The activation of inert oxygen(O_(2))often consumes enormous amounts of energy and resources,which is a global challenge in the field of environmental remediation and fuel cells.Organic pollutants are abundant in elec...The activation of inert oxygen(O_(2))often consumes enormous amounts of energy and resources,which is a global challenge in the field of environmental remediation and fuel cells.Organic pollutants are abundant in electrons and are promising alternative electron donors.Herein,we implement sustainable microactivation of dissolved oxygen(DO)by using the electrons and adsorption energy of pollutants by creating a nonequilibrium microsurface on nanoparticle-integrated molybdenum(Mo)lattice-doped zinc sulfide(ZnS)composites(MZS-1).Organic pollutants were quickly removed by DO microactivation in the MZS-1 system under natural conditions without any additional energy or electron donor.The turnover frequency(TOF,per Mo atom basis)is 5 orders of magnitude higher than those of homogeneous systems.Structural and electronic characterization technologies reveal the change in the crystalline phase(Zn-S-Mo)and the activation of π-electrons on six-membered rings of ZnS after Mo doping,which results in the formation of a nonequilibrium microsurface on MZS-1.This is the key for the strong interfacial interaction and directional electron transfer from pollutants to MZS-1 through the delocalized π-π conjugation effect and from MZS-1 to DO via Zn-S-Mo,as demonstrated by electron paramagnetic resonance(EPR)techniques and density functional theory(DFT)calculations.This process achieves the efficient use of pollutants and the low-energy activation of O_(2) through the construction of a nonequilibrium microsurface,which shows new significance for water treatment.展开更多
基金financially supported by the National Natural Science Foundation of China(52122009,52070046 and 51838005)the Introduced Innovative Research and Development Team Project under the“Pearl River Talent Recruitment Program”of Guangdong Province(2019ZT08L387)+2 种基金the National College Students’Innovation and Entrepreneurship Training Program,China(202111078021,202111078019,and 202011078019)the Special Funds for the Cultivation of Guangdong College Students’Scientific and Technological Innovation-“Climbing Program”Special Funds(pdjh2021b0395)the Guangdong Province Universities and Colleges Pearl River Scholar Funded Scheme(Young Scholar).
文摘The activation of inert oxygen(O_(2))often consumes enormous amounts of energy and resources,which is a global challenge in the field of environmental remediation and fuel cells.Organic pollutants are abundant in electrons and are promising alternative electron donors.Herein,we implement sustainable microactivation of dissolved oxygen(DO)by using the electrons and adsorption energy of pollutants by creating a nonequilibrium microsurface on nanoparticle-integrated molybdenum(Mo)lattice-doped zinc sulfide(ZnS)composites(MZS-1).Organic pollutants were quickly removed by DO microactivation in the MZS-1 system under natural conditions without any additional energy or electron donor.The turnover frequency(TOF,per Mo atom basis)is 5 orders of magnitude higher than those of homogeneous systems.Structural and electronic characterization technologies reveal the change in the crystalline phase(Zn-S-Mo)and the activation of π-electrons on six-membered rings of ZnS after Mo doping,which results in the formation of a nonequilibrium microsurface on MZS-1.This is the key for the strong interfacial interaction and directional electron transfer from pollutants to MZS-1 through the delocalized π-π conjugation effect and from MZS-1 to DO via Zn-S-Mo,as demonstrated by electron paramagnetic resonance(EPR)techniques and density functional theory(DFT)calculations.This process achieves the efficient use of pollutants and the low-energy activation of O_(2) through the construction of a nonequilibrium microsurface,which shows new significance for water treatment.
