Electrochemical valorization of HS in natural gas to sulfate under mild conditions.

HS capture and valorization from polluted natural gas offer environmental and resource recovery benefits, but current approaches produce moderate-value sulfur with intensive carbon footprint. Herein, we develop an electrochemical deep oxidation method that converts HS from polluted natural gas into value-added KSO using in-situ cathodically generated HO. We first validate this concept using commercial HO and then in-situ generated HO in H-cell, revealing the importance of high HO concentration for deep HS oxidation, especially sluggish SO-to-SO conversion.

Ligand Tuning of Molecular Ag Catalysts Enables Efficient Direct Propylene Electrooxidation to Propylene Glycol.

Renewable-electricity-driven direct oxidation of propylene (CH) presents a sustainable route for propylene glycol (PG) production. Silver (Ag) shows a 30-fold lower price compared to other active noble metals (platinum and palladium) but suffers from low activity. Here, we report a ligand-tuning strategy in Ag-based molecular catalysts for efficient direct CH-to-PG conversion.

Electrocatalytic Upgrading of Plastic and Biomass-Derived Polyols to Formamide under Ambient Conditions.

Electrocatalytic upgrading of wasted plastic and renewable biomass represents a sustainable method to produce chemicals but is limited to carbohydrates, leaving other value-added chemicals, such as organonitrogen compounds, being scarcely explored. Herein, we reported an electrocatalytic oxidation strategy to transform polyethylene terephthalate (PET) plastic-derived ethylene glycol (EG) and biomass-derived polyols into formamide, in the presence of ammonia (NH) over a tungsten oxide (WO) catalyst. Taking EG-to-formamide as an example, we achieved a high formamide productivity of 537.

Steering Selectivity in Electrocatalytic Furfural Reduction via Electrode-Electrolyte Interface Modification.

Electrocatalytic reduction of biomass-derived furfural (FF) represents a sustainable route to produce furfuryl alcohol (FA) and 2-methylfuran (MF) as a value-added chemical and a biofuel, respectively. However, achieving high selectivity for MF as well as tuning the selectivity between FA and MF within one reaction system remain challenging. Herein, we have reported an electrode-electrolyte interface modification strategy, enabling FA and MF selectivity steering under the same reaction conditions.

Electrochemical carbon-carbon coupling with enhanced activity and racemate stereoselectivity by microenvironment regulation.

Enzymes are characteristic of catalytic efficiency and specificity by maneuvering multiple components in concert at a confined nanoscale space. However, achieving such a configuration in artificial catalysts remains challenging. Herein, we report a microenvironment regulation strategy by modifying carbon paper with hexadecyltrimethylammonium cations, delivering electrochemical carbon-carbon coupling of benzaldehyde with enhanced activity and racemate stereoselectivity.

An Adjacent Atomic Platinum Site Enables Single-Atom Iron with High Oxygen Reduction Reaction Performance.

The modulation effect has been widely investigated to tune the electronic state of single-atomic M-N-C catalysts to enhance the activity of oxygen reduction reaction (ORR). However, the in-depth study of modulation effect is rarely reported for the isolated dual-atomic metal sites. Now, the catalytic activities of Fe-N moiety can be enhanced by the adjacent Pt-N moiety through the modulation effect, in which the Pt-N acts as the modulator to tune the 3d electronic orbitals of Fe-N active site and optimize ORR activity.