Atomically precise bimetallic metal ensembles with tailorable synergistic effects
Source abstract
Abstract
The large-scale synthesis of supported multinuclear catalysts with controllable metal nuclearity and constituent composition remains a formidable challenge. We report the stepwise assembly of supported atom-precise bimetallic ligand-mediated metal ensembles (LMMEs) by exploiting the underlying principles of coordination chemistry and solid-state chemistry. Lewis di-basic 2-methylimidazole is used to bridge multiple Cu2+ and M2+ (M = Co, Ni, Cu, and Zn) ions within ZSM-5 zeolites. We observe the metal constituent composition of the LMMEs by mass spectroscopy. The adjacent metal nuclei in the LMMEs offer substantial synergistic effects that enhance the catalytic performance by at least an order of magnitude in the model catalytic “click” reaction. It is envisaged that this stepwise assembly approach to develop supported multinuclear catalysts with atom precision could effectively bridge homogeneous and heterogeneous catalysis.
Source: openalex_inverted_index · Quality: baseline
Research context
OpenAlex topics: Metal-Organic Frameworks: Synthesis and Applications · Catalytic Processes in Materials Science · Asymmetric Hydrogenation and Catalysis
SciVX discovery tags are terminology-based. OpenAlex topics are source-provided classifications.
References (36)
Show source-provided references
1. Exceptional oxidation activity with size-controlled supported gold clusters of low atomicity10.1038/nchem.1721 ↗
2. Water oxidation on a mononuclear manganese heterogeneous catalyst10.1038/s41929-018-0158-6 ↗
3. Matching the kinetics of natural enzymes with a single-atom iron nanozyme10.1038/s41929-021-00609-x ↗
4. Olefin cyclopropanation via carbene transfer catalyzed by engineered cytochrome P450 enzymes10.1126/science.1231434 ↗
5. Coordination and activation of nitrous oxide by iron zeolites10.1038/s41929-021-00602-4 ↗
6. Regulating coordination number in atomically dispersed Pt species on defect-rich graphene for n-butane dehydrogenation reaction10.1038/s41467-021-22948-w ↗
7. Atomic-layered Au clusters on α-MoC as catalysts for the low-temperature water-gas shift reaction10.1126/science.aah4321 ↗
8. Shape-selective C–H activation of aromatics to biarylic compounds using molecular palladium in zeolites10.1038/s41929-020-00533-6 ↗
9. Sub-nanometre metal clusters for catalytic carbon-carbon and carbon-heteroatom cross-coupling reactions10.1039/C7DT03203J ↗
10. Multinuclear late transition metal catalysts for olefin polymerization10.1016/j.ccr.2021.213788 ↗
11. Effective binuclear Pd(II) complexes for Suzuki reactions in water10.1002/aoc.3034 ↗
12. Xia · J. Am. Chem. Soc. · 2003 · 125 · 1036210.1021/ja0355325 ↗
13. Structural transformation of highly active metal–organic framework electrocatalysts during the oxygen evolution reaction10.1038/s41560-020-00709-1 ↗
14. Low temperature oxidation of ethane to oxygenates by oxygen over iridium-cluster catalysts10.1021/jacs.9b06986 ↗
15. High turnover catalysis at bimetallic sites of the hydration of nitriles to carboxamides co-catalysed by acid. Highly specific hydration of acrylonitrile to acrylamide10.1039/c39880000112 ↗
16. Dynamic titanium phosphinoamides as unique bidentate phosphorus ligands for platinum10.1021/om0509600 ↗
17. Transition-metal-bridged bimetallic clusters with multiple uranium–metal bonds10.1038/s41557-018-0195-4 ↗
18. Configuring bonds between first-row transition metals10.1021/acs.accounts.5b00336 ↗
19. Nickel(II)-, copper(II)- and zinc(II)-complexes of some substituted imidazole ligands10.1016/S0162-0134(98)10027-2 ↗
20. Silver clusters in zeolites: from self-assembly to ground-breaking luminescent properties10.1021/acs.accounts.7b00295 ↗
21. Recent advances of precise Cu nanoclusters in microporous materials10.1002/asia.202000331 ↗
22. Fully exposed cluster catalyst (FECC): toward rich surface sites and full atom utilization efficiency10.1021/acscentsci.0c01486 ↗
23. Double rotors with fluxional axles: domino rotation and azide–alkyne huisgen cycloaddition catalysis10.1002/anie.202002739 ↗
24. Complementarity of solvent-free MALDI TOF and solid-state NMR spectroscopy in spectral analysis of polylactides10.1021/ac9020006 ↗
25. Nanoparticle MALDI-TOF mass spectrometry without fragmentation: Au 25 (SCH 2 CH 2 Ph) 18 and mixed monolayer Au 25 (SCH 2 CH 2 Ph) 18− x (L) x10.1021/ja710323t ↗
26. Synthesis, structure and gas-phase reactivity of a silver hydride complex [Ag 3 {(PPh 2 ) 2 CH 2 } 3 (μ 3 -H)(μ 3 -Cl)]BF 410.1002/anie.201302436 ↗
27. Characterization of Cu-exchanged SSZ-13: a comparative FTIR, UV-Vis, and EPR study with Cu-ZSM-5 and Cu-β with similar Si/Al and Cu/Al ratios10.1039/c3dt50732g ↗
28. Identification and quantification of copper sites in zeolites by electron paramagnetic resonance spectroscopy10.1007/s11244-016-0731-7 ↗
29. Differential adsorption of l- and d-lysine on achiral MFI zeolites as determined by synchrotron X-ray powder diffraction and thermogravimetric analysis10.1002/anie.201909352 ↗
30. The contribution of synchrotron X-ray powder diffraction to modern zeolite applications: a mini-review and prospects10.1016/j.chempr.2018.04.018 ↗
31. Elucidation of adsorbate structures and interactions on brønsted acid sites in H-ZSM-5 by synchrotron X-ray powder diffraction10.1002/anie.201600487 ↗
32. Decarboxylation of lactones over Zn/ZSM-5: elucidation of the structure of the active site and molecular interactions10.1002/anie.201704347 ↗
33. Evaluation of Brønsted and Lewis acid sites in H-ZSM-5 and H-USY with or without metal modification using probe molecule-synchrotron X-ray powder diffraction10.1016/j.apcata.2020.117528 ↗
34. Force field for molecular dynamics computations in flexible ZIF-8 framework10.1021/jp209463a ↗
35. MOF catalysis in relation to their homogeneous counterparts and conventional solid catalysts10.1039/c4sc00265b ↗
36. Direct evidence of a dinuclear copper intermediate in Cu(I)-catalyzed azide-alkyne cycloadditions10.1126/science.1229506 ↗