The presence of persistent pollutants in water poses a severe environmental threat,driving an urgent need for efficient and eco-friendly remediation strategies.In response,the scientific community is increasingly focu...The presence of persistent pollutants in water poses a severe environmental threat,driving an urgent need for efficient and eco-friendly remediation strategies.In response,the scientific community is increasingly focused on developing catalytic processes that maximize efficiency while minimizing environmental impact.In this context,we introduce recyclable catalysts based on NiPd nanoparticles(NPs)that feature tunable phase distributions and compositions.By varying Pd doping levels through Reactive Laser Ablation in Liquids(RLAL),we precisely control the catalytic and magnetic properties of these NPs.Notably,a nanocatalyst featuring the NiPd alloyed phase exhibits exceptional catalytic performance,achieving a turnover frequency of 3680 h^(-1) and 98.5%selectivity in the model transformation of 4-nitrophenol into 4-aminophenol.Additionally,it demonstrates remarkable efficiency in the chemoselective hydrogenation of various nitroarenes to functionalized anilines under mild conditions(atmospheric H_(2) pressure,33℃).Furthermore,the synergistic properties arising from the internal structure of these NPs allow them to surpass the performance of nanocatalysts made from their monometallic counterparts and simple mixtures.Overall,this study represents a significant advancement in the precise control of nanocatalyst synthesis and their associated physicochemical properties,paving the way for more efficient redox catalytic protocols,including industrially demanding hydrogenation reactions.展开更多
基金supported by the European Union’s Horizon Europe Widera 2021 Programme under the SURRI project,Grant Agreement No.101079345support from the European Union’s Horizon Europe Research and Innovation Programme under Marie Sklodowska-Curie grant agreements LYMON number 101151748.M.C.thanks the project DKRVO(RP/CPS/2024-28/007)+4 种基金supported by the Ministry of Education,Youth and Sports of the Czech Republic.I.S.thanks the Gen-T Plan of the Generalitat Valenciana through the program“Suport a l’estabilitzacióde les persones investigadores amb talent contractades amb càrrec a les convocatòries 2023 i anteriors del Pla GenT”(ESGENT/016/2024)Furthermore,the Grant CNS_(2)022-136183 funded by MICIU/AEI/10.13039/501100011033by“European Union NextGenerationEU/PRTR”the Grant PID2022-143164OA-I00 funded by MICIU/AEI/10.13039/501100011033 and by“ERDF/EU”Universitat Jaume I(GACUJIMA/2024/13)are also gratefully acknowledged.
文摘The presence of persistent pollutants in water poses a severe environmental threat,driving an urgent need for efficient and eco-friendly remediation strategies.In response,the scientific community is increasingly focused on developing catalytic processes that maximize efficiency while minimizing environmental impact.In this context,we introduce recyclable catalysts based on NiPd nanoparticles(NPs)that feature tunable phase distributions and compositions.By varying Pd doping levels through Reactive Laser Ablation in Liquids(RLAL),we precisely control the catalytic and magnetic properties of these NPs.Notably,a nanocatalyst featuring the NiPd alloyed phase exhibits exceptional catalytic performance,achieving a turnover frequency of 3680 h^(-1) and 98.5%selectivity in the model transformation of 4-nitrophenol into 4-aminophenol.Additionally,it demonstrates remarkable efficiency in the chemoselective hydrogenation of various nitroarenes to functionalized anilines under mild conditions(atmospheric H_(2) pressure,33℃).Furthermore,the synergistic properties arising from the internal structure of these NPs allow them to surpass the performance of nanocatalysts made from their monometallic counterparts and simple mixtures.Overall,this study represents a significant advancement in the precise control of nanocatalyst synthesis and their associated physicochemical properties,paving the way for more efficient redox catalytic protocols,including industrially demanding hydrogenation reactions.