Atomic-level design of biomimetic iron-sulfur clusters for biocatalysis

X Zhang, S Zhou, D Liu, K Fan, H Liu - Nanoscale, 2024 - pubs.rsc.org
Designing biomimetic materials with high activity and customized biological functions by
mimicking the central structure of biomolecules has become an important avenue for the …

An Artificial [Fe4S4]-Containing Metalloenzyme for the Reduction of CO2 to Hydrocarbons

V Waser, M Mukherjee, R Tachibana… - Journal of the …, 2023 - ACS Publications
Iron–sulfur clusters have been reported to catalyze various redox transformations, including
the multielectron reduction of CO2 to hydrocarbons. Herein, we report the design and …

Inorganic Fe-O and Fe-S oxidoreductases: paradigms for prebiotic chemistry and the evolution of enzymatic activity in biology

XL Huang, JR Harmer, G Schenk, G Southam - Frontiers in Chemistry, 2024 - frontiersin.org
Oxidoreductases play crucial roles in electron transfer during biological redox reactions.
These reactions are not exclusive to protein-based biocatalysts; nano-size (< 100 nm), fine …

Three-coordinate nickel and metal–metal interactions in a heterometallic iron–sulfur cluster

DWN Wilson, MS Fataftah, Z Mathe… - Journal of the …, 2024 - ACS Publications
Biological multielectron reactions often are performed by metalloenzymes with
heterometallic sites, such as anaerobic carbon monoxide dehydrogenase (CODH), which …

An iron–sulfur cluster with a highly pyramidalized three-coordinate iron center and a negligible affinity for dinitrogen

AC Brown, DLM Suess - Journal of the American Chemical …, 2023 - ACS Publications
Attempts to generate open coordination sites for N2 binding at synthetic Fe–S clusters often
instead result in cluster oligomerization. Recently, it was shown for Mo–Fe–S clusters that …

Highly Activated Terminal Carbon Monoxide Ligand in an Iron–Sulfur Cluster Model of FeMco with Intermediate Local Spin State at Fe

LNV Le, JP Joyce, PH Oyala, S DeBeer… - Journal of the …, 2024 - ACS Publications
Nitrogenases, the enzymes that convert N2 to NH3, also catalyze the reductive coupling of
CO to yield hydrocarbons. CO-coordinated species of nitrogenase clusters have been …

Opportunities for insight into the mechanism of efficient CO2/CO interconversion at a nickel-iron cluster in CO dehydrogenase

SH Newman-Stonebraker, TJ Gerard, PL Holland - Chem, 2024 - cell.com
The reduction of CO 2 with low overpotential and high selectivity is a crucial challenge in
catalysis. Fortunately, natural systems have evolved enzymes that achieve this catalytic …

Understanding the Electronic Structure Basis for N2 Binding to FeMoco: A Systematic Quantum Mechanics/Molecular Mechanics Investigation

Y Pang, R Bjornsson - Inorganic Chemistry, 2023 - ACS Publications
The FeMo cofactor (FeMoco) of Mo nitrogenase is responsible for reducing dinitrogen to
ammonia, but it requires the addition of 3–4 e–/H+ pairs before N2 even binds. A binding …

Terminal Hydride Complex of High-Spin Mn

A Drena, A Fraker, NB Thompson… - Journal of the …, 2024 - ACS Publications
The iron–molybdenum cofactor of nitrogenase (FeMoco) catalyzes fixation of N2 via Fe
hydride intermediates. Our understanding of these species has relied heavily on the …

Exploiting molecular symmetry to quantitatively map the excited-state landscape of iron–sulfur clusters

BA Skeel, DLM Suess - Journal of the American Chemical Society, 2023 - ACS Publications
Cuboidal [Fe4S4] clusters are ubiquitous cofactors in biological redox chemistry. In the
[Fe4S4] 1+ state, pairwise spin coupling gives rise to six arrangements of the Fe valences …