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

и другие.

Acta Physico-Chimica Sinica, Год журнала: 2023, Номер 0(0), С. 2308027 - 2308027

Опубликована: Янв. 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.

Язык: Английский

Synergy of Ni Nanoclusters and Single Atom Site: Size Effect on the Performance of Electrochemical CO2 Reduction Reaction and Rechargeable Zn−CO2 Batteries DOI

Kanghua Miao,

Jundi Qin,

Jun Yang

и другие.

Advanced Functional Materials, Год журнала: 2024, Номер 34(33)

Опубликована: Апрель 18, 2024

Abstract The design of bifunctional electrocatalysts toward reduction reaction carbon dioxide (ECO 2 RR) and oxygen evolution (OER) in aqueous rechargeable Zn─CO batteries (ZABs) still poses a significant challenge. Herein, Ni clusters (Ni x ) 0.5 0.8 nm diameter coupled with single site (Ni−N 4 −C), denoted as Ni−N /Ni 5 8 , respectively, are synthesized the size effect nanoclusters studied. exhibits an ≈100% Faradaic efficiency ( FE CO ECO RR for from −0.4 to −0.8 V versus reversible hydrogen electrode, superior that −C = 55.0%) 80.0%). OER performance or comparable commercial RuO but outperform −C. Theoretical calculation indicates * COOH intermediates bond synergistically atom site, promoting activation reducing energy barrier potential determining step RR. Such is strongly size‐dependent larger result too strong binding intermediates, impede formation CO. As cathode electrocatalyst alkaline ZABs, peak power density 11.7 mW cm −2 cycling durability over 1200 cycles 420 h.

Язык: Английский

Процитировано

28
Cobalt phthalocyanine promoted copper catalysts toward enhanced electro reduction of CO2 to C2: Synergistic catalysis or tandem catalysis? DOI

Yan Luo,

Jun Yang,

Jundi Qin

и другие.

Journal of Energy Chemistry, Год журнала: 2024, Номер 92, С. 499 - 507

Опубликована: Янв. 18, 2024

Язык: Английский

Процитировано

24
Targeted C-O bond cleavage of *CH2CHO at copper active sites for efficient electrosynthesis of ethylene from CO2 reduction DOI
Huiying Zhang, Xiaojun Wang,

Yanfei Sun

и другие.

Applied Catalysis B Environment and Energy, Год журнала: 2024, Номер 351, С. 123992 - 123992

Опубликована: Апрель 24, 2024

Язык: Английский

Процитировано

20
Probing Photocatalytic Reduction Pathways of CO2 by Catalyst PbBiO2Br Using In-Situ Raman Spectroscopy DOI Creative Commons

Kang-Yu Hsiao,

Fuyu Liu,

Chiing‐Chang Chen

и другие.

ACS Catalysis, Год журнала: 2025, Номер unknown, С. 3153 - 3161

Опубликована: Фев. 6, 2025

Язык: Английский

Процитировано

2
The green chemistry paradigm in modern organic synthesis DOI
Sergei G. Zlotin, Ksenia S. Egorova, Valentine P. Ananikov

и другие.

Russian Chemical Reviews, Год журнала: 2023, Номер 92(12), С. RCR5104 - RCR5104

Опубликована: Дек. 1, 2023

After the appearance of green chemistry concept, which was introduced in vocabulary early 1990s, its main statements have been continuously developed and modified. Currently, there are 10–12 cornerstones that should form basis for an ideal chemical process. This review analyzes accumulated experience achievements towards design products processes reduce or eliminate use generation hazardous substances. The presents views leading Russian scientists specializing various fields this subject, including homogeneous heterogeneous catalysis, fine basic organic synthesis, electrochemistry, polymer chemistry, based on bio-renewable feedstocks energetic compounds materials. A new approach to quantitative evaluation environmental friendliness by authors is described. <br> bibliography includes 1761.

Язык: Английский

Процитировано

39
In-situ characterization technologies and theoretical calculations in carbon dioxide reduction: In-depth understanding of reaction mechanisms and rational design of electrocatalysts DOI
Rutao Wang, Xiaokun Yang, Jianpeng Zhang

и другие.

Coordination Chemistry Reviews, Год журнала: 2025, Номер 533, С. 216541 - 216541

Опубликована: Фев. 28, 2025

Язык: Английский

Процитировано

1
Selectivity of Electrochemical CO2 Reduction toward Ethanol and Ethylene: The Key Role of Surface-Active Hydrogen DOI
Yixin Ouyang, Li Shi, Xiaowan Bai

и другие.

ACS Catalysis, Год журнала: 2023, Номер 13(23), С. 15448 - 15456

Опубликована: Ноя. 15, 2023

Electrochemical reduction offers promise for converting CO2 into a range of hydrocarbons and oxygenates, yet the production alcohols remains an ongoing challenge. The elusive understanding underlying factors governing alcohol selectivity has hindered optimization yields. Herein, we clarify insight mechanism enhanced ethanol over modified copper catalysts via explicit solvent models combined with slow-growth molecular dynamics. surface-active hydrogen, introduced by guest metals high-facet atomic arrangements, emerges as pivotal factor in promoting kinetics surface-coupled hydrogenation intermediates while indirectly inhibiting intermediates. This intricate interplay unlocks reaction pathway toward products. Moreover, evaluation hydrogen activity allows rapid screening Cu-based catalyst aiming alcohols, qualitative agreement available experimental results, turn, confirms rationality mechanism. study discloses that suppressing are two fundamental strategies to improve selectivity, which provides insights design catalytic systems electrochemical desired

Язык: Английский

Процитировано

20
Enhanced CO2 Electroreduction to Multi‐Carbon Products on Copper via Plasma Fluorination DOI Creative Commons

Ziqian Zhou,

Xiao Hu,

Jiye Li

и другие.

Advanced Science, Год журнала: 2024, Номер 11(22)

Опубликована: Март 27, 2024

Abstract The electroreduction of carbon dioxide (CO 2 ) to multi‐carbon (C 2+ compounds offers a viable approach for the up‐conversion greenhouse gases into valuable fuels and feedstocks. Nevertheless, current industrial applications face limitations due unsatisfactory conversion efficiency high overpotential. Herein, facile scalable plasma fluorination method is reported. Concurrently, self‐evolution during CO employed control active sites Cu catalysts. copper catalyst modified with fluorine exhibits an impressive C Faradaic (FE) 81.8% at low potential −0.56 V (vs reversible hydrogen electrode) in alkaline flow cell. presence leads exposure stabilization high‐activity + species, enhancing adsorption *CO intermediates generation *CHO, facilitating subsequent dimerization. This results notably improved 13.1% significant reduction overpotential (≈100 mV) products. Furthermore, superior FE 81.6% 250 mA cm −2 , coupled energy 31.0%, can be achieved two‐electrode membrane electrode assembly electrolyzer utilizing fluorine‐modified catalyst. strategy provides novel insights controllable electronic modification surface reconstruction electrocatalysts practical potential.

Язык: Английский

Процитировано

7
Phosphorus Coordination in Second Shell of Single-Atom Cu Catalyst toward Acetate Production in CO Electroreduction DOI

Kanghua Miao,

Jingbo Wen,

Mi Luo

и другие.

Nano Letters, Год журнала: 2024, Номер unknown

Опубликована: Сен. 6, 2024

It is challenging to achieve highly efficient CO-CO coupling toward C

Язык: Английский

Процитировано

6
Criteria and cutting-edge catalysts for CO₂ electrochemical reduction at the industrial scale DOI Creative Commons

Asma Al Harthi,

Mohammed Al‐Abri, Hussein A. Younus

и другие.

Journal of CO2 Utilization, Год журнала: 2024, Номер 83, С. 102819 - 102819

Опубликована: Май 1, 2024

Converting waste or hazardous chemicals into valuable products is a paramount consideration from economic, environmental, and sustainability standpoints. Diverse strategies are under exploration to convert CO₂ fine chemicals, encompassing electrocatalysis, thermo- photo-catalysis, chemical fixation. Amid these avenues, the electrochemical reduction reaction (CO₂RR) emerges as exceptionally promising, driven by its manifold advantages growing accessibility of renewable electricity sources. While CO₂RR has witnessed substantial advancements, most endeavors remain in proof-of-concept phase, necessitating improved catalytic efficiency stability enable industrialization. Realizing industrial viability technology mandates meticulous myriad electrocatalyst-related factors. This review delves critical criteria recent materials with potential drive at an scale. These factors, akin other processes, closely relate activity, product selectivity, catalyst/system stability, catalyst cost. In this context, we investigated that define electrocatalysts industrially feasible, considering factors such Faradaic efficiency, current density, energy overpotential, choice materials. Furthermore, highlight prime examples demonstrating high for process categorize them based on products. To offer comprehensive perspective, also discusses fundamental principles CO₂RR, covering physicochemical properties CO₂, cell configurations, electrolyte compositions, role electrocatalysts. We address economic significance various

Язык: Английский

Процитировано

5