Reaction intermediate-mediated electrocatalyst synthesis favors specified facet and defect exposure for efficient nitrate–ammonia conversion

Energy & Environmental Science, Год журнала: 2021, Номер 14(9), С. 4989 - 4997

Опубликована: Янв. 1, 2021

An intermediate-mediated approach was proposed to synthesize copper, rich in (100) facets and defects, for highly efficient nitrate reduction.

Язык: Английский

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Construction of C–N bonds from small-molecule precursors through heterogeneous electrocatalysis

Nature Reviews Chemistry, Год журнала: 2022, Номер 6(5), С. 303 - 319

Опубликована: Апрель 25, 2022

Язык: Английский

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Dynamic Reconstitution Between Copper Single Atoms and Clusters for Electrocatalytic Urea Synthesis

Advanced Materials, Год журнала: 2023, Номер 35(18)

Опубликована: Фев. 6, 2023

Electrocatalytic CN coupling between carbon dioxide and nitrate has emerged to meet the comprehensive demands of footprint closing, valorization waste, sustainable manufacture urea. However, identification catalytic active sites design efficient electrocatalysts remain a challenge. Herein, synthesis urea catalyzed by copper single atoms decorated on CeO2 support (denoted as Cu1 -CeO2 ) is reported. The catalyst exhibits an average yield rate 52.84 mmol h-1 gcat.-1 at -1.6 V versus reversible hydrogen electrode. Operando X-ray absorption spectra demonstrate reconstitution (Cu1 clusters (Cu4 during electrolysis. These electrochemically reconstituted Cu4 are real for electrocatalytic synthesis. Favorable reactions formation validated using operando synchrotron-radiation Fourier transform infrared spectroscopy theoretical calculations. Dynamic transformations single-atom configurations occur when applied potential switched open-circuit potential, endowing with superior structural electrochemical stabilities.

Язык: Английский

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Everything You Wanted to Know about Deep Eutectic Solvents but Were Afraid to Be Told

Annual Review of Chemical and Biomolecular Engineering, Год журнала: 2023, Номер 14(1), С. 141 - 163

Опубликована: Март 8, 2023

Are deep eutectic solvents (DESs) a promising alternative to conventional solvents? Perhaps, but their development is hindered by plethora of misconceptions. These are carefully analyzed here, beginning with the very meaning DESs, which has strayed far beyond its original scope mixtures Lewis or Brønsted acids and bases. Instead, definition that grounded on thermodynamic principles distinguishes between encouraged, types precursors can be used prepare DESs reviewed. Landmark works surrounding sustainability, stability, toxicity, biodegradability these also discussed, revealing piling evidence numerous reported thus far, particularly those choline based, lack sufficient sustainability-related traits considered green solvents. Finally, emerging DES applications reviewed, emphasizing most remarkable feature: ability liquefy solid compound target property, allowing use as liquid solvent.

Язык: Английский

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Prospects and challenges of green ammonia synthesis

Nature Synthesis, Год журнала: 2023, Номер 2(7), С. 612 - 623

Опубликована: Май 25, 2023

Язык: Английский

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Designing Efficient Nitrate Reduction Electrocatalysts by Identifying and Optimizing Active Sites of Co-Based Spinels

Journal of the American Chemical Society, Год журнала: 2023, Номер 146(5), С. 2967 - 2976

Опубликована: Дек. 29, 2023

Cobalt-based spinel oxides (i.e., Co

Язык: Английский

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N‐Coordinated Cu–Ni Dual‐Single‐Atom Catalyst for Highly Selective Electrocatalytic Reduction of Nitrate to Ammonia

Small, Год журнала: 2023, Номер 19(20)

Опубликована: Фев. 15, 2023

As a traditional method of ammonia (NH3 ) synthesis, Haber-Bosch expends vast amount energy. An alternative route for NH3 synthesis is proposed from nitrate (NO3- via electrocatalysis. However, the structure-activity relationship remains challenging and requires in-depth research both experimentally theoretically. Here an N-coordinated Cu-Ni dual-single-atom catalyst anchored in N-doped carbon (Cu/Ni-NC) reported, which has competitive activity with maximal Faradaic efficiency 97.28%. Detailed characterizations demonstrate that high Cu/Ni-NC mainly comes contribution dual active sites. That is, (1) electron transfer (Ni → Cu) reveals strong interaction dual-single-atom; (2) hybridizations Cu 3d-and Ni 3d-O 2p orbitals NO3- can accelerate dual-site to ; (3) effectively decrease rate-limiting step barriers, suppress N-N coupling N2 O formation hydrogen production.

Язык: Английский

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Review of ammonia production and utilization: Enabling clean energy transition and net-zero climate targets

Energy Conversion and Management, Год журнала: 2024, Номер 300, С. 117869 - 117869

Опубликована: Янв. 1, 2024

Язык: Английский

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Recent Advances in Designing Efficient Electrocatalysts for Electrochemical Nitrate Reduction to Ammonia

Small Structures, Год журнала: 2022, Номер 4(6)

Опубликована: Окт. 6, 2022

As a raw material for producing chemical fertilizers, ammonia plays an essential role in human production and life. Due to the severe energy consumption pollution caused by industrial Haber–Bosch process of NH 3 synthesis, developing synthesis reaction under ambient conditions is vital. Electrochemical nitrogen reduction (NRR) has recently emerged as potential method. However, its limited yield selectivity are unsatisfactory. NO − , oxidized form nitrogen, universally exists drinking water (<50 mg L −1 ) wastewater (2000‐4000 ). nitrate (NO RR), with higher Faradaic efficiency, promising strategy treatment production. In this review, detailed overview recent progress RR precious group metal (PGM) electrocatalysts, PGM‐free nonmetal electrocatalysts summarized. addition, effective design strategies efficient existing challenges, research prospects next stage also discussed. This review may provide some directions improving electrocatalytic offer inspiration electrochemical process.

Язык: Английский

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Electrocatalytic Nitrate and Nitrite Reduction toward Ammonia Using Cu₂O Nanocubes: Active Species and Reaction Mechanisms

Journal of the American Chemical Society, Год журнала: 2024, Номер 146(14), С. 9665 - 9678

Опубликована: Апрель 1, 2024

The electrochemical reduction of nitrate (NO3–) and nitrite (NO2–) enables sustainable, carbon-neutral, decentralized routes to produce ammonia (NH3). Copper-based materials are promising electrocatalysts for NOx– conversion NH3. However, the underlying reaction mechanisms role different Cu species during catalytic process still poorly understood. Herein, by combining quasi in situ X-ray photoelectron spectroscopy (XPS) operando absorption (XAS), we unveiled that is mostly metallic form highly selective NO3–/NO2– On contrary, Cu(I) predominant a potential region where two-electron NO3– NO2– major reaction. Electrokinetic analysis Raman was also used propose possible steps intermediates leading NH3, respectively. This work establishes correlation between performance dynamic changes chemical state Cu, provides crucial mechanistic insights into pathways electrocatalytic reduction.

Язык: Английский

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