Ultrathin Metal–Organic Framework Nanosheets with Ultrahigh Loading of Single Pt Atoms for Efficient Visible‐Light‐Driven Photocatalytic H<sub>2</sub> Evolution

Zuo, Quan; Liu, Tingting; Chen, Chuanshuang; Ji, Yi; Gong, X. G.; Mai, Yiyong; Zhou, Yongfeng

doi:10.1002/anie.201904058

Cited by 471 publications

(336 citation statements)

References 59 publications

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“…Extended X-Ray absorption fine structure (EXAFS) and X-ray absorption near edge structure (XANES) are promising techniques to determine the coordination of the metal clusters of MOFs and their tuneable interaction with incorporated molecules. Quan Zuo et al 11 . investigated the Pt-N coordination through XPS, XANES and EXAFS and reported the ultrahigh loading of Pt in ultrathin nanosheets of Cu based MOF for efficient photocatalytic performance.…”

Section: Introductionmentioning

confidence: 99%

Investigation of Ionic Liquid interaction with ZnBDC-Metal Organic Framework through Scanning EXAFS and Inelastic Neutron Scattering

Dutta

Rao

Kumar

2019

Sci Rep

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Zn based Metal-Organic Framework (MOF), Zinc 1,4-benzenedicarboxylate (ZnBDC) has been synthesized and incorporated with ionic liquid (IL) 1-butyl-3 methylimidazolium bromide (BMIMBr) at optimum 50 wt% of IL. Interaction of BMIMBr in the micropores of ZnBDC-MOF is investigated by XPS, scanning EXAFS and inelastic neutron spectroscopy. Significant increase in binding energies of Zn spin-orbit peaks upon IL incorporation is observed from XPS spectra indicating motion of Br− anions of the IL BMIMBr towards the unsaturated Zn cluster of ZnBDC-MOF. The k-space periodicity as well as the local coordination geometry of Zn K-edge is investigated from the scanning EXAFS and XANES spectra. Asymmetric oscillation periodicity has been observed from the k-space scanning XANES spectra upon IL incorporation. Difference in peak positions of oxygen and zinc are observed from the R-space scanning EXAFS spectra suggesting change in coordination geometry due to dehydration of Zn2+ ion in the ZnBDC-MOF upon IL incorporation. Incorporation of IL in the pores of ZnBDC-MOF gives rise to increased scattering intensity in the Inelastic Neutron Scattering (INS) spectra, which is attributed to the displacement of IL ions in the MOF pores.

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Section: Introductionmentioning

confidence: 99%

Investigation of Ionic Liquid interaction with ZnBDC-Metal Organic Framework through Scanning EXAFS and Inelastic Neutron Scattering

Dutta

Rao

Kumar

2019

Sci Rep

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“…[19,20] For H 2 evolution, the binding energy of H* on photocatalysts can be tuned to favor the subsequent reaction. [21,22] However, the current photocatalysts are still faced with severe challenges such as fast charge-carrier recombination, leading to poor performance. [23,24] Therefore, it is essential to develop efficient and durable photocatalysts for driving water splitting into hydrogen.…”

Section: Introductionmentioning

confidence: 99%

Recent Progress in Single‐Atom Catalysts for Photocatalytic Water Splitting

Zhang

Guan

2020

Solar RRL

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Photocatalytic water splitting can realize a direct conversion from solar energy into green hydrogen energy, which is conducive to effectively mitigate energy crisis and environmental issues. Single‐atom catalysts (SACs) have shown great potential in photocatalytic hydrogen evolution, with unique geometric and electronic structures that help to boost mass and charge transfer during photocatalytic processes. Herein, recent advances of SACs in photocatalytic water splitting are focused upon. To decrease aggregation and realize sufficient utilization of metal atoms, different synthesis strategies for SACs are documented. For photocatalytic hydrogen evolution, the catalytic performances, active sites, and structure–property relationships of SACs including Al, Co, Ni, Pd, Ag, and Pt single sites are highlighted. The existing challenges and future directions of SACs in photocatalytic water splitting are provided.

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“…The facile alkali-etched strategy for creating defects in MOF has been reported, which is used to fabricate D-Ni-MOF in our work. [23][24][25] The corresponding morphology and structure variation from Ni-MOF to D-Ni-MOF was firstly investigated. As shown in Figure 2a and Figures S1a and S2a (Supporting Information) scanning electron microscope (SEM) images illustrate the smooth and cross linked Ni-MOF nanosheets were orderly grown on the conductor substrate with the average diameter and thickness of ≈1 µm and ≈10 nm, respectively.…”

Section: Resultsmentioning

confidence: 99%

Alkali‐Etched Ni(II)‐Based Metal–Organic Framework Nanosheet Arrays for Electrocatalytic Overall Water Splitting

Zhou

Dou

et al. 2020

Small

118

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However, only limited MOFs were explored for electrocatalytic water splitting, mainly due to the poor structure stability of most MOFs in water system, especially under acidic/alkaline conditions. [11-13] Most importantly, metal nodes in most MOFs are coordinately saturated with ligand/ solvent molecules, [14,15] which are inert in electrocatalysis, even if these metal sites are highly exposed by rich pores. [16] For instance, Zhang and co-workers reported a new metal azolate framework [Co 2 (µ-Cl) 2 (bbta)], [12] but showing poor OER activity. The metal sites became active only on the functionalization by hydroxide ligands, and then exhibited efficient electrocatalysis performance. In addition, the low electrical conductivity for most MOFs also affects the electrocatalytic activity. [17] The principal reason is that the larger inner impedance of most organic ligands and rigid pore structures are not conducive to long-range charge transport. [18,19] Despite few of efforts including synthesis of ultrathin 2D layers or introduction of conductive materials in channels for exposing more active sites or improving their conductivity, the electrocatalytic activity enhancement is still not prominent. [20,21] Thus, it is desired to rationally design or optimize the structure and composition of MOFs to improve water spitting activity. Herein, we propose that the construction of defects into MOFs could be a feasible strategy to create highly active sites and improve conductivity for optimizing electrocatalytic properties. As a proof of concept, a Ni(II)-based MOF [Ni 2 (OH) 2 (BDC); BDC = 1,4-benzenedicarboxylate] with intrinsic 2D metal-oxide layers connected by BDC ligands [22] was selected and its defectrich nanosheet array (as D-Ni-MOF NSA) was prepared via a simply alkali-etched strategy (Figure 1). The intrusion of KOH leads to partial breaking of NiO bonds in the MOF, accompanied with the generation of open unsaturated Ni sites and the introduction of extra-framework K cations. Subsequently, the unsaturated Ni sites were attacked by the OH − ions, leading to the exposed active site NiO(OH), while the original framework topology is still well maintained. Theoretical/experimental results reveal that the above features could endow the D-Ni-MOF with richer active sites and largely improved conductivity, compared with pristine Ni-MOF. Finally, the assembled D-Ni-MOF||D-Ni-MOF electrolyte cell could achieve comparable electrocatalytic performance with that of the noble metal-based benchmark catalysts, demonstrating a promising bifunctional electrocatalyst for overall water splitting. The exploration of efficient electrocatalysts is the central issue for boosting the overall efficiency of water splitting. Herein, pertinently creating active sites and improving conductivity for metal-organic frameworks (MOFs) is proposed to tailor electrocatalytic properties for overall water splitting. An Ni(II)-MOF nanosheet array is presented as an ideal material model and a facile alkali-etched strategy is developed to break its NiO b...

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Ultrathin Metal–Organic Framework Nanosheets with Ultrahigh Loading of Single Pt Atoms for Efficient Visible‐Light‐Driven Photocatalytic H₂ Evolution

Cited by 471 publications

References 59 publications

Investigation of Ionic Liquid interaction with ZnBDC-Metal Organic Framework through Scanning EXAFS and Inelastic Neutron Scattering

Investigation of Ionic Liquid interaction with ZnBDC-Metal Organic Framework through Scanning EXAFS and Inelastic Neutron Scattering

Recent Progress in Single‐Atom Catalysts for Photocatalytic Water Splitting

Alkali‐Etched Ni(II)‐Based Metal–Organic Framework Nanosheet Arrays for Electrocatalytic Overall Water Splitting

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Ultrathin Metal–Organic Framework Nanosheets with Ultrahigh Loading of Single Pt Atoms for Efficient Visible‐Light‐Driven Photocatalytic H2 Evolution

Cited by 471 publications

References 59 publications

Investigation of Ionic Liquid interaction with ZnBDC-Metal Organic Framework through Scanning EXAFS and Inelastic Neutron Scattering

Investigation of Ionic Liquid interaction with ZnBDC-Metal Organic Framework through Scanning EXAFS and Inelastic Neutron Scattering

Recent Progress in Single‐Atom Catalysts for Photocatalytic Water Splitting

Alkali‐Etched Ni(II)‐Based Metal–Organic Framework Nanosheet Arrays for Electrocatalytic Overall Water Splitting

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Product

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Ultrathin Metal–Organic Framework Nanosheets with Ultrahigh Loading of Single Pt Atoms for Efficient Visible‐Light‐Driven Photocatalytic H₂ Evolution