Journal of Materials Chemistry A, Год журнала: 2022, Номер 10(25), С. 13170 - 13189
Опубликована: Янв. 1, 2022
Advanced optimization strategies for Ir-based oxygen evolution catalysts include morphological regulation, heteroatomic doping, crystal phase control, and support introduction.
Язык: Английский
Advanced Functional Materials, Год журнала: 2022, Номер 32(28)
Опубликована: Апрель 13, 2022
Abstract The single‐phase oxides with elemental complexity and compositional diversity, usually named high entropy oxides, feature homogeneously dispersed multi‐metallic elements in equiatomic concentration. unusual properties of endow their potential application clean‐energy‐related electrocatalysis. However, the possible fundamental relationship between configuration underlying catalytic mechanism is still not well understood established. Herein, a perovskite cobaltate consisting five equimolar metals B‐site (Mg, Mn, Fe, Co, Ni) employed as an electrocatalyst for oxygen evolution reaction (OER). serves effective tool to promote intrinsic activity Co reactive site manipulate OER mechanism. demonstrates lower overpotential 320 mV at current density 10 mA cm −2 , outperforming other counterparts. X‐ray spectroscopies disclose synergistic charge‐exchange effect among different cations formation new hole state. Combinatorially computational experimental results unveil enigma that leads random occupation cations, facilitates surface reconstruction, benefits stable vacancies. Owing these merits, O 2 found be kinetically favorable via lattice
Язык: Английский
Процитировано
202
Advanced Materials, Год журнала: 2022, Номер 34(29)
Опубликована: Май 17, 2022
Tuning the reactivity of lattice oxygen is significance for lowering energy barriers and accelerating evolution reaction (OER). Herein, single-atomic Mo sites are anchored on Ni-Fe oxyhydroxide nanoarrays by a facile metal-organic-framework-derived strategy, exhibiting superior performance toward OER in alkaline media. In situ electrochemical spectroscopy isotope-labeling experiments reveal involvement during cycles. Combining theoretical experimental investigations electronic configuration, it comprehensively confirmed that incorporation enables higher oxidation state metal strengthened metal-oxygen hybridization, as well formation oxidized ligand holes above Fermi level. word, considerable acceleration water achieved via enhancing triggering activation. This work may provide new insights designing ideal electrocatalysts tuning chemical activating anions ligands.
Язык: Английский
Процитировано
196
Coordination Chemistry Reviews, Год журнала: 2022, Номер 475, С. 214869 - 214869
Опубликована: Окт. 14, 2022
Язык: Английский
Процитировано
183
Nature Communications, Год журнала: 2023, Номер 14(1)
Опубликована: Сен. 27, 2023
The oxygen evolution reaction is known to be a kinetic bottleneck for water splitting. Triggering the lattice oxidation mechanism (LOM) can break theoretical limit of conventional adsorbate and enhance kinetics, yet unsatisfied stability remains grand challenge. Here, we report high-entropy MnFeCoNiCu layered double hydroxide decorated with Au single atoms O vacancies (AuSA-MnFeCoNiCu LDH), which not only displays low overpotential 213 mV at 10 mA cm-2 high mass activity 732.925 A g-1 250 in 1.0 M KOH, but also delivers good 700 h continuous operation ~100 cm-2. Combining advanced spectroscopic techniques density functional theory calculations, it demonstrated that synergistic interaction between incorporated leads an upshift 2p band weakens metal-O bond, thus triggering LOM, reducing energy barrier, boosting intrinsic activity.
Язык: Английский
Процитировано
181
Nature Communications, Год журнала: 2022, Номер 13(1)
Опубликована: Июнь 30, 2022
Abstract The redox center of transition metal oxides and hydroxides is generally considered to be the site. Interestingly, proton oxygen in lattice recently are found actively involved catalytic reactions, critically determine reactivity. Herein, taking glycerol electrooxidation reaction as model reaction, we reveal systematically impact anion (de)intercalation processes on elementary steps. Combining density functional theory calculations advanced spectroscopy techniques, find that doping Co into Ni-hydroxide promotes deintercalation from catalyst surface. vacancies formed NiCo hydroxide during increase d -band filling sites, facilitating charge transfer surface cleaved molecules 2 nd C-C bond cleavage. Consequently, exhibits enhanced activity, with a current 100 mA/cm at 1.35 V formate selectivity 94.3%.
Язык: Английский
Процитировано
168
Chemical Society Reviews, Год журнала: 2023, Номер 52(23), С. 8319 - 8373
Опубликована: Янв. 1, 2023
In this review, we provide a comprehensive summary of recent advances in the synthesis strategies, design principles, and characterization technologies high entropy alloys, their applications various electrocatalytic conversion reactions.
Язык: Английский
Процитировано
161
Nano-Micro Letters, Год журнала: 2023, Номер 15(1)
Опубликована: Фев. 16, 2023
The electrocatalytic water splitting technology can generate high-purity hydrogen without emitting carbon dioxide, which is in favor of relieving environmental pollution and energy crisis achieving neutrality. Electrocatalysts effectively reduce the reaction barrier increase efficiency. Facet engineering considered as a promising strategy controlling ratio desired crystal planes on surface. Owing to anisotropy, with different orientations usually feature facet-dependent physical chemical properties, leading differences adsorption energies oxygen or intermediates, thus exhibit varied activity toward evolution (HER) (OER). In this review, brief introduction basic concepts, fundamental understanding mechanisms well key evaluating parameters for both HER OER are provided. formation facets comprehensively overviewed aiming give scientific theory guides realize dominant planes. Subsequently, three strategies selective capping agent, etching coordination modulation tune summarized. Then, we present an overview significant contributions facet-engineered catalysts HER, OER, overall splitting. particular, highlight that density functional calculations play indispensable role unveiling structure–activity correlation between plane catalytic activity. Finally, remaining challenges provided future prospects designing advanced electrocatalysts discussed.
Язык: Английский
Процитировано
149
Chem, Год журнала: 2023, Номер 9(7), С. 1882 - 1896
Опубликована: Апрель 6, 2023
Язык: Английский
Процитировано
144
Angewandte Chemie International Edition, Год журнала: 2023, Номер 62(24)
Опубликована: Март 21, 2023
The development of productive catalysts for the oxygen evolution reaction (OER) remains a major challenge requiring significant progress in both mechanism and material design. Conventionally, thermodynamic barrier lattice oxidation (LOM) is lower than that absorbate (AEM) because former can overcome certain limitations. However, controlling OER pathway from AEM to LOM by exploiting intrinsic properties catalyst challenging. Herein, we incorporated F anions into vacancies spinel ZnCo2 O4 established link between electronic structure catalytic mechanism. Theoretical density calculations revealed upshifts O 2p center activates redox capability O, successfully triggering pathway. Moreover, high electronegativity favourable balancing residual protonation, which stabilize catalyst.
Язык: Английский
Процитировано
132
SusMat, Год журнала: 2021, Номер 1(4), С. 460 - 481
Опубликована: Дек. 1, 2021
Abstract Proton exchange membrane (PEM) water electrolysis represents one of the most promising technologies to achieve green hydrogen production, but currently its practical viability is largely affected by slow reaction kinetics anodic oxygen evolution (OER) in an acidic environment. While noble metal‐based catalysts containing iridium or ruthenium are excellent for OER, their use PEM electrolyzers hindered due low abundance and high cost. Most recently, metal–organic frameworks (MOFs) have been demonstrated as a perfect platform facilitate design OER with both efficiency cost‐effectiveness. Here, we provide timely comprehensive overview recent progress on MOF‐based catalysts. The fundamental mechanisms first introduced, followed summary development pristine MOFs MOF derivatives Importantly, number catalyst strategies discussed aiming at improving catalytic performance candidates. integration into real also included. Finally, future research directions provided better operational environments devices.
Язык: Английский
Процитировано
129