Preparation of Au@Pd Core–Shell Nanorods with fcc-2H-fcc Heterophase for Highly Efficient Electrocatalytic Alcohol Oxidation

Journal of the American Chemical Society, Journal Year: 2021, Volume and Issue: 144(1), P. 547 - 555

Published: Dec. 21, 2021

Controlled construction of bimetallic nanostructures with a well-defined heterophase is great significance for developing highly efficient nanocatalysts and investigating the structure-dependent catalytic performance. Here, wet-chemical synthesis method used to prepare Au@Pd core-shell nanorods unique fcc-2H-fcc (fcc: face-centered cubic; 2H: hexagonal close-packed stacking sequence "AB"). The obtained exhibit superior electrocatalytic ethanol oxidation performance mass activity as high 6.82 A mgPd-1, which 2.44, 6.96, 6.43 times those 2H-Pd nanoparticles, fcc-Pd commercial Pd/C, respectively. operando infrared reflection absorption spectroscopy reveals C2 pathway fast reaction kinetics on prepared nanorods. Our experimental results together density functional theory calculations indicate that enhanced can be attributed unconventional 2H phase, 2H/fcc phase boundary, lattice expansion Pd shell. Moreover, also serve an catalyst electrochemical methanol, ethylene glycol, glycerol. work in area engineering nanomaterials (PENs) opens way high-performance electrocatalysts toward future practical applications.

Language: Английский

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Lattice‐Strain Engineering for Heterogenous Electrocatalytic Oxygen Evolution Reaction

Advanced Materials, Journal Year: 2023, Volume and Issue: 35(39)

Published: Jan. 14, 2023

Abstract The energy efficiency of metal–air batteries and water‐splitting techniques is severely constrained by multiple electronic transfers in the heterogenous oxygen evolution reaction (OER), high overpotential induced sluggish kinetics has become an uppermost scientific challenge. Numerous attempts are devoted to enabling activity, selectivity, stability via tailoring surface physicochemical properties nanocatalysts. Lattice‐strain engineering as a cutting‐edge method for tuning geometric configuration metal sites plays pivotal role regulating interaction catalytic surfaces with adsorbate molecules. By defining d‐band center descriptor structure–activity relationship, individual contribution strain effects within state‐of‐the‐art electrocatalysts can be systematically elucidated OER optimization mechanism. In this review, fundamentals advancements strain‐catalysts showcased innovative trigger strategies enumerated, particular emphasis on feedback mechanism between precise regulation lattice‐strain optimal activity. Subsequently, modulation various attributes categorized impediments encountered practicalization strained effect discussed, ending outlook future research directions burgeoning field.

Language: Английский

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Recent progress on the synthesis and oxygen reduction applications of Fe-based single-atom and double-atom catalysts

Journal of Materials Chemistry A, Journal Year: 2021, Volume and Issue: 9(35), P. 19489 - 19507

Published: Jan. 1, 2021

Single-atom and double-atom catalysts have emerged as a new Frontier in many fields due to their high atom-utilization efficiency, excellent catalytic properties good durability.

Language: Английский

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Mesoporous Pt@Pt-skin Pt3Ni core-shell framework nanowire electrocatalyst for efficient oxygen reduction

Nature Communications, Journal Year: 2023, Volume and Issue: 14(1)

Published: March 18, 2023

The design of Pt-based nanoarchitectures with controllable compositions and morphologies is necessary to enhance their electrocatalytic activity. Herein, we report a rational synthesis anisotropic mesoporous Pt@Pt-skin Pt3Ni core-shell framework nanowires for high-efficient electrocatalysis. catalyst has uniform structure an ultrathin atomic-jagged Pt nanowire core Pt-skin shell, possessing high activity, stability utilisation efficiency. For the oxygen reduction reaction, demonstrated exceptional mass specific activities 6.69 A/mgpt 8.42 mA/cm2 (at 0.9 V versus reversible hydrogen electrode), exhibited negligible activity decay after 50,000 cycles. configuration combines advantages three-dimensional open mesopore molecular accessibility compressive surface strains, which results in more catalytically active sites weakened chemisorption oxygenated species, thus boosting its catalytic towards

Language: Английский

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Pd–Pt Tesseracts for the Oxygen Reduction Reaction

Journal of the American Chemical Society, Journal Year: 2021, Volume and Issue: 143(1), P. 496 - 503

Published: Jan. 1, 2021

Hollow frame structures are of special interest in the realm catalysis since they hold only ridges and hollow interiors, enabling accessibility active sites to most extent. Herein, we prepared Pd–Pt composed double-shell cubes linked by body diagonals as an efficient catalyst toward oxygen reduction reaction (ORR), inspired 4D analogue a cube, denoted tesseract. The etching process involves selective removal Pd atoms subsequent rearrangement remaining Pt atoms. successful preparation tesseracts via lies selection Pd/Pt ratio initial nanocubes. With various ratios nanocubes templates, obtained octapods, tesseracts, nanoframes, respectively. During ORR, exhibited highest mass activity 1.86 A mg–1Pt among these nanocrystals. On basis mechanistic studies, high derived from optimal adsorption energy due facet effect composition effect.

Language: Английский

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Recent Progress of Amorphous Nanomaterials

Chemical Reviews, Journal Year: 2023, Volume and Issue: 123(13), P. 8859 - 8941

Published: June 26, 2023

Amorphous materials are metastable solids with only short-range order at the atomic scale, which results from local intermolecular chemical bonding. The lack of long-range typical crystals endows amorphous nanomaterials unconventional and intriguing structural features, such as isotropic environments, abundant surface dangling bonds, highly unsaturated coordination, etc. Because these features ensuing modulation in electronic properties, display potential for practical applications different areas. Motivated by elements, here we provide an overview unique general synthetic methods, covered contemporary research nanomaterials. Furthermore, discussed possible theoretical mechanism nanomaterials, examining how properties configurations contribute to their exceptional performance. In particular, benefits well enhanced electrocatalytic, optical, mechanical thereby clarifying structure–function relationships, highlighted. Finally, a perspective on preparation utilization establish mature systems superior hierarchy various is introduced, outlook future challenges opportunities frontiers this rapidly advancing field proposed.

Language: Английский

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Material Evolution with Nanotechnology, Nanoarchitectonics, and Materials Informatics: What will be the Next Paradigm Shift in Nanoporous Materials?

Advanced Materials, Journal Year: 2021, Volume and Issue: 34(7)

Published: Oct. 13, 2021

Abstract Materials science and chemistry have played a central significant role in advancing society. With the shift toward sustainable living, it is anticipated that development of functional materials will continue to be vital for sustaining life on our planet. In recent decades, rapid progress has been made owing advances experimental, analytical, computational methods, thereby producing several novel useful materials. However, most problems material are highly complex. Here, best strategy via implementation three key concepts discussed: nanotechnology as game changer, nanoarchitectonics an integrator, informatics super‐accelerator. Discussions from conceptual viewpoints example developments, chiefly focused nanoporous materials, presented. It coupling these strategies together open advanced routes swift design exploratory search truly solving real‐world problems. These result evolution

Language: Английский

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Dynamic Evolution of Active Sites in Electrocatalytic CO₂ Reduction Reaction: Fundamental Understanding and Recent Progress

Advanced Functional Materials, Journal Year: 2022, Volume and Issue: 32(16)

Published: Jan. 5, 2022

Abstract Advancing the development of electrocatalytic CO 2 reduction reaction (CO RR) to address environmental issues caused by excessive consumption fossil fuels requires rational design remarkable electrocatalysts, where identification active sites and further understanding structure–performance relationship are bases. However, notable dynamic evolution often appears on catalysts, with typical examples Cu‐based under operating conditions, causing great difficulty in identifying real correlations between structure catalytic property. In this context, process catalytically during RR is particular importance, which inspires organize present review. Herein, fundamental principles including thermodynamics kinetics aspects, followed introduction operando techniques employed probe conditions first highlighted. The behaviors, involving atomic rearrangement change chemical state, catalysts discussed, emphasis behaviors properties (activity, selectivity, stability). emerging pulsed electrolysis technique that behaves promise manipulate future opportunities finally discussed.

Language: Английский

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Atomically Reconstructed Palladium Metallene by Intercalation-Induced Lattice Expansion and Amorphization for Highly Efficient Electrocatalysis

ACS Nano, Journal Year: 2022, Volume and Issue: 16(9), P. 13715 - 13727

Published: Aug. 10, 2022

As an emerging class of materials with distinctive physicochemical properties, metallenes are deemed as efficient catalysts for energy-related electrocatalytic reactions. Engineering the lattice strain, electronic structure, crystallinity, and even surface porosity metallene provides a great opportunity to further enhance its catalytic performance. Herein, we rationally developed reconstruction strategy Pd at atomic scale generate series nonmetallic atom-intercalated (M-Pdene, M = H, N, C) expansion S-doped (S-Pdene) amorphous structure. Catalytic performance evaluation demonstrated that N-Pdene exhibited highest mass activities 7.96 A mg-1, which was 10.6 8.5 time greater than those commercial Pd/C Pt/C, respectively, methanol oxidation reaction (MOR). Density functional theory calculations suggested well-controlled tensile strain well strong p-d hybridization interaction between N resulted in enhanced OH adsorption weakened CO MOR catalysis on N-Pdene. When tested hydrogen evolution (HER) catalysts, S-Pdene delivered superior activity durability relative crystalline counterparts because disordered elongated bond length downshifted d-band center. This work effective engineering nanomaterials high electrocatalysts.

Language: Английский

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Recent advances in one-dimensional noble-metal-based catalysts with multiple structures for efficient fuel-cell electrocatalysis

Coordination Chemistry Reviews, Journal Year: 2021, Volume and Issue: 450, P. 214244 - 214244

Published: Oct. 18, 2021

Language: Английский

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