Template-Assisted, Seed-Mediated Synthesis of Hierarchically Mesoporous Core–Shell UiO-66: Enhancing Adsorption Capacity and Catalytic Activity through Iterative Growth

Zhang, Furui; Hu, Xiaobing; Roth, Eric W.; Kim, Yonghwi; Nguyen, SonBinh T.

doi:10.1021/acs.chemmater.0c01065

Cited by 19 publications

(8 citation statements)

References 83 publications

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“…First, to initiate capping agent dissociation, we tried to increase the concentration of linkers. This need could be satisfied by the use of tetrafluoroterephthalic acid (BDC-F 4 ) as the MOF linker to synthesize UiO-66, which is chosen for its high solubility in aqueous solution. , Second, cetyltrimethylammonium chloride (CTAC) was used as capping agents to substitute CTAB due to its weaker binding strength with metal surface than that of CTAB . The kinetic capping agent exchange was conducted by exposing Au-CTAB NPs to an aqueous solution with a high concentration of CTAC.…”

Section: Results and Discussionmentioning

confidence: 99%

Creating an Aligned Interface between Nanoparticles and MOFs by Concurrent Replacement of Capping Agents

Yang

Zhang

et al. 2021

J. Am. Chem. Soc.

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Applying metal–organic frameworks (MOFs) on the surface of other materials to form multifunctional materials has recently attracted great attention; however, directing the MOF overgrowth is challenging due to the orders of magnitude differences in structural dimensions. In this work, we developed a universal strategy to mediate MOF growth on the surface of metal nanoparticles (NPs), by taking advantage of the dynamic nature of weakly adsorbed capping agents. During this colloidal process, the capping agents gradually dissociate from the metal surface, replaced in situ by the MOF. The MOF grows to generate a well-defined NP-MOF interface without a trapped capping agent, resulting in a uniform core–shell structure of one NP encapsulated in one single-crystalline MOF nanocrystal with specific facet alignment. The concept was demonstrated by coating ZIF-8 and UiO-66-type MOFs on shaped metal NPs capped by cetyltrimethylammonium surfactants, and the formation of the well-defined NP-MOF interface was monitored by spectroscopies. The defined interface outperforms ill-defined ones generated via conventional methods, displaying a high selectivity to unsaturated alcohols for the hydrogenation of an α,β-unsaturated aldehyde. This strategy opens a new route to create aligned interfaces between materials with vastly different structural dimensions.

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Section: Results and Discussionmentioning

confidence: 99%

Creating an Aligned Interface between Nanoparticles and MOFs by Concurrent Replacement of Capping Agents

Yang

Zhang

et al. 2021

J. Am. Chem. Soc.

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“…Thermogravimetric analysis of as-synthesized composites are displayed in Figure c,d. All UiO/GO-based adsorbents can be divided into three weight-loss stages: First, the removal of water at 100 °C and the weight loss at 100–280 °C is attributed to the removal of GO and polyimide-coated on UiO. , When the temperature is higher than 550 °C, the weight of the material does not change after reaching the platformthis is attributed to the complete decomposition of the UiO skeleton. , Evidently, the stability of PI-UiO/GOs composite is obviously improved before 280 °C, after doping GO and wrapping the PI polymer on the surface. In addition, the PI- and GO-modified adsorbents have superior thermal stability to endure the normal flue gas temperature for CO 2 separation.…”

Section: Results and Discussionmentioning

confidence: 99%

A Novel Strategy to Enhance the Performance of CO₂ Adsorption Separation: Grafting Hyper-cross-linked Polyimide onto Composites of UiO-66-NH₂ and GO

Ning

Yang

Yin

et al. 2021

ACS Appl. Mater. Interfaces

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Graphene oxide (GO) is widely used to improve the pore structure, dispersion capacity, adsorption selectivity, resistance to acids and bases, and thermal stability of metal–organic frameworks (MOFs). However, it remains a daunting challenge to enhance selectivity simply by modifying the pore surface polarity and producing a suitable pore structure for CO2 molecules through a combination of GO with MOFs. Herein, we demonstrate a novel porous hyper-cross-linked polyimide–UiO–graphene composite adsorbent for CO2 capture via in situ chemical knitting and condensation reactions. Specifically, a network of polyimides rich in carbonyl and nitrogen atoms with amino terminations was synthesized via the reaction of 4,4′-oxydiphthalic anhydride (ODPA) and 2,4,6-trimethyl-1,3-phenylenediamine (DAM). The product plays a crucial role in the separation of CO2 from N2. As expected, the resulting composite (PI-UiO/GO-1) exhibited a 3-fold higher CO2 capacity (8.24 vs 2.8 mmol·g–1 at 298 K and 30 bar), 4.2 times higher CO2/N2 selectivity (64.71 vs 15.43), and significantly improved acid–base resistance stability compared with those values of pristine UiO-66-NH2. Furthermore, breakthrough experiments verified that the porous composites can effectively separate CO2 from simulated fuel gas (CO2/N2 = 15/85 vol %) with great potential in industrial applications. More importantly, this strategy can be extended to prepare other MOF-based composites. This clearly advances the development of MOF–polymer materials for gas capture.

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“…Thanks to the open mesochannels and designable topology, full advantages of hierarchical mesoporous Zr-based metal–organic frameworks (mesoMOFs) could be taken for constructing such a heterogeneous system. − Their rigid and stable mesochannels could work as exoskeletons to immobilize and protect natural SOX. − Meanwhile, the phosphorescent carboxylated metalloporphyrin of TCPP-Pt could serve as colinker to be well incorporated into the surrounding microporous walls as oxygen-sensitive signal units (Scheme ). Metallic nodes in MOFs could effectively isolate TCPP-Pt, thus avoiding the aggregation-induced quenching effect .…”

Section: Introductionmentioning

confidence: 99%

Specific Screening of Prostate Cancer Individuals Using an Enzyme-Assisted Substrate Sensing Platform Based on Hierarchical MOFs with Tunable Mesopore Size

et al. 2021

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Rapid and specific identification of tumor metabolic markers is of great significance. Herein, a convenient, reliable and specific strategy was proposed to screen prostate cancer (PCa) individuals through indirectly quantifying sarcosine, an early indicator of PCa, in the clinical urine samples. The success roots in the rational design of a cascade response model, which takes integrated sarcosine oxidase (SOX) as a specific recognition unit and oxygen-sensitive molecule as a signal reporter. The newly developed hierarchical mesoporous Zr-based metal–organic frameworks with continuously tunable mesopore size ensure the synergetic work of the SOX and response unit spatially separated in their neighboring mesoporous and microporous domains, respectively. The large mesopore up to 12.1 nm not only greatly enhances the loading capacity of SOX but also spares enough space for the free diffusion of sarcosine. On this basis, the probe is competent to specifically check out the tiny concentration change of sarcosine in the urine sample between PCa patients and healthy humans. Such a concept of enzyme-assisted substrate sensing could be simply extended by altering the type of immobilized enzymes, hopefully setting a guideline for the rational design of multiple probes to quantify specific biomarkers in complex biological samples.

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Template-Assisted, Seed-Mediated Synthesis of Hierarchically Mesoporous Core–Shell UiO-66: Enhancing Adsorption Capacity and Catalytic Activity through Iterative Growth

Cited by 19 publications

References 83 publications

Creating an Aligned Interface between Nanoparticles and MOFs by Concurrent Replacement of Capping Agents

Creating an Aligned Interface between Nanoparticles and MOFs by Concurrent Replacement of Capping Agents

A Novel Strategy to Enhance the Performance of CO₂ Adsorption Separation: Grafting Hyper-cross-linked Polyimide onto Composites of UiO-66-NH₂ and GO

Specific Screening of Prostate Cancer Individuals Using an Enzyme-Assisted Substrate Sensing Platform Based on Hierarchical MOFs with Tunable Mesopore Size

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Template-Assisted, Seed-Mediated Synthesis of Hierarchically Mesoporous Core–Shell UiO-66: Enhancing Adsorption Capacity and Catalytic Activity through Iterative Growth

Cited by 19 publications

References 83 publications

Creating an Aligned Interface between Nanoparticles and MOFs by Concurrent Replacement of Capping Agents

Creating an Aligned Interface between Nanoparticles and MOFs by Concurrent Replacement of Capping Agents

A Novel Strategy to Enhance the Performance of CO2 Adsorption Separation: Grafting Hyper-cross-linked Polyimide onto Composites of UiO-66-NH2 and GO

Specific Screening of Prostate Cancer Individuals Using an Enzyme-Assisted Substrate Sensing Platform Based on Hierarchical MOFs with Tunable Mesopore Size

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A Novel Strategy to Enhance the Performance of CO₂ Adsorption Separation: Grafting Hyper-cross-linked Polyimide onto Composites of UiO-66-NH₂ and GO