Oxygen Evolution/Reduction Reaction Catalysts: From In Situ Monitoring and Reaction Mechanisms to Rational Design

Chemical Reviews, Год журнала: 2023, Номер 123(9), С. 6257 - 6358

Опубликована: Март 21, 2023

The oxygen evolution reaction (OER) and reduction (ORR) are core steps of various energy conversion storage systems. However, their sluggish kinetics, i.e., the demanding multielectron transfer processes, still render OER/ORR catalysts less efficient for practical applications. Moreover, complexity catalyst–electrolyte interface makes a comprehensive understanding intrinsic mechanisms challenging. Fortunately, recent advances in situ/operando characterization techniques have facilitated kinetic monitoring under conditions. Here we provide selected highlights mechanistic studies with main emphasis placed on heterogeneous systems (primarily discussing first-row transition metals which operate basic conditions), followed by brief outlook molecular catalysts. Key sections this review focused determination true active species, identification sites, reactive intermediates. For in-depth insights into above factors, short overview metrics accurate characterizations is provided. A combination obtained time-resolved information reliable activity data will then guide rational design new Strategies such as optimizing restructuring process well overcoming adsorption-energy scaling relations be discussed. Finally, pending current challenges prospects toward development homogeneous presented.

Язык: Английский

---

Clusters Induced Electron Redistribution to Tune Oxygen Reduction Activity of Transition Metal Single‐Atom for Metal–Air Batteries

Angewandte Chemie International Edition, Год журнала: 2021, Номер 61(12)

Опубликована: Дек. 27, 2021

Oxygen reduction reaction (ORR) activity can be effectively tuned by modulating the electron configuration and optimizing chemical bonds. Herein, a general strategy to optimize of metal single-atoms is achieved decoration clusters via coating-pyrolysis-etching route. In this unique structure, are able induce redistribution modulate M-N species bond lengths. As result, M-ACSA@NC exhibits superior ORR compared with nanoparticle-decorated counterparts. The performance enhancement attributed optimized intermediates desorption benefiting from electronic configuration. Theoretical analysis reinforces significant roles correlating cluster-induced charge transfer. proof-of-concept, various metal-air batteries assembled Fe-ACSA@NC deliver remarkable power densities capacities. This an effective universal technique for modulation M-N-C, which shows great potential in application energy storage devices.

Язык: Английский

---

Capabilities and limitations of rotating disk electrodes versus membrane electrode assemblies in the investigation of electrocatalysts

Nature Catalysis, Год журнала: 2022, Номер 5(5), С. 363 - 373

Опубликована: Май 23, 2022

Язык: Английский

---

High‐Entropy Alloys for Electrocatalysis: Design, Characterization, and Applications

Small, Год журнала: 2021, Номер 18(7)

Опубликована: Ноя. 5, 2021

Abstract High‐entropy alloys (HEAs) are expected to function well as electrocatalytic materials, owing their widely adjustable composition and unique physical chemical properties. Recently, HEA catalysts extensively studied in the field of electrocatalysis; this motivated authors investigate relationship between structure HEAs performance. In review, latest advances electrocatalysts systematically summarized, with special focus on nitrogen fixation, carbon cycle, water splitting, fuel cells; addition, by combining characterization analysis microstructures, rational design strategies for optimizing electrocatalysts, including controllable preparation, component regulation, strain engineering, defect theoretical prediction proposed. Moreover, existing issues future trends predicted, which will help further develop these high‐entropy materials.

Язык: Английский

---

Scalable Molten Salt Synthesis of Platinum Alloys Planted in Metal–Nitrogen–Graphene for Efficient Oxygen Reduction

Angewandte Chemie International Edition, Год журнала: 2021, Номер 61(6)

Опубликована: Дек. 11, 2021

Fuel cells are considered as a promising alternative to the existing traditional energy systems towards sustainable future. Nevertheless, synthesis of efficient and robust platinum (Pt) based catalysts remains challenge for practical applications. In this work, we present simple scalable molten-salt method producing low-platinum nanoalloy implanted in metal-nitrogen-graphene. The as-prepared low-Pt alloyed graphene exhibits high oxygen reduction activity 1.29 A mgPt-1 excellent durability over 30 000 potential cycles. catalyst nanoarchitecture encased Pt provides capability against nanoparticle migration corrosion due strong metal-support interaction. Similarly, advanced characterization theoretical calculations show that multiple active sites synergistically account improved reduction. This work not only an but also facile design idea preparation technique integrated achieve more profound applications fuel beyond.

Язык: Английский

---

Oxidation‐Reduction Molecular Junction Covalent Organic Frameworks for Full Reaction Photosynthesis of H₂O₂

Angewandte Chemie International Edition, Год журнала: 2022, Номер 62(9)

Опубликована: Дек. 30, 2022

The full reaction photosynthesis of H2 O2 that can combine water-oxidation and oxygen-reduction without sacrificial agents is highly demanded to maximize the light-utilization overcome complex reaction-process anthraquinone-oxidation. Here, a kind oxidation-reduction molecular junction covalent-organic-framework (TTF-BT-COF) has been synthesized through covalent-coupling tetrathiafulvalene (photo-oxidation site) benzothiazole (photo-reduction site), which presents visible-light-adsorption region, effective electron-hole separation-efficiency photo-redox sites enables generation . Specifically, record-high yield (TTF-BT-COF, ≈276 000 μM h-1 g-1 ) for achieved among porous crystalline photocatalysts. This first work design COFs , might extend scope in production.

Язык: Английский

---

An integrated platinum-nanocarbon electrocatalyst for efficient oxygen reduction

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

Опубликована: Ноя. 7, 2022

Abstract Efficient and robust platinum-carbon electrocatalysts are of great significance for the long-term service high-performance fuel cells. Here, we report a Pt alloy integrated in cobalt-nitrogen-nanocarbon matrix by multiscale design principle efficient oxygen reduction reaction. This catalyst demonstrates an increased mass activity, 11.7 times higher than that commercial catalyst, retains stability 98.7% after 30,000 potential cycles. Additionally, this delivers current density 1.50 A cm −2 at 0.6 V hydrogen-air cell achieves power 980 mW . Comprehensive investigations demonstrate synergistic contribution components structure is responsible high-efficiency ORR

Язык: Английский

---

A Facile “Double‐Catalysts” Approach to Directionally Fabricate Pyridinic NB‐Pair‐Doped Crystal Graphene Nanoribbons/Amorphous Carbon Hybrid Electrocatalysts for Efficient Oxygen Reduction Reaction

Advanced Materials, Год журнала: 2022, Номер 34(13)

Опубликована: Янв. 17, 2022

Carbon material is a promising electrocatalyst for the oxygen reduction reaction (ORR). Doping of heteroatoms, most widely used modulating strategy, has attracted many efforts in past decade. Despite all this, catalytic activity heteroatoms-modulated carbon hard to compare that metal-based electrocatalysts. Here, "double-catalysts" (Fe salt, H3 BO3 ) strategy presented directionally fabricate porous structure crystal graphene nanoribbons (GNs)/amorphous doped by pyridinic NB pairs. The and GNs accelerate ion/mass electron transport, respectively. N percentage pairs accounts ≈80% species. pair drives ORR via an almost 4e- transfer pathway with half-wave potential (0.812 V vs reversible hydrogen electrode (RHE)) onset (0.876 RHE) alkaline solution. performance as-prepared catalysts approximates commercial Pt/C outperforms prior carbon-based catalysts. assembled Zn-air battery exhibits high peak power density 94 mW cm-2 . Density functional theory simulation reveals possesses highest among configurations, due charge at C active sites neighboring B, which enhances interaction strength intermediates p-band center.

Язык: Английский

---

Atomically precise electrocatalysts for oxygen reduction reaction

Chem, Год журнала: 2023, Номер 9(2), С. 280 - 342

Опубликована: Фев. 1, 2023

Язык: Английский

---

Recent Advances on MOF Derivatives for Non-Noble Metal Oxygen Electrocatalysts in Zinc-Air Batteries

Nano-Micro Letters, Год журнала: 2021, Номер 13(1)

Опубликована: Июнь 7, 2021

Oxygen electrocatalysts are of great importance for the air electrode in zinc-air batteries (ZABs). Owing to high specific surface area, controllable pore size and unsaturated metal active sites, metal-organic frameworks (MOFs) derivatives have been widely studied as oxygen ZABs. To date, many strategies developed generate efficient from MOFs improving performance In this review, latest progress MOF-derived non-noble metal-oxygen ZABs is reviewed. The these catalysts toward reduction, evolution reactions discussed based on categories metal-free carbon materials, single-atom catalysts, cluster/carbon composites compound/carbon composites. Moreover, we provide a comprehensive overview design various their structure-performance relationship. Finally, challenges perspectives provided further advancing

Язык: Английский

---