Molecular Modulation of Sequestered Copper Sites for Efficient Electroreduction of Carbon Dioxide to Methane DOI
Kefan Zhang, Jie Xu,

Tianran Yan

et al.

Advanced Functional Materials, Journal Year: 2023, Volume and Issue: 33(17)

Published: Feb. 1, 2023

Abstract The sustainable production of methane (CH 4 ) via the electrochemical conversion carbon dioxide (CO 2 is an appealing approach to simultaneously mitigating emissions and achieving energy storage in chemical bonds. Copper (Cu) a unique material produce hydrocarbons oxygenates. However, selective generation on Cu remains great challenge due preferential *CO dimerization pathway toward multi‐carbon (C 2+ products at neighboring catalytic sites. Herein, conjugated copper phthalocyanine polymer (CuPPc) designed by facile solid‐state method for highly CO ‐to‐CH conversion. spatially isolated CuN sites CuPPc favor protonation generate key *CHO intermediate, thus significantly promoting formation CH . As result, catalyst exhibits high Faradaic efficiency 55% partial current density 18 mA cm −2 −1.25 V versus reversible hydrogen electrode. It also stably operates 12 h. This study may offer new solution regulating environment active development efficient copper‐based catalysts reduction.

Language: Английский

Electrochemical CO2RR to C2+ products: A vision of dynamic surfaces of Cu-based catalysts DOI
Jinxin Wang, Jiaqi Zhang, Chen Chen

et al.

CHINESE JOURNAL OF CATALYSIS (CHINESE VERSION), Journal Year: 2025, Volume and Issue: 68, P. 83 - 102

Published: Jan. 1, 2025

Language: Английский

Citations

3
Selective and Stable Ethanol Synthesis via Electrochemical CO2 Reduction in a Solid Electrolyte Reactor DOI
Tae‐Ung Wi,

Zachary Levell,

Shaoyun Hao

et al.

ACS Energy Letters, Journal Year: 2025, Volume and Issue: unknown, P. 822 - 829

Published: Jan. 15, 2025

Electrochemical CO2 reduction to ethanol faces challenges such as low selectivity, a product mixture with liquid electrolyte, and poor catalyst/reactor stability. Here, we developed grain-rich zinc-doped Cu2O precatalyst that presented high Faradaic efficiency of over 40% under current density 350 mA·cm–2. Our functional theory (DFT) simulation suggested Zn atoms inside the structure have greater carbophilicity than Cu help facilitate *CHCHO formation, key reaction intermediate toward instead other C2 products. A ratio between ethylene (FEEtOH/FEC2H4) reached 2.34 in precatalyst, representing an 4-fold improvement compared bare precatalyst. By integrating this Cu-based catalyst into porous solid electrolyte (PSE) reactor salt-managing design, achieved stable production for 180 h 250 mA·cm–2 while maintaining selectivity at ∼30%.

Language: Английский

Citations

2
A Cation Concentration Gradient Approach to Tune the Selectivity and Activity of CO2 Electroreduction DOI
Wenhao Ren, Aoni Xu, Karen Chan

et al.

Angewandte Chemie International Edition, Journal Year: 2022, Volume and Issue: 61(49)

Published: Oct. 14, 2022

The linear scaling relationship of the binding energies different intermediates limits catalyst performance in CO2 electroreduction. Here we demonstrate a cation concentration gradient strategy to promote activity and tune selectivity electroreduction, thereby breaking relationship. In optimal concentrations potassium acetate (KAc) electrolyte, Cu, Ag catalysts deliver current densities that are 7.1, 3.2, 2.7 times higher than those obtained 0.5 M KAc for C2 H4 , CO, formate production, respectively. Increasing also changes from CO on Ag, products Cu. situ surface-enhanced Raman spectroscopy computational simulations reveal changed at electrolyte concentrations, which is due local electrostatic interaction modulated by cations electrode surface.

Language: Английский

Citations

59
Electrochemical carbon–carbon coupling with enhanced activity and racemate stereoselectivity by microenvironment regulation DOI Creative Commons

Kejian Kong,

An-Zhen Li,

Ye Wang

et al.

Nature Communications, Journal Year: 2023, Volume and Issue: 14(1)

Published: Oct. 30, 2023

Enzymes are characteristic of catalytic efficiency and specificity by maneuvering multiple components in concert at a confined nanoscale space. However, achieving such configuration artificial catalysts remains challenging. Herein, we report microenvironment regulation strategy modifying carbon paper with hexadecyltrimethylammonium cations, delivering electrochemical carbon-carbon coupling benzaldehyde enhanced activity racemate stereoselectivity. The modified electrode-electrolyte interface creates an optimal for electrocatalysis-it engenders dipolar interaction the reaction intermediate, giving 2.2-fold higher rate (from 0.13 to 0.28 mmol h

Language: Английский

Citations

40
High‐Concentration Electrosynthesis of Formic Acid/Formate from CO2: Reactor and Electrode Design Strategies DOI Creative Commons

Yizhu Kuang,

Hesamoddin Rabiee, Lei Ge

et al.

Energy & environment materials, Journal Year: 2023, Volume and Issue: 6(6)

Published: Feb. 2, 2023

The electrochemical CO 2 reduction reaction (CO RR), driven by renewable energy, provides a potential carbon‐neutral avenue to convert into valuable fuels and feedstocks. Conversion of formic acid/formate is considered one the economical feasible methods, owing their high energy densities, ease distribution storage. separation from mixtures accounts for majority overall RR process cost, while increment product concentration can lead remarkably. In this paper, we give an overview recent strategies highly concentrated products in RR. complex with several different products, as it has intermediates pathways. Therefore, review focuses on study that enhance targeted yield, such all‐solid‐state reactor design deliver during electrolyzer. Firstly, some novel electrolyzers are introduced engineering strategy improve reduce cost downstream separations. Also, planar gas diffusion electrodes (GDEs) high‐concentration summarized. Finally, existing technological challenges highlighted, further research recommendations achieve This provide inspiration future economic benefits

Language: Английский

Citations

38
Advanced Catalyst Design and Reactor Configuration Upgrade in Electrochemical Carbon Dioxide Conversion DOI

Zhitong Wang,

Yansong Zhou, Peng Qiu

et al.

Advanced Materials, Journal Year: 2023, Volume and Issue: 35(52)

Published: Aug. 20, 2023

Abstract Electrochemical carbon dioxide reduction reaction (CO 2 RR) driven by renewable energy shows great promise in mitigating and potentially reversing the devastating effects of anthropogenic climate change environmental degradation. The simultaneous synthesis energy‐dense chemicals can meet global demand while decoupling emissions from economic growth. However, development CO RR technology faces challenges catalyst discovery device optimization that hinder their industrial implementation. In this contribution, a comprehensive overview current state research is provided, starting with background motivation for technology, followed fundamentals evaluated metrics. Then underlying design principles electrocatalysts are discussed, emphasizing structure–performance correlations advanced electrochemical assembly cells increase selectivity throughput. Finally, review looks to future identifies opportunities innovation mechanism discovery, material screening strategies, assemblies move toward carbon‐neutral society.

Language: Английский

Citations

38
Promoting CO2 Electroreduction to Multi‐Carbon Products by Hydrophobicity‐Induced Electro‐Kinetic Retardation DOI

Mengjiao Zhuansun,

Yue Liu, Ruihu Lu

et al.

Angewandte Chemie International Edition, Journal Year: 2023, Volume and Issue: 62(41)

Published: Aug. 23, 2023

Advancing the performance of Cu-catalyzed electrochemical CO2 reduction reaction (CO2 RR) is crucial for its practical applications. Still, wettable pristine Cu surface often suffers from low exposure to , reducing Faradaic efficiencies (FEs) and current densities multi-carbon (C2+ ) products. Recent studies have proposed that increasing availability by cation-exchange ionomers can enhance C2+ product formation rates. However, due rapid consumption *CO, such promotion in kinetics shorten residence *CO whose adsorption determines selectivity, thus resulting FEs remain low. Herein, we discover electro-kinetic retardation caused strong hydrophobicity quaternary ammonium group-functionalized polynorbornene greatly prolong on Cu. This unconventional effect demonstrated increased Tafel slopes decreased sensitivity coverage change potentials. As a result, strongly hydrophobic electrodes exhibit ≈90 % at partial density 223 mA cm-2 more than twice bare or hydrophilic surfaces.

Language: Английский

Citations

34
Electrode and cell design for CO2 reduction: A viewpoint DOI Creative Commons
Claudio Ampelli,

Francesco Tavella,

Daniele Giusi

et al.

Catalysis Today, Journal Year: 2023, Volume and Issue: 421, P. 114217 - 114217

Published: May 18, 2023

The electrocatalytic reduction of carbon dioxide (CO2RR) is a crucial technology to develop the decarbonisation strategy for circularity and producing solar fuels substituting fossil fuels. This viewpoint discusses role electrode reactor design as main factor in determining performance CO2RR, at least under reaction conditions relevant industrial scalability, evidencing need overturn current strategic vision focused more on improving characteristics materials. Many parameters characterising performances (such Faradaic efficiency, selectivity potential onset, besides density) are strongly influenced typically dominated (under conditions) by effective population adspecies surface, which is, turn, related mass control transport resistances, local pH changes, multiphase boundaries, wettability other aspects. Even preliminary screening catalysts could be incorrect, not operating representative conditions, thus without properly choosing reactor. Advanced electrode/reactor designs, e.g., based gas-diffusion electrodes (GDEs) that avoid having liquid electrolyte (zero-gap design), necessary improve CO2RR scalability applications. situ catalyst nanoparticle reconstruction may depend these Electrochemical characterization methods like electrochemical impedance spectroscopy (EIS) right approach study reactions, providing indications controlling elements determine electrocatalyst/electrode performances.

Language: Английский

Citations

33
Theory-guided synthesis of heterostructured [email protected] catalyst towards superior electrochemical reduction of CO2 to C2 products DOI
Dong Xiang,

Kunzhen Li,

Manzhi Li

et al.

Materials Today Physics, Journal Year: 2023, Volume and Issue: 33, P. 101045 - 101045

Published: March 14, 2023

Language: Английский

Citations

29
A Universal Approach for Sustainable Urea Synthesis via Intermediate Assembly at the Electrode/Electrolyte Interface DOI

Xiaojin Tu,

Xiaorong Zhu,

Shuowen Bo

et al.

Angewandte Chemie International Edition, Journal Year: 2023, Volume and Issue: 63(3)

Published: Dec. 7, 2023

Abstract Electrocatalytic C−N coupling process is indeed a sustainable alternative for direct urea synthesis and co‐upgrading of carbon dioxide nitrate wastes. However, the main challenge lies in unactivated process. Here, we proposed strategy intermediate assembly with alkali metal cations to activate at electrode/electrolyte interface. Urea activity follows trend Li + <Na <Cs <K . In presence K , world‐record performance was achieved yield rate 212.8±10.6 mmol h −1 g on single‐atom Co supported TiO 2 catalyst −0.80 V versus reversible hydrogen electrode. Theoretical calculations operando synchrotron‐radiation Fourier transform infrared measurements revealed that energy barriers were significantly decreased via mediated assembly. By applying this various catalysts, demonstrate interface universal approach boost synthesis.

Language: Английский

Citations

28