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Instruments / Technical Area	Publication Details	Published
B18-Core EXAFS	AuxPdy-based heterogeneous nanocatalysts for plasmon-mediated enhanced catalysis under visible light irradiation Priyanka Verma , Panashe M. Mhembere , Paolo Tallone , Maela Manzoli , Giuseppina Cerrato , Ryo Watanabe , Choji Fukuhara , Robert Raja , Hiromi Yamashita Chemnanomat 400 DOI: 10.1002/cnma.202300053 Show Abstract ▼ Abstract: The formation of hybrid plasmonic nanocatalysts made of Au nanoparticles (NPs) combined with catalytically active NPs has gained great attention owing to their interesting properties and efficient catalysis under visible light irradiation. However, the research on the combination of plasmonic metal NPs with unique support frameworks is still limited. In this report, the varying ratio of AuxPdy prepared by the extrusion method on the CuClP framework has been correlated to its optimized catalysis in the Suzuki-Miyaura coupling reaction in dark and under visible light irradiation. The prepared catalysts AuxPdy/CuClP were characterized by spectroscopic techniques to understand the structural and electronic modification with different metal ratios. The presence of bimetallic NPs on the surface was confirmed by HR-TEM measurements and [MCl4]n− species in the framework were validated by XPS, FT-EXAFS, DR UV-Vis-NIR, and Raman analysis. The obtained results display the superior catalytic performance and highest plasmonic enhancement factor over Au1Pd1/CuClP under visible light irradiation, which was facilely recycled and reused for several cycles. The hot-electron transfer mechanism has been discussed for enhanced catalysis in the plasmon-driven Suzuki−Miyaura coupling reaction. These results are highly significant in the rational design of new plasmonic photocatalysts combined with unique support materials.	Apr 2023
B18-Core EXAFS	Amine functionalization within hierarchically‐porous zeotype framework for plasmonic catalysis over PdAu nanoparticles Priyanka Verma , Kohsuke Mori , Yasutaka Kuwahara , Maela Manzoli , Sara Morandi , Choji Fukuhara , Robert Raja , Hiromi Yamashita Chemcatchem DOI: 10.1002/cctc.202201182 Diamond Proposal Number(s): [19850, 29271] Show Abstract ▼ Abstract: Plasmonic catalysis has revealed improved product yield and selectivity in various chemical transformation reactions. In this report, we have investigated the effect of tertiary amine (-NR3) functionalization on the surface of hierarchically-porous zeotype (HP-AlPO-5) materials to enhance the plasmon-mediated catalysis, utilizing a combination of the plasmonic antenna (Au) and catalytic reactor (Pd) nanoparticles (NPs). The catalysts have been characterized using enhanced techniques such as HAADF-STEM, FT-EXAFS, and probe-based FT-IR to reveal the proximity and interaction between bimetallic NPs, and thermal stability of amines. Interestingly, a four-fold enhancement in the Suzuki-Miyaura coupling reaction was obtained over PdAu/HP-AlPO-5-NR3 when compared with the analogous plasmonic catalyst with no amine functionalization under visible light irradiation. A range of amines were functionalized and their influence in the nucleation, uniform growth and stabilization of catalytic active site (Pd) and formation of electron-rich species under visible light irradiation has also been investigated. The presence of tertiary amine in the nanostructured catalyst enhanced the turnover number significantly under light irradiation conditions. This study provides an enriched understanding of plasmon-driven chemistry, where the maximized reaction rate enhancement requires the existence of active metal species and the formation of electron-enriched species under light irradiation conditions.	Jan 2023
B18-Core EXAFS	Bimetallic PdAu catalysts within hierarchically porous architectures for aerobic oxidation of benzyl alcohol Priyanka Verma , Matthew E. Potter , Alice E. Oakley , Panashe M. Mhembere , Robert Raja Nanomaterials 11 DOI: 10.3390/nano11020350 Diamond Proposal Number(s): [19850] Open Access Show Abstract ▼ Abstract: Hierarchically porous (HP) zeotype materials (possessing both micropores and mesopores) offer improved diffusional access to intra-framework active sites, analogous to mesoporous materials, yet retain the high selectivity of the microporous (MP) bulk. We have recently designed crystalline hierarchically porous silicoaluminophosphates (SAPOs) with enhanced mass-transport characteristics, which can lead to significant improvement in catalytic activity and catalyst lifetime. In this study, we have prepared PdAu bimetallic nanostructures supported on HP-SAPO frameworks by an incipient impregnation of metal precursors followed by H2 reduction at 300 °C, for the aerobic oxidation of benzyl alcohol to benzaldehyde. PdAu NPs supported on HP framework displayed significantly enhanced catalytic activities, when compared with their MP analogues, clearly highlighting the benefits of introducing hierarchical porosity in the SAPO support matrix.	Feb 2021

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