Reaction Environment Regulation for Electrocatalytic CO₂ Reduction in Acids

Angewandte Chemie International Edition, Год журнала: 2024, Номер 63(26)

Опубликована: Апрель 19, 2024

The electrocatalytic CO

Язык: Английский

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Electronic Structure Design of Transition Metal-Based Catalysts for Electrochemical Carbon Dioxide Reduction

ACS Nano, Год журнала: 2024, Номер 18(14), С. 9823 - 9851

Опубликована: Март 28, 2024

With the increasingly serious greenhouse effect, electrochemical carbon dioxide reduction reaction (CO2RR) has garnered widespread attention as it is capable of leveraging renewable energy to convert CO2 into value-added chemicals and fuels. However, performance CO2RR can hardly meet expectations because diverse intermediates complicated processes, necessitating exploitation highly efficient catalysts. In recent years, with advanced characterization technologies theoretical simulations, exploration catalytic mechanisms gradually deepened electronic structure catalysts their interactions intermediates, which serve a bridge facilitate deeper comprehension structure-performance relationships. Transition metal-based (TMCs), extensively applied in CO2RR, demonstrate substantial potential for further modulation, given abundance d electrons. Herein, we discuss representative feasible strategies modulate catalysts, including doping, vacancy, alloying, heterostructure, strain, phase engineering. These approaches profoundly alter inherent properties TMCs interaction thereby greatly affecting rate pathway CO2RR. It believed that rational design modulation fundamentally provide viable directions development toward conversion many other small molecules.

Язык: Английский

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Coordination Environment Engineering of Metal Centers in Coordination Polymers for Selective Carbon Dioxide Electroreduction toward Multicarbon Products

ACS Nano, Год журнала: 2024, Номер 18(9), С. 7192 - 7203

Опубликована: Фев. 22, 2024

Electrocatalytic carbon dioxide reduction reaction (CO2RR) toward value-added chemicals/fuels has offered a sustainable strategy to achieve carbon-neutral energy cycle. However, it remains great challenge controllably and precisely regulate the coordination environment of active sites in catalysts for efficient generation targeted products, especially multicarbon (C2+) products. Herein we report engineering metal centers polymers electroreduction CO2 C2+ products under neutral conditions. Significantly, Cu polymer with Cu–N2S2 configuration (Cu–N–S) demonstrates superior Faradaic efficiencies 61.2% 82.2% ethylene respectively, compared selective formic acid on an analogous Cu–I2S2 mode (Cu–I–S). In situ studies reveal balanced formation atop bridge *CO intermediates Cu–N–S, promoting C–C coupling production. Theoretical calculations suggest that can induce electronic modulations sites, where d-band center is upshifted Cu–N–S stronger selectivity Consequently, displays trend while Cu–I–S favors due suppression couplings pathways large barriers.

Язык: Английский

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Site‐selective Growth of fcc‐2H‐fcc Copper on Unconventional Phase Metal Nanomaterials for Highly Efficient Tandem CO₂ Electroreduction

Advanced Materials, Год журнала: 2024, Номер 36(32)

Опубликована: Май 29, 2024

Abstract Copper (Cu) nanomaterials are a unique kind of electrocatalysts for high‐value multi‐carbon production in carbon dioxide reduction reaction (CO 2 RR), which holds enormous potential attaining neutrality. However, phase engineering Cu remains challenging, especially the construction unconventional Cu‐based asymmetric heteronanostructures. Here site‐selective growth on unusual gold (Au) nanorods, obtaining three kinds heterophase fcc‐2H‐fcc Au–Cu heteronanostructures is reported. Significantly, resultant Janus nanostructures (JNSs) break symmetric mode Au. In electrocatalytic CO RR, JNSs exhibit excellent performance both H‐type and flow cells, with Faradaic efficiencies 55.5% 84.3% ethylene products, respectively. situ characterizations theoretical calculations reveal co‐exposure 2H‐Au 2H‐Cu domains diversifies CO* adsorption configurations promotes spillover subsequent C–C coupling toward generation reduced energy barriers.

Язык: Английский

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Simultaneous Defect and Size Control of Metal–Organic Framework Nanostructures for Highly Efficient Carbon Dioxide Electroreduction to Multicarbon Products

ACS Materials Letters, Год журнала: 2023, Номер 5(8), С. 2121 - 2130

Опубликована: Июль 11, 2023

Electrocatalytic carbon dioxide (CO2) reduction reaction (CO2RR) has offered a sustainable approach in converting an anthropogenic CO2 source to chemicals and fuels promote neutral. However, it remains challenging prepare high-performance catalysts for efficient selective electroreduction, especially toward the high-vaule multicarbon products. Here we report facile synthesis of four kinds nearly monodispersed CuTrz (HTrz = 1H,1,2,4-triazole) metal–organic framework (MOF) nanostructures with different sizes by controlling kinetics. Significantly, small demonstrate much superior CO2RR performance over large counterparts production neutral electrolytes, optimized Faradaic efficiency 55.4% 81.8% ethylene products, respectively. Detailed structural characterizations reveal that are polycrystalline rich grain boundaries, while ones single crystalline. This work highlights importance simultaneous defect size control MOFs boosting their production.

Язык: Английский

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Electrocatalysis of nitrogen pollution: transforming nitrogen waste into high-value chemicals

Chemical Society Reviews, Год журнала: 2023, Номер 53(2), С. 557 - 565

Опубликована: Дек. 15, 2023

This viewpoint focuses on electrocatalytic NW reduction and highlights the challenges in its practical application. It also discusses future directions to meet requirements of upstream downstream industries by optimizing production processes.

Язык: Английский

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Steering the Selectivity of Carbon Dioxide Electroreduction from Single-Carbon to Multicarbon Products on Metal–Organic Frameworks via Facet Engineering

Nano Letters, Год журнала: 2024, Номер 24(5), С. 1553 - 1562

Опубликована: Янв. 24, 2024

Although metal-organic frameworks (MOFs) have attracted more attention for the electrocatalytic CO

Язык: Английский

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Modulating Interfacial Hydrogen-Bond Environment by Electrolyte Engineering Promotes Acidic CO₂ Electrolysis

ACS Catalysis, Год журнала: 2024, Номер 14(14), С. 10529 - 10537

Опубликована: Июнь 27, 2024

Язык: Английский

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Ethylene Electrosynthesis via Selective CO₂ Reduction: Fundamental Considerations, Strategies, and Challenges

Advanced Energy Materials, Год журнала: 2024, Номер unknown

Опубликована: Июнь 11, 2024

Abstract The electrochemical carbon dioxide reduction reaction (CO 2 RR) is a promising approach for reducing atmospheric ) emissions, allowing harmful CO to be converted into more valuable carbon‐based products. On one hand, single (C 1 products have been obtained with high efficiency and show great promise industrial capture. However, multi‐carbon 2+ possess market value demonstrated significant as potential RR. Due RR's multiple pathways similar equilibrium potentials, the extended mechanisms necessary form C continue reduce overall selectivity of ‐to‐C electroconversion. Meanwhile, RR whole faces many challenges relating system optimization, owing an intolerance low surface pH, systemic stability utilization issues, competing side in H evolution (HER). Ethylene 4 remains incredibly within chemical industry; however, current established method producing ethylene (steam cracking) contributes emission atmosphere. Thus, strategies significantly increase this technology are essential. This review will discuss vital factors influencing forming summarize recent advancements electrosynthesis.

Язык: Английский

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Flow-electrode capacitive separation of organic acid products and recovery of alkali cations after acidic CO ₂ electrolysis

Proceedings of the National Academy of Sciences, Год журнала: 2024, Номер 121(41)

Опубликована: Окт. 3, 2024

Acidic CO

Язык: Английский

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