Asymmetrically coordinated main group atomic In-S_(1)N_(3)interface sites for promoting electrochemical CO_(2)reduction

Designing catalysts with highly active,selectivity,and stability for electrocatalytic CO_(2)to formate is currently a severe challenge.Herein,we developed an electronic structure engineering on carbon nano frameworks embedded with nitrogen and sulfur asymmetrically dual-coordinated indium active sites toward the efficient electrocatalytic CO_(2)reduction reaction.As expected,atomically dispersed In-based catalysts with In-S_(1)N_(3)atomic interface with asymmetrically coordinated exhibited high efficiency for CO_(2)reduction reaction(CO_(2)RR)to formate.It achieved a maximum Faradaic efficiency(FE)of 94.3%towards formate generation at−0.8 V vs.reversible hydrogen electrode(RHE),outperforming that of catalysts with In-S2N2 and In-N4 atomic interface.And at a potential of−1.10 V vs.RHE,In-S_(1)N_(3)achieves an impressive Faradaic efficiency of 93.7%in flow cell.The catalytic performance of In-S_(1)N_(3)sites was confirmed to be enhanced through in-situ X-ray absorption near-edge structure(XANES)measurements under electrochemical conditions.Our discovery provides the guidance for performance regulation of main group metal catalysts toward CO_(2)RR at atomic scale.

Atomically Dispersed Main Group Magnesium on Cadmium Sulfide as the Active Site for Promoting Photocatalytic Hydrogen Evolution Catalysis

Photoabsorption charge separation/transfer and surface reaction are the three main factors influencing the efficiency of photocatalysis.Band structure engineering has been extensively applied to improve the light absorption of photocatalysts,however,most of the developed photocatalysts still suffer from low photocatalytic performance due to the limited active site(s)and fast recombination of photogenerated charge carriers.In this work,atomically dispersed main group magnesium(Mg)is introduced onto CdS monodispersed nanospheres,which greatly enhances the photocatalytic hydrogen evolution reaction.The photocatalytic hydrogen evolution reaction rate reaches 30.6 mmol·gcatalyst^(-1)·h^(-1),which is about 11.8 and 2.5 times that of pure CdS and Pt(2 wt.%)-CdS.The atomically dispersed Mg on CdS acts as an electron sink to trap photogenerated electrons,and at the same time,greatly reduces the Gibbs free energy of hydrogen evolution reaction(HER)and accelerates HER.

Mechanically Strong Heterogeneous Catalysts via Immobilization of Powderous Catalysts to Porous Plastic Tablets

Main observation and conclusion We describe a practical and general protocol for immobilization of heterogeneous catalysts to mechanically robust porous ultra-high molecular weight polyethylene tablets using inter-facial Lifshitz-van der Waals Interactions.Diverse types of powderous catalysts,including Cu,Pd/C,Pd/Al2O3,Pt/C,and Rh/C have been immobilized successfully.The immobilized catalysts are mechanistically robust towards stirring in solutions,and they worked well in diverse synthetic reactions.The immobilized catalyst tablets are easy to handle and reused.Moreover,the metal leaching of immobilized catalysts was reduced significantly.