Metal–Organic Frameworks for Electrocatalysis: Catalyst or Precatalyst?

Zheng, Weiran; Lee, Yoon Suk

doi:10.1021/acsenergylett.1c01350

Cited by 208 publications

(156 citation statements)

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“…Indeed, the study of MOFs as NRR electrocatalysts is still in the early stage, and most of them show unsatisfactory performance. − Meanwhile, recent studies showed that some MOFs are precatalysts and new species as active sites are formed from MOFs during the electrocatalytic process. The periodically distributed metal ions in MOFs transformed into active catalysts which inherited the merits of MOFs such as high dispersity of metal ions and high surface areas. , Besides, the in situ growth of MOFs on conductive substrates to form a self-supporting electrode without using a polymeric binder can facilitate the charge transport of the electrode and avoid the peeling off of MOFs during electrocatalysis; the porous and conductive substrates such as copper mesh are also favorable for enhanced mass transport. − Recent studies showed that Ce-based compounds, such as CeO 2 with abundant oxygen vacancies, are promising NRR electrocatalysts. − Moreover, the pristine Ce-MOF has been found to be active for the photodriven NRR . The Ce coordination unsaturated sites (Ce-CUS) on the Ce-MOF surface can provide unoccupied and occupied 4f orbitals for N 2 adsorption and activation. , However, the NH 3 yield is not satisfactory because of the low utilization efficiency for solar energy.…”

Section: Introductionmentioning

confidence: 99%

Structural Reconstruction of Ce-MOF with Active Sites for Efficient Electrocatalytic N₂ Reduction

Liu

Peng

et al. 2021

ACS Appl. Energy Mater.

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The electrochemical synthesis of ammonia from N 2 under mild conditions is a promising alternative to the energy-consuming Haber−Bosch process. Metal−organic frameworks (MOFs) are promising electrocatalysts for the N 2 reduction reaction, but most of them are active for the undesirable and competitive hydrogen evolution reaction. Herein, we developed a facile strategy to grow a Ce-MOF on copper mesh substrate. The Ce-MOF with a self-supporting structure could be directly used as an electrode for the N 2 reduction reaction, demonstrating highly efficient electrocatalytic performance with an NH 3 yield of 14.83 μg h −1 cm −2 and a Faradaic efficiency of 10.81% at −0.2 V versus a reversible hydrogen electrode. Structural characterizations of Ce-MOF after electrocatalysis revealed that Ce-MOF as precatalyst underwent structural reconstruction at negative potential, forming catalytically active CeO 2 with oxygen vacancies embedded in the amorphous Ce-MOF. In addition, the self-supporting structure formed by in situ growth of Ce-MOF on porous and conductive cooper mesh endowed the electrocatalyst with enhanced stability, conductivity, and mass transport. This work demonstrated the structural transformation of Ce-MOF during the electrocatalytic process and provided new insight for the rational design of MOF-based electrocatalysts.

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Section: Introductionmentioning

confidence: 99%

Structural Reconstruction of Ce-MOF with Active Sites for Efficient Electrocatalytic N₂ Reduction

Liu

Peng

et al. 2021

ACS Appl. Energy Mater.

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“…5f), where the percentage of O-Fe increases obviously, together with the emergence of new peaks which can be assigned to O-H, further demonstrating that the electrocatalyst should be converted into FeOOH on the surfaces during the OER. 62,63 As a consequence, an increase in the positive charge of Fe species makes it easier to capture highly polarized OH À and H 2 O, and the formed FeOOH can be used as a promoter to facilitate the cleavage of H-O* bonds for enhancing OER catalytic performance in alkaline solution. 58 To further elucidate the role of S in improving electrocatalytic performance, operando Raman spectroscopy was employed.…”

Section: Resultsmentioning

confidence: 99%

A self-supported S-doped Fe-based organic framework platform enhances electrocatalysis toward highly efficient oxygen evolution in alkaline media

Lin

Leng

et al. 2022

J. Mater. Chem. A

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“…While structural instability of MOFs has been recognized during the reaction process, [ 96 ] numerous fundamental questions regarding the detailed process of local coordination evolution remain unanswered. It has been observed that ultrathin NiCo bimetallic MOF nanosheets show outstanding OER activity, [ 36 ] but the details about structure evolution of MOFs was not revealed.…”

Section: In Situ X‐ray Related Techniquesmentioning

confidence: 99%

In Situ Investigation on Life‐Time Dynamic Structure–Performance Correlation Toward Electrocatalyst Service Behavior in Water Splitting

Xie

Sun

Tao

et al. 2022

Adv Funct Materials

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Electrocatalytic water splitting is recognized as quite a promising protocol for the renewable hydrogen energy production, and significant effort has been devoted to the design of high‐performance electrocatalysts that can efficiently alleviate the critical issue of fossil fuel scarcity. However, the vast majority of traditional design strategies restrictedly focus on the pristine electrocatalyst structure and ultimate performance results, which may lead to the incorrect or even opposite understanding of catalytic structure–performance correlations. With the burgeoning development of in situ techniques, the dynamic service behaviors of electrocatalysts during water splitting have been growingly investigated from enriched perspectives, only by which can the life‐time dynamic structure–performance correlations be established. Herein, to shed new light on the next‐stage development of in situ investigations for water splitting electrocatalysts, a series of dynamic service behavior that existed in water splitting process and highlight their key role for understanding the life‐time dynamic structure–performance correlations is comprehensively summarized. Besides, a wide variety of in situ techniques are systematically dissected in terms of their functional features, advantages, and limitations. Critical challenges and prospects are also discussed for establishing the life‐time dynamic structure–performance correlations of water splitting electrocatalysts.

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Metal–Organic Frameworks for Electrocatalysis: Catalyst or Precatalyst?

Cited by 208 publications

References 50 publications

Structural Reconstruction of Ce-MOF with Active Sites for Efficient Electrocatalytic N₂ Reduction

Structural Reconstruction of Ce-MOF with Active Sites for Efficient Electrocatalytic N₂ Reduction

A self-supported S-doped Fe-based organic framework platform enhances electrocatalysis toward highly efficient oxygen evolution in alkaline media

In Situ Investigation on Life‐Time Dynamic Structure–Performance Correlation Toward Electrocatalyst Service Behavior in Water Splitting

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Metal–Organic Frameworks for Electrocatalysis: Catalyst or Precatalyst?

Cited by 208 publications

References 50 publications

Structural Reconstruction of Ce-MOF with Active Sites for Efficient Electrocatalytic N2 Reduction

Structural Reconstruction of Ce-MOF with Active Sites for Efficient Electrocatalytic N2 Reduction

A self-supported S-doped Fe-based organic framework platform enhances electrocatalysis toward highly efficient oxygen evolution in alkaline media

In Situ Investigation on Life‐Time Dynamic Structure–Performance Correlation Toward Electrocatalyst Service Behavior in Water Splitting

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Structural Reconstruction of Ce-MOF with Active Sites for Efficient Electrocatalytic N₂ Reduction

Structural Reconstruction of Ce-MOF with Active Sites for Efficient Electrocatalytic N₂ Reduction