4.8 Article

Directing the Selectivity of CO Electrolysis to Acetate by Constructing Metal-Organic Interfaces

相关参考文献

注意:仅列出部分参考文献,下载原文获取全部文献信息。
Article Nanoscience & Nanotechnology

Coverage-driven selectivity switch from ethylene to acetate in high-rate CO2/CO electrolysis

Pengfei Wei et al.

Summary: Tuning catalyst microenvironments by electrolytes and organic modifications improves the performance of CO2 electrolysis. The influence of mixed CO/CO2 feeds from incomplete industrial combustion on catalyst microenvironments has been investigated. CO/CO2 co-electrolysis over CuO nanosheets was studied in an alkaline membrane electrode assembly electrolyser. The optimized conditions achieved high Faradaic efficiency, partial current density, selectivity, and yield, outperforming thermocatalytic CO hydrogenation. The scale-up demonstration using an electrolyser stack showed high rates of ethylene and acetate formation.

NATURE NANOTECHNOLOGY (2023)

Article Chemistry, Physical

Promoting Electrolysis of Carbon Monoxide toward Acetate and 1-Propanol in Flow Electrolyzer

Shengyuan Guo et al.

Summary: Acetic acid/acetate is an important precursor for chemical manufacturing and biofuel synthesis. Carbon monoxide electrolysis can enhance the selectivity for multicarbon products, and this research explores practical approaches to improve acetate and 1-propanol selectivity and yield using a copper catalyst. The pH and catalyst loading were found to strongly influence the performance, and in situ Raman and multiphysics modeling provided insights into the mechanism of improvement.

ACS ENERGY LETTERS (2023)

Article Chemistry, Multidisciplinary

Interfacial Synergy between the Cu Atomic Layer and CeO2 Promotes CO Electrocoupling to Acetate

Tang Yang et al.

Summary: Spraying atomically layered Cu atoms onto CeO2 nanorods (Cu-CeO2) enables the rational design of a catalyst for highly selective CO/CO2 reduction to C2+ liquid products such as acetate.

ACS NANO (2023)

Article Chemistry, Multidisciplinary

Synergy of Cu/C3N4 Interface and Cu Nanoparticles Dual Catalytic Regions in Electrolysis of CO to Acetic Acid

Xupeng Yan et al.

Summary: It was discovered that Cu nanoparticles supported on graphitic carbon nitride (Cu-CN) with the appropriate size exhibited a high acetate faradaic efficiency of 62.8% and a partial current density of 188 mA cm(-2) in the electrochemical reduction of CO to acetic acid. Experimental and theoretical studies revealed that the Cu/C3N4 interface and metallic Cu surface synergistically promoted the conversion of CO to acetic acid. The continuous production of acetic acid in a porous solid electrolyte reactor further demonstrated the potential of Cu-CN catalyst in industrial applications.

ANGEWANDTE CHEMIE-INTERNATIONAL EDITION (2023)

Article Chemistry, Multidisciplinary

Metal-Organic Framework Derived Cu-Ag Interface for Selective Carbon Monoxide Electroreduction to Acetate

Chang Liu et al.

Summary: Researchers have developed a two-dimensional Ag-modified Cu metal-organic framework that shows high selectivity to acetate at high current density.

CHEMISTRY-A EUROPEAN JOURNAL (2023)

Article Multidisciplinary Sciences

Constrained C2 adsorbate orientation enables CO-to-acetate electroreduction

Jian Jin et al.

Summary: The carbon dioxide and carbon monoxide electroreduction reactions are promising pathways for decarbonization of chemical manufacture. By dispersing a low concentration of copper atoms in a host metal, acetate can be selectively synthesized from carbon monoxide. Through catalyst design and reactor engineering, high selectivity and Faradaic efficiency for acetate production have been achieved.

NATURE (2023)

Article Chemistry, Physical

Atomically Dispersed Cu-Au Alloy for Efficient Electrocatalytic Reduction of Carbon Monoxide to Acetate

Qian Sun et al.

Summary: We report a Cu-Au alloy catalyst with abundant atomic Cu-Au interfaces for efficient electrocatalytic carbon monoxide reduction reaction (CORR) towards acetate production. The atomic Cu-Au interfaces exhibit unique geometric and electronic structures, resulting in improved acetate activity and selectivity surpassing metallic Cu nanoparticles and CuAu bulk alloys. A high Faradaic efficiency of 39% and large partial current density of 217 mA cm-2 were achieved in an alkaline flow cell.

ACS CATALYSIS (2023)

Article Chemistry, Physical

Amino-Functionalized Cu for Efficient Electrochemical Reduction of CO to Acetate

Yinyin Wang et al.

Summary: Selective electrochemical reduction of CO to acetate can be achieved on an amino functionalized Cu surface. The Cu@NH2 catalyst shows significant catalytic performance with a CO-to-acetate Faradaic efficiency of 51.5% and an acetate partial current density of around 150 mA cm-2 at -0.75 V versus RHE. The amino groups on the Cu surface help maintain the low valence state of Cu and the H delta+ in the amino groups stabilize the oxygen-containing intermediates, promoting the formation of acetate through *CO-*CHO coupling.

ACS CATALYSIS (2023)

Article Chemistry, Multidisciplinary

Coordination Polymer Electrocatalysts Enable Efficient CO-to-Acetate Conversion

Mingchuan Luo et al.

Summary: Upgrading carbon dioxide/monoxide to multi-carbon C2+ products using renewable electricity offers a sustainable approach to fuel and chemical production. A new coordination polymer catalyst consisting of Cu(I) and benzimidazole units linked via Cu(I)-imidazole coordination bonds enables selective reduction of CO to acetate with a 61% Faradaic efficiency. The catalyst integrated in a cation exchange membrane-based membrane electrode assembly allows stable acetate electrosynthesis and achieves concentrated acetate collection, high CO-to-acetate conversion efficiency, and good acetate full-cell energy efficiency.

ADVANCED MATERIALS (2023)

Article Chemistry, Physical

Electrochemical CO2 Reduction over Copper Phthalocyanine Derived Catalysts with Enhanced Selectivity for Multicarbon Products

Jie Zhang et al.

Summary: Metal complexes have been found to be selective and active catalysts for electrochemical CO2 reduction (CO2RR). Using in situ Raman, X-ray photoelectron spectroscopy, and advanced electron microscopy, researchers have discovered that copper phthalocyanine (CuPc) undergoes reconstruction during CO2RR. Further investigations have revealed that CuPc demetalates to Cu atoms, which then agglomerate to form Cu clusters and Cu nanoparticles (NPs). The size of the Cu NPs is highly dependent on experimental parameters, and the selectivity of multicarbon products is positively correlated with NP size. This study provides important insights for future applications of metal complex catalysts in CO2RR and inspires the design of advanced electrocatalysts for other electrochemical reactions.

ACS CATALYSIS (2023)

Article Chemistry, Physical

Trends in Electrocatalysis: The Microenvironment Moves to Center Stage

Marcel Schreier et al.

ACS Energy Letters (2023)

Article Energy & Fuels

Imidazolium-functionalized Mo3P nanoparticles with an ionomer coating for electrocatalytic reduction of CO2 to propane

Mohammadreza Esmaeilirad et al.

Summary: Research shows that ionomer-coated imidazolium-functionalized Mo3P nanoparticles produce propane with high activity and selectivity by electrochemical reduction of CO2, which is significant for achieving the direct production of C3+ molecules from CO2.

NATURE ENERGY (2023)

Article Chemistry, Physical

Experimental evidence of distinct sites for CO2-to-CO and CO conversion on Cu in the electrochemical CO2 reduction reaction

Wenqiang Gao et al.

Summary: The electrochemical CO2 reduction reaction on Cu is believed to occur via two consecutive and orthogonal reaction steps, but we provide experimental evidence challenging this assumption. We show that CO2 promotes the electrochemical CO reduction reaction and there are at least two types of Cu sites, with one being more active in CO2-to-CO conversion and the other favoring further reduction to C2+. CO adsorbed on Cu-CO is more active towards C2+ formation compared to Cu-CO2. Isotopic labelling experiments suggest Cu-CO2 and Cu-CO correspond to Cu(111)-like and defect sites, respectively. These insights suggest the possibility of controlling selectivity in the CO2 reduction reaction.

NATURE CATALYSIS (2023)

Article Chemistry, Multidisciplinary

Tailoring acidic microenvironments for carbon-efficient CO2 electrolysis over a Ni-N-C catalyst in a membrane electrode assembly electrolyzer

Hefei Li et al.

Summary: A carbon-efficient CO2 electrolysis strategy using a zero-gap acidic membrane electrode assembly electrolyzer is proposed to convert CO2 into valuable fuels and chemicals. The microenvironments of a Ni-N-C catalyst are optimized by adjusting the anolyte composition and CO2 pressure. Under optimal conditions, a CO faradaic efficiency of 95% and a CO production rate of 13 mL min(-1) are achieved. This strategy shows higher energy efficiency and reduced carbon loss compared to alkaline CO2 electrolysis.

ENERGY & ENVIRONMENTAL SCIENCE (2023)

Article Chemistry, Physical

Amino-Functionalized Cu for Efficient Electrochemical Reduction of CO to Acetate

Yinyin Wang et al.

Summary: Electrosynthesis of valuable chemicals from CO2 or CO offers a promising approach to store renewable electricity and reduce carbon emission. In this study, amino functionalized Cu surface (Cu@NH2) derived from in situ electroreduction of copper ammonia chloride complexes exhibits significant catalytic performance for CO reduction to acetate. The amino groups on the Cu surface play a crucial role in maintaining the low valence state of Cu and stabilizing the oxygen-containing intermediates, thus promoting the coupling reaction between *CO and *CHO to form acetate.

ACS CATALYSIS (2023)

Article Chemistry, Multidisciplinary

Electrocatalysts Derived from Copper Complexes Transform CO into C2+ Products Effectively in a Flow Cell

Shaoxuan Ren et al.

Summary: In this study, a copper phthalocyanine catalyst layer was used to successfully electrolyze CO2 into high-value chemicals and fuels. Compared to traditional CO2 electrolysis, CO electrolysis can produce products containing two or more carbon atoms more efficiently. These findings provide new strategies for the development of sustainable carbon-neutral chemicals and fuels.

CHEMISTRY-A EUROPEAN JOURNAL (2022)

Article Chemistry, Physical

Asymmetrical C-C Coupling for Electroreduction of CO on Bimetallic Cu-Pd Catalysts

Hao Shen et al.

Summary: This study reports the selective reduction of CO to acetate using Cu-Pd bimetallic electrocatalysts and explores the underlying mechanism. The results demonstrate that the bimetallic catalyst exhibits high activity and selectivity for the conversion of CO to acetate.

ACS CATALYSIS (2022)

Article Chemistry, Physical

Selective CO-to-acetate electroreduction via intermediate adsorption tuning on ordered Cu-Pd sites

Yali Ji et al.

Summary: In this study, a novel copper-palladium intermetallic compound catalyst was developed to enhance the hydrogenation reduction of carbon monoxide, thereby promoting the formation of acetate. The catalyst exhibited high selectivity and efficiency for acetate production, and demonstrated good performance in long-term stability tests.

NATURE CATALYSIS (2022)

Article Chemistry, Physical

Upcycling CO2 into energy-rich long-chain compounds via electrochemical and metabolic engineering

Tingting Zheng et al.

Summary: Upcycling carbon dioxide into value-added products is a promising solution to environmental issues and achieving a circular economy. This study presents a hybrid electro-biosystem that efficiently converts CO2 to glucose and can be extended to produce other products.

NATURE CATALYSIS (2022)

Article Energy & Fuels

2022 roadmap on low temperature electrochemical CO2 reduction

Ifan E. L. Stephens et al.

Summary: This article reviews recent progress in electrochemical CO2 reduction, discusses the challenges towards commercialization, and highlights opportunities for further research. The goal is to establish a low- or zero-emission carbon cycle.

JOURNAL OF PHYSICS-ENERGY (2022)

Article Chemistry, Multidisciplinary

Few-Atom Copper Catalyst for the Electrochemical Reduction of CO to Acetate: Synergetic Catalysis between Neighboring Cu Atoms

Weifeng Rong et al.

Summary: A study reveals that the synergetic interaction between neighboring copper atoms greatly enhances the production of acetate in the CO electroreduction reaction. Experimental results show that the copper few-atom catalyst (Cu FAC) exhibits high efficiency, high purity, and excellent stability in producing acetate. Theoretical studies provide insights into the mechanism of this synergetic catalysis.

CCS CHEMISTRY (2022)

Article Energy & Fuels

Bifunctional ionomers for efficient co-electrolysis of CO2 and pure water towards ethylene production at industrial-scale current densities

Wenzheng Li et al.

Summary: The use of bifunctional ionomers as polymer electrolytes enables CO2 activation and ethylene synthesis in solid-state polymer electrolyzers running on pure water.

NATURE ENERGY (2022)

Article Chemistry, Physical

Enhancing acetate selectivity by coupling anodic oxidation to carbon monoxide electroreduction

Sean Overa et al.

Summary: This study presents an internally coupled purification strategy to improve the concentration and purity of acetate in CO electrolysis. By utilizing an alkaline-stable anion exchange membrane and a selective ethanol partial oxidation anode, the CO reduction product stream was controlled, resulting in stable operation of the CO electrolyzer and production of high concentration and high purity acetate product stream.

NATURE CATALYSIS (2022)

Article Chemistry, Multidisciplinary

The mechanism for acetate formation in electrochemical CO(2) reduction on Cu: selectivity with potential, pH, and nanostructuring

Hendrik H. Heenen et al.

Summary: Nanostructured Cu catalysts have been found to enhance the selectivities and geometric activities for high value C-C coupled products in electrochemical CO(2) reduction reaction. The selectivity mechanism for acetate formation has been elucidated through ab initio simulations, kinetic-transport model, and loading dependent experiments, indicating that the selectivity is influenced by variations in electrolyte pH and local mass transport properties rather than Cu's intrinsic activity.

ENERGY & ENVIRONMENTAL SCIENCE (2022)

Article Multidisciplinary Sciences

Direct and continuous generation of pure acetic acid solutions via electrocatalytic carbon monoxide reduction

Peng Zhu et al.

Summary: The direct and continuous generation of pure acetic acid solutions via electrochemical CO reduction is demonstrated through rational designs in a Cu catalyst and PSE reactor. The Cu nanocube catalyst shows unprecedented acetate performance with a maximal Faradaic efficiency of 43% and ultrahigh relative purity of up to 98 wt%, along with excellent stability of over 150 hours continuous operation.

PROCEEDINGS OF THE NATIONAL ACADEMY OF SCIENCES OF THE UNITED STATES OF AMERICA (2021)

Article Chemistry, Physical

Electrochemical CO2-to-ethylene conversion on polyamine-incorporated Cu electrodes

Xinyi Chen et al.

Summary: A Cu-polyamine hybrid catalyst was developed to significantly enhance the selectivity for ethylene production in CO2 electrochemical conversion. Incorporating polyamine altered surface reactivity, leading to improved product selectivity at high current densities.

NATURE CATALYSIS (2021)

Article Chemistry, Physical

Cascade CO2 electroreduction enables efficient carbonate-free production of ethylene

Adnan Ozden et al.

Summary: CO2 electroreduction is a promising method to convert waste emissions into chemicals, but the process suffers from CO2 loss to carbonate, consuming a large amount of energy input. By coupling a cascade SOEC-MEA approach, the energy efficiency can be improved, reducing energy intensity.
Article Multidisciplinary Sciences

Molecular tuning of CO2-to-ethylene conversion

Fengwang Li et al.

NATURE (2020)

Article Chemistry, Multidisciplinary

Control of Molecular Bonding Strength on Metal Catalysts with Organic Monolayers for CO2 Reduction

Jing Zhang et al.

JOURNAL OF THE AMERICAN CHEMICAL SOCIETY (2020)

Editorial Material Multidisciplinary Sciences

The future of low-temperature carbon dioxide electrolysis depends on solving one basic problem

Joshua A. Rabinowitz et al.

NATURE COMMUNICATIONS (2020)

Letter Materials Science, Multidisciplinary

N-modulated Cu+ for efficient electrochemical carbon monoxide reduction to acetate

Fenglou Ni et al.

SCIENCE CHINA-MATERIALS (2020)

Article Chemistry, Multidisciplinary

Electrocatalysis at Organic-Metal Interfaces: Identification of Structure-Reactivity Relationships for CO2 Reduction at Modified Cu Surfaces

Aya K. Buckley et al.

JOURNAL OF THE AMERICAN CHEMICAL SOCIETY (2019)

Review Chemistry, Multidisciplinary

Progress and Perspectives of Electrochemical CO2 Reduction on Copper in Aqueous Electrolyte

Stephanie Nitopi et al.

CHEMICAL REVIEWS (2019)

Article Multidisciplinary Sciences

Molecular electrocatalysts can mediate fast, selective CO2 reduction in a flow cell

Shaoxuan Ren et al.

SCIENCE (2019)

Article Chemistry, Physical

Transition state and product diffusion control by polymer-nanocrystal hybrid catalysts

Andrew R. Riscoe et al.

NATURE CATALYSIS (2019)

Editorial Material Chemistry, Physical

HETEROGENEOUS CATALYSIS Confined microenvironment for catalysis control

Qiang Fu et al.

NATURE CATALYSIS (2019)

Article Multidisciplinary Sciences

Active sites of copper-complex catalytic materials for electrochemical carbon dioxide reduction

Zhe Weng et al.

NATURE COMMUNICATIONS (2018)

Article Chemistry, Physical

High-rate electroreduction of carbon monoxide to multi-carbon products

Matthew Jouny et al.

NATURE CATALYSIS (2018)

Article Chemistry, Physical

Raman Spectroscopic Observation of Gradual Polymorphic Transition and Phonon Modes in CuPc Nanorod

Uttam K. Ghorai et al.

JOURNAL OF PHYSICAL CHEMISTRY C (2017)

Article Chemistry, Physical

Spectroscopic Observation of Reversible Surface Reconstruction of Copper Electrodes under CO2 Reduction

Charuni M. Gunathunge et al.

JOURNAL OF PHYSICAL CHEMISTRY C (2017)

Article Chemistry, Multidisciplinary

Enhancing CO2 Electroreduction with the Metal-Oxide Interface

Dunfeng Gao et al.

JOURNAL OF THE AMERICAN CHEMICAL SOCIETY (2017)

Article Chemistry, Physical

Tuning Catalytic Selectivity at the Mesoscale via Interparticle Interactions

Hemma Mistry et al.

ACS CATALYSIS (2016)

Article Multidisciplinary Sciences

A Local Proton Source Enhances CO2 Electroreduction to CO by a Molecular Fe Catalyst

Cyrille Costentin et al.

SCIENCE (2012)

Article Chemistry, Physical

Universal transition state scaling relations for (de)hydrogenation over transition metals

S. Wang et al.

PHYSICAL CHEMISTRY CHEMICAL PHYSICS (2011)

Article Chemistry, Multidisciplinary

How copper catalyzes the electroreduction of carbon dioxide into hydrocarbon fuels

Andrew A. Peterson et al.

ENERGY & ENVIRONMENTAL SCIENCE (2010)

Article Chemistry, Multidisciplinary

Semiempirical GGA-type density functional constructed with a long-range dispersion correction

Stefan Grimme

JOURNAL OF COMPUTATIONAL CHEMISTRY (2006)

Article Materials Science, Multidisciplinary

A fast and robust algorithm for Bader decomposition of charge density

Graeme Henkelman et al.

COMPUTATIONAL MATERIALS SCIENCE (2006)

Article Chemistry, Physical

The Bronsted-Evans-Polanyi relation and the volcano curve in heterogeneous catalysis

T Bligaard et al.

JOURNAL OF CATALYSIS (2004)