Understanding the structure-performance relationship of active sites at atomic scale

Nano Research, Journal Year: 2022, Volume and Issue: 15(8), P. 6888 - 6923

Published: June 14, 2022

Language: Английский

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

Chemical Reviews, Journal Year: 2023, Volume and Issue: 123(9), P. 6257 - 6358

Published: March 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.

Language: Английский

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Atomically dispersed materials: Ideal catalysts in atomic era

Nano Research, Journal Year: 2023, Volume and Issue: 17(1), P. 18 - 38

Published: May 25, 2023

Language: Английский

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Water electrolysis for hydrogen production: from hybrid systems to self-powered/catalyzed devices

Energy & Environmental Science, Journal Year: 2023, Volume and Issue: 17(1), P. 49 - 113

Published: Nov. 7, 2023

This perspective highlights recent advancements in innovative strategies to provide valuable insights into the potential for energy-saving hydrogen production through water electrolysis.

Language: Английский

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Microenvironment Engineering of Single/Dual‐Atom Catalysts for Electrocatalytic Application

Advanced Materials, Journal Year: 2023, Volume and Issue: 35(31)

Published: Feb. 23, 2023

Single/dual-metal atoms supported on carbon matrix can be modulated by coordination structure and neighboring active sites. Precisely designing the geometric electronic uncovering structure-property relationships of single/dual-metal confront with grand challenges. Herein, this review summarizes latest progress in microenvironment engineering single/dual-atom sites via a comprehensive comparison single-atom catalyst (SACs) dual-atom catalysts (DACs) term design principles, modulation strategy, theoretical understanding structure-performance correlations. Subsequently, recent advances several typical electrocatalysis process are discussed to get general reaction mechanisms finely-tuned SACs DACs. Finally, full-scaled summaries challenges prospects given for This will provide new inspiration development atomically dispersed electrocatalytic application.

Language: Английский

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Simultaneously Engineering the Synergistic-Effects and Coordination-Environment of Dual-Single-Atomic Iron/Cobalt-sites as a Bifunctional Oxygen Electrocatalyst for Rechargeable Zinc-Air Batteries

ACS Catalysis, Journal Year: 2023, Volume and Issue: 13(4), P. 2313 - 2325

Published: Jan. 30, 2023

Single-atom introduced carbon nanomaterials show favorable oxygen-reduction reaction (ORR) and oxygen-evolution (OER) performance for renewable energy applications. Nevertheless, the electronic-structure regulation by decorating heterogeneous single-metal-atoms engineering of a single-atom active-sites' microenvironment need to be optimized simultaneously, which is challenging. Herein, we develop an atomic-interfacial-regulation approach fabricate dual single Fe/Co atoms synchronized with both nitrogen/sulfur on defective/graphitic/porous nanosheets (Fe,Co/DSA-NSC). The unsymmetrically organized N S coordinated bridged atomic-sites [Fe-(N2S)/Co-(N2S) moiety] are established prompt charge-transfer, lowering barrier oxygenated reaction-intermediates leading boost reaction-kinetics. As estimated, Fe,Co/DSA-NSC exhibits improved ORR/OER activity higher half-wave potential lower overpotential (E1/2 = 879 mV η10 210 mV, respectively) also good cycling stability toward zinc-air batteries. This discovery hence provides widespread scheme synergistic-principles dual-single-atom catalysts controlled

Language: Английский

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Breaking the Scaling Relationship Limit: From Single-Atom to Dual-Atom Catalysts

Accounts of Materials Research, Journal Year: 2022, Volume and Issue: 3(6), P. 584 - 596

Published: May 17, 2022

ConspectusRecent decades have witnessed the rapid development of catalytic science, especially after Taylor and Armstrong proposed notion "active site" in 1925. By optimizing reaction paths reducing activation energies reactions, catalysts appear more than 90% chemical production involving homogeneous catalysis, heterogeneous enzyme catalysis. Because 100% efficiency active atom utilization adjustable microenvironment metal centers, single-atom (SACs) shine various fields for enhancing rate, conversion, selectivity reactions. Nevertheless, a solo site determines fixed adsorption mode, intermediates from multistep reactions linking with are related to each other. For specific reaction, it is almost impossible optimally adjust every intermediate on simultaneously. This phenomenon termed scaling relationship limit (SRL) an unavoidable obstacle pure SACs.Dual-atom (DACs), perfectly inheriting advantages SACs, can exhibit better performance simple SACs thus gradually gained researchers' attention. Depending dual-metal structure, sites (DMSs) DACs be divided into two separated heterometal sites, linked homometal sites. Two prescribe distance between electron interaction. Currently, origins summarized following three points: (1) electronic effect, which only one center serves as other plays regulatory role; (2) synergistic centers separately catalyze different core steps improve together; (3) offering additional changes structures break SRL based SACs. Among origins, structure upon DMSs most effective technologies boost property basis To date, few contributions focused catalysis environments, including O2 reduction evolution H2 CO2 N2 conversion reactions.In this Account, summary recent progress regarding will presented. First, unpopular discovery research hot spot illustrated through timeline. In next section, categories, potential revealed by comparison addition, techniques constructing systematically summarized, preparation carbonous, pyrolysis-free, noncarbon-supported, complex-type DACs. Furthermore, underlying energy- environment-related introduced detail assistance theoretical calculations. Finally, we affirm contribution particularly electrocatalysis, provide outlook direction discussing major challenges. It anticipated that Account inspire researchers propel advance

Language: Английский

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Toward Electrocatalytic Methanol Oxidation Reaction: Longstanding Debates and Emerging Catalysts

Advanced Materials, Journal Year: 2023, Volume and Issue: 35(26)

Published: Jan. 27, 2023

The study of direct methanol fuel cells (DMFCs) has lasted around 70 years, since the first investigation in early 1950s. Though enormous effort been devoted this field, it is still far from commercialization. oxidation reaction (MOR), as a semi-reaction DMFCs, bottleneck that restricts overall performance DMFCs. To date, there intense debate on complex six-electron reaction, but barely any reviews have systematically discussed topic. end, controversies and progress regarding electrocatalytic mechanisms, evaluations well design science toward MOR electrocatalysts are summarized. This review also provides comprehensive introduction recent development emerging with focus innovation alloy, core-shell structure, heterostructure, single-atom catalysts. Finally, perspectives future outlook mechanisms provided.

Language: Английский

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Asymmetric CoN₃P₁ Trifunctional Catalyst with Tailored Electronic Structures Enabling Boosted Activities and Corrosion Resistance in an Uninterrupted Seawater Splitting System

Advanced Materials, Journal Year: 2022, Volume and Issue: 34(34)

Published: July 5, 2022

Employing seawater splitting systems to generate hydrogen can be economically advantageous but still remains challenging, particularly for designing efficient and high Cl- -corrosion resistant trifunctional catalysts toward the oxygen reduction reaction (ORR), evolution (OER), (HER). Herein, single CoNC with well-defined symmetric CoN4 sites are selected as atomic platforms electronic structure tailoring. Density function theory reveals that P-doping into lead formation of asymmetric CoN3 P1 symmetry-breaking structures, enabling affinity strong oxygen-containing intermediates, moderate H adsorption, weak adsorption. Thus, ORR/OER/HER activities stability optimized simultaneously resistance. The based catalyst boosted performance endows seawater-based Zn-air batteries (S-ZABs) superior long-term over 750 h allows operate continuously 1000 h. A self-driven powered by S-ZABs gives ultrahigh H2 production rates 497 μmol h-1 . This work is first advance scientific understanding competitive adsorption mechanism between intermediates from perspective structure, paving way synthesis

Language: Английский

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Facilitating two-electron oxygen reduction with pyrrolic nitrogen sites for electrochemical hydrogen peroxide production

Nature Communications, Journal Year: 2023, Volume and Issue: 14(1)

Published: July 22, 2023

Abstract Electrocatalytic hydrogen peroxide (H 2 O ) production via the two-electron oxygen reduction reaction is a promising alternative to energy-intensive and high-pollution anthraquinone oxidation process. However, developing advanced electrocatalysts with high H yield, selectivity, durability still challenging, because of limited quantity easy passivation active sites on typical metal-containing catalysts, especially for state-of-the-art single-atom ones. To address this, we report graphene/mesoporous carbon composite high-rate high-efficiency 2e − catalysis. The coordination pyrrolic-N -modulates adsorption configuration *OOH species provide kinetically favorable pathway production. Consequently, yield approaches 30 mol g −1 h Faradaic efficiency 80% excellent durability, yielding concentration 7.2 L . This strategy manipulating reactants multiple non-metal provides design efficient durable metal-free electrocatalyst reduction.

Language: Английский

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