Keggin-type SiW12 encapsulated in MIL-101(Cr) as efficient heterogeneous photocatalysts for nitrogen fixation reaction

Su, Senda; Li, Xiaoman; Zhang, Xu; Zhu, Jingting; Liu, Guodong; Tan, Mengyao; Wang, Yingying; Luo, Min

doi:10.1016/j.jcis.2022.04.006

Cited by 53 publications

(35 citation statements)

References 46 publications

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“…The SiW 12 diffraction peaks in the PXRD pattern of SiW 12 @NU-1000 are not visible as POM moieties occupy the pores of NU-1000 and are not present on the surface of MOF. These results are in agreement with the related literature data. − The characterization by PXRD can also be affected by the crystallinity decline of SiW 12 when incorporated into SiW 12 @NU-1000. However, the diffraction peaks of both components were observed in the PXRD pattern of the physical mixture of SiW 12 and NU-1000 (Figure S1, SI).…”

Section: Resultssupporting

confidence: 92%

Postsynthetic Modification of NU-1000 for Designing a Polyoxometalate-Containing Nanocomposite with Enhanced Third-Order Nonlinear Optical Performance

et al. 2022

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For the advancement of laser technologies and optical engineering, various types of new inorganic and organic materials are emerging. Metal−organic frameworks (MOFs) reveal a promising use in nonlinear optics, given the presence of organic linkers, metal cluster nodes, and possible delocalization of π-electron systems. These properties can be further enhanced by the inclusion of solely inorganic materials such as polyoxometalates as prospective low-cost electron-acceptor species. In this study, a novel hybrid nanocomposite, namely, SiW 12 @NU-1000 composed of SiW 12 (H 4 SiW 12 O 40 ) and Zrbased MOF (NU-1000), was assembled, completely characterized, and thoroughly investigated in terms of its nonlinear optical (NLO) performance. The third-order NLO behavior of the developed system was assessed by Z-scan measurements using a 532 nm laser. The effect of two-photon absorption and self-focusing was significant in both NU-1000 and SiW 12 @NU-1000. Experimental studies suggested a much superior NLO performance of SiW 12 @NU-1000 if compared to that of NU-1000, which can be assigned to the charge-energy transfer between SiW 12 and NU-1000. Negligible light scattering, good stability, and facile postsynthetic fabrication method can promote the applicability of the SiW 12 @NU-1000 nanocomposite for various optoelectronic purposes. This research may thus open new horizons to improve and enhance the NLO performance of MOF-based materials through π-electron delocalization and compositing metal−organic networks with inorganic molecules as electron acceptors, paving the way for the generation of novel types of hybrid materials for prospective NLO applications.

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Section: Resultssupporting

confidence: 92%

Postsynthetic Modification of NU-1000 for Designing a Polyoxometalate-Containing Nanocomposite with Enhanced Third-Order Nonlinear Optical Performance

et al. 2022

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“…These results indicated the construction of the expected MIL-88B. The comparison of the FT-IR pattern of MIL-88B and TSA/MIL-88B shows the presence of H 4 SiW 12 O 40 structures in the latter, especially by characteristic peaks of WO, Si–O, W–O b –W, and W–O c –W at 973, 926, 883, and 804 cm –1 , respectively. , Furthermore, the absorption peak of WO shows a slight red-shift from 983 to 973 cm –1 after the loading due to the generation of hydrogen bonds between the carrier and silicotungstic acid . It is inferred that perhaps heteropolyacid is anchored on the MIL-88B successfully.…”

Section: Resultsmentioning

confidence: 78%

“…As shown in Figure d, the binding energy of the W–O in the catalyst has been shifted from 531.58 to 530.92 eV and electron cloud density around oxygen atoms increases. In addition, another peak located at 532.01 eV is attributed to the carboxyl group of the ligand in MIL-88B . Therefore, the synthesized catalyst is formed by hydrogen bonds between MOF and silicotungstic acid, which efficiently prevents the leaching of TSA from the iron–organic framework supporter, improving the reusability of the catalyst.…”

Section: Resultsmentioning

confidence: 99%

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Iron–Organic Framework Nanoparticle-Supported Tungstosilicic Acid as a Catalyst for the Biginelli Reaction

Zhang

Liu

et al. 2022

ACS Appl. Nano Mater.

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In this work, a metal−organic framework with an octahedral morphology supported by a tungstosilicic acid (TSA) nanocatalyst has been successfully synthesized through a postsynthetic modification approach and referred to as TSA/MIL-88B. The as-prepared catalyst was efficiently obtained from Biginelli reactions among benzaldehyde, urea, and 1,3-dicarbonyl compound. Depending on the synergistic effect of exposed metal iron sites and the supported Brønsted acid sites, the hybrid materials exhibited high catalytic activity. Additionally, the environmentally friendly nanocatalyst could be recycled seven times with a little reduction in the catalytic performance. This study also provides a way for the application of such porous organic polymer functionalization in organic synthesis.

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“…To overcome this issue, some strategies have been developed to reinforce its stability during NRR, including adhesive ( Tianyu Wang et al, 2020 ), coupling with MOFs ( Tianyu Wang et al, 2021 ), and interfacial interaction ( Yuan Feng et al, 2022 ). For example, Su et al (2022 ) fabricated SiW 12 encapsulated Cr-MOFs (MIL-101(Cr)) hybrids, which were applied to N 2 photocatalysis affording an NH 3 yield rate of 75.56 μmol h −1 g −1 , about 10 times that of Na 4 SiW 12 O 40 . SiW 12 of polyoxometalates was supposed to be the active center, which could be regulated to locate in different cavities of MIL-101(Cr) by controlling the synthesis method.…”

Section: Tungsten-based and Related Photocatalysts For Nrrmentioning

confidence: 99%

Recent progress of photocatalysts based on tungsten and related metals for nitrogen reduction to ammonia

et al. 2022

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Photocatalytic nitrogen reduction reaction (NRR) to ammonia holds a great promise for substituting the traditional energy-intensive Haber–Bosch process, which entails sunlight as an inexhaustible resource and water as a hydrogen source under mild conditions. Remarkable progress has been achieved regarding the activation and solar conversion of N2 to NH3 with the rapid development of emerging photocatalysts, but it still suffers from low efficiency. A comprehensive review on photocatalysts covering tungsten and related metals as well as their broad ranges of alloys and compounds is lacking. This article aims to summarize recent advances in this regard, focusing on the strategies to enhance the photocatalytic performance of tungsten and related metal semiconductors for the NRR. The fundamentals of solar-to-NH3 photocatalysis, reaction pathways, and NH3 quantification methods are presented, and the concomitant challenges are also revealed. Finally, we cast insights into the future development of sustainable NH3 production, and highlight some potential directions for further research in this vibrant field.

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Keggin-type SiW12 encapsulated in MIL-101(Cr) as efficient heterogeneous photocatalysts for nitrogen fixation reaction

Cited by 53 publications

References 46 publications

Postsynthetic Modification of NU-1000 for Designing a Polyoxometalate-Containing Nanocomposite with Enhanced Third-Order Nonlinear Optical Performance

Postsynthetic Modification of NU-1000 for Designing a Polyoxometalate-Containing Nanocomposite with Enhanced Third-Order Nonlinear Optical Performance

Iron–Organic Framework Nanoparticle-Supported Tungstosilicic Acid as a Catalyst for the Biginelli Reaction

Recent progress of photocatalysts based on tungsten and related metals for nitrogen reduction to ammonia

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