Polymer-Derived Heteroatom-Doped Porous Carbon Materials

Chemical Reviews, Год журнала: 2020, Номер 120(17), С. 9363 - 9419

Опубликована: Авг. 6, 2020

Heteroatom-doped porous carbon materials (HPCMs) have found extensive applications in adsorption/separation, organic catalysis, sensing, and energy conversion/storage. The judicious choice of precursors is crucial for the manufacture HPCMs with specific usages maximization their functions. In this regard, polymers as demonstrated great promise because versatile molecular nanoscale structures, modulatable chemical composition, rich processing techniques to generate textures that, combination proper solid-state chemistry, can be maintained throughout carbonization. This Review comprehensively surveys progress polymer-derived functional terms how produce control porosities, heteroatom doping effects, morphologies related use. First, we summarize discuss synthetic approaches, including hard soft templating methods well direct synthesis strategies employing pores and/or heteroatoms HPCMs. Second, effects on thermal stability, electronic optical properties, surface chemistry Specifically, effect, which involves both single-type codoping two or more types into network, discussed. Considering significance application spectrum, potential choices suitable polymeric precisely regulate are presented. Finally, provide our perspective predefine structures by using realize current fields generation/conversion environmental remediation. We believe that these analyses deductions valuable a systematic understanding will serve source inspiration design future

Язык: Английский

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Intrinsic Electrocatalytic Activity Regulation of M–N–C Single‐Atom Catalysts for the Oxygen Reduction Reaction

Angewandte Chemie International Edition, Год журнала: 2020, Номер 60(9), С. 4448 - 4463

Опубликована: Апрель 21, 2020

Abstract Single‐atom catalysts (SACs) with highly active sites atomically dispersed on substrates exhibit unique advantages regarding maximum atomic efficiency, abundant chemical structures, and extraordinary catalytic performances for multiple important reactions. In particular, M–N–C SACs (M=transition metal atom) demonstrate optimal electrocatalytic activity the oxygen reduction reaction (ORR) have attracted extensive attention recently. Despite substantial efforts in fabricating various SACs, principles regulating intrinsic of their not been sufficiently studied. this Review, we summarize regulation strategies promoting ORR by modulation center atoms, coordinated environmental guest groups. Theoretical calculations experimental investigations are both included to afford a comprehensive understanding structure–performance relationship. Finally, future directions developing advanced other analogous reactions proposed.

Язык: Английский

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Coexisting Single‐Atomic Fe and Ni Sites on Hierarchically Ordered Porous Carbon as a Highly Efficient ORR Electrocatalyst

Advanced Materials, Год журнала: 2020, Номер 32(42)

Опубликована: Сен. 16, 2020

The development of oxygen reduction reaction (ORR) electrocatalysts based on earth-abundant nonprecious materials is critically important for sustainable large-scale applications fuel cells and metal-air batteries. Herein, a hetero-single-atom (h-SA) ORR electrocatalyst presented, which has atomically dispersed Fe Ni coanchored to microsized nitrogen-doped graphitic carbon support with unique trimodal-porous structure configured by highly ordered macropores interconnected through mesopores. Extended X-ray absorption fine spectra confirm that Fe- Ni-SAs are affixed the via FeN4 NiN4 coordination bonds. resultant Fe/Ni h-SA exhibits an outstanding activity, outperforming SA only or Ni-SAs, benchmark Pt/C. obtained experimental results indicate achieved performance from synergetic enhancement induced coexisting sites, superior mass-transfer capability promoted trimodal-porous-structured support.

Язык: Английский

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Electrocatalytic Refinery for Sustainable Production of Fuels and Chemicals

Angewandte Chemie International Edition, Год журнала: 2021, Номер 60(36), С. 19572 - 19590

Опубликована: Фев. 19, 2021

Abstract Compared to modern fossil‐fuel‐based refineries, the emerging electrocatalytic refinery (e‐refinery) is a more sustainable and environmentally benign strategy convert renewable feedstocks energy sources into transportable fuels value‐added chemicals. A crucial step in conducting e‐refinery processes development of appropriate reactions optimal electrocatalysts for efficient cleavage formation chemical bonds. However, compared well‐studied primary (e.g., O 2 reduction, water splitting), mechanistic aspects materials design complex are yet be settled. To address this challenge, herein, we first present fundamentals heterogeneous electrocatalysis some reactions, then implement these establish framework by coupling situ generated intermediates (integrated reactions) or products (tandem reactions). We also set principles strategies efficiently manipulate reaction pathways.

Язык: Английский

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Atomically dispersed iron sites with a nitrogen–carbon coating as highly active and durable oxygen reduction catalysts for fuel cells

Nature Energy, Год журнала: 2022, Номер 7(7), С. 652 - 663

Опубликована: Июль 7, 2022

Язык: Английский

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MIL‐101‐Derived Mesoporous Carbon Supporting Highly Exposed Fe Single‐Atom Sites as Efficient Oxygen Reduction Reaction Catalysts

Advanced Materials, Год журнала: 2021, Номер 33(23)

Опубликована: Апрель 29, 2021

Abstract Fe single‐atom catalysts (Fe SACs) with atomic FeN x active sites are very promising alternatives to platinum‐based for the oxygen reduction reaction (ORR). The pyrolysis of metal–organic frameworks (MOFs) is a common approach preparing SACs, though most MOF‐derived reported date microporous and thus suffer from poor mass transfer high proportion catalytically inaccessible sites. Herein, NH 2 ‐MIL‐101(Al), MOF possessing mesoporous cage architecture, used as precursor prepare series N‐doped carbon supports (denoted herein NC‐MIL101‐T) well‐defined structure at different temperatures. NC‐MIL101‐T then impregnated Fe(II)‐phenanthroline complex, heated again yield SAC‐MIL101‐T rich in accessible single atom best performing SAC‐MIL101‐1000 catalyst offers outstanding ORR activity alkaline media, evidenced by an half‐wave potential 0.94 V (vs RHE) 0.1 m KOH, well excellent performance both aqueous primary zinc–air batteries (a near maximum theoretical energy density 984.2 Wh kg Zn −1 ) solid‐state peak power 50.6 mW cm −2 specific capacity 724.0 mAh ).

Язык: Английский

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Metal–Organic Frameworks Derived Functional Materials for Electrochemical Energy Storage and Conversion: A Mini Review

Nano Letters, Год журнала: 2021, Номер 21(4), С. 1555 - 1565

Опубликована: Фев. 11, 2021

With many apparent advantages including high surface area, tunable pore sizes and topologies, diverse periodic organic–inorganic ingredients, metal–organic frameworks (MOFs) have been identified as versatile precursors or sacrificial templates for preparing functional materials advanced electrodes high-efficiency catalysts electrochemical energy storage conversion (EESC). In this Mini Review, we first briefly summarize the material design strategies to show rich possibilities of chemical compositions physical structures MOFs derivatives. We next highlight latest advances focusing on composition/structure/performance relationship discuss their practical applications in various EESC systems, such supercapacitors, rechargeable batteries, fuel cells, water electrolyzers, carbon dioxide/nitrogen reduction reactions. Finally, provide some our own insights into major challenges prospective solutions MOF-derived EESC, hoping shed light future development highly exciting field.

Язык: Английский

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Strategies to suppress hydrogen evolution for highly selective electrocatalytic nitrogen reduction: challenges and perspectives

Energy & Environmental Science, Год журнала: 2021, Номер 14(3), С. 1176 - 1193

Опубликована: Янв. 1, 2021

This review underlines the strategies to suppress HER for selective NRR in view of proton-/electron-transfer kinetics, thermodynamics, and electrocatalyst design on basis deep understanding mechanisms.

Язык: Английский

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Porphyrin-based frameworks for oxygen electrocatalysis and catalytic reduction of carbon dioxide

Chemical Society Reviews, Год журнала: 2021, Номер 50(4), С. 2540 - 2581

Опубликована: Янв. 1, 2021

The recent progress made on porphyrin-based frameworks and their applications in energy-related conversion technologies (e.g., ORR, OER CO₂RR) storage Zn–air batteries).

Язык: Английский

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Dual‐Sites Coordination Engineering of Single Atom Catalysts for Flexible Metal–Air Batteries

Advanced Energy Materials, Год журнала: 2021, Номер 11(30)

Опубликована: Июнь 19, 2021

Abstract Dual‐sites single atom catalysts hold promise for efficiently regulating multiple reaction processes and explicitly explaining the underlying mechanisms. However, delicate atomic engineering dual‐site remains a huge challenge. Herein, atomically dispersed Fe‐Ni atoms embedded in nitrogen‐doped carbon matrix (FeNi SAs/NC) are successfully developed with extraordinary activity electrocatalytic oxygen reduction evolution reactions (ORR/OER). The FeNi SAs/NC catalyst displays high onset potential (0.98 V) half‐wave (0.84 ORR, as well as, low overpotential of (270 mV) at 10 mA cm −2 OER. density functional theory calculations indicate that Fe site active center can facilitate four‐electron process, while Ni sites regulate electronic structure further reduce energy barrier rate‐determining step. In addition, prevents metal from aggregation corrosion, leading to improvement durability. As proof concept, flexible quasi‐solid‐state zinc– aluminum–air batteries assembled exhibit superior peak power densities discharging specific capacities outperforming commercial Pt/C. This work provides rational guidance synthesis bifunctional electrocatalysts next‐generation devices consumer electronics.

Язык: Английский

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