Transferring enzyme features to molecular CO2 reduction catalysts DOI Creative Commons

Matthías Huber,

Corinna R. Hess

Current Opinion in Chemical Biology, Journal Year: 2024, Volume and Issue: 83, P. 102540 - 102540

Published: Nov. 15, 2024

Language: Английский

Molecular Co-Catalyst Confined within a Metallacage for Enhanced Photocatalytic CO2 Reduction DOI
Dongdong Liu,

Huirong Ma,

Chao Zhu

et al.

Journal of the American Chemical Society, Journal Year: 2024, Volume and Issue: 146(3), P. 2275 - 2285

Published: Jan. 12, 2024

The construction of structurally well-defined supramolecular hosts to accommodate catalytically active species within a cavity is promising way address catalyst deactivation. resulting catalysts can significantly improve the utilization catalytic sites, thereby achieving highly efficient chemical conversion. In this study, Co-metalated phthalocyanine (

Language: Английский

Citations

45
Ligand-Bound CO2 as a Nonclassical Route toward Efficient Photocatalytic CO2 Reduction with a Ni N-Confused Porphyrin DOI

Huihong Yuan,

Akash Krishna,

Zhihe Wei

et al.

Journal of the American Chemical Society, Journal Year: 2024, Volume and Issue: 146(15), P. 10550 - 10558

Published: April 8, 2024

Implementing the synergistic effects between metal and ligand has successfully streamlined energetics for CO2 activation gained high catalytic activities, establishing important breakthroughs in photocatalytic reduction. Herein, we describe a Ni(II) N-confused porphyrin complex (NiNCP) featuring an acidic N–H group. It is readily deprotonated exists anion form during catalysis. Owing to this functional site, NiNCP gave rise outstanding turnover number (TON) as 217,000 with 98% selectivity reduction CO, while parent (NiTPP) was found be nearly inactive. Our mechanistic analysis revealed nonclassical reaction pattern where effectively activated via attack of Lewis-basic ligand. The resulting ligand-bound adduct could further reduced produce CO. This new metal–ligand effect anticipated inspire design highly active catalysts small molecule activations.

Language: Английский

Citations

23
Heterobimetallic NiFe Complex for Photocatalytic CO2 Reduction: United Efforts of NiFe Dual Sites DOI
Yao Xiao,

Hongtao Zhang,

Ming‐Tian Zhang

et al.

Journal of the American Chemical Society, Journal Year: 2024, Volume and Issue: 146(42), P. 28832 - 28844

Published: Oct. 8, 2024

Catalytic CO

Language: Английский

Citations

6
STRUCTURES, ELECTRONIC, AND MAGNETIC PROPERTIES OF TRANSITION METAL-INSERTED H2DBP CLUSTERS DOI
Zhi Li, Shu-qi Yang,

Jia-Hui Yin

et al.

Surface Review and Letters, Journal Year: 2024, Volume and Issue: 31(11)

Published: Jan. 27, 2024

The configurations, electronic, and magnetic properties of the H 2 DBP-M clusters have been investigated via density functional theory. results reveal that TM atoms for ([Formula: see text], Y, Zr, Nb, Lu, Hf) deviate from center planes clusters. Lu) display largest dipole magnitudes. Based on binding energy per atom HOMO-LUMO gap, DBP-Ni DBP-Lu are most favorable synthesis. charge transfer amounts Zn, Cd, Hf, Hg) larger. TM-d orbitals text]Co Cu) contribute significantly to Fermi levels. spin densities reduce 0 except text]) DBP-V

Language: Английский

Citations

5
Why alkali metals and alkaline earth metals are not loaded the metal–organic frameworks DOI
Zhen Zhao, Shu-qi Yang,

Jia-hui Yin

et al.

Research on Chemical Intermediates, Journal Year: 2024, Volume and Issue: 50(5), P. 2383 - 2394

Published: March 19, 2024

Language: Английский

Citations

5
Redox-active ligand promoted multielectron reactivity at earth-abundant transition metal complexes DOI Creative Commons
Minzhu Zou, Kate M. Waldie

Inorganic Chemistry Frontiers, Journal Year: 2024, Volume and Issue: 11(18), P. 5795 - 5809

Published: Jan. 1, 2024

This review highlights the application of redox-active ligands for achieving substrate activation and reactivity through multielectron transfer at earth-abundant transition metal complexes.

Language: Английский

Citations

5
Pendant Catechol Group Improves the Performance of Iron Porphyrin CO2 Reduction Catalysts DOI
Ana Sonea, Jeffrey J. Warren

ACS Catalysis, Journal Year: 2025, Volume and Issue: 15(3), P. 1444 - 1454

Published: Jan. 9, 2025

In this work, we prepared chloroiron 5-(2,3-dihydroxyphenyl)-10,15,20-triphenyl porphyrin (Fe(Cat)TPP) and investigated its properties for CO2 reduction. Iron porphyrins make up a class of compounds that are known to efficiently convert carbon monoxide (CO). There exist many different derivatives reduce with some leading examples, including structures place hydrogen bond donors and/or proton near the iron ion active site. Here, presence an internal H-bond in 2,3-dihydroxyphenyl group Fe(Cat)TPP increases observed reduction rate constants by factor 10 respect parent chloroiron-5,10,15,20-tetraphenyl 3 only one hydroxyphenyl (i.e., 5-(2-hydroxyphenyl)-10,15,20-triphenyl porphyrin). The is proposed facilitate proton-coupled electron transfer process carbon–oxygen breaking, which has been established as rate-limiting step CO2-to-CO conversion. molecule, those like it, important improving designs molecular electrocatalysts. ongoing development platforms can rapidly selectively mediate electrochemical transformation dioxide (CO2) valorized products great technical challenge.

Language: Английский

Citations

0
Enhancing photocatalytic CO2-to-CO conversion by iron complexes through 8-hydroxyquinoline ligand regulation DOI
Zhichao Xu, Xin Huang, Liyan Zhang

et al.

Journal of Molecular Structure, Journal Year: 2025, Volume and Issue: unknown, P. 142039 - 142039

Published: March 1, 2025

Language: Английский

Citations

0
Carbon nanotube heterogenization improves cobalt pyridyldiimine complex CO2 reduction activity in aqueous carbonate buffer DOI

Baptiste Andrin,

Paulo Jorge Marques Cordeiro,

David Provost

et al.

Chemical Communications, Journal Year: 2024, Volume and Issue: 60(38), P. 5022 - 5025

Published: Jan. 1, 2024

We present two cobalt pyridyldiimine complexes functionalized with pyrene for selective CO 2 electroreduction in water upon immobilization on multi-walled carbon nanotubes.

Language: Английский

Citations

3
Three Oxidation States of Cobalt(I/II/III) Complexes by Thiaporphyrin DOI
Fang Wang,

Zi-Bin Zhong,

Rixin Jia

et al.

Inorganic Chemistry, Journal Year: 2024, Volume and Issue: 63(16), P. 7233 - 7240

Published: April 8, 2024

Reaction of tetraphenyl-21-thiaporphyrin (HSTPP) with cobalt salt yields a pentacoordinated high-spin 3/2 [CoIICl(STTP)] (1). Through ion exchange, roughly square-planar-geometry low-spin 1/2 CoIISTTP(BArF24) (2) complex was isolated. These two paramagnetic precursors were examined by single X-ray diffraction, nuclear magnetic resonance, electron superconducting quantum interference device, and density functional theory calculations. allowed the development one reduction oxidation to give [CoI(STTP)] (3), [CoIII(STTP)Cl(CH3CN)](BF4) (4), [CoIII(STTP)Cl2] (5). The products chemical redox reactions isolated fully characterized. In addition, reactivity (1) azide (N3), cyanate (OCN), thiocyanate (SCN) featured preferential N-coordination metal.

Language: Английский

Citations

1