Converting CO_(2) under mild conditions by employing semiconductor photocatalysts is promising to address global environmental issues.However,the current CO_(2) conversion efficiency is limited by the difficulty activ...Converting CO_(2) under mild conditions by employing semiconductor photocatalysts is promising to address global environmental issues.However,the current CO_(2) conversion efficiency is limited by the difficulty activating the thermodynamically stable CO_(2) molecules.Constructing plasmonic nanoalloy-based photocatalytic systems with significant localized surface plasmon resonance(LSPR)is full of po-tential but remains a vast challenge.In this work,AuAg plasmonic nanoalloys were incorporated on CeO_(2) nanorods(designated as AuAg–CeO_(2))to achieve selective photoreduction of CO_(2).The result displays that Ag can serve as a superior electron modifier to promote the electron enrichment of Au,thus producing asymmetric charge distributions to boost the selective conversion of CO_(2).Furthermore,the improved LSPR effect on AuAg–CeO_(2) induces the generation of high-energy hot electrons under irradiation,enhancing the reactivity of electrons for CO_(2) photo-reduction.Due to the aforementioned effects,AuAg–CeO_(2) exhibits a high CO_(2)-to-CH4 performance of 92.6μmol g-1 through a 3-h test and a high CH4 selectivity of 94.5%,up to 2.6,8.7,and 17.1 times higher than the activity of Au–CeO_(2),pure CeO_(2),and Ag–CeO_(2),respectively.This work can provide a new perspective for con-structing high-performance catalysts for photocatalytic CO_(2) reduction.展开更多
基金financially supported by the Key R&D Program of Shaanxi Province(No.2023-YBGY-323)Joint Funds of the National Natural Science Foundation of China(No.U22A20391)+4 种基金the National Natural Science Foundation of China(Nos.22078256,22308272)the High-level Innovation and Entrepreneurship Talent Project of Qinchuangyuan(No.2021QCYRC4-24)Innovation Capability Support Program of Shaanxi(No.2023-CX-TD-26)the“Young Talent Support Plan”of Xi'an Jiaotong University(No.HG6J021)the Higher Education Institution Academic Discipline Innovation and Talent Introduction Plan(“111 Plan”,No.B23025).
文摘Converting CO_(2) under mild conditions by employing semiconductor photocatalysts is promising to address global environmental issues.However,the current CO_(2) conversion efficiency is limited by the difficulty activating the thermodynamically stable CO_(2) molecules.Constructing plasmonic nanoalloy-based photocatalytic systems with significant localized surface plasmon resonance(LSPR)is full of po-tential but remains a vast challenge.In this work,AuAg plasmonic nanoalloys were incorporated on CeO_(2) nanorods(designated as AuAg–CeO_(2))to achieve selective photoreduction of CO_(2).The result displays that Ag can serve as a superior electron modifier to promote the electron enrichment of Au,thus producing asymmetric charge distributions to boost the selective conversion of CO_(2).Furthermore,the improved LSPR effect on AuAg–CeO_(2) induces the generation of high-energy hot electrons under irradiation,enhancing the reactivity of electrons for CO_(2) photo-reduction.Due to the aforementioned effects,AuAg–CeO_(2) exhibits a high CO_(2)-to-CH4 performance of 92.6μmol g-1 through a 3-h test and a high CH4 selectivity of 94.5%,up to 2.6,8.7,and 17.1 times higher than the activity of Au–CeO_(2),pure CeO_(2),and Ag–CeO_(2),respectively.This work can provide a new perspective for con-structing high-performance catalysts for photocatalytic CO_(2) reduction.
