Chemical Engineering Journal, Год журнала: 2023, Номер 478, С. 147415 - 147415
Опубликована: Ноя. 17, 2023
Язык: Английский
Chemical Engineering Journal, Год журнала: 2023, Номер 478, С. 147415 - 147415
Опубликована: Ноя. 17, 2023
Язык: Английский
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
154Advanced Functional Materials, Год журнала: 2023, Номер 33(45)
Опубликована: Сен. 1, 2023
Abstract Oxygen evolution reaction (OER) remains a bottleneck for electrocatalytic water‐splitting to generate hydrogen. However, the traditional adsorbed mechanism (AEM) possesses sluggish kinetics due scaling relationship, while lattice oxygen (LOM) triggers an unstable structure escaping of oxygen. Herein, proof‐of‐concept Fe‐Co(OH) 2 /Fe O 3 heterostructure is put forward, where following AEM can complete rapidly deprotonation process Fe LOM trigger O─O coupling step. Combining theoretical and experimental investigation confirmed that redistributed space‐charge junction optimize synergistically oxygen, facilitate synchronously OER activity stability. As result, shows excellent performance with low overpotential only 219 249 mV reach current density 10 100 mA cm −2 . Specifically, electrocatalyst maintains long‐term stability h at large This work paves avenue break through limit conventional mechanism.
Язык: Английский
Процитировано
127Angewandte Chemie International Edition, Год журнала: 2023, Номер 62(43)
Опубликована: Сен. 6, 2023
Metal-organic frameworks (MOFs) have been increasingly applied in oxygen evolution reaction (OER), and the surface of MOFs usually undergoes structural transformation to form metal oxyhydroxides serve as catalytically active sites. However, controllable regulation reconstruction process remains a great challenge. Here we report defect engineering strategy facilitate during OER with enhanced activity. Defective (denoted NiFc'x Fc1-x ) abundant unsaturated sites are constructed by mixing ligands 1,1'-ferrocene dicarboxylic acid (Fc') defective ferrocene carboxylic (Fc). series more prone be transformed compared non-defective (NiFc'). Moreover, as-formed derived from contain vacancies. NiFc'Fc grown on nickel foam exhibits excellent catalytic activity an overpotential 213 mV at current density 100 mA cm-2 , superior that undefective NiFc'. Experimental results theoretical calculations suggest vacancies adsorption oxygen-containing intermediates centers, thus significantly improving
Язык: Английский
Процитировано
124Advanced Science, Год журнала: 2023, Номер 10(22)
Опубликована: Май 30, 2023
Valence tuning of transition metal oxides is an effective approach to design high-performance catalysts, particularly for the oxygen evolution reaction (OER) that underpins solar/electric water splitting and metal-air batteries. Recently, high-valence (HVOs) are reported show superior OER performance, in association with fundamental dynamics charge transfer intermediates. Particularly considered adsorbate mechanism (AEM) lattice oxygen-mediated (LOM). High-valence states enhance performance mainly by optimizing e
Язык: Английский
Процитировано
120Nano-Micro Letters, Год журнала: 2023, Номер 15(1)
Опубликована: Фев. 11, 2023
Rechargeable zinc-air batteries (ZABs) are a promising energy conversion device, which rely critically on electrocatalysts to accelerate their rate-determining reactions such as oxygen reduction (ORR) and evolution (OER). Herein, we fabricate range of bifunctional M-N-C (metal-nitrogen-carbon) catalysts containing M-Nx coordination sites M/MxC nanoparticles (M = Co, Fe, Cu) using new class γ-cyclodextrin (CD) based metal-organic framework the precursor. With two types active interacting with each other in catalysts, obtained Fe@C-FeNC Co@C-CoNC display superior alkaline ORR activity terms low half-wave (E1/2) potential (~ 0.917 0.906 V, respectively), higher than Cu@C-CuNC 0.829 V) commercial Pt/C 0.861 V). As electrocatalyst, exhibits best performance, showing ORR/OER overpotential (ΔE) ~ 0.732 is much lower that 0.831 1.411 V), well most robust reported date. Synchrotron X-ray absorption spectroscopy density functional theory simulations reveal strong electronic correlation between metallic Co atomic Co-N4 catalyst can increase d-electron near Fermi level thus effectively optimize adsorption/desorption intermediates ORR/OER, resulting an enhanced electrocatalytic performance. The Co@C-CoNC-based rechargeable ZAB exhibited maximum power 162.80 mW cm-2 at 270.30 mA cm-2, combination + RuO2 158.90 265.80 cm-2) catalysts. During galvanostatic discharge 10 delivered almost stable voltage 1.2 V for 140 h, signifying virtue excellent activity.
Язык: Английский
Процитировано
105Nano-Micro Letters, Год журнала: 2023, Номер 15(1)
Опубликована: Июль 29, 2023
Abstract The electrochemical oxygen reduction reaction (ORR) and evolution (OER) are fundamental processes in a range of energy conversion devices such as fuel cells metal–air batteries. ORR OER both have significant activation barriers, which severely limit the overall performance that utilize ORR/OER. Meanwhile, is another very important involving has been widely investigated. occurs aqueous solutions via two pathways: direct 4-electron or 2-electron pathways from O 2 to water (H O) hydrogen peroxide ). Noble metal electrocatalysts often used catalyze ORR, despite fact noble certain intrinsic limitations, low storage. Thus, it urgent develop more active stable low-cost electrocatalysts, especially for severe environments (e.g., acidic media). Theoretically, an ideal electrocatalyst should provide adequate binding species. Transition metals not belonging platinum group metal-based oxides substance could give d orbital species binding. As result, transition regarded substitute typical precious electrocatalysts. However, development oxide catalysts reactions still faces challenges, e.g., catalytic activity, stability, cost, mechanism. We discuss principles underlying design catalysts, including influence crystal structure, electronic structure on their performance. also challenges associated with developing potential strategies overcome these challenges.
Язык: Английский
Процитировано
81Chemical Reviews, Год журнала: 2023, Номер 123(8), С. 4972 - 5019
Опубликована: Март 27, 2023
Scanning electrochemical probe microscopy (SEPM) techniques can disclose the local reactivity of interfaces in single-entity and sub-entity studies. Operando SEPM measurements consist using a tip to investigate performance electrocatalysts, while interface is simultaneously modulated. This powerful combination correlate activity with changes surface properties, e.g., topography structure, as well provide insight into reaction mechanisms. The focus this review reveal recent progress catalytic toward reduction evolution O2 H2 conversion CO2. capabilities SEPMs are showcased, possibility coupling other presented. Emphasis given scanning (SECM), ion conductance (SICM), tunneling (EC-STM), cell (SECCM).
Язык: Английский
Процитировано
80Chemical Engineering Journal, Год журнала: 2023, Номер 463, С. 142380 - 142380
Опубликована: Март 16, 2023
Язык: Английский
Процитировано
65Nano-Micro Letters, Год журнала: 2023, Номер 16(1)
Опубликована: Ноя. 30, 2023
The formation of multiple oxygen intermediates supporting efficient evolution reaction (OER) are affinitive with hydroxyl adsorption. However, ability the catalyst to capture and maintain continuous supply at active sits remains a tremendous challenge. Herein, an affordable Ni
Язык: Английский
Процитировано
58Small, Год журнала: 2023, Номер 19(49)
Опубликована: Авг. 7, 2023
Abstract The precatalyst undergoes surface reconstruction during the oxygen evolution reaction (OER) process, and reconstituted material is one that really plays a catalytic role. However, degree of seriously affects performance. For this reason, it important to establish link between activity based on deep understanding OER mechanism for rational design high‐performance electrocatalysts. Here, briefly introduced, competition adsorbate (AEM) lattice oxygen‐mediated (LOM) discussed, several descriptors are summarized. strategies realize controllable emphatically including ion leaching, element doping, regulating catalyst size, heterogeneous structure engineering, self‐reconstruction. A mechanistic perspective emphasized understand relationship dynamic electronic structure. Controlled reconfiguration can break limitation proportional brought by traditional AEM mechanism, also switching LOM thus realizing ultra‐low overpotential. This review will provide some reference transition metal‐based catalysts reasonable development ideal
Язык: Английский
Процитировано
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