, remains elusive.In this study, Cu nanoparticles were prepared functionalized with set amine derivatives, including hexadecylamine (HDA), N-methylhexadecylamine (N-MHDA), hexadecyldimethylamine (HDDMA), palmitamide (PMM).The impact structure surfactants on was systematically explored through both experiments theoretical calculations.X-ray photoelectron spectroscopy density functional theory calculations revealed that HDA catalyst surface resulted negative charge transfer from molecules Cu. ECO2RR examined 1.0 mol•L -1 KOH aqueous electrolyte.HDA achieved highest Faradaic efficiency (FE) 73.5% C2 46.4% C2H4, respectively.It also provided partial current 131.4 mA•cm -2 -0.9 V vs. reversible hydrogen electrode (RHE) among these derivatives catalysts.In contrast, FE pristine only 27.0% 50.5 , respectively.Theoretical studies bonding interactions intermediates enriched CO2, CO, other lowered kinetic energy barrier CO-CHO coupling thereby promoted products.Replacing H atoms group methyl groups N-MHDA HDDMA dominant evolution (HER) eCO2RR.PMM Cu-O bond, instead Cu-N as HDA, HDDMA, preferred ethanol production.In situ Raman indicated CO adsorption atop sites HDA-capped catalysts, bridge site clean surfaces, possibly due former case.HDA increased local pH relative catalysts.The Cu-HDA-based rechargeable Zn-CO2 battery exhibited superior maximum power 6.48 mW•cm discharge 16 remarkable durability 60 h, outperforming most reported literature.This work enhances CO2-C2 conversion tuning Cu-based materials, unravels provides new insights promoting organic molecules.

Language: Английский

Citations

2