A facile complexing agent-assistant single atom Ag-N3S1 site photodeposition strategy

Li, Mingyang; Liu, Xuxiao; Fu, Diqin; Xie, Zhixun; Zou, Xingfu; Liu, Wuran; Yu, Yueyang; Wang, Jihui; Wang, Hanqing; Tong, Chaobo; Cheng, Zhiming; Wu, Songmei; Ding, Kejian; Yu, Yu

doi:10.1016/j.apcatb.2022.121896

Cited by 13 publications

(8 citation statements)

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“…Moreover, iced photocatalytic reduction reaction enables Cu 2p 3/2 peak to move to a bit lower bonding energy, indicating the reduction of Cu ions into SA state with lower valence electron by photo‐excited electrons from terephthalic acid (ATA) linkers. [ 17 ] Fourier‐transformed (FT) extended X‐ray absorption fine structure (EXAFS) curves are shown in Figure 2b. Cu SA@UiO‐66‐NH 2 sample demonstrates only one notable peak at ≈1.50 Å, which should be assigned to Cu−N contribution.…”

Section: Resultsmentioning

confidence: 99%

Ligand‐Assistant Iced Photocatalytic Reduction to Synthesize Atomically Dispersed Cu Implanted Metal‐Organic Frameworks for Photo‐Enhanced Uranium Extraction from Seawater

Liu

Wei

et al. 2023

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and natural seawater. [5] Recently, porous framework materials (e.g., metal-organic framework (MOF), [6] covalent organic framework (COF), [7] hydrogen-bonded organic framework (HOF) [8] ) have been developed for uranium uptake by combination of ligand complexation and photocatalytic reduction. Most photocatalysts still suffer from inefficient ligand-tometal charge transfer (LMCT), [9] which severely restrict the photocatalytic activity. Recently, single-atom (SA) catalysts have attracted considerable research interest in heterogeneous catalysis over the recent years. [10] Some studies have reported a continuous decrease in catalytic activity with increasing particle size. [11] Hence, it is of great significance to rationally design and control the synthesis of monodispersed metal at the atomic level. Inspired by the iced-photochemical synthesis, [12] we developed ligand-assistant frozen photoreduction approach to anchor atomically dispersed Cu on aminofunctionalized Zr-MOF (Cu SA@UiO-66-NH 2 ). High angle annular dark-field scanning transmission electron microscopy (HAADF-STEM) and X-ray absorption fine structure (XAFS) spectroscopy measurements confirm the atomically dispersed Cu in the form of N-Cu-N. By contrast, there are Cu nanoclusters decorated on UiO-66-NH 2 support (Cu Clu@UiO-66-NH 2 ) by the routine photochemical solution-phase reaction. Compared to the agglomerated active sites, isolated dispersed Cu sites contribute to higher photocatalytic activity, which endow Cu SA@UiO-66-NH 2 adsorbent with enhanced photoreduction-assistant uranium extraction performance from natural seawater together with superior antibacterial ability. Results and Discussion Synthesis and Structure CharacterizationUiO-66-NH 2 crystals were synthesized by the traditional solvothermal method [13] and then employed as the catalyst support. The Cu SA@UiO-66-NH 2 sample was prepared through ligandassistant iced photocatalytic reduction route, as illustrated in Uranium extraction from natural seawater is one of the most promising routes to address the shortage of uranium resources. By combination of ligand complexation and photocatalytic reduction, porous framework-based photocatalysts have been widely applied to uranium enrichment. However, their practical applicability is limited by poor photocatalytic activity and low adsorption capacity. Herein, atomically dispersed Cu implanted UiO-66-NH 2 (Cu SA@UiO-66-NH 2 ) photocatalysts are prepared via ligand-assistant iced photocatalytic reduction route. N-Cu-N moiety acts as an effective electron acceptor to potentially facilitate charge transfer kinetics. By contrast, there exist Cu sub-nanometer clusters by the typical liquid phase photoreduction, resulting in a relatively low photocatalytic activity. Cu SA@UiO-66-NH 2 adsorbents exhibit superior antibacterial ability and improved photoreduction conversion of the adsorbed U(VI) to insoluble U(IV), leading to a high uranium sorption capacity of 9.16 mg-U/g-Ads from natural seawater. This study provides new insight for enhancing uranium...

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Section: Resultsmentioning

confidence: 99%

Ligand‐Assistant Iced Photocatalytic Reduction to Synthesize Atomically Dispersed Cu Implanted Metal‐Organic Frameworks for Photo‐Enhanced Uranium Extraction from Seawater

Liu

Wei

et al. 2023

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“…37 The valence change of Ag is not in the same potential window as that of SnO 2 (−1.0 to 0.3 V vs REH), which could not impact the CV curve of Ag/SnO 2 . For H* adsorption/desorption over Ag, previous reports show that the ΔG H* of Ag is about 0.4−0.5 eV, 25,38 suggesting that H* is difficult to be adsorbed on Ag. Therefore, there are no obvious H* adsorption/desorption peaks in the CV curves over Ag.…”

Section: ■ Results and Discussionmentioning

confidence: 99%

Promoting Electrocatalytic Hydrogenation of 5-Hydroxymethylfurfural over a Cooperative Ag/SnO₂ Catalyst in a Wide Potential Window

Guo,

Fu,

Yang

et al. 2023

ACS Catal.

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Electrochemical reduction of biomass-derived 5hydroxymethylfurfural (HMF) to produce 2,5-dihydroxymethylfuran (DHMF) is a promising approach for biomass upgrading. The achievement of high activity and Faradaic efficiency (FE) in a wide potential window is critical for mature applications considering the significantly varied voltages supplied by different renewable energies. However, it is still challenging due to multiple reaction pathways and the competitive hydrogen evolution reaction. Herein, we synthesized a cooperative catalyst by supporting Ag nanoparticles (AgNPs) on SnO 2 nanosheet arrays, which realizes the electrochemical HMF reduction to DHMF with a high FE (>95%) in a wide potential window (from −0.62 to −1.12 V vs reversible hydrogen electrode). Electrochemical and in situ measurements reveal that the AgNPs promote water splitting to generate reactive hydrogen (H*) species, which effectively react with HMF via a Langmuir−Hinshelwood mechanism. Moreover, the AgNPs accelerate the formation of oxygen vacancies on SnO 2 under reaction conditions, which act as electrophilic sites to realize the selective adsorption and hydrogenation of the carbonyl bond (C�O) in HMF to yield DHMF. Finally, we designed a coupling system to simultaneously realize the electrochemical reduction and oxidation of HMF to produce DHMF and 2,5-furandicarboxylic acid, showing lower potential at the same current density than that of traditional cathodic HMF reduction coupling anodic oxygen evolution reaction, in an economical manner.

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“…66,88,89 It is noteworthy that careful selection of the sacrificial agents is crucial in the photochemical preparation of atomically dispersed catalysts, as they can often accelerate the deposition rate of metal ions and may lead to agglomeration. 63 Besides, added reagents generally serve multiple purposes in one system, which makes it difficult to understand the photochemical reaction.…”

Section: Process Control In Photochemical Synthesismentioning

confidence: 99%

A review on the photochemical synthesis of atomically dispersed catalysts

Chen,

Liu

2024

Mater. Chem. Front.

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A facile complexing agent-assistant single atom Ag-N3S1 site photodeposition strategy

Cited by 13 publications

References 52 publications

Ligand‐Assistant Iced Photocatalytic Reduction to Synthesize Atomically Dispersed Cu Implanted Metal‐Organic Frameworks for Photo‐Enhanced Uranium Extraction from Seawater

Ligand‐Assistant Iced Photocatalytic Reduction to Synthesize Atomically Dispersed Cu Implanted Metal‐Organic Frameworks for Photo‐Enhanced Uranium Extraction from Seawater

Promoting Electrocatalytic Hydrogenation of 5-Hydroxymethylfurfural over a Cooperative Ag/SnO₂ Catalyst in a Wide Potential Window

A review on the photochemical synthesis of atomically dispersed catalysts

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A facile complexing agent-assistant single atom Ag-N3S1 site photodeposition strategy

Cited by 13 publications

References 52 publications

Ligand‐Assistant Iced Photocatalytic Reduction to Synthesize Atomically Dispersed Cu Implanted Metal‐Organic Frameworks for Photo‐Enhanced Uranium Extraction from Seawater

Ligand‐Assistant Iced Photocatalytic Reduction to Synthesize Atomically Dispersed Cu Implanted Metal‐Organic Frameworks for Photo‐Enhanced Uranium Extraction from Seawater

Promoting Electrocatalytic Hydrogenation of 5-Hydroxymethylfurfural over a Cooperative Ag/SnO2 Catalyst in a Wide Potential Window

A review on the photochemical synthesis of atomically dispersed catalysts

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Promoting Electrocatalytic Hydrogenation of 5-Hydroxymethylfurfural over a Cooperative Ag/SnO₂ Catalyst in a Wide Potential Window