<i>ACS Central Science</i> Virtual Issue on Bioinspired Catalysis

Ward, Thomas R.

doi:10.1021/acscentsci.9b01045

Cited by 8 publications

(5 citation statements)

References 35 publications

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“…2,3 More recently, inspired by nature, the metal–ligand cooperative processes observed in catalytic reactions mediated by enzymes have been mimicked based on ligand design to develop cooperative catalysts in which both, the metal and the ligand, play a part in the catalytic reaction. 4 A wide variety of systems having diverse metal–ligand bonds have proven very effective for the activation of diverse small molecules. 5 Recently, the growing interest in first-row transition metal catalysts has also motivated the design of cooperative platforms based on these metals.…”

Section: Introductionmentioning

confidence: 99%

Ambiphilic boryl groups in a neutral Ni(ii) complex: a new activation mode of H₂

et al. 2021

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Section: Introductionmentioning

confidence: 99%

Ambiphilic boryl groups in a neutral Ni(ii) complex: a new activation mode of H₂

et al. 2021

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“…An array of terms describes this area of research, often associated with specific subdisciplines of catalysis from which they are derived. Bioinspired catalyst, 42 biomimetic catalyst, 43 biohybrid, 44 artificial enzyme, 45 nanozyme, 46 designer enzyme, 47 enzyme models, 48 enzyme-inspired, 49 and bionic 50 are among the names used. In general, definitions and distinctions between these terms is not clear, though some terms are more widely accepted within subsets of the community.…”

Section: ■ Introductionmentioning

confidence: 99%

Bioinspired Catalyst Design Principles: Progress in Emulating Properties of Enzymes in Synthetic Catalysts

Ginovska,

Gutiérrez,

Karkamkar

et al. 2023

ACS Catal.

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Catalysis enables many aspects of modern life, including fuels, products, plastics, and medicines. Recent advances in catalysis have enabled us to realize higher efficiencies and new processes. Ideally, we seek to achieve high rates of selective conversions using catalysts derived from abundantly available elements and operating under mild conditions, specifically lower reaction temperatures and pressures. Such catalysts could enable decentralized, on-demand synthesis of chemicals and energy carriers. Nature has demonstrated the feasibility of this approach with enzymes, which showcase catalytic processes at low temperatures and pressures with nonprecious metals. Current thinking holds that in addition to the active site, the complexity of the enzyme structure, specifically the protein scaffold, is also critical to achieving this performance. Recreating this environment has been a long-standing scientific goal. However, we still understand the functions of enzymes better than we understand the de novo design of catalysts that mimic enzymes features, while also retaining their activity and selectivity under more demanding conditions. In this Perspective, we will critically examine four key areas of catalyst design that incorporate the chemical and structural properties of enzymes into synthetic catalysts: (i) the use of confinement to enhance catalytic activity, (ii) tailoring the environment around the active site, (iii) proton transport, and (iv) bifunctionality and cooperativity.

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“…Although the interactions of metal ions with various biological molecules, including peptides, have been well studied, the focus of these examinations is primarily under the purview of metallodrugs and metal toxicity [ 1 , 2 , 3 , 4 , 5 ]. However, modified biocompatible or biologically relevant frameworks are also applied to the mimic natural catalyst’s design [ 6 ].…”

Section: Introductionmentioning

confidence: 99%

“…Bioinspired applications make use of modified biocompatible or biologically relevant frameworks to imitate the natural catalyst design [ 6 ]. Weakly coordinating chelates may be incorporated into the design of metal complexes to function as an “on-off” switch during catalysis.…”

Section: Introductionmentioning

confidence: 99%

Synthesis, Characterization, and Reaction Studies of Pd(II) Tripeptide Complexes

et al. 2021

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The aqueous synthesis of Pd(II) complexes with alkylated tripeptides led to the hydrolysis of the peptides at low pH values and mixtures of complexed peptides were formed. A non-aqueous synthetic route allowed the formation and isolation of single products and their characterization. Pd(II) complexes with α-Asp(OR)AlaGly(OR), β-Asp(OR)AlaGly(OR), and TrpAlaGly(OR) (R = H or alkyl) as tri and tetradentate chelates were characterized. The tridentate coordination mode was accompanied by a fourth monodentate ligand that was shown to participate in both ligand exchange reactions and a direct removal to form the tetradentate coordination mode. The tetradentate coordination revealed a rare a hemi labile carbonyl goup coordination mode to Pd(II). Reactivity with small molecules such as ethylene, acids, formate, and episulfide was investigated. Under acidic conditions and in the presence of ethylene; acetaldehyde was formed. The Pd(II) is a soft Lewis acid and thiophilic and the complexes abstract sulfur from episulfide at apparent modest catalytic rates. The complexes adopt a square planar geometry according to a spectroscopic analysis and DFT calculations that were employed to evaluate the most energetically favorable coordination geometry and compared with the observed infrared and NMR data.

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ACS Central Science Virtual Issue on Bioinspired Catalysis

Cited by 8 publications

References 35 publications

Ambiphilic boryl groups in a neutral Ni(ii) complex: a new activation mode of H₂

Ambiphilic boryl groups in a neutral Ni(ii) complex: a new activation mode of H₂

Bioinspired Catalyst Design Principles: Progress in Emulating Properties of Enzymes in Synthetic Catalysts

Synthesis, Characterization, and Reaction Studies of Pd(II) Tripeptide Complexes

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ACS Central Science Virtual Issue on Bioinspired Catalysis

Cited by 8 publications

References 35 publications

Ambiphilic boryl groups in a neutral Ni(ii) complex: a new activation mode of H2

Ambiphilic boryl groups in a neutral Ni(ii) complex: a new activation mode of H2

Bioinspired Catalyst Design Principles: Progress in Emulating Properties of Enzymes in Synthetic Catalysts

Synthesis, Characterization, and Reaction Studies of Pd(II) Tripeptide Complexes

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Product

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Ambiphilic boryl groups in a neutral Ni(ii) complex: a new activation mode of H₂

Ambiphilic boryl groups in a neutral Ni(ii) complex: a new activation mode of H₂