Superiority of Dual‐Atom Catalysts in Electrocatalysis: One Step Further Than Single‐Atom Catalysts

Advanced Energy Materials, Journal Year: 2022, Volume and Issue: 12(9)

Published: Jan. 18, 2022

Abstract In recent years, dual‐atom catalysts (DACs) have attracted extensive attention, as an extension of single‐atom (SACs). Compared with SACs, DACs higher metal loading and more complex flexible active sites, thus achieving better catalytic performance providing opportunities for electrocatalysis. This review introduces the research progress in years on how to design new enhance Firstly, advantages increasing are introduced. Then, role changing adsorption condition reactant molecules atoms is discussed. Moreover, ways which can reduce reaction energy barrier key steps change path explored. Catalytic applications different electrocatalytic reactions, including carbon dioxide reduction reaction, oxygen evolution hydrogen nitrogen followed. Finally, a brief summary made challenges prospects

Language: Английский

---

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

---

Fe/Cu diatomic catalysts for electrochemical nitrate reduction to ammonia

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

Published: June 19, 2023

Electrochemical conversion of nitrate to ammonia offers an efficient approach reducing pollutants and a potential technology for low-temperature low-pressure synthesis. However, the process is limited by multiple competing reactions NO3- adsorption on cathode surfaces. Here, we report Fe/Cu diatomic catalyst holey nitrogen-doped graphene which exhibits high catalytic activities selectivity production. The enables maximum Faradaic efficiency 92.51% (-0.3 V(RHE)) NH3 yield rate 1.08 mmol h-1 mg-1 (at - 0.5 V(RHE)). Computational theoretical analysis reveals that relatively strong interaction between promotes discharge anions. Nitrogen-oxygen bonds are also shown be weakened due existence hetero-atomic dual sites lowers overall reaction barriers. dual-site hetero-atom strategy in this work provides flexible design further development expands electrocatalytic techniques reduction

Language: Английский

---

Metal-metal interactions in correlated single-atom catalysts

Science Advances, Journal Year: 2022, Volume and Issue: 8(17)

Published: April 29, 2022

Single-atom catalysts (SACs) include a promising family of electrocatalysts with unique geometric structures. Beyond conventional ones fully isolated metal sites, an emerging class the adjacent single atoms exhibiting intersite metal-metal interactions appear in recent years and can be denoted as correlated SACs (C-SACs). This type provides more opportunities to achieve substantial structural modification performance enhancement toward wider range electrocatalytic applications. On basis clear identification interactions, this review critically examines research progress C-SACs. It shows that control enables regulation atomic structure, local coordination, electronic properties atoms, which facilitate modulation behavior Last, we outline directions for future work design development C-SACs, is indispensable creating high-performing new SAC architectures.

Language: Английский

---

Isolated Fe-Co heteronuclear diatomic sites as efficient bifunctional catalysts for high-performance lithium-sulfur batteries

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

Published: Jan. 18, 2023

The slow redox kinetics of polysulfides and the difficulties in decomposition Li2S during charge discharge processes are two serious obstacles to practical application lithium-sulfur batteries. Herein, we construct Fe-Co diatomic catalytic materials supported by hollow carbon spheres achieve high-efficiency catalysis for conversion simultaneously. Fe atom center is beneficial accelerate reaction process, Co favorable charging process. Theoretical calculations combined with experiments reveal that this excellent bifunctional activity originates from synergy between atom. As a result, assembled cells exhibit high rate performance (the specific capacity achieves 688 mAh g-1 at 5 C) cycle stability decay 0.018% 1000 cycles 1 C).

Language: Английский

---

A review of Ni based powder catalyst for urea oxidation in assisting water splitting reaction

Advanced Powder Materials, Journal Year: 2022, Volume and Issue: 1(3), P. 100030 - 100030

Published: Jan. 10, 2022

Water splitting has been regarded as a sustainable and environmentally-friendly technique to realize green hydrogen generation, while more energy is consumed due the high overpotentials required for anode oxygen evolution reaction. Urea electrooxidation, an ideal substitute, thus received increasing attention in assisting water-splitting reactions. Note that highly efficient catalysts are still drive urea oxidation, facile generation of valence state species significant reaction based on electrochemical-chemical mechanisms. The cost rareness make noble metal impossible further consideration large-scale application. Ni-based very promising their cheap price, structure tuning, good compatibility, easy active phase formation. In light advances made recently, herein, we reviewed recent powder oxidation fundamental firstly presented clarify mechanism urea-assisted water splitting, then prevailing evaluation indicators briefly expressed electrochemical measurements. catalyst design principle including synergistic effect, electronic defect construction surface reconstruction well main fabrication approaches various assisted summarized discussed. problems challenges also concluded fabrication, performance evaluation, Considering key influencing factors catalytic process application, should be given structure−property relationship deciphering, novel development real device; specifically, effort directed with multi-functions simultaneously promote steps anti-corrosion ability by revealing local integration practical We believe current summarization will instructive helpful understanding action via technique.

Language: Английский

---

Long‐Range Interactions in Diatomic Catalysts Boosting Electrocatalysis

Angewandte Chemie International Edition, Journal Year: 2022, Volume and Issue: 61(52)

Published: Oct. 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.

Language: Английский

---

Precisely Constructing Orbital Coupling-Modulated Dual-Atom Fe Pair Sites for Synergistic CO₂ Electroreduction

ACS Energy Letters, Journal Year: 2022, Volume and Issue: 7(2), P. 640 - 649

Published: Jan. 14, 2022

Electrochemical reduction of CO2 (CO2RR) provides an attractive pathway to achieve a carbon-neutral energy cycle. Single-atom catalysts (SAC) have shown unique potential in heterogeneous catalysis, but their structural simplicity prevents them from breaking linear scaling relationships. In this study, we develop feasible strategy precisely construct series electrocatalysts featuring well-defined single-atom and dual-site iron anchored on nitrogen-doped carbon matrix (Fe1–N–C Fe2–N–C). The Fe2–N–C dual-atom electrocatalyst (DAC) achieves enhanced CO Faradaic efficiency above 80% wider applied ranges along with higher turnover frequency (26,637 h–1) better durability compared SAC counterparts. Furthermore, based in-depth experimental theoretical analysis, the orbital coupling between dual sites decreases gap antibonding bonding states *CO adsorption. This research presents new insights into structure–performance relationship CO2RR at atomic scale extends application DACs for electrocatalysis beyond.

Language: Английский

---

Atomically Dispersed Ni/Cu Dual Sites for Boosting the CO₂ Reduction Reaction

ACS Catalysis, Journal Year: 2021, Volume and Issue: 11(20), P. 12673 - 12681

Published: Oct. 1, 2021

Developing diatomic catalysts (DACs) for the CO2 reduction reaction (CO2RR) has emerged as a promising leading-edge research area owing to their maximum atomic utility and more sophisticated functionalities. However, proper design of DACs at an level understanding synergistic mechanism binary sites remain challenging. Herein, N-rich carbon matrix with precisely controlled Ni/Cu dual is synthesized through assistance metal–organic frameworks. The as-prepared catalyst presents high CO Faradaic efficiency over 95% from −0.39 −1.09 V vs reversible hydrogen electrode (RHE) value 99.2% −0.79 RHE long-term durability 60 h electrolysis. Density functional theory studies reveal that electronic redistribution band gap narrowing induced by adjacent NiN4 CuN4 moieties enhance electron conductivity strengthen bonding interactions between *COOH intermediates Ni centers, thus lowering overall barriers promoting generation.

Language: Английский

---

Strain Engineering in Electrocatalysts: Fundamentals, Progress, and Perspectives

Advanced Energy Materials, Journal Year: 2021, Volume and Issue: 12(5)

Published: Dec. 22, 2021

Abstract Strain engineering of nanomaterials, namely, designing, tuning, or controlling surface strains nanomaterials is an effective strategy to achieve outstanding performance in different for their various applications. This article summarizes recent progress and achievements the development strain‐rich electrocatalysts (SREs) applications field electrochemical energy conversion technologies. It starts from definition lattice strains, followed by classification where mechanisms strain formation reported methods regulate related are elaborated. The SRE characterization techniques overviewed, focusing deeply on clarification strain‐property relationship these SREs. Their electrocatalytic reactions further highlighted, including hydrogen evolution reaction, oxygen reduction alcohol oxidation carbon dioxide nitrogen reaction. Related reaction SREs interpreted after taking catalytic performance, as well between properties into account. challenges future opportunities finally outlined discussed together with potential fields.

Language: Английский

---