Fuels and industrial chemicals that are conventionally derived from fossil resources could potentially be produced in a renewable, sustainable manner by an electrochemical process that operates at room temperature and atmospheric pressure, using only water, CO2, and electricity as inputs. To enable this technology, improved catalysts must be developed. Herein, we report trends in the electrocatalytic conversion of CO2 on a broad group of seven transition metal surfaces: Au, Ag, Zn, Cu, Ni, Pt, and Fe. Contrary to conventional knowledge in the field, all metals studied are capable of producing methane or methanol. We quantify reaction rates for these two products and describe catalyst activity and selectivity in the framework of CO binding energies for the different metals. While selectivity toward methane or methanol is low for most of these metals, the fact that they are all capable of producing these products, even at a low rate, is important new knowledge. This study reveals a richer surface chemistry ...

Electrocatalytic Conversion of Carbon Dioxide to Methane and Methanol on Transition Metal Surfaces

Methods that fix atmospheric nitrogen to ammonia under mild conditions could offer a more environmentally benign alternative to the Haber–Bosch process. Now, a Ru-loaded electride, [Ca24Al28O64]4+(e−)4, is reported that acts as an efficient electron donor and reversible hydrogen store, and is demonstrated to function as an efficient catalyst for ammonia synthesis.

Ammonia synthesis using a stable electride as an electron donor and reversible hydrogen store

Interaction of hydrogen with solid surfaces

Carbide and Nitride Overlayers on Early Transition Metal Surfaces: Preparation, Characterization, and Reactivities.

Pathways and kinetics through which chlorinated ethylenes and their daughter products react with Fe(0) particles were investigated through batch experiments. Substantial intra- and interspecies inhibitory effects were observed, requiring the use of a modified Langmuir−Hinshelwood−Hougen−Watson (LHHW) kinetic model in which species compete for a limited number of reactive sites at the particle−water interface. Results indicate that reductive β-elimination accounts for 87% of tetrachloroethylene (PCE), 97% of trichloroethylene (TCE), 94% of cis-dichloroethylene (cis-DCE), and 99% of trans-dichloroethylene (trans-DCE) reaction. Reaction of 1,1-DCE gives rise to ethylene, consistent with a reductive α-elimination pathway. For the highly reactive chloro- and dichloroacetylene intermediates produced from the reductive elimination of TCE and PCE, 100% and 76% of the reaction, respectively, occur via hydrogenolysis to lesser chlorinated acetylenes. The branching ratios for reactions of PCE or TCE (and their daugh...

Pathways and Kinetics of Chlorinated Ethylene and Chlorinated Acetylene Reaction with Fe(0) Particles

${\mathrm{N}}_{2}$ chemisorbed on Fe(111) is identified by photoelectron spectroscopy and high-resolution electron energy-loss spectroscopy as a $\ensuremath{\pi}$-bonded surface complex in which both nitrogen atoms interact with the metal. This species forms the immediate precursor to dissociation.

π -Bonded N 2 on Fe(111): The Precursor for Dissociation

Interaction of Co with an Fe(111) surface

A vibrational spectroscopy study on the interaction of N2 with clean and K-promoted Fe(111) surfaces: π-bonded dinitrogen as precursor for dissociation

M.-C. Tsai

Papers

π -Bonded N 2 on Fe(111): The Precursor for Dissociation

Interaction of Co with an Fe(111) surface

A vibrational spectroscopy study on the interaction of N2 with clean and K-promoted Fe(111) surfaces: π-bonded dinitrogen as precursor for dissociation

Interaction of acetylene and ethylene with an Fe(111) surface