High-rate CO2-to-CH4 Electrosynthesis by Undercoordinated Cu Sites in Alkaline-Earth-Metal Perovskites with Strong Basicity

Article Chemistry, Multidisciplinary

MOF Encapsulating N-Heterocyclic Carbene-Ligated Copper Single-Atom Site Catalyst towards Efficient Methane Electrosynthesis

Shenghua Chen et al.

Summary: This study introduces an efficient CO2RR electrocatalyst with NHC-coordinated Cu SAS embedded in MOF, which exhibits high CH4 FE and TOF, attributed to the σ donation of NHC and the porosity of the catalyst.

ANGEWANDTE CHEMIE-INTERNATIONAL EDITION (2022)

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Article Chemistry, Multidisciplinary

Cation-Deficiency-Dependent CO2 Electroreduction over Copper-Based Ruddlesden-Popper Perovskite Oxides

Jiawei Zhu et al.

Summary: By engineering A-site cation deficiencies, the CO2 electroreduction properties of Cu-based RP perovskite oxides can be greatly enhanced, with specific relationships between selectivity and activity demonstrated at different levels of cation deficiencies. Such optimized properties are attributed to the introduction of oxygen vacancies and CuO/RP hybrids induced by the cation deficiencies, leading to improved adsorption/activation of key reaction species and manipulated reaction pathways.

ANGEWANDTE CHEMIE-INTERNATIONAL EDITION (2022)

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Article Chemistry, Multidisciplinary

Imparting CO2 Electroreduction Auxiliary for Integrated Morphology Tuning and Performance Boosting in a Porphyrin-based Covalent Organic Framework

Yi-Rong Wang et al.

Summary: This study has successfully prepared COF nanosheets with superior performance using a functionalizing exfoliation agent, providing a new possibility for the development of efficient CO2 electroreduction catalysts.

ANGEWANDTE CHEMIE-INTERNATIONAL EDITION (2022)

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Article Chemistry, Multidisciplinary

Selective methane electrosynthesis enabled by a hydrophobic carbon coated copper core-shell architecture

Xin Yu Zhang et al.

Summary: By using a copper-carbon-based catalyst with a hydrophobic core-shell architecture, the selectivity and activity of deep-reduction products (DRPs) for methane generation can be significantly improved, with a high Faradaic efficiency, showing potential applications in electrosynthesis.

ENERGY & ENVIRONMENTAL SCIENCE (2022)

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Article Chemistry, Multidisciplinary

Stabilizing Cu2+ Ions by Solid Solutions to Promote CO2 Electroreduction to Methane

Xianlong Zhou et al.

Summary: This study proposes a solid solution strategy to stabilize Cu2+ ions by incorporating them into a CeO2 matrix, which improves the performance of Cu-based catalysts in CO2 reduction reaction and enhances the efficiency of CH4 production.

JOURNAL OF THE AMERICAN CHEMICAL SOCIETY (2022)

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Article Chemistry, Multidisciplinary

The Role of Cation Acidity on the Competition between Hydrogen Evolution and CO2 Reduction on Gold Electrodes

Mariana C. O. Monteiro et al.

Summary: The presence of multivalent cations has been shown to affect CO2 electroreduction and competing hydrogen evolution reactions, with acidic cations favoring CO2RR at low overpotentials in acidic media. Cation acidity correlates with the activity and onset of the water reduction reaction, with weakly hydrated trivalent species exhibiting the highest activity. Among the nonacidic cations, Cs+, Ba2+, and Nd3+ show coordination to adsorbed CO2, enabling stabilization of the *CO2- intermediate and barrierless protonation to COOH and other reduction products.

JOURNAL OF THE AMERICAN CHEMICAL SOCIETY (2022)

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Article Chemistry, Multidisciplinary

Lithium Vacancy-Tuned [CuO4] Sites for Selective CO2 Electroreduction to C2+ Products

Chen Peng et al.

Summary: Utilizing an electrochemical delithiation strategy, a lithium vacancy-tuned Li2CuO2 catalyst was developed to enhance the efficiency and selectivity of electrochemical CO2 reduction to valuable multi-carbon (C2+) products. The introduction of lithium vacancies led to improved CO-CO coupling, resulting in a high Faradaic efficiency of 90.6 +/- 7.6% for C2+ and an outstanding partial current density of -706 +/- 32 mA cm(-2) under certain conditions. This work demonstrates a promising approach to produce controllable alkali metal vacancy-tuned Cu catalytic sites for C2+ products in electrochemical CO2 reduction.

SMALL (2022)

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Article Chemistry, Multidisciplinary

Constructing Cu-C Bonds in a Graphdiyne-Regulated Cu Single-Atom Electrocatalyst for CO2 Reduction to CH4

Guodong Shi et al.

Summary: By anchoring Cu single atoms on graphdiyne, we successfully constructed a Cu-C bond, which promotes the formation of CH4 during CO2 reduction and enhances catalytic performance.

ANGEWANDTE CHEMIE-INTERNATIONAL EDITION (2022)

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Article Chemistry, Physical

Electrochemically reconstructed perovskite with cooperative catalytic sites for CO2-to-formate conversion

Meng-Nan Zhu et al.

Summary: This study reveals that the reconstructed BaBiO3 perovskite can facilitate CO2-to-formate conversion through cooperative catalysis between A (Ba) and B (Bi) site elements. The electrochemical reduction triggers atom rearrangement and generates efficient Bi metallene, while the release of Ba2+ promotes CO2 adsorption and conversion.

APPLIED CATALYSIS B-ENVIRONMENTAL (2022)

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Article Chemistry, Physical

Stabilization of Undercoordinated Cu Sites in Strontium Copper Oxides for Enhanced Formation of C2+Products in ElectrochemicalCO2 Reduction

Xiao Kun Lu et al.

Summary: The electrochemical CO2 reduction reaction is a promising method for generating renewable fuels and commodities using renewable energy. By tuning the properties of copper oxide, the stability of undercoordinated and higher-valence-state copper sites can be improved, thereby enhancing ECO2RR performance.

ACS CATALYSIS (2022)

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Article Chemistry, Physical

Highly-Exposed Single-Interlayered Cu Edges Enable High-Rate CO2-to-CH4 Electrosynthesis

Chen Peng et al.

Summary: In this study, ultrathin CuGaO2 nanosheets with highly exposed single-interlayered Cu edges were synthesized, and they exhibited excellent CO2 electroreduction catalytic activity towards CH4. The results suggest a design strategy for promoting CH4 electrosynthesis by tuning both the crystal facets and Cu-Cu distance.

ADVANCED ENERGY MATERIALS (2022)

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Article Chemistry, Multidisciplinary

Engineering Water Molecules Activation Center on Multisite Electrocatalysts for Enhanced CO2 Methanation

Shenghua Chen et al.

Summary: This study presents a novel tandem catalyst that efficiently converts CO2 to CH4, improving CH4 yield and increasing Faradaic efficiency, offering a promising strategy for the rational design of high-efficiency multisite catalytic systems.

JOURNAL OF THE AMERICAN CHEMICAL SOCIETY (2022)

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Article Chemistry, Physical

Ga doping disrupts C-C coupling and promotes methane electroproduction on CuAl catalysts

Armin Sedighian Rasouli et al.

Summary: The effect of doping CuAl catalysts with elements such as Au, Zn, and Ga on the electrochemical CO2 reduction reaction (CO2RR) was studied. It was found that the presence of uniformly dispersed Ga is crucial in enhancing the performance of CO2RR-to-methane.

CHEM CATALYSIS (2022)

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Article Chemistry, Multidisciplinary

Emerging Electrochemical Processes to Decarbonize the Chemical Industry

Rong Xia et al.

Summary: This Perspective discusses the potential of electrification as an approach to reduce carbon emissions in the chemical industry. The authors analyze the current CO2 emissions in manufacturing and survey state-of-the-art electrosynthesis methods in three emission-intensive areas. They identify technical bottlenecks in electrifying chemical production and propose strategies to overcome these issues. The authors also provide their views on how electrochemical manufacturing can contribute to reducing carbon emissions, with the aim of inspiring further research efforts in this field.

JACS AU (2022)

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Review Chemistry, Multidisciplinary

Recent Progress in Electrocatalytic Methanation of CO2 at Ambient Conditions

Runbo Zhao et al.

Summary: This review systematically reviews the latest research on different electrocatalysts for the conversion of CO2 to CH4, as well as strategies for enhancing catalytic activity and selectivity. The review also highlights the importance of electrolyte influence on the activity and selectivity of CO2 electrocatalysis to CH4.

ADVANCED FUNCTIONAL MATERIALS (2021)

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Article Chemistry, Multidisciplinary

Enhanced Cuprophilic Interactions in Crystalline Catalysts Facilitate the Highly Selective Electroreduction of CO2 to CH4

Lei Zhang et al.

Summary: Cu(I)-based catalysts are essential for the electrocatalytic CO2 reduction, and in this study, two stable copper(I)-based catalysts with inherent cuprophilic interactions were synthesized for highly selective CO2-to-CH4 conversion. The substitution of sulfate radicals with hydroxyl radicals led to a dynamic crystal structure transition, enhancing the cuprophilic interactions inside the catalyst structure. The enhanced cuprophilic interactions in NNU-33(H) showed outstanding CH4 selectivity, representing the best crystalline catalyst for electrocatalytic CO2-to-CH4 conversion.

JOURNAL OF THE AMERICAN CHEMICAL SOCIETY (2021)

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Article Multidisciplinary Sciences

Coordination environment dependent selectivity of single-site-Cu enriched crystalline porous catalysts in CO2 reduction to CH4

Yu Zhang et al.

Summary: The study demonstrates that the ECR selectivity depends strongly on the Cu site coordination environment in crystalline porous catalysts, with Cu-DBC showing higher selectivity and activity due to the lower energy barriers of Cu-O-4 sites during the ECR process. This provides a platform for constructing highly selective ECR catalysts with potential applications in the energy conversion field.

NATURE COMMUNICATIONS (2021)

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Article Chemistry, Physical

High-purity and high-concentration liquid fuels through CO2 electroreduction

Peng Zhu et al.

Summary: Liquid fuels generated from the electrochemical CO2 reduction reaction have high energy densities and storage advantages, but are often produced in low concentrations and mixed with impurities due to limitations in current traditional CO2 electrolyzers and CO2RR catalysts. Strategies in reactor engineering and catalyst improvement are proposed to overcome these challenges and make electrochemical production of liquid fuels more competitive in the future.

NATURE CATALYSIS (2021)

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Article Multidisciplinary Sciences

Self-assembly of anthraquinone covalent organic frameworks as 1D superstructures for highly efficient CO2 electroreduction to CH4

Ming Liu et al.

Summary: This study presents the design of selective and efficient COFs-based electrocatalysts with tunable morphology for efficient CO2 reduction reaction (CO2RR) to CH4. By introducing a specific reaction, COFs with tunable morphology were produced, demonstrating the importance of these superstructures for efficient CO2RR. The obtained COF-based superstructures showed superior performance in electrocatalytic CO2RR, providing a general methodology for exploring morphology-controlled COFs.

SCIENCE BULLETIN (2021)

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Article Chemistry, Multidisciplinary

Lithiation-Enabled High-Density Nitrogen Vacancies Electrocatalyze CO2 to C2 Products

Chen Peng et al.

Summary: This study demonstrates that high-density nitrogen vacancies formed on cubic copper nitrite can efficiently catalyze the CO-CO coupling to form key OCCO* intermediate for the production of valuable C-2 products in electrochemical CO2 reduction. The Cu3Nx catalyst with abundant nitrogen vacancies shows one of the highest Faradaic efficiencies towards C-2 products and outstanding electrochemical stability at high current densities, providing an attractive approach for the creation of catalytic centers towards multicarbon products in electrochemical CO2 reduction.

ADVANCED MATERIALS (2021)

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Article Chemistry, Multidisciplinary

Geometric Modulation of Local CO Flux in Ag@Cu2O Nanoreactors for Steering the CO2RR Pathway toward High-Efficacy Methane Production

Likun Xiong et al.

Summary: A novel CO2RR catalyst with a yolk-shell nanocell structure was developed, allowing for the regulation of the CO2RR pathway by adjusting the Ag core and Cu2O shell. Density functional theory simulations showed that lower CO coverage favored methane formation by stabilizing the intermediate *CHO. The catalyst demonstrated excellent CO2RR performance in a flow cell, achieving high methane selectivity and efficiency.

ADVANCED MATERIALS (2021)

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Article Chemistry, Multidisciplinary

Implanting Numerous Hydrogen-Bonding Networks in a Cu-Porphyrin-Based Nanosheet to Boost CH4 Selectivity in Neutral-Media CO2 Electroreduction

Yi-Rong Wang et al.

Summary: This study successfully utilized a Cu-porphyrin-based large-scale and ultrathin nanosheet as an electrocatalyst for CO2RR, achieving high CO2 conversion efficiency under neutral conditions. By constructing hydrogen-bonding networks, proton migration and intermediate stabilization were facilitated, providing a new pathway for efficient CO2RR catalyst development.

ANGEWANDTE CHEMIE-INTERNATIONAL EDITION (2021)

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Article Materials Science, Multidisciplinary

Evaluation of Ca2CuO3 as an oxygen carrier material

A. A. Burdina et al.

Summary: The study found that Ca2CuO3 can be used as an effective oxygen carrier material with promising applications in chemical looping combustion. It has a fast rate of oxygen release, high oxygen storage capacity, and produces hydrocarbon oxidation products free of CO.

MATERIALS LETTERS (2021)

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Article Multidisciplinary Sciences

CO2 reduction on pure Cu produces only H2 after subsurface O is depleted: Theory and experiment

Guiji Liu et al.

Summary: Experimental validation shows that maintaining sufficient subsurface oxygen on Cu catalysts is essential for long-term C2 production, with Cu2O significantly increasing the rate of C2 production compared to pure Cu.

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

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Review Chemistry, Multidisciplinary

New advances in using Raman spectroscopy for the characterization of catalysts and catalytic reactions

Christian Hess

Summary: Raman spectroscopy is a powerful vibrational spectroscopic technique that has been widely used for the characterization of catalysts and catalytic reactions. It provides important information on catalyst structures, adsorbates, and reaction intermediates, offering key insights into studying working catalysts.

CHEMICAL SOCIETY REVIEWS (2021)

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Article Chemistry, Multidisciplinary