Recent advances in nanostructured heterogeneous catalysts for N-cycle electrocatalysis

Deleted Journal, Год журнала: 2022, Номер 1, С. e9120010 - e9120010

Опубликована: Май 30, 2022

To restore the natural nitrogen cycle (N-cycle), artificial N-cycle electrocatalysis with flexibility, sustainability, and compatibility can convert intermittent renewable energy (e.g., wind) to harmful or value-added chemicals minimal carbon emissions. The background of such N-cycles, as fixation, ammonia oxidation, nitrate reduction, is briefly introduced here. discussion emerging nanostructures in various conversion reactions focused on architecture/compositional design, electrochemical performances, reaction mechanisms, instructive tests. Energy device advancements for achieving more functions well in situ/operando characterizations toward understanding key steps are also highlighted. Furthermore, some recently proposed less discussed C–N coupling summarized. We classify inorganic sources that each other under an applied voltage into three types, namely, abundant nitrogen, toxic (nitrite), oxides, useful compounds ammonia, hydrazine, hydroxylamine, goal providing critical insights strategies facilitate development our circular economy.

Язык: Английский

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Porous organic polymers for electrocatalysis

Chemical Society Reviews, Год журнала: 2022, Номер 51(2), С. 761 - 791

Опубликована: Янв. 1, 2022

Porous organic polymers (POPs) composed of building units linked via covalent bonds are a class lightweight porous network materials with high surface areas, tuneable pores, and designable components structures. Owing to their well-preserved characteristics in terms structure composition, POPs applied as electrocatalysts have shown promising activity achieved considerable advances numerous electrocatalytic reactions, including the hydrogen evolution reaction, oxygen reduction CO2 N2 nitrate/nitrite nitrobenzene oxidation benzyl alcohol reaction. Herein, we present systematic overview recent applications these reactions. The synthesis strategies, specific active sites, catalytic mechanisms summarized this review. fundamental principles some reactions also concluded. We further discuss current challenges perspectives on for applications. Meanwhile, possible future directions highlighted afford guidelines development efficient POP electrocatalysts.

Язык: Английский

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Precisely Constructing Orbital Coupling-Modulated Dual-Atom Fe Pair Sites for Synergistic CO₂ Electroreduction

ACS Energy Letters, Год журнала: 2022, Номер 7(2), С. 640 - 649

Опубликована: Янв. 14, 2022

Electrochemical reduction of CO2 (CO2RR) provides an attractive pathway to achieve a carbon-neutral energy cycle. Single-atom catalysts (SAC) have shown unique potential in heterogeneous catalysis, but their structural simplicity prevents them from breaking linear scaling relationships. In this study, we develop feasible strategy precisely construct series electrocatalysts featuring well-defined single-atom and dual-site iron anchored on nitrogen-doped carbon matrix (Fe1–N–C Fe2–N–C). The Fe2–N–C dual-atom electrocatalyst (DAC) achieves enhanced CO Faradaic efficiency above 80% wider applied ranges along with higher turnover frequency (26,637 h–1) better durability compared SAC counterparts. Furthermore, based in-depth experimental theoretical analysis, the orbital coupling between dual sites decreases gap antibonding bonding states *CO adsorption. This research presents new insights into structure–performance relationship CO2RR at atomic scale extends application DACs for electrocatalysis beyond.

Язык: Английский

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Nickel dual-atom sites for electrochemical carbon dioxide reduction

Nature Synthesis, Год журнала: 2022, Номер 1(9), С. 719 - 728

Опубликована: Авг. 18, 2022

Язык: Английский

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Design strategies for markedly enhancing energy efficiency in the electrocatalytic CO₂ reduction reaction

Energy & Environmental Science, Год журнала: 2022, Номер 15(9), С. 3603 - 3629

Опубликована: Янв. 1, 2022

The review summarizes the recent strategies to improve energy efficiency of CO 2 electroreduction, a guiding metric for industrial application and economic feasibility, with emphasis on designing remarkable catalyst advanced electrolysis system.

Язык: Английский

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Electrochemical reduction of carbon dioxide to multicarbon (C₂₊) products: challenges and perspectives

Energy & Environmental Science, Год журнала: 2023, Номер 16(11), С. 4714 - 4758

Опубликована: Янв. 1, 2023

This review analyzes advanced catalysts and C 2+ synthesis mechanisms based on theoretical explorations in situ / operando characterizations. Triphasic interface optimization is discussed for the potential of industry-compatible stability.

Язык: Английский

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A Tandem Strategy for Enhancing Electrochemical CO₂ Reduction Activity of Single‐Atom Cu‐S₁N₃ Catalysts via Integration with Cu Nanoclusters

Angewandte Chemie International Edition, Год журнала: 2021, Номер 60(45), С. 24022 - 24027

Опубликована: Сен. 9, 2021

We developed a tandem electrocatalyst for CO2 -to-CO conversion comprising the single Cu site co-coordinated with N and S anchored carbon matrix (Cu-S1 N3 ) atomically dispersed clusters (Cux ), denoted as Cu-S1 /Cux . The as-prepared composite presents 100 % Faradaic efficiency towards CO generation (FECO at -0.65 V vs. RHE high FECO over 90 from -0.55 to -0.75 V, outperforming analogues Cu-N4 only 54 -0.7 V) 70 configurations. unsymmetrical atomic interface in basal plane possesses an optimized binding energy key intermediate *COOH compared site. At same time, adjacent Cux effectively promotes protonation of *CO2- by accelerating water dissociation offering *H active sites. This work provides strategy facilitating proton-coupled electron transfer atomic-level catalytic

Язык: Английский

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Breaking the Scaling Relationship Limit: From Single-Atom to Dual-Atom Catalysts

Accounts of Materials Research, Год журнала: 2022, Номер 3(6), С. 584 - 596

Опубликована: Май 17, 2022

ConspectusRecent decades have witnessed the rapid development of catalytic science, especially after Taylor and Armstrong proposed notion "active site" in 1925. By optimizing reaction paths reducing activation energies reactions, catalysts appear more than 90% chemical production involving homogeneous catalysis, heterogeneous enzyme catalysis. Because 100% efficiency active atom utilization adjustable microenvironment metal centers, single-atom (SACs) shine various fields for enhancing rate, conversion, selectivity reactions. Nevertheless, a solo site determines fixed adsorption mode, intermediates from multistep reactions linking with are related to each other. For specific reaction, it is almost impossible optimally adjust every intermediate on simultaneously. This phenomenon termed scaling relationship limit (SRL) an unavoidable obstacle pure SACs.Dual-atom (DACs), perfectly inheriting advantages SACs, can exhibit better performance simple SACs thus gradually gained researchers' attention. Depending dual-metal structure, sites (DMSs) DACs be divided into two separated heterometal sites, linked homometal sites. Two prescribe distance between electron interaction. Currently, origins summarized following three points: (1) electronic effect, which only one center serves as other plays regulatory role; (2) synergistic centers separately catalyze different core steps improve together; (3) offering additional changes structures break SRL based SACs. Among origins, structure upon DMSs most effective technologies boost property basis To date, few contributions focused catalysis environments, including O2 reduction evolution H2 CO2 N2 conversion reactions.In this Account, summary recent progress regarding will presented. First, unpopular discovery research hot spot illustrated through timeline. In next section, categories, potential revealed by comparison addition, techniques constructing systematically summarized, preparation carbonous, pyrolysis-free, noncarbon-supported, complex-type DACs. Furthermore, underlying energy- environment-related introduced detail assistance theoretical calculations. Finally, we affirm contribution particularly electrocatalysis, provide outlook direction discussing major challenges. It anticipated that Account inspire researchers propel advance

Язык: Английский

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Electrochemical C–N coupling of CO₂and nitrogenous small molecules for the electrosynthesis of organonitrogen compounds

Chemical Society Reviews, Год журнала: 2023, Номер 52(6), С. 2193 - 2237

Опубликована: Янв. 1, 2023

Electrochemical C–N coupling reaction by renewable electricity for the electrosynthesis of organonitrogen compounds with abundant CO 2 and nitrogenous small molecules as carbon nitrogen sources, respectively, is a promising sustainable synthetic strategy.

Язык: Английский

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Atomically Dispersed Ni–Cu Catalysts for pH‐Universal CO₂ Electroreduction

Advanced Materials, Год журнала: 2023, Номер 35(13)

Опубликована: Янв. 10, 2023

CO2 electroreduction is of great significance to reduce emissions and complete the carbon cycle. However, unavoidable carbonate formation low utilization efficiency in neutral or alkaline electrolytes hinder its application at commercial scale. The development reduction under acidic conditions provides a promising strategy, but inhibition hydrogen evolution reaction difficult. Herein, first work design Ni-Cu dual atom catalyst supported on hollow nitrogen-doped reported for pH-universal CO. shows high CO Faradaic ≈99% acidic, neutral, electrolytes, partial current densities reach 190 ± 11, 225 10, 489 14 mA cm-2 , respectively. In particular, reaches 64.3%, which twice as that conditions. Detailed study indicates existence electronic interaction between Ni Cu atoms. atoms push d-band center further toward Fermi level, thereby accelerating *COOH. addition, operando characterizations density functional theory calculation are used elucidate possible mechanism electrolytes.

Язык: Английский

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