Interplay of electrochemical and electrical effects induces structural transformations in electrocatalysts

Li, Feng; Medvedeva, Xenia V.; Medvedev, Jury J.; Khairullina, Evgeniia M.; Engelhardt, Helen; Chandrasekar, Skandan; Guo, Yinzhou; Jin, Jian; Lee, Anna; Thérien-Aubin, Héloı̈se; Ahmed, Aftab; Pang, Yuanjie

doi:10.1038/s41929-021-00624-y

Cited by 75 publications

(124 citation statements)

References 45 publications

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“…[27] At the microscopic level, the detailed rearrangement behavior stems from atomic migration or diffusion process. [40,48] It should be mentioned that here we focus on the atomic rearrangement without considering the change in chemical state or forming of oxide.…”

Section: Fundamental Understanding Of Atomic Rearrangementmentioning

confidence: 99%

“…First, the element type would influence the migration barrier ( E mig ) [ 40,69 ] that DFT calculations demonstrate the migration energy barrier difference between Au and Pd atoms on similar models, for example, on (110) facet, about 0.7 eV for Au and 2.1 eV for Pd counterpart. The higher barrier of Pd nanocrystal inhibits the atomic detachment from catalyst surface and contributes to its better structural stability, consistent with the well‐maintained catalytic current density during 5 h of CO 2 electrolysis.…”

Section: Fundamentals For Dynamic Evolution Of Active Sites: Thermody...mentioning

confidence: 99%

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Dynamic Evolution of Active Sites in Electrocatalytic CO₂ Reduction Reaction: Fundamental Understanding and Recent Progress

Lai

Zhang

et al. 2022

Adv Funct Materials

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Advancing the development of electrocatalytic CO2 reduction reaction (CO2RR) to address the environmental issues caused by excessive consumption of fossil fuels requires rational design of remarkable electrocatalysts, where the identification of active sites and further understanding of structure–performance relationship are the bases. However, the notable dynamic evolution often appears on the catalysts, with typical examples of Cu‐based catalysts, under operating conditions, causing great difficulty in identifying the real active sites and further understanding the correlations between structure and catalytic property. In this context, understanding the dynamic evolution process of catalytically active sites during CO2RR is of particular importance, which inspires to organize the present review. Herein, the fundamental principles of dynamic evolution in CO2RR including thermodynamics and kinetics aspects, followed by the introduction of operando techniques employed to probe the evolution under operating conditions are first highlighted. The dynamic evolution behaviors, involving atomic rearrangement and change in chemical state, on typical catalysts are further discussed, with emphasis on the correlations between evolution behaviors and catalytic properties (activity, selectivity, and stability). The emerging CO2 pulsed electrolysis technique that behaves promise to manipulate the dynamic evolution and future opportunities are finally discussed.

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Section: Fundamental Understanding Of Atomic Rearrangementmentioning

confidence: 99%

Section: Fundamentals For Dynamic Evolution Of Active Sites: Thermody...mentioning

confidence: 99%

Dynamic Evolution of Active Sites in Electrocatalytic CO₂ Reduction Reaction: Fundamental Understanding and Recent Progress

Lai

Zhang

et al. 2022

Adv Funct Materials

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show abstract

“…In addition, strong binding of intermediate species produced during CO 2 RR on a catalyst surface (e.g., adsorbed CO) can weaken the metal–metal bonds at the surface and readily induce migration of surface atoms. 8 , 9 Metal electromigration has also been recently proposed as another mechanism for the phenomenon of structural reconstruction. 8 …”

Section: Structural Transformation Of Nanocatalyst During Co ...mentioning

confidence: 99%

“… 8 , 9 Metal electromigration has also been recently proposed as another mechanism for the phenomenon of structural reconstruction. 8 …”

Section: Structural Transformation Of Nanocatalyst During Co ...mentioning

confidence: 99%

The Interactive Dynamics of Nanocatalyst Structure and Microenvironment during Electrochemical CO₂ Conversion

Louisia

Yang

2022

JACS Au

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In the pursuit of a decarbonized society, electrocatalytic CO 2 conversion has drawn tremendous research interest in recent years as a promising route to recycling CO 2 into more valuable chemicals. To achieve high catalytic activity and selectivity, nanocatalysts of diverse structures and compositions have been designed. However, the dynamic structural transformation of the nanocatalysts taking place under operating conditions makes it difficult to study active site configurations present during the CO 2 reduction reaction (CO 2 RR). In addition, although recognized as consequential to the catalytic performance, the reaction microenvironment generated near the nanocatalyst surface during CO 2 RR and its impact are still an understudied research area. In this Perspective, we discuss current understandings and difficulties associated with investigating such dynamic aspects of both the surface reaction site and its surrounding reaction environment as a whole. We further highlight the interactive influence of the structural transformation and the microenvironment on the catalytic performance of nanocatalysts. We also present future research directions to control the structural evolution of nanocatalysts and tailor their reaction microenvironment to achieve an ideal catalyst for improved electrochemical CO 2 RR.

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“…Therefore, there is an urgent need to investigate catalysts for the hydrogen production. 1–5 The layered materials such as 2D transition metal dichalcogenides (TMDs), i.e. MoS 2 and WS 2 , have been widely investigated as a promising electrocatalyst for the HER.…”

Section: Introductionmentioning

confidence: 99%

Layered MAX phase electrocatalyst activity is driven by only a few hot spots

2022

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Interplay of electrochemical and electrical effects induces structural transformations in electrocatalysts

Cited by 75 publications

References 45 publications

Dynamic Evolution of Active Sites in Electrocatalytic CO₂ Reduction Reaction: Fundamental Understanding and Recent Progress

Dynamic Evolution of Active Sites in Electrocatalytic CO₂ Reduction Reaction: Fundamental Understanding and Recent Progress

The Interactive Dynamics of Nanocatalyst Structure and Microenvironment during Electrochemical CO₂ Conversion

Layered MAX phase electrocatalyst activity is driven by only a few hot spots

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Interplay of electrochemical and electrical effects induces structural transformations in electrocatalysts

Cited by 75 publications

References 45 publications

Dynamic Evolution of Active Sites in Electrocatalytic CO2 Reduction Reaction: Fundamental Understanding and Recent Progress

Dynamic Evolution of Active Sites in Electrocatalytic CO2 Reduction Reaction: Fundamental Understanding and Recent Progress

The Interactive Dynamics of Nanocatalyst Structure and Microenvironment during Electrochemical CO2 Conversion

Layered MAX phase electrocatalyst activity is driven by only a few hot spots

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Product

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Dynamic Evolution of Active Sites in Electrocatalytic CO₂ Reduction Reaction: Fundamental Understanding and Recent Progress

Dynamic Evolution of Active Sites in Electrocatalytic CO₂ Reduction Reaction: Fundamental Understanding and Recent Progress

The Interactive Dynamics of Nanocatalyst Structure and Microenvironment during Electrochemical CO₂ Conversion