Name: preparation of silver-palladium alloyed nanoparticles for plasmonic catalysis under visible-light illumination
Uploaded: 2020-08-18T15:00:00
Description: Watch this Scientific Journal Video about Preparation of Silver-Palladium Alloyed Nanoparticles for Plasmonic Catalysis under Visible-Light Illumination at JoVE.com

Dette arbejde blev støttet af Universitetet i Helsinki og Jane og Aatos Erkko Foundation. S.H. takker Erasmus+ EU-midler for stipendiet.

1. Sammenfatning af AG-Pd/ZrO2 NPs 
BEMÆRK: I denne procedure svarede Pd mol% i Ag-Pd til 1%, og Ag-Pd-belastningen på ZrO2 svarede til 3 wt.%.
<ol><li>Placer 1 g ZrO2 pulver i et 250 mL bægerglas.</li>
	<li>Der tilsættes 50 mL af en AgNO3 (aq) (0,0059 mol/L) og 9,71 mL af en K2PdCl4 (aq) (0,00031 mol/L) opløsninger til bægeret under kraftig magnetisk omrøring (500 omdrejninger) ved stuetemperatur.</li>...

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De fund, der er beskrevet i denne metode, viser , at pds iboende katalytiske aktivitet (eller anden katalytisk, men ikke plasonisk metal) kan forbedres betydeligt ved LSPR-excitation via synlig lysbestråling i bimetallegeret NPs35. I dette tilfælde er Ag (eller et andet plasonisk metal) i stand til at høste energi fra synlig lysbestråling via LSPR-excitation. LSPR-excitationen fører til dannelse af varme ladebærere (varme elektroner og huller) og lokaliseret opvarmning5</su...

Blandt de mange anvendelser af metal nanopartikler (NPs), katalyse fortjener særlig opmærksomhed. Katalyse spiller en central rolle i en bæredygtig fremtid, der bidrager til mindre energiforbrug, bedre udnyttelse af råmaterialer og muliggør renere reaktionsforhold1,2,3,4. Således kan fremskridt inden for katalyse give værktøjer til at forbedre den atomare effektivitet af kemiske processer, hvilket gør dem renere, mere økonomisk levedygtige og mere miljøvenlige. Metal NPs omfatter sølv (Ag), guld (Au) eller kobber (Cu) kan vise interessante optiske egenskaber i det synlige område, der opstår fra den unikke måde, disse systemer interagerer med lys på nanoskala via den lokaliserede overflade plasmon resonans (LSPR) excitation5,6,7,8. I disse NPs, benævnt plasmoniske NPs, LSPR omfatter resonans interaktion mellem hændelsen fotoner (fra en indgående elektromagnetisk bølge) med den kollektive bevægelse af elektroner5,6,7,8. Dette fænomen finder sted med en karakteristisk frekvens, der er afhængig af miljøets størrelse, form, sammensætning og dielektriske konstant9,10,11. For Ag, Au og Cu kan disse frekvenserf.eks.
For nylig er det blevet påvist, at LSPR-excitationen i plasmoniske NPs kan bidrage til at fremskynde satserne og kontrollere selektiviteten af molekylære transformationer5,14,15,16,17,18,19. Dette fødte et feltkaldetplasmonisk katalyse, der fokuserer på at bruge energi fra lys til at accelerere, drive og / eller kontrollere kemiske transformationer 5,14,15,16,17,18,19. I denne forbindelse er det blevet fastslået, at LSPR excitation i plasmoniske NPs kan føre til dannelsen af energiske varme elektroner og huller, benævnt LSPR-ophidsede varme bærere. Disse bærere kan interagere med adsorberede arter gennem elektronisk eller vibrationel aktivering15,16. Ud over øgede reaktionshastigheder kan denne proces også give alternative reaktionsveje , der ikke er tilgængelige via traditionelle termokemisk drevne processer, hvilket åbner nye muligheder for kontrol over reaktions selektivitet20,21,22,23,24,25. Det er vigtigt at bemærke, at plasmon henfald også kan føre til termisk spredning, hvilket fører til en temperaturstigning i nærheden af NPs, som også kan bidrage til at fremskynde reaktionshastigheder15,16.
På grund af disse interessante funktioner er plasmonisk katalyse med succes blevet anvendt til en række molekylære transformationer18. Ikke desto mindre er der stadig en vigtig udfordring. Mens plasmoniske NPs såsom Ag og Au viser fremragende optiske egenskaber i de synlige og nær-IR-intervaller, er deres katalytiske egenskaber begrænset med hensyn til omfanget af transformationer. Med andre ord viser de ikke gode katalytiske egenskaber til flere transformationer. Derudover understøtter metaller, der er vigtige i katalyse, såsom palladium (Pd) og platin (Pt), ikke LSPR-excitation i de synlige eller nær-IR-intervaller. For at bygge bro over denne kløft repræsenterer bimetalliske NP'er , der indeholder et plasonisk og katalytisk metal , en effektiv strategi20,26,27,28,29. I disse systemer kan plasmonisk metal bruges som antenne til at høste energi fra lys excitation gennem LSPR, som derefter bruges til at drive, accelerere og kontrollere molekylære transformationer ved det katalytiske metal. Derfor giver denne strategi os mulighed for at udvide plasmonisk katalyse ud over traditionelle plasmoniske metal-NPs20,26,27,28,29.
Denne protokol beskriver facile syntesen af bimetallic sølv-palladium (Ag-Pd) legeret NPs understøttet på ZrO2 (Ag-Pd/ZrO2), der kan fungere som en plasmonisk-katalytisk system til plasmonisk katalyse. Ag-Pd/ZrO2 NP'erne blev fremstillet ved co-imprægnering af de tilsvarende metalprækursorer på ZrO2-støtten efterfulgt af samtidig reduktion30. Denne fremgangsmåde førte til dannelsen af bimetalliske NPs omkring 10 nm i størrelse (diameter) direkte på overfladen af ZrO2 støtte. NP'erne bestod af 1 mol% af Pd for at minimere udnyttelsen af det katalytiske metal og samtidig maksimere de optiske egenskaber af de resulterende Ag-Pd NPs. Der blev påvist en protokol for anvendelse af AG-Pd/ZrO2 IP'er i plasmonisk katalyse med henblik på reduktion af nitrobenzen. Vi brugte 425 nm LED-belysning til LSPR-excitationen. Gaskromatografi blev udført for at overvåge omdannelsen og selektiviteten af reduktionsreaktionen under de mørke og lyse bestrålingsforhold. LSPR-excitation førte til forbedret katalytisk ydeevne og kontrol over selektivitet i Ag-Pd/ZrO2 NP'er i forhold til rent termisk drevne forhold. Den metode, der er beskrevet i denne protokol, er baseret på en simpel fotokatalytisk reaktionsopsætning kombineret med gaskromatografi og kan tilpasses en bred vifte af molekylære transformationer og NPs-sammensætninger. Således gør denne metode det muligt at karakterisere fotokatalytisk aktivitet med hensyn til konvertering og reaktions selektivitet af forskellige NPs og for et utal af væskefasetransformationer. Vi mener, at denne artikel vil give vigtige retningslinjer og indsigter til både nyankomne og mere erfarne forskere på området.

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preparation of silver-palladium alloyed nanoparticles for plasmonic catalysis under visible-light illumination

Lokaliseret overfladeplasmon resonans (LSPR) i plasmoniske nanopartikler (NPs) kan accelerere og kontrollere selektiviteten af en række molekylære transformationer. Dette åbner muligheder for brug af synligt eller nær-IR-lys som et bæredygtigt input til at drive og kontrollere reaktioner, når plasmoniske nanopartikler, der understøtter LSPR-excitation i disse serier, anvendes som katalysatorer. Desværre er dette ikke tilfældet for flere katalytiske metaller som palladium (Pd). En strategi for at overvinde denne begrænsning er at anvende bimetalliske NPs indeholder plasmoniske og katalytiske metaller. I dette tilfælde kan LSPR-excitationen i plasmonisk metal bidrage til at fremskynde og kontrollere transformationer drevet af den katalytiske komponent. Den metode, der rapporteres heri, fokuserer på syntesen af bimetallisk sølvpaladium (Ag-Pd) NPs understøttet på ZrO2 (Ag-Pd/ZrO2),der fungerer som et plasonisk-katalytisk system. NP'erne blev udarbejdet ved co-imprægnering af tilsvarende metalprækursorer på ZrO2-støtten efterfulgt af samtidig reduktion, hvilket førte til dannelsen af bimetalliske NPs direkte på ZrO2-støtten. Ag-Pd/ZrO2 NP'er blev derefter brugt som plasmoniske katalysatorer til reduktion af nitrobenzen under 425 nm belysning af LED-lamper. Ved hjælp af gaskromatografi (GC) kan omdannelsen og selektiviteten af reduktionsreaktionen under de mørke og lyse bestrålingsforhold overvåges, hvilket viser den forbedrede katalytiske ydeevne og kontrol over selektivitet under LSPR-excitation efter legering af ikke-plasonisk Pd med plasonisk metal Ag. Denne teknik kan tilpasses en bred vifte af molekylære transformationer og NPs-kompositioner, hvilket gør den nyttig til karakterisering af den plasmoniske katalytiske aktivitet af forskellige typer katalyse med hensyn til konvertering og selektivitet.

Figur 1A viser digitale fotografier af de faste prøver, der indeholder den rene ZrO2-oxid (til venstre) og AG-Pd/ZrO2-NPs (højre). Denne farveændring fra hvid (i ZrO2) til brun (Ag-Pd/ZrO2)giver den første kvalitative dokumentation for depositionen af AG-Pd NPs på ZrO2-overfladen. Figur 1B viser UV-synlige absorptionsspektre fra AG-Pd/ZrO2 NP'er (blåt spor) samt ZrO2 (sort spor) o...

Watch this Scientific Journal Video about Preparation of Silver-Palladium Alloyed Nanoparticles for Plasmonic Catalysis under Visible-Light Illumination at JoVE.com

Preparation of Silver-Palladium Alloyed Nanoparticles for Plasmonic Catalysis under Visible-Light Illumination

Præsenteret her er en protokol for syntese af sølv-palladium (Ag-Pd) legering nanopartikler (NPs) understøttet på ZrO2 (Ag-Pd/ZrO2). Dette system gør det muligt at høste energi fra synlig lysbestråling for at fremskynde og kontrollere molekylære transformationer. Dette illustreres af nitrobenzenreduktion under let bestråling katalyseret af Ag-Pd/ZrO2 NPs.

Forberedelse af sølv-palladium legerede nanopartikler til plasmonisk katalyse under synlig lysbelysning

Localized surface plasmon resonance (LSPR) in plasmonic nanoparticles (NPs) can accelerate and control the selectivity of a variety of molecular ...

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