Subnanometric Ru clusters with upshifted D band center improve performance for alkaline hydrogen evolution reaction

Nature Communications, Год журнала: 2022, Номер 13(1)

Опубликована: Июль 8, 2022

Abstract Subnanometric metal clusters usually have unique electronic structures and may display electrocatalytic performance distinctive from single atoms (SAs) larger nanoparticles (NPs). However, the of clusters, especially size-activity relationship at sub-nanoscale, is largely unexplored. Here, we synthesize a series Ru nanocrystals atoms, subnanometric to nanoparticles, aiming investigating size-dependent activity hydrogen evolution in alkaline media. It found that d band center downshifts nearly linear with increase diameter, closer Femi level stronger water dissociation ability thus superior than SAs nanoparticles. Benefiting high utilization strong ability, manifest an ultrahigh turnover frequency 43.3 s −1 overpotential 100 mV, 36.1-fold commercial Pt/C.

Язык: Английский

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Descriptors for the Evaluation of Electrocatalytic Reactions: d‐Band Theory and Beyond

Advanced Functional Materials, Год журнала: 2021, Номер 32(4)

Опубликована: Окт. 13, 2021

Abstract Closing the carbon‐, hydrogen‐, and nitrogen cycle with renewable electricity holds promises for mitigation of facing environment energy crisis, along continuing prosperity human society. Descriptors bridge gap between physicochemical factors electrocatalysts their boosted activity serve as guiding principles during rational design electrocatalysts. The optimal adsorption strength key intermediates is potentially accessed under tendentious guidelines proposed by indicators, such d‐band center, Δ G H , E O* coordination number (CN), bond length, etc. Here, in this review, a comprehensive summary recent advances achieved regarding descriptors that aims recycling C/H/N‐containing chemicals offered. review initiated providing necessity development efficient then physics behind center introduced. Then progress relating to guidance reviewed. Following that, an extended discussion experimental or theoretical characterization beyond it provided. Finally, perspectives challenges area are

Язык: Английский

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Interfacial engineering of the NiSe2/FeSe2 p-p heterojunction for promoting oxygen evolution reaction and electrocatalytic urea oxidation

Applied Catalysis B Environment and Energy, Год журнала: 2021, Номер 299, С. 120638 - 120638

Опубликована: Авг. 19, 2021

Язык: Английский

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Vertically-interlaced NiFeP/MXene electrocatalyst with tunable electronic structure for high-efficiency oxygen evolution reaction

Science Bulletin, Год журнала: 2021, Номер 66(11), С. 1063 - 1072

Опубликована: Март 2, 2021

Язык: Английский

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Synergistic effect of multiple vacancies to induce lattice oxygen redox in NiFe-layered double hydroxide OER catalysts

Applied Catalysis B Environment and Energy, Год журнала: 2022, Номер 323, С. 122091 - 122091

Опубликована: Ноя. 3, 2022

Язык: Английский

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Cation‐Tuning Induced d‐Band Center Modulation on Co‐Based Spinel Oxide for Oxygen Reduction/Evolution Reaction

Angewandte Chemie International Edition, Год журнала: 2021, Номер 61(16)

Опубликована: Дек. 31, 2021

Atomic substitutions at the tetrahedral site (ATd ) could theoretically achieve an efficient optimization of charge octahedral (BOh through ATd -O-BOh interactions in spinel oxides (AB2 O4 ). Despite substantial progress having been made, precise control and adjustment are still challenging owing to complexity their crystal structure. In this work, we demonstrate a simple solvent method tailor structures use oxide composites (ACo2 /NCNTs, A=Mn, Co, Ni, Cu, Zn) for oxygen electrocatalysis. The optimized MnCo2 /NCNTs exhibit high activity excellent durability reduction/evolution reactions. Remarkably, rechargeable liquid Zn-air battery equipped with cathode affords specific capacity 827 mAh gZn-1 power density 74.63 mW cm-2 no voltage degradation after 300 cycles charging-discharging rate (5 mA functional theory (DFT) calculations reveal that substitution regulate ratio Co3+ /Co2+ thereby lead modulation electronic structure accompanied movement d-band center. sites interact Mn-O-Co, Co3+Oh optimal allows more suitable binding interaction between active center oxygenated species, resulting superior electrocatalytic performance.

Язык: Английский

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Cation‐Vacancy‐Enriched Nickel Phosphide for Efficient Electrosynthesis of Hydrogen Peroxides

Advanced Materials, Год журнала: 2022, Номер 34(16)

Опубликована: Фев. 22, 2022

Electrocatalytic hydrogen peroxide (H2 O2 ) synthesis via the two-electron oxygen reduction reaction (2e ORR) pathway is becoming increasingly important due to green production process. Here, cationic vacancies on nickel phosphide, as a proof-of-concept regulate catalyst's physicochemical properties, are introduced for efficient H2 electrosynthesis. The as-fabricated Ni (VNi )-enriched Ni2-x P-VNi electrocatalyst exhibits remarkable 2e ORR performance with molar fraction of >95% and Faradaic efficiencies >90% in all pH conditions under wide range applied potentials. Impressively, as-created VNi possesses superb long-term durability over 50 h, suppassing recently reported catalysts Operando X-ray absorption near-edge spectroscopy (XANES) synchrotron Fourier transform infrared (SR-FTIR) combining theoretical calculations reveal that excellent catalytic originates from -induced geometric electronic structural optimization, thus promoting adsorption favored "end-on" configuration. It believed demonstrated cation vacancy engineering an effective strategy toward creating active heterogeneous atomic precision.

Язык: Английский

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Single Iridium Atom Doped Ni₂P Catalyst for Optimal Oxygen Evolution

Journal of the American Chemical Society, Год журнала: 2021, Номер 143(34), С. 13605 - 13615

Опубликована: Авг. 16, 2021

Single-atom catalysts (SACs) with 100% active sites have excellent prospects for application in the oxygen evolution reaction (OER). However, further enhancement of catalytic activity OER is quite challenging, particularly development stable SACs overpotentials <180 mV. Here, we report an iridium single atom on Ni2P catalyst (IrSA-Ni2P) a record low overpotential 149 mV at current density 10 mA·cm–2 1.0 M KOH. The IrSA-Ni2P delivers up to ∼28-fold higher than that widely used IrO2 1.53 V vs RHE. Both experimental results and computational simulations indicate Ir atoms preferentially occupy Ni top surface. reconstructed Ir–O–P/Ni–O–P bonding environment plays vital role optimal adsorption desorption intermediate species, which leads marked activity. Additionally, dynamic "top-down" specific structure Ni@Ir particles responsible robust single-atom and, thus, stability property. This offers novel simplifying decoration strategies enhancing performance.

Язык: Английский

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Self-supported bimetallic phosphides with artificial heterointerfaces for enhanced electrochemical water splitting

Applied Catalysis B Environment and Energy, Год журнала: 2021, Номер 304, С. 120914 - 120914

Опубликована: Ноя. 15, 2021

Язык: Английский

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Oxygen Evolution Reaction in Energy Conversion and Storage: Design Strategies Under and Beyond the Energy Scaling Relationship

Nano-Micro Letters, Год журнала: 2022, Номер 14(1)

Опубликована: Апрель 28, 2022

The oxygen evolution reaction (OER) is the essential module in energy conversion and storage devices such as electrolyzer, rechargeable metal-air batteries regenerative fuel cells. adsorption scaling relations between intermediates, however, impose a large intrinsic overpotential sluggish kinetics on OER catalysts. Developing advanced electrocatalysts with high activity stability based non-noble metal materials still grand challenge. Central to rational design of novel high-efficiency catalysts development understanding quantitative structure-activity relationships, which correlate catalytic activities structural electronic descriptors. This paper comprehensively reviews benchmark descriptors for electrolysis, aiming give an in-depth origins electrocatalytic further contribute building theory electrocatalysis. Meanwhile, cutting-edge research frontiers proposing new paradigms crucial strategies circumvent relationship are also summarized. Challenges, opportunities perspectives discussed, intending shed some light concepts advance more efficient enhancing performance.

Язык: Английский

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