Low-Valence Znδ+ (0<δ<2) Single-Atom Material as Highly Efficient Electrocatalyst for CO2 Reduction

Monica R. Madsen, Magnus H. Rønne, Marvin Heuschen, Dusanka Golo, Mårten S. G. Ahlquist, Troels Skrydstrup, Steen U. Pedersen, and Kim Daasbjerg. https://doi.org/10.1002/anie.202107550 A nitrogen-stabilized single-atom catalyst containing low-valence zinc atoms (Znδ+-NC) is reported. It contains saturated four-coordinate (Zn-N4) and unsaturated three-coordinate (Zn-N3) sites. The latter makes Zn a low-valence state, as deduced from X-ray photoelectron spectroscopy, X-ray absorption spectroscopy, electron…

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Synthesis and depolymerization of self-immolative poly(disulfide)s with saturated aliphatic backbones

Magnus Hansen-Felby, Andreas Sommerfeldt, Martin Lahn Henriksen, Steen Uttrup Pedersen, and Kim Daasbjerg. https://doi.org/10.1039/D1PY01412A Self-immolative polymers (SIPs) are a class of degradable stimuli-responsive polymers, which, upon removal of labile end-caps, depolymerize selectively and stepwise to small molecules. In light of our recent discovery of poly(dithiothreitol) (pDTT), a versatile SIP with a remarkably simple synthesis procedure, we…

Promoting Selective Generation of Formic Acid from CO2 Using Mn(bpy)(CO)3Br as Electrocatalyst and Triethylamine/Isopropanol as Additives

Monica R. Madsen, Magnus H. Rønne, Marvin Heuschen, Dusanka Golo, Mårten S. G. Ahlquist, Troels Skrydstrup, Steen U. Pedersen, and Kim Daasbjerg. https://pubs.acs.org/doi/10.1021/jacs.1c10805 Urgent solutions are needed to efficiently convert the greenhouse gas CO2 into higher‑value products. In this work, fac-Mn(bpy)(CO)3Br (bpy = 2,2′-bipyridine) is employed as electrocatalyst in reductive CO2 conversion. It is shown that product selectivity can be shifted…

New NNF Center

We are exceedingly happy to announce that we are a part of the forthcoming Novo Nordisk Foundation (NNF) CO2 center which is a new, unique research center to be launched. One of the most important global challenges of the modern era is to curb climate change, and the resultant upheavals facing society in the coming…

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…

Incorporation of nickel single atoms into carbon paper as self-standing electrocatalyst for CO2 reduction

Li, S., Ceccato, M., Lu, X., Frank, S., Lock, N., Roldan, A., Hu, X. M., Skrydstrup, T. & Daasbjerg, K. 10.1039/d0ta08433f The design of selective and efficient catalysts for electrochemical CO2 reduction is highly desirable yet still challenging, in particular, if the aim is to make them binder-free and self-standing. Here, we report a new and straightforward…

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…

Evaluation of Surface-initiated Polymer brush as Anti-scaling Coating for Plate Heat Exchangers

Jakob Ege Friis, Guruprakash Subbiahdoss, Gorm Gerved, Allan Hjarbæk Holm, Olga Santos, Anders Bank Blichfeld, Saeed Zajforoushan Moghaddam, Esben Thormann, Kim Daasbjerg, Joseph Iruthayaraj, Rikke Louise Meyer https://doi.org/10.1016/j.porgcoat.2019.06.042 Inorganic fouling is one of the challenging problems in heat exchanger applications. One approach to mitigate fouling is to employ surface coatings. In this study, we evaluated…