Temperature dependent product distribution of electrochemical CO2 reduction on CoTPP/MWCNT Composite

As the sole metal that could reduce CO2 to substantial amounts of hydrocarbons, Cu plays an important role in electrochemical CO2 reduction, despite its low energy efficiency. Surface morphology modification is an effective method to improve its reaction activity and selectivity. Different from the pretreated modification method, in which the catalysts self-reconstruction process was ignored, we present operando synthesis by simultaneous electro-dissolution and electro-redeposition of copper during the CO2 electroreduction process. Through controlling the cathodic potential and CO2 flow rate, various high-curvature morphologies including microclusters, microspheres, nanoneedles, and nanowhiskers have been obtained, for which the real-time activity and product distribution is analyzed. The best CO2 electro-reduction activity and favored C2H4 generation activity, with around 10% faradic efficiency, can be realized through extensively distributed copper nanowhiskers synthesized under 40 mL/min flow rate and −2.1 V potential.

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Temperature dependent product distribution in photolysis of o-alkylphenacyl benzoates

Tetrahedron Letters ◽

10.1016/j.tetlet.2013.10.109 ◽

2013 ◽

Vol 54 (52) ◽

pp. 7175-7179 ◽

Cited By ~ 2

Author(s):

Mi Jang ◽

Bum Hee Lim ◽

Hyuk Jun Ryu ◽

Bong Ser Park

Keyword(s):

Product Distribution ◽

Temperature Dependent ◽

Dependent Product

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Flash pyrolysis of coals. Temperature-dependent product distribution

Journal of Analytical and Applied Pyrolysis ◽

10.1016/0165-2370(94)00826-m ◽

1995 ◽

Vol 32 ◽

pp. 51-63 ◽

Cited By ~ 29

Author(s):

Jesper V. Christiansen ◽

Anders Feldthus ◽

Lars Carlsen

Keyword(s):

Product Distribution ◽

Temperature Dependent ◽

Flash Pyrolysis ◽

Dependent Product

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Molecular Inhibition for Selective CO2 Conversion

10.26434/chemrxiv-2022-63b91 ◽

2022 ◽

Author(s):

Charles Creissen ◽

José Guillermo Rivera de la Cruz ◽

Dilan Karapinar ◽

Dario Taverna ◽

Moritz Schreiber ◽

...

Keyword(s):

Heterogeneous Catalysts ◽

Co2 Reduction ◽

Copper Catalysts ◽

Reaction Rates ◽

Product Distribution ◽

Flow Cell ◽

Novel Approach ◽

Electrochemical Co2 Reduction ◽

Conventional Material ◽

Formate Production

Electrochemical CO2 reduction presents a sustainable route to the production of chemicals and fuels. Achieving a narrow product distribution with copper catalysts is challenging and conventional material modifications offer limited control over selectivity. Here, we show that the mild cathodic potentials required to reach high currents in an alkaline gas-fed flow cell permits retention of a surface-bound thiol (4-mercaptopyridine), enabling molecule-directed selective formate generation at high reaction rates. Combined experimental and computational results showed that formate production is favoured due to the inhibition of a CO producing pathway caused by destabilising interactions with the anchored molecule. The immobilisation of molecules to inhibit specific carbon-based products therefore offers a novel approach to rationally tune the selectivity of heterogeneous catalysts.

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An NADH-Inspired Redox Mediator Strategy to Promote Second-Sphere Electron and Proton Transfer for Cooperative Electrochemical CO2 Reduction Catalyzed by Iron Porphyrin

10.26434/chemrxiv.12159207.v1 ◽

2020 ◽

Cited By ~ 1

Author(s):

Peter T. Smith ◽

Sophia Weng ◽

Christopher Chang

Keyword(s):

Proton Transfer ◽

Co2 Reduction ◽

Iron Porphyrin ◽

Redox Mediators ◽

Reservoir Properties ◽

Proton Reduction ◽

Electrochemical Co2 Reduction ◽

Starting Point ◽

Rate Improvement ◽

Molecular Catalysts

We present a bioinspired strategy for enhancing electrochemical carbon dioxide reduction catalysis by cooperative use of base-metal molecular catalysts with intermolecular second-sphere redox mediators that facilitate both electron and proton transfer. Functional synthetic mimics of the biological redox cofactor NADH, which are electrochemically stable and are capable of mediating both electron and proton transfer, can enhance the activity of an iron porphyrin catalyst for electrochemical reduction of CO2 to CO, achieving a 13-fold rate improvement without altering the intrinsic high selectivity of this catalyst platform for CO2 versus proton reduction. Evaluation of a systematic series of NADH analogs and redox-inactive control additives with varying proton and electron reservoir properties reveals that both electron and proton transfer contribute to the observed catalytic enhancements. This work establishes that second-sphere dual control of electron and proton inventories is a viable design strategy for developing more effective electrocatalysts for CO2 reduction, providing a starting point for broader applications of this approach to other multi-electron, multi-proton transformations.

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