Confined interface engineering of self-supported Cu@N-doped graphene for electrocatalytic CO_(2) reduction with enhanced selectivity towards ethanol

Electroreduction of greenhouse gas CO_(2) into value-added fuels and chemicals provides a promising pathway to address the issues of energy crisis and environmental change.However,the regulations of the selectivity towards C2 product and the competing hydrogen evolution reaction(HER)are major challenges for CO_(2) reduction reaction(CO_(2)RR).Here,we develop an interface-enhanced strategy by depositing a thin layer of nitrogen-doped graphene(N-G)on a Cu foam surface(Cu-N-G)to selectively promote the ethanol pathway in CO_(2)RR.Compared to the undetectable ethanol selectivity of pure Cu and Cu@graphene(Cu-G),Cu-N-G has boosted the ethanol selectivity to 33.1%in total Faradic efficiency(FE)at−0.8 V vs.reversible hydrogen electrode(RHE).The experimental and density functional theory(DFT)results verify that the interconnected graphene coating can not only serve as the fast charge transport channel but also provide confined nanospace for mass transfer.The N doping can not only trigger the intrinsic interaction between N in N-G and CO_(2) molecule for enriching the local concentration of reactants but also promote the average valence state of Cu for C–C coupling pathways.The confinement effect at the interface of Cu-N-G can not only provide high adsorbed hydrogen(Had)coverage but also stabilize the key*HCCHOH intermediate towards ethanol pathway.The provided interface-enhanced strategy herein is expected to inspire the design of Cubased CO_(2)RR electrocatalysts towards multi-carbon products.

Clusterphene:A new two-dimensional structure from cluster selfassembly

Since the advent of graphene in 2004,two-dimensional(2D)materials had ignited the development of fascinating functional materials for almost 20 years.Currently,the main members of 2D materials family are graphene,transition metal dichalcogenides(TMDs,MoS_(2),WS_(2),and others),MXenes(Ti_(3)C_(2),Ta_(4)C_(3),and others),Xenes(B,Si,P,Ge,and Sn),organic materials(COF,covalent organic frameworks),etc.The unique sheet-like morphology(single-or few-atomic-layer thickness)endow 2D materials with unconventional physicochemical properties for promising applications in catalysis,energy storage/conversion,electronics,biomedicine,sensors,etc.Nevertheless,the exploration and preparation of novel twodimensional materials with desired characteristics through highly controlled strategy remains one of the major challenges in this field.In a recent work from Nature Chemistry published on 10 February 2022,Liu et al.reported a new member,clusterphene,in the family of two-dimensional materials.