Dual-Responsive Material Based on Catechol Modified Self-Immolative Poly(Disulfide) Backbones

Asger Holm Agergaard, Andreas Sommerfeldt, Steen Uttrup Pedersen, Henrik Birkedal, Kim Daasbjerg https://doi.org/10.1002/anie.202108698 Functional materials engineered to degrade upon triggering are in high demand due their potentially lower impact on the environment as well as their use in sensing and in medical applications. Here, stimuli‑responsive polymers are prepared by decorating a self-immolative poly(dithiothreitol) backbone with pendant catechol units. The…

Mechanistic Elucidation of Dimer Formation and Strategies for Its Suppression in Electrochemical Reduction of Fac-Mn(bpy)(CO)3Br

Dr. Magnus H. Rønne, Monica R. Madsen, Prof. Dr. Troels Skrydstrup, Assoc. Prof. Dr. Steen U. Pedersen,Prof. Dr. Kim Daasbjerg https://doi.org/10.1002/celc.202100279 Development of new catalytic approaches for reduction of small molecules is an aspiring technology to alleviate increasing energy demands without use of fossil fuels. One of the most promising molecular catalysts for reduction of CO2 is fac-Mn(bpy)(CO)3Br (bpy=2,2’-bipyridine). In this work, the mechanism…

Highly Scalable Conversion of Blood Protoporphyrin to Efficient Electrocatalyst for CO2-to-CO Conversion

Matteo Miola, Simin Li, Xin-Ming Hu, Marcel Ceccato, Annette-E. Surkus, Edmund Welter, Steen U. Pedersen, Henrik Junge, Troels Skrydstrup, Matthias Beller, Kim Daasbjerg https://doi.org/10.1002/admi.202100067 Electrochemical CO2 reduction to valuable chemicals represents a green and sustainable approach to close the anthropogenic carbon cycle, but has been impeded by low efficiency and high cost of electrocatalysts. Here, a cost-effective hybrid catalyst consisting of hemin (chloroprotoporphyrin IX iron(III)), a…

A novel approach toward attachment of graphene oxide on copper using electrochemical grafting of an organic interlayer with enhanced corrosion performance

Adel-Mehraban, F., Raeissi, K., Karimzadeh, F., Pedersen, S. U., Salehzadeh, H. & Daasbjerg, K. https://doi.org/10.1016/j.porgcoat.2021.106185 This paper proposes a novel approach for attaching a graphene oxide (GO) film to a Cu substrate using diazonium chemistry. For this purpose, Cu was covalently modified using electrochemical grafting of p-phenylenebis(diazonium) salt (p-PBDS) followed by immersion in a basic GO suspension.…

Are Amines the Holy Grail for Facilitating CO2 Reduction?

Jakobsen, J. B., Rønne, M. H., Daasbjerg, K. & Skrydstrup, T. https://doi.org/10.1002/anie.202014255 The selective and efficient reduction of carbon dioxide represents a key solution to producing non-fossil-fuel-based feedstocks for the chemical industry, while alleviating the increasing atmospheric concentration of this greenhouse gas. A variety of catalytic methods for the CO2 reduction reaction (CO2RR) have been developed, including…

Homogeneous Electrochemical Reduction of CO2. From Homogeneous to Supported Systems

Costentin, C., Daasbjerg, K. & Robert, M. The development of supported molecular catalysts deposited at conductive electrodes has recently (re)opened a wide range of new possibilities to investigate CO2 reduction with the catalytic selectivity traditionally offered by molecules, and the increased stability usually encountered with heterogeneous materials. The various methods for immobilizing molecules (non-covalent, covalent, periodic systems)…

Hydrophobic Copper Interfaces Boost Electroreduction of Carbon Dioxide to Ethylene in Water

Liang, H. Q., Zhao, S., Hu, X. M., Ceccato, M., Skrydstrup, T. & Daasbjerg, K. https://doi.org/10.1021/acscatal.0c03766 Cu is in the spotlight as it represents the only metal capable of catalyzing CO2 reduction to multicarbon products. However, its catalytic performance is determined collectively by a number of parameters including its composition and structure, electrolyte, and cell configuration. It…

Mode I debonding under large deformation conditions including notes on cleavage-peeling transition

Heide-Jørgensen, S., Budzik, M. K., Buhl, K. B., Hinge, M., Pedersen, S. U., Daasbjerg, K. & Kongsfelt, M. https://doi.org/10.1016/j.engfracmech.2020.107413 Peeling and cleavage are common load cases for studying and evaluating adhesion between materials. The former is suitable for testing adhesion of thin or highly flexible materials for which the bending energy is negligible while the latter…

Main element chemistry enables gas-cylinder-free hydroformylations

Pedersen, S. K., Gudmundsson, H. G., Nielsen, D. U., Donslund, B. S., Hammershøj, H. C. D., Daasbjerg, K. & Skrydstrup, T. https://doi.org/10.1038/s41929-020-00510-z Industrially, aldehydes are produced annually on a multimillion-tonne scale via the hydroformylation of olefins with syngas (CO/H2 mixture). Nonetheless, this transformation has not found frequent use in the laboratory. Here we report on a simple…