Simultaneous introduction of various palladium active sites into MOF via one-pot synthesis: Pd@[Cu3−xPdx(BTC)2]n

Zhang, Wenhua; Chen, Zhihao; Naji, Mohamed; Guo, Ping; Cwik, Stefan; Halbherr, Olesia; Wang, Yuemin; Wilde, Nicole; Gläser, Roger; Fischer, Roland A.

doi:10.1039/c6dt02893d

Cited by 31 publications

(21 citation statements)

References 58 publications

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“…By using this approach, the properties of a known and promising framework structure can be extended and altered without changing the framework topology. For the HKUST‐1 structure, some mixed‐metal structures with the metal combinations Cu/Ru, Cu/Zn, Cu/Ni, Cu/Pd, Cu/Ag, Cu/Mn, Cu/Fe and Cu/Co have already been reported. The first four have been synthesized via direct syntheses, while the latter ones used post‐synthetic metal exchange.…”

Section: Introductionmentioning

confidence: 88%

“…Moreover, even completely new structures containing two types of metals might be obtained as undesired side products. Furthermore, a metal–organic framework structure with metal nanoparticles within the pores, as reported by Zhang et al., is generally possible as well. Hence, a careful characterization of the synthesized materials is of high importance.…”

Section: Introductionmentioning

confidence: 99%

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Experimental Evidence for the Incorporation of Two Metals at Equivalent Lattice Positions in Mixed‐Metal Metal–Organic Frameworks

Bitzer

Otterbach

Thangavel

et al. 2020

Chemistry A European J

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Metal-organic frameworksc ontaining multiple metals distributed over crystallographically equivalent framework positions (mixed-metal MOFs) represent an interesting class of materials, since the closev icinity of isolated metal centerso ften gives rise to synergistic effects. However,a ppropriate characterization techniques for detailed investigations of these mixed-metal metal-organicf ramework materials, particularlya ddressing the distribution of metalsw ithin the lattice,a re rarely available.T he synthesis of mixed-metal FeCuBTC materials in direct syntheses provedt ob ed ifficult and only at horough characterizationu sing varioust echniques,l ike powder X-ray diffraction, X-ray absorption spectroscopy and electron paramagnetic resonance spectroscopy,u nambiguously evidencedt he formationof am ixed-metalF eCuBTC materialw ith HKUST-1s tructure, which containedb imetallic FeÀCu paddlewheels as wella sm onometallic CuÀCu andF e ÀFe units under optimizeds ynthesis conditions. The in-depthc haracterization showedt hat other synthetic procedures led to impurities, whichc ontained the majority of the applied iron and were impossible or difficult to identify using solely standard characterization techniques. Therefore, this studys hows the necessity to characterize mixed-metal MOFs extensively to unambiguously prove the incorporationo fb oth metals at the desiredp ositions. The controlled positioning of metal centers in mixed-metal metal-organicf ramework materials and the thorough characterization thereof is particularly important to derive structure-property or structure-activity correlations.Supporting information and the ORCID identification number(s) for the author(s) of this article can be found under: https://doi.org/10.Figure 1. Schematic framework structure (a) andthe characteristic paddlewheel unit (b) of amixed-metal FeCuBTCmaterial with HKUST-1 structure.Figure 5. Best fit calculations and experimentally obtained EXAFS spectra(a+ b), Fourier-transformed EXAFS spectra (c + d) and Fourier back-transformed spectra (e + f) of FeCuBTC at the Cu K-edge (a,c,e) and the Fe K-edge (b,d,f).

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Section: Introductionmentioning

confidence: 88%

Section: Introductionmentioning

confidence: 99%

Experimental Evidence for the Incorporation of Two Metals at Equivalent Lattice Positions in Mixed‐Metal Metal–Organic Frameworks

Bitzer

Otterbach

Thangavel

et al. 2020

Chemistry A European J

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“…The Pd@[Cu 3−x Pd x (btc) 2 ] n MOFs featuring both incorporated Pd 2+ nodes and loaded Pd 0 NPs show substantially enhanced catalytic activity toward the aqueous-phase hydrogenation of p-nitrophenol with NaBH 4 to p-aminophenol, as contrasted with the pristine Cu-MOFs (HKUST-1). Furthermore, it was evident that the Pd 2+ species play a key role in this reaction and are predominantly responsible for the observed high catalytic activity [127].…”

Section: Mixed-metal Demofs: Metal Node Engineeringmentioning

confidence: 98%

“…Recently, the mixed metal Pd@[Cu 3−x Pdx(btc) 2 ] n with various levels of doping with Pd were obtained via one-pot synthesis [127]. The XPS results provided evidence for the simultaneous introduction of Pd 2+ -doped framework nodes and Pd 0 NPs embedded into MOFs.…”

Section: Mixed-metal Demofs: Metal Node Engineeringmentioning

confidence: 99%

Chemical Reactions at Isolated Single-Sites Inside Metal–Organic Frameworks

Wang

Wöll

2018

Catal Lett

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Isolated, coordinatively unsaturated metal sites within metal-organic framework (MOF) materials feature interesting chemical properties and offer applications as single-site catalysts. Here, we report on the recent progress in providing fundamental insight into chemical reactions occurring inside MOFs. In addition to the common form, powders, we discuss the potential of MOF thin films (SURMOFs). The combined spectroscopic and modeling approach applied to selected systems demonstrated that the catalytic activity of MOFs can be precisely tuned. A particular interesting case is the so-called defect-engineering, where structural imperfections are created in a controlled fashion. The chemical properties of MOF materials can be further modified by integration and decoration of linkers or loading with guest species, such as metal or metal-oxide nanoparticles or nanoclusters. A particularly interesting aspect of layer-by-layer approaches for the fabrication of MOF thin films is the prospect to realize tandem catalysts. Graphical AbstractKeywords Metal-organic frameworks · Thin films · Single-site catalysts · Infrared spectroscopy · Defects · Active sites

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“…Recently, the paddlewheel SBU of HKUST-1 was modified with catalytically active sites, such as Pd, and the activity improved [344]. The observed catalytic activity was further improved when Pd NP are loaded into the Pd substituted MOF.…”

Section: Catalysismentioning

confidence: 99%

Metal–organic frameworks in Germany: From synthesis to function

Evans

Garai

Reinsch

et al. 2019

Coordination Chemistry Reviews

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104

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Metal-organic frameworks (MOFs) are constructed from a combination of inorganic and organic units to produce materials which display high porosity, among other unique and exciting properties. MOFs have shown promise in many wide ranging applications, such as catalysis and gas separations. In this review, we highlight MOF research conducted by Germany-based research groups. Specifically, we feature approaches for the synthesis of new MOFs, high-throughput MOF production, advanced characterization methods and examples of advanced functions and properties.

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Simultaneous introduction of various palladium active sites into MOF via one-pot synthesis: Pd@[Cu_3−xPd_x(BTC)₂]_n

Cited by 31 publications

References 58 publications

Experimental Evidence for the Incorporation of Two Metals at Equivalent Lattice Positions in Mixed‐Metal Metal–Organic Frameworks

Experimental Evidence for the Incorporation of Two Metals at Equivalent Lattice Positions in Mixed‐Metal Metal–Organic Frameworks

Chemical Reactions at Isolated Single-Sites Inside Metal–Organic Frameworks

Metal–organic frameworks in Germany: From synthesis to function

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