Electrocatalytic oxygen reduction reaction(ORR)to prepare H_(2)O_(2)in acidic medium has the advantages of green,safety,and portability,which shows broad development prospects.However,it still suffers from low catalys...Electrocatalytic oxygen reduction reaction(ORR)to prepare H_(2)O_(2)in acidic medium has the advantages of green,safety,and portability,which shows broad development prospects.However,it still suffers from low catalyst activity,insufficient selectivity,and high cost.Herein,Pt_(1)/CoSe_(2)with ultralow 0.01 wt.%Pt atomic distribution was synthesized by a simple hydrothermal method.The Pt_(1)/CoSe_(2)with ultralow Pt content exhibits high activity,high selectivity,and long-term stability for ORR to H_(2)O_(2)in O_(2)-saturated 0.1 M HClO_(4).The onset potential is as low as 0.75 V versus reversible hydrogen electrode(RHE),H_(2)O_(2)selectivity is as high as 84%(0.4 V vs.RHE),and the electron transfer number is 2.3(0.4 V vs.RHE).Moreover,the hydrogen peroxide yield using the flow cell testing is 110.02 mmol g_(cat).^(−1)h^(−1) with high Faradaic efficiency of 78%(0 V vs.RHE)at 0.1 M HClO_(4),and the catalyst did not deactivate significantly after 60 h stability testing.Mechanistic studies and in situ X-ray photoelectron spectroscopy characterization confirm that the ultralow Pt content on CoSe_(2)can effectively regulate the electronic structure of Co as the real active site around the Pt site,which gives a suitable Δ_(dp) value(the difference between the d-band center of the active metal site and the p-band center of the terminal oxygen in*OOH),provides an ideal*OOH binding energy,and inhibits the O-O bond breakage.This work successfully improves the intrinsic activity of the Co active sites around Pt in Pt_(1)/CoSe_(2)for acidic ORR to H_(2)O_(2)by constructing ultralow-content Pt single atom.展开更多
基金Natural Science Foundation of Shandong,Grant/Award Numbers:ZR2022QB236,ZR2020KB011China Postdoctoral Science Foundation,Grant/Award Number:2022M722363+1 种基金National Natural Science Foundation of China,Grant/Award Numbers:21878063,22005168Taishan Scholars Program,Grant/Award Number:tsqn201909119。
文摘Electrocatalytic oxygen reduction reaction(ORR)to prepare H_(2)O_(2)in acidic medium has the advantages of green,safety,and portability,which shows broad development prospects.However,it still suffers from low catalyst activity,insufficient selectivity,and high cost.Herein,Pt_(1)/CoSe_(2)with ultralow 0.01 wt.%Pt atomic distribution was synthesized by a simple hydrothermal method.The Pt_(1)/CoSe_(2)with ultralow Pt content exhibits high activity,high selectivity,and long-term stability for ORR to H_(2)O_(2)in O_(2)-saturated 0.1 M HClO_(4).The onset potential is as low as 0.75 V versus reversible hydrogen electrode(RHE),H_(2)O_(2)selectivity is as high as 84%(0.4 V vs.RHE),and the electron transfer number is 2.3(0.4 V vs.RHE).Moreover,the hydrogen peroxide yield using the flow cell testing is 110.02 mmol g_(cat).^(−1)h^(−1) with high Faradaic efficiency of 78%(0 V vs.RHE)at 0.1 M HClO_(4),and the catalyst did not deactivate significantly after 60 h stability testing.Mechanistic studies and in situ X-ray photoelectron spectroscopy characterization confirm that the ultralow Pt content on CoSe_(2)can effectively regulate the electronic structure of Co as the real active site around the Pt site,which gives a suitable Δ_(dp) value(the difference between the d-band center of the active metal site and the p-band center of the terminal oxygen in*OOH),provides an ideal*OOH binding energy,and inhibits the O-O bond breakage.This work successfully improves the intrinsic activity of the Co active sites around Pt in Pt_(1)/CoSe_(2)for acidic ORR to H_(2)O_(2)by constructing ultralow-content Pt single atom.
