Recent Advances on Carbon‐Based Metal‐Free Electrocatalysts for Energy and Chemical Conversions

Advanced Materials, Journal Year: 2024, Volume and Issue: unknown

Published: July 25, 2024

Over the last decade, carbon-based metal-free electrocatalysts (C-MFECs) have become important in electrocatalysis. This field is started thanks to initial discovery that nitrogen atom doped carbon can function as a electrode alkaline fuel cells. A wide variety of nanomaterials, including 0D dots, 1D nanotubes, 2D graphene, and 3D porous carbons, has demonstrated high electrocatalytic performance across applications. These include clean energy generation storage, green chemistry, environmental remediation. The applicability C-MFECs facilitated by effective synthetic approaches, e.g., heteroatom doping, physical/chemical modification. methods enable creation catalysts with properties useful for sustainable transformation storage (e.g., cells, Zn-air batteries, Li-O

Language: Английский

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Electronic Structure Regulation of MnCo₂O₄ via Surface‐Phosphorization Coupling to Monolithic Carbon for Oxygen Electrocatalysis in Zn–Air Batteries

Advanced Functional Materials, Journal Year: 2024, Volume and Issue: unknown

Published: July 1, 2024

Abstract An urgent challenge to the development of rechargeable Zn–air batteries (RZABs) is highly active, durable, and low‐cost catalysts for oxygen reduction reaction evolution (ORR OER). Herein, a carbon‐based monolithic catalyst designed via anchoring P‐modified MnCo 2 O 4 inverse spinel nanoparticles on biomass‐derived carbon (P‐MnCo @PWC). The introduction surface P atoms regulates electronic structures valences metal by adjusting coordination fields (P‐O) δ– Metal‐P. optimization adsorption behavior key intermediates facilitates activation conversion species. structure beneficial construction three‐phase interface efficient mass transfer high electrical conductivity. P‐MnCo @PWC displays outstanding bifunctional catalytic properties with thin Δ E (the difference between OER potential at 10 mA cm – ORR halfwave potential) 0.66 V. RZAB as cathode delivers an exceptional peak power density (160 mW ) remarkable cycle life (over 1200 cycles), overcoming those noble counterparts. This research provides promising general surface‐phosphorization way design electrocatalysts high‐value utilization biomass.

Language: Английский

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Structure–Activity Relationships in Oxygen Electrocatalysis

Advanced Materials, Journal Year: 2024, Volume and Issue: unknown

Published: Sept. 30, 2024

Abstract Oxygen electrocatalysis, as the pivotal circle of many green energy technologies, sets off a worldwide research boom in full swing, while its large kinetic obstacles require remarkable catalysts to break through. Here, based on summarizing reaction mechanisms and situ characterizations, structure–activity relationships oxygen electrocatalysts are emphatically overviewed, including influence geometric morphology chemical structures electrocatalytic performances. Subsequently, experimental/theoretical is combined with device applications comprehensively summarize cutting‐edge according various material categories. Finally, future challenges forecasted from perspective catalyst development applications, favoring researchers promote industrialization electrocatalysis at an early date.

Language: Английский

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Heteroatoms Modulate the Copper Single Atom Catalytic Host Materials for Promoting the Redox Reaction in Aqueous Zinc‐Selenium Batteries

Advanced Functional Materials, Journal Year: 2024, Volume and Issue: unknown

Published: Oct. 18, 2024

Abstract Aqueous zinc‐selenium (Zn‐Se) batteries have garnered much attention due to their inherent safety and high specific capacity. Unfortunately, the problem of sluggish redox reaction represents a significant obstacle development aqueous Zn‐Se batteries. Here, nitrogen‐phosphorus asymmetrically coordinated copper single atom catalytic host material (CuN 3 P 1 @C) is synthesized for an battery. The CuN @C exhibits rich porous structure, high‐loading Cu atoms, unique asymmetric coordination environment, which significantly reduces energy barrier between Se Zn, enhancing electrochemical performance Consequently, Se/CuN cathode achieves capacity 756 mAh g −1 at 0.2 A cycling stability 4 000 cycles 5.0 (capacity decay 0.0044% per cycle). Meanwhile, conversion mechanism battery systematically explored via systematical characteristics density functional theory calculations. This work opens up novel approach boosting by modulating atom‐based materials heteroatoms.

Language: Английский

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Mo2N nanoclusters and FeMo dual atomic active sites confined in N-doped hollow carbon nanocages for synergistic improvement in oxygen reduction and Zn-air battery

Chemical Engineering Journal, Journal Year: 2025, Volume and Issue: unknown, P. 160442 - 160442

Published: Feb. 1, 2025

Language: Английский

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Structural and coordination microenvironment regulated MOF with phosphorylurea group to boost uranium adsorption

Separation and Purification Technology, Journal Year: 2024, Volume and Issue: 346, P. 127409 - 127409

Published: April 7, 2024

Language: Английский

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Manipulating the Electronic Properties of an Fe Single Atom Catalyst via Secondary Coordination Sphere Engineering to Provide Enhanced Oxygen Electrocatalytic Activity in Zinc‐Air Batteries

Advanced Materials, Journal Year: 2024, Volume and Issue: 36(44)

Published: Sept. 16, 2024

Abstract Oxygen reduction and evolution reactions are two key processes in electrochemical energy conversion technologies. Synthesis of nonprecious metal, carbon‐based electrocatalysts with high oxygen bifunctional activity stability is a crucial, yet challenging step to achieving conversion. Here, an approach address this issue: synthesis atomically dispersed Fe electrocatalyst (Fe 1 /NCP) over porous, defect‐containing nitrogen‐doped carbon support, described. Through incorporation phosphorus atom into the second coordination sphere iron, durability boundaries catalyst pushed unprecedented level alkaline environments, such as those found zinc‐air battery. The rationale delicately incorporate P heteroatoms defects close central metal sites (FeN 4 ‐OH) order break local symmetry electronic distribution. This enables suitable binding strength oxygenated intermediates. In situ characterizations theoretical studies demonstrate that these synergetic interactions responsible for stability. These intrinsic advantages /NCP enable potential gap mere 0.65 V power density 263.8 mW cm −2 when incorporated findings underscore importance design principles access high‐performance green

Language: Английский

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Harnessing Multi‐Asymmetric Engineering: A New Horizon in Bifunctional Oxygen Electrocatalysis with Iron‐Group Atom‐Cluster Nanohybrid

Advanced Functional Materials, Journal Year: 2024, Volume and Issue: unknown

Published: Sept. 27, 2024

Abstract Integrating active sites for oxygen reduction and evolution reactions (ORR OER) is pivotal advancing bifunctional electrodes. Addressing the geometric/electronic properties of these essential to disrupt linear scaling relationship between adsorption desorption complex intermediates. Herein, a proof‐of‐concept presented constructing asymmetric trinuclear employing both composition‐ size‐based coupling strategies. These comprise ORR‐active Fe single atom (Fe SA ), OER‐active atomically clustered species AC Ni as modulators. This AC‐SA ‐Ni @N‐doped carbon exhibits excellent catalytic activities, with narrow potential gap 0.661 V an ORR half‐wave 0.931 OER 1.592 at 10 mA cm −2 . The Zn‐air battery this material achieves peak power density 293 mW , specific capacity 748 mAh g Zn −1 remarkable stability. Experimental findings theoretical simulations reveal that induced strong electronic among centers, facilitating charge redistribution optimizing barriers enhances rapid release * OH during efficient transformation from O OOH OER. study presents novel strategy developing robust

Language: Английский

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Self‐Encapsulated Ni Nanoparticles on Delignified Wood Carbon for Efficient Urea‐Assisted Hydrogen Production

Advanced Functional Materials, Journal Year: 2024, Volume and Issue: unknown

Published: Oct. 8, 2024

Abstract Developing efficient, low‐cost electrocatalysts for industrial‐level hydrogen production remains a significant challenge. Here lattice‐distorted Ni nanoparticles (NPs) encapsulated within nitrogen‐doped carbon shell on delignified wood (Ni‐NC@DWC) are constructed through chitosan‐induced assembly and the pyrolysis process. Experimental theoretical results indicate that lattice distortion due to strong metal‐support interactions, boosts electron transfer reaction intermediate adsorption/desorption, enhancing both urea oxidation (UOR) evolution (HER). Interestingly, active center 3+ ‐O is dynamically cyclically generated during UOR. When utilized as self‐standing electrode in an alkaline electrolyte, Ni‐NC@DWC exhibits low potentials of 24 mV 1.244 V at 100 mA cm −2 HER UOR, respectively. Moreover, achieves ultrasmall cell voltage 1.13 urea‐assisted water splitting can operate stably over 1000 h. Furthermore, when it self‐assembled anion exchange membrane (AEM) electrolyzer, requires only 1.62 2000 industrial operates 150 h without degradation, confirming highly attractive economical, sustainable, scalable production.

Language: Английский

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Nonmetallic High‐Entropy‐Engineered Nanocarbons for Advanced ORR Electrocatalysis

Angewandte Chemie International Edition, Journal Year: 2025, Volume and Issue: unknown

Published: March 10, 2025

High-entropy materials are poised to revolutionize science and industrial applications due their design flexibility, peculiar performance, broad applicability. In this study, we present a proof-of-concept high-entropy engineered nanocarbon (HENC) co-doped with five nonmetal elements (B, F, P, S, N), synthesized via in situ polymerization modification of ZIF-8 followed by pyrolysis. The HENC exhibits outstanding performance as electrocatalyst for the oxygen reduction reaction (ORR), activity on par benchmark Pt/C electrocatalysts superior cyclic stability. Simulations all-site calculations reveal that synergistic effects abundant heteroatoms increased system entropy facilitate formation *O2 species, N, S acting key active elements, while co-doping B F further enhances Notably, HENCs have been validated cathode catalysts zinc-air batteries, achieving an impressive peak power density 604 mW cm-2 demonstrating long-term stability over 16-day period, outpacing commercial catalyst (542 cm-2). This work not only enriches concept high advances understanding but also opens new avenue development high-performance low-cost catalysts.

Language: Английский

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