Chemistry in the Center for Catalytic Hydrocarbon Functionalization: An Energy Frontier Research Center

Abstract

Selective catalysts that activate small molecules such as hydrocarbons, dioxygen, water, carbon dioxide and dihydrogen are central to new technologies for the use of alternative energy sources. For example, controlled hydrocarbon functionalization can lead to high impact technologies, but such catalysts require a level of molecular control beyond current means. The Center for Catalytic Hydrocarbon Functionalization facilitates collaborations among research groups in catalysis, materials, electrochemistry, bioinorganic chemistry and quantum mechanics to develop, validate and optimize new methods to rearrange the bonds of hydrocarbons, activate and transform water and carbon dioxide, implement enzymatic strategies into synthetic systems and design optimal environments for catalysis.

Catalytic and Mechanistic Insights of the Low‐Temperature Selective Oxidation of Methane over Cu‐Promoted Fe‐ZSM‐5

“…This may be accounted for by the rapid over-oxidation of, in particular, H 2 CÀ(OH) 2 to HCOOH. However, it is also possible that H 2 CO and H 2 C(OH) 2 were not produced during the reaction. Indeed, evaluation of the stability of possible reaction products under our experimental conditions demonstrated that at least H 2 CO, if formed, should be detected during the reaction.…”

“…[1] Methane, the major component of fossil resources such as natural gas and clathrate fields, is one such promising alternative feedstock. [2] In spite of its significant natural abundance and its relatively inexpensive commodity price, methane is still a hugely underutilised resource. Although methods of converting methane to value-added products and fuels are practiced industrially, [3] these are not economically viable in remote regions where a significant fraction of the worlds reserves are found.…”

Low‐Temperature Transformation of Methane to Methanol on Pd1O4 Single Sites Anchored on the Internal Surface of Microporous Silicate

“…[1] Hydraulic fracturing supplies much of this earth-abundant source from shale,w hich make chemical and energy transformations economical. Thermodynamic calculations suggest that the reaction toward methanol production is highly favorable compared to formation of ab yproduct, methyl peroxide.…”

“…

Direct conversion of methane to chemical feedstocks such as methanol under mild conditions is ac hallenging but ideal solution for utilization of methane.P d 1 O 4 single-sites anchored on the internal surface of micropores of am icroporous silicate exhibit high selectivity and activity in transforming CH 4 to CH 3 OH at 50-95 8 8Cinaqueous phase through partial oxidation of CH 4 with H 2 O 2 .T he selectivity for methanol production remains at 86.4 %, while the activity for methanol production at 95 8 8Ci sa bout 2.78 molecules per Pd 1 O 4 site per second when 2.0 wt %C uO is used as ac ocatalyst with the Pd 1 O 4 @ZSM-5. Thec onversion rate of CH 4 to CH 3 OH at as olid-liquid interface pioneered by Hutchings et al [4a,5] is typically higher than these at as olid-gas interface, [3a,b] though the rate is still relatively low.Although catalytic activity for direct oxidation of CH 4 to CH 3 OH on these catalysts at solid-gas and solid-liquid interfaces was reported, [1,[3][4][5][6] challenges remain before ad irect oxidation process under mild conditions could be considered as ap otential approach in the chemical industry. [1] Hydraulic fracturing supplies much of this earth-abundant source from shale,w hich make chemical and energy transformations economical.

…”

“…[1] Hydraulic fracturing supplies much of this earth-abundant source from shale,w hich make chemical and energy transformations economical. [1] Hydraulic fracturing supplies much of this earth-abundant source from shale,w hich make chemical and energy transformations economical.…”