Direct Synthesis of 1-Butanol with High Faradaic Efficiency from CO Utilizing Cascade Catalysis at a Ni-Enhanced (CrO)GaO Electrocatalyst.

Electrochemical transformation of CO into energy-dense liquid fuels provides a viable solution to challenges regarding climate change and nonrenewable resource dependence. Here, we report on the modification of a Cr-Ga oxide electrocatalyst through the introduction of nickel to generate a catalyst that generates 1-butanol at unprecedented faradaic efficiencies (ξ = 42%). This faradaic efficiency occurs at -1.

Exploiting Metal-Ligand Cooperativity to Sequester, Activate, and Reduce Atmospheric Carbon Dioxide with a Neutral Zinc Complex.

As atmospheric levels of carbon dioxide (CO) continue to increase, there is an immediate need to balance the carbon cycle. Current approaches require multiple processes to fix CO from the atmosphere or flue gas and then reduce it to value-added products. The zinc(II) catalyst Zn(DMTH) (DMTH = diacetyl-2-(4-methyl-3-thiosemicarbazonate)-3-(2-pyridinehydrazonato)) reduces CO from air to formate with a faradaic efficiency of 15.

Utilizing Charge Effects and Minimizing Intramolecular Proton Rearrangement to Improve the Overpotential of a Thiosemicarbazonato Zinc HER Catalyst.

The zinc(II) complex of diacetyl-2-(4-methyl-3-thiosemicarbazone)-3-(2-hydrazonepyridine), ZnL (), was prepared and evaluated as a precatalyst for the hydrogen evolution reaction (HER) under homogeneous conditions in acetonitrile. Complex is protonated on the noncoordinating nitrogen of the hydrazonepyridine moiety to yield the active catalyst Zn(HL)OAc () upon addition of acetic acid. Addition of methyl iodide to yields the corresponding methylated derivative ZnLI ().

Metal-Assisted Ligand-Centered Electrocatalytic Hydrogen Evolution upon Reduction of a Bis(thiosemicarbazonato)Cu(II) Complex.

In this study, we report the electrocatalytic behavior of the neutral, monomeric Cu(II) complex of diacetyl-bis(N-4-methyl-3-thiosemicarbazonato), CuL, for metal-assisted ligand-centered hydrogen evolution in acetonitrile and dimethylformamide. CuL displays a maximum turnover frequency (TOF) of 10 000 s in acetonitrile and 5100 s in dimethylformamide at an overpotential of 0.80 and 0.