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

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Emerging low-nuclearity supported metal catalysts with atomic level precision for efficient heterogeneous catalysis

Nano Research, Год журнала: 2022, Номер 15(9), С. 7806 - 7839

Опубликована: Июнь 2, 2022

Язык: Английский

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Quasi-solid-state Zn-air batteries with an atomically dispersed cobalt electrocatalyst and organohydrogel electrolyte

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

Опубликована: Июнь 27, 2022

Abstract Quasi-solid-state Zn-air batteries are usually limited to relatively low-rate ability (<10 mA cm −2 ), which is caused in part by sluggish oxygen electrocatalysis and unstable electrochemical interfaces. Here we present a high-rate robust quasi-solid-state battery enabled atomically dispersed cobalt sites anchored on wrinkled nitrogen doped graphene as the air cathode polyacrylamide organohydrogel electrolyte with its hydrogen-bond network modified addition of dimethyl sulfoxide. This design enables cycling current density 100 over 50 h at 25 °C. A low-temperature stability 300 (at 0.5 ) 90% capacity retention −60 °C broad temperature adaptability (−60 60 °C) also demonstrated.

Язык: Английский

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Designing a Built-In Electric Field for Efficient Energy Electrocatalysis

ACS Nano, Год журнала: 2022, Номер 16(12), С. 19959 - 19979

Опубликована: Дек. 15, 2022

To utilize intermittent renewable energy as well achieve the goals of peak carbon dioxide emissions and neutrality, various electrocatalytic devices have been developed. However, reactions, e.g., hydrogen evolution reaction/oxygen reaction in overall water splitting, polysulfide conversion lithium–sulfur batteries, formation/decomposition lithium peroxide lithium–oxygen nitrate reduction to degrade sewage, suffer from sluggish kinetics caused by multielectron transfer processes. Owing merits accelerated charge transport, optimized adsorption/desorption intermediates, raised conductivity, regulation microenvironment, ease combine with geometric characteristics, built-in electric field (BIEF) is expected overcome above problems. Here, we give a Review about very recent progress BIEF for efficient electrocatalysis. First, construction strategies characterization methods (qualitative quantitative analysis) are summarized. Then, up-to-date overviews engineering electrocatalysis, attention on electron structure optimization microenvironment modulation, analyzed discussed detail. In end, challenges perspectives proposed. This gives deep understanding design electrocatalysts next-generation storage devices.

Язык: Английский

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Atomically dispersed materials: Ideal catalysts in atomic era

Nano Research, Год журнала: 2023, Номер 17(1), С. 18 - 38

Опубликована: Май 25, 2023

Язык: Английский

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Long‐Range Interactions in Diatomic Catalysts Boosting Electrocatalysis

Angewandte Chemie International Edition, Год журнала: 2022, Номер 61(52)

Опубликована: Окт. 6, 2022

Abstract The simultaneous presence of two active metal centres in diatomic catalysts (DACs) leads to the occurrence specific interactions between sites. Such interactions, referred as long‐range (LRIs), play an important role determining rate and selectivity a reaction. optimal combination must be determined achieve targeted efficiency. To date, various types DACs have been synthesised applied electrochemistry. However, LRIs not systematically summarised. Herein, regulation, mechanism, electrocatalytic applications are comprehensively summarised discussed. In addition basic information above, challenges, opportunities, future development proposed order present overall view reference for research.

Язык: Английский

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Defect engineering of two-dimensional materials for advanced energy conversion and storage

Chemical Society Reviews, Год журнала: 2023, Номер 52(5), С. 1723 - 1772

Опубликована: Янв. 1, 2023

Defective two-dimensional (2D) materials show huge potential for energy-related fields. This review overviews the formation/evolution mechanisms and engineering strategies of defects in 2D materials, which enable enhanced electrode reaction kinetics.

Язык: Английский

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Single‐atom catalysis for carbon neutrality

Carbon Energy, Год журнала: 2022, Номер 4(6), С. 1021 - 1079

Опубликована: Июль 14, 2022

Abstract Currently, more than 86% of global energy consumption is still mainly dependent on traditional fossil fuels, which causes resource scarcity and even emission high amounts carbon dioxide (CO 2 ), resulting in a severe “Greenhouse effect.” Considering this situation, the concept “carbon neutrality” has been put forward by 125 countries one after another. To achieve goals neutrality,” two main strategies to reduce CO emissions develop sustainable clean can be adopted. Notably, these are crucial for synthesis advanced single‐atom catalysts (SACs) energy‐related applications. In review, we highlight unique SACs conversion into high‐efficiency energy, example, through photocatalytic, electrocatalytic, thermal catalytic hydrogenation technologies, convert hydrocarbon fuels (CO, CH 4 , HCOOH, 3 OH, multicarbon [C 2+ ] products). addition, introduce technologies devices replace polluting such as photocatalytic electrocatalytic water splitting produce hydrogen oxygen reduction reaction (ORR) fuel cells. Impressively, several representative examples (including d ‐, ds p f ‐blocks) conversion, H ORR discussed describe methods, characterization, corresponding activity. Finally, review concludes with description challenges outlooks future applications contributing toward neutrality.

Язык: Английский

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Synergistic Fe−Se Atom Pairs as Bifunctional Oxygen Electrocatalysts Boost Low‐Temperature Rechargeable Zn‐Air Battery

Angewandte Chemie International Edition, Год журнала: 2023, Номер 62(15)

Опубликована: Фев. 18, 2023

Herein, we successfully construct bifunctional electrocatalysts by synthesizing atomically dispersed Fe-Se atom pairs supported on N-doped carbon (Fe-Se/NC). The obtained Fe-Se/NC shows a noteworthy oxygen catalytic performance with low potential difference of 0.698 V, far superior to that reported Fe-based single-atom catalysts. theoretical calculations reveal p-d orbital hybridization around the leads remarkably asymmetrical polarized charge distributions. based solid-state rechargeable Zn-air batteries (ZABs-Fe-Se/NC) present stable charge/discharge 200 h (1090 cycles) at 20 mA cm-2 25 °C, which is 6.9 times ZABs-Pt/C+Ir/C. At extremely temperature -40 ZABs-Fe-Se/NC displays an ultra-robust cycling 741 (4041 1 , about 11.7 More importantly, could be operated for 133 (725 even 5 °C.

Язык: Английский

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Dual‐Atom Support Boosts Nickel‐Catalyzed Urea Electrooxidation

Angewandte Chemie International Edition, Год журнала: 2023, Номер 62(22)

Опубликована: Март 24, 2023

Nickel-based catalysts have been regarded as one of the most promising electrocatalysts for urea oxidation reaction (UOR), however, their activity is largely limited by inevitable self-oxidation Ni species (NSOR) during UOR. Here, we proposed an interface chemistry modulation strategy to trigger occurrence UOR before NSOR via constructing a 2D/2D heterostructure that consists ultrathin NiO anchored Ru-Co dual-atom support (Ru-Co DAS/NiO). Operando spectroscopic characterizations confirm this unique triggering mechanism on surface DAS/NiO. Consequently, fabricated catalyst exhibits outstanding with low potential 1.288 V at 10 mA cm-2 and remarkable long-term durability more than 330 h operation. DFT calculations demonstrate favorable electronic structure induced heterointerface endows energetically NSOR.

Язык: Английский

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