Green Carbon Science: Efficient Carbon Resource Processing, Utilization, and Recycling towards Carbon Neutrality

Angewandte Chemie International Edition, Год журнала: 2021, Номер 61(15)

Опубликована: Дек. 17, 2021

Green carbon science is defined as the "study and optimization of transformation carbon-containing compounds relevant processes involved in entire cycle from resource processing, energy utilization, CO2 fixation, recycling to utilize resources efficiently minimize net emission."[1] related closely neutrality, fields have developed quickly last decade. In this Minireview, we propose concept index, recent progress petroleum refining, production liquid fuels, chemicals, materials using coal, methane, , biomass, waste plastics highlighted combination with green science. An outlook for these important provided final section.

Язык: Английский

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Phosphorus Induced Electron Localization of Single Iron Sites for Boosted CO₂ Electroreduction Reaction

Angewandte Chemie International Edition, Год журнала: 2021, Номер 60(44), С. 23614 - 23618

Опубликована: Авг. 31, 2021

Electrochemical reduction of carbon dioxide (CO2 ) into chemicals and fuels has recently attracted much interest, but normally suffers from a high overpotential low selectivity. In this work, single P atoms were introduced N-doped supported Fe atom catalyst (Fe-SAC/NPC) mainly in the form P-C bonds for CO2 electroreduction to CO an aqueous solution. This exhibited Faradaic efficiency ≈97 % at 320 mV, Tafel slope only 59 mV dec-1 , comparable state-of-the-art gold catalysts. Experimental analysis combined with DFT calculations suggested that coordination shells (n≥3), particular third shell center enhanced electronic localization Fe, which improved stabilization key *COOH intermediate on leading superior electrochemical performance overpotentials.

Язык: Английский

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Coordination Symmetry Breaking of Single‐Atom Catalysts for Robust and Efficient Nitrate Electroreduction to Ammonia

Advanced Materials, Год журнала: 2022, Номер 34(36)

Опубликована: Июль 16, 2022

Nitrate electrocatalytic reduction (NO3 RR) for ammonia production is a promising strategy to close the N-cycle from nitration contamination, as well an alternative Haber-Bosch process with less energy consumption and carbon dioxide release. However, current long-term stability of NO3 RR catalysts usually tens hours, far requirements industrialization. Here, symmetry-broken Cusingle-atom are designed, catalytic activity retained after operation more than 2000 h, while average rate 27.84 mg h-1 cm-2 at industrial level density 366 mA achieved, obtaining good balance between stability. Coordination symmetry breaking achieved by embedding one Cu atom in graphene nanosheets two N O atoms cis-configuration, effectively lowering coordination symmetry, rendering active site polar, accumulating NO3- near electrocatalyst surface. Additionally, cis-coordination splits 3d orbitals, which generates orbital-symmetry-matched π-complex key intermediate *ONH reduces barrier, compared σ-complex generated other catalysts. These results reveal critical role single-atom catalysts, prompting design coordination-symmetry-broken electrocatalysts toward possible

Язык: Английский

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Single‐atom catalysis for carbon neutrality

Carbon Energy, Год журнала: 2022, Номер 4(6), С. 1021 - 1079

Опубликована: Июль 14, 2022

Abstract Currently, more than 86% of global energy consumption is still mainly dependent on traditional fossil fuels, which causes resource scarcity and even emission high amounts carbon dioxide (CO 2 ), resulting in a severe “Greenhouse effect.” Considering this situation, the concept “carbon neutrality” has been put forward by 125 countries one after another. To achieve goals neutrality,” two main strategies to reduce CO emissions develop sustainable clean can be adopted. Notably, these are crucial for synthesis advanced single‐atom catalysts (SACs) energy‐related applications. In review, we highlight unique SACs conversion into high‐efficiency energy, example, through photocatalytic, electrocatalytic, thermal catalytic hydrogenation technologies, convert hydrocarbon fuels (CO, CH 4 , HCOOH, 3 OH, multicarbon [C 2+ ] products). addition, introduce technologies devices replace polluting such as photocatalytic electrocatalytic water splitting produce hydrogen oxygen reduction reaction (ORR) fuel cells. Impressively, several representative examples (including d ‐, ds p f ‐blocks) conversion, H ORR discussed describe methods, characterization, corresponding activity. Finally, review concludes with description challenges outlooks future applications contributing toward neutrality.

Язык: Английский

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Highly Efficient Electrocatalytic Uranium Extraction from Seawater over an Amidoxime‐Functionalized In–N–C Catalyst

Advanced Science, Год журнала: 2022, Номер 9(23)

Опубликована: Июнь 17, 2022

Seawater contains uranium at a concentration of ≈3.3 ppb, thus representing rich and sustainable nuclear fuel source. Herein, an adsorption-electrocatalytic platform is developed for extraction from seawater, comprising atomically dispersed indium anchored on hollow nitrogen-doped carbon capsules functionalized with flexible amidoxime moieties (In-N

Язык: Английский

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Dynamic Stability of Copper Single-Atom Catalysts under Working Conditions

Journal of the American Chemical Society, Год журнала: 2022, Номер 144(37), С. 17140 - 17148

Опубликована: Сен. 12, 2022

The long-term stability of single-atom catalysts is a major factor affecting their large-scale commercial application. How to evaluate the dynamic under working conditions still lacking. Here, taking single copper atom embedded in N-doped graphene as an example, "constant-potential hybrid-solvation model" used reversible transformation between atoms and clusters realistic reaction conditions. It revealed that adsorption H vital driving force for leaching Cu from catalyst surface. more negative electrode potential, stronger H. As result, competitive hydrogen evolution inhibited, Cu-N bonds are weakened, resulting some being tethered on surface dissolved aqueous solution. collision two states forms transient cluster structure true catalytic active site promote CO2 reduction ethanol. applied potential released or switched positive value, hydroxyl radicals (OH•) play dominant role oxidation process cluster, then returns initial atomic dispersion state by redeposition, completing reconstruction cycle catalyst. Our work provides fundamental understanding at level calls reassessment currently reported considering

Язык: Английский

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Recent advances on electrocatalytic CO2 reduction to resources: Target products, reaction pathways and typical catalysts

Chemical Engineering Journal, Год журнала: 2022, Номер 453, С. 139663 - 139663

Опубликована: Окт. 8, 2022

Язык: Английский

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Adjacent Copper Single Atoms Promote C–C Coupling in Electrochemical CO₂ Reduction for the Efficient Conversion of Ethanol

Journal of the American Chemical Society, Год журнала: 2023, Номер 145(31), С. 17253 - 17264

Опубликована: Июль 27, 2023

The electrochemical CO2 reduction reaction (CO2RR) using renewable electricity is one of the most promising strategies for reaching goal carbon neutrality. Multicarbonous (C2+) products have broad applications, and ethanol a valuable chemical fuel. Many Cu-based catalysts been reported to be efficient electrocatalytic CO2RR C2+ products, but they generally offer limited selectivity current density toward ethanol. Herein, we proposed silica-mediated hydrogen-bonded organic framework (HOF)-templated approach preparing ultrahigh-density Cu single-atom (SACs) on thin-walled N-doped nanotubes (TWN). content in prepared by this method could up 13.35 wt %. It was found that showed outstanding performance ethanol, Faradaic efficiency (FE) increased with increase Cu-N3 site density. FE over % reach ∼81.9% partial 35.6 mA cm-2 an H-type cell, which best result date. In addition, catalyst stably used more than 25 h. Experimental functional theory (DFT) studies revealed adjacent active sites (one atom coordinates three N) were reaction, their high crucial because short distance promote C-C coupling synergistically.

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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Sulfur‐Dopant‐Promoted Electroreduction of CO₂ over Coordinatively Unsaturated Ni‐N₂ Moieties

Angewandte Chemie International Edition, Год журнала: 2021, Номер 60(43), С. 23342 - 23348

Опубликована: Авг. 27, 2021

Abstract Atomically dispersed nickel–nitrogen–carbon (Ni‐N‐C) moieties are promising for efficient electrochemical CO 2 ‐to‐CO conversion. To improve the intrinsic electrocatalytic activity, it is essential but challenging to steer coordination environment of Ni centers promoting formation kinetics. Here, we introduce alien sulfur atoms tune local electronic density unsaturated NiN species. A coordinated structure evolution detected and S vacancies generated at high overpotentials, as confirmed by X‐ray absorption spectroscopy. The dopants enhance selectivity activity over normal structure, reaching a Faradaic efficiency 97 % large current 40.3 mA cm −2 in H‐cell −0.8 V −0.9 (vs. RHE), respectively. DFT calculations reveal both doped evolved contribute reduced energy barriers electroreduction CO.

Язык: Английский

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