The contamination of nitric oxide presents a significant environmental challenge,necessitating the development of efficient photocatalysts for remediation.Conventional heterojunctions encounter obstacles such as large...The contamination of nitric oxide presents a significant environmental challenge,necessitating the development of efficient photocatalysts for remediation.Conventional heterojunctions encounter obstacles such as large contact barriers,sluggish charge transport,and compromised redox capacity.Here,we introduce an innovative S-type heterostructure photocatalyst,UiO-66-NH_(2)/ZnS(en)0.5,designed specifically to overcome these challenges.The synthesis,employing a unique microwave solvothermal method,strategically aligns the lowest unoccupied molecular orbital of UiO-66-NH_(2)with the highest occupied molecular orbital of ZnS(en)0.5,fostering the formation of a stepped heterojunction.The resulting intimate interface contact generates a built-in electric field,facilitating charge separation and migration,as evidenced by time-resolved photoluminescence spectroscopy and photoelectrochemical tests.The abundant active sites in the porous UiO-66-NH_(2)counterpart provide adsorption and activation sites for nitrogen monoxide(NO)oxidation.Performance evaluation reveals exceptional photocatalytic NO removal,achieving 70%efficiency and 99%selectivity toward nitrates under simulated solar illumination.Evidence from X-ray photoelectron spectroscopy and trapping experiments supports the effectiveness of the S-type heterostructure,showcasing refined reactive oxygen species,particularly superoxide.Thus,this study introduces a new perspective on advanced NO oxidation and unlocks the potential of S-scheme heterojunctions to refine reactive oxygen species for NO remediation.展开更多
基金National Natural Science Foundation of China,Grant/Award Numbers:22106105,22201180Innovation Program of Shanghai Municipal Education Commission,Grant/Award Number:2019‐01‐07‐00‐E00015+3 种基金Shanghai Scientific and Technological Innovation Project,Grant/Award Number:21DZ1206300Central Guidance on Local Science and Technology Development Fund of Shanghai,Grant/Award Number:YDZX20213100003002Science and Technology Commission of Shanghai Municipality,Grant/Award Number:20060502200Program for Professor of Special Appointment,Shanghai Sailing Program,Grant/Award Number:20YF1432200。
文摘The contamination of nitric oxide presents a significant environmental challenge,necessitating the development of efficient photocatalysts for remediation.Conventional heterojunctions encounter obstacles such as large contact barriers,sluggish charge transport,and compromised redox capacity.Here,we introduce an innovative S-type heterostructure photocatalyst,UiO-66-NH_(2)/ZnS(en)0.5,designed specifically to overcome these challenges.The synthesis,employing a unique microwave solvothermal method,strategically aligns the lowest unoccupied molecular orbital of UiO-66-NH_(2)with the highest occupied molecular orbital of ZnS(en)0.5,fostering the formation of a stepped heterojunction.The resulting intimate interface contact generates a built-in electric field,facilitating charge separation and migration,as evidenced by time-resolved photoluminescence spectroscopy and photoelectrochemical tests.The abundant active sites in the porous UiO-66-NH_(2)counterpart provide adsorption and activation sites for nitrogen monoxide(NO)oxidation.Performance evaluation reveals exceptional photocatalytic NO removal,achieving 70%efficiency and 99%selectivity toward nitrates under simulated solar illumination.Evidence from X-ray photoelectron spectroscopy and trapping experiments supports the effectiveness of the S-type heterostructure,showcasing refined reactive oxygen species,particularly superoxide.Thus,this study introduces a new perspective on advanced NO oxidation and unlocks the potential of S-scheme heterojunctions to refine reactive oxygen species for NO remediation.
