查看更多>>摘要：The electrochemical reduction of CO2 is an extremely potential technique to achieve the goal of carbon neutrality,but the development of electrocatalysts with high activity,excellent product selectivity,and long-term durability remains a great challenge.Herein,the role of metal-supports interaction(MSI)between different active sites(including single and bimetallic atom sites consisting of Cu and Ni atoms)and carbon-based supports(including C2N,C3N4,N-coordination graphene,and graphdiyne)on catalytic activity,prod-uct selectivity,and thermodynamic stability towards CO2 reduction reaction(CRR)is systematically investi-gated by first principles calculations.Our results show that MSI is mainly related to the charge transfer behavior from metal sites to supports,and different MSI leads to diverse magnetic moments and d-band centers.Subsequently,the adsorption and catalytic performance can be efficiently improved by tuning MSI.Notably,the bimetallic atom supported graphdiyne not only exhibits a better catalytic activity,higher product selec-tivity,and higher thermodynamic stability,but also effectively inhibits the hydrogen evolution reaction.This finding provides a new research idea and optimization strategy for the rational design of high-efficiency CRR catalysts.
查看更多>>摘要：Antibiotic pollution in aqueous solutions seriously endangers the natural environment and public health.In this work,Mo-doped transition metal FeCo-Se metal aerogels(MAs)were investigated as bifunctional catalysts for the removal of sulfamethazine(SMT)in solution.The optimal Mo0.3Fe1Co3-Se catalyst can remove 97.7％of SMT within 60 min(SMT content:10 mg/L,current intensity:10 mA/cm2).The unique porous cross-linked structure of aerogel confered the catalyst sufficient active sites and efficient mass transfer channels.For the anode,Mo0.3Fe1Co3-Se MAs exhibits superior oxygen evolution reaction(OER)property,with an overpotential of only 235 mV(10 mA/cm2).Compared with FeiCo3 MAs or Mo0.3Fe1Co3 MAs,density functional theory(DFT)demonstrated that the better catalytic capacity of Mo0.3Fe1Co3-Se MAs is attributed to the doping of Mo species and selenization lowers the energy barrier for the*OOH to O2 step in the OER process.Excellent OER perfor-mance ensures the self-oxygenation in this system,avoiding the addition of air or oxygen in the traditional electro-Fenton process.For the cathode,Mo doping can lead to the lattice contraction and metallic character of CoSe2,which is beneficial to accelerate electron transfer.The adjacent Co active sites effectively adsorb*OOH and inhibit the breakage of the O-O bond.Rotating ring disk electrode(RRDE)test indicated that Mo0.3Fe1Co3-Se MAs has an excellent 2e ORR activity with H2O2 selectivity up to 88％,and the generated H2O2 is activated by the adjacent Fe site through heterogeneous Fenton process to generate OH.
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