| 1. |
- Li, Yingzheng, et al.
(author)
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Influence of O-O formation pathways and charge transfer mediator on lipid bilayer membrane-like photoanodes for water oxidation
- 2024
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In: Journal of Energy Chemistry. - : Elsevier. - 2095-4956 .- 2096-885X. ; 93, s. 526-537
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Journal article (peer-reviewed)abstract
- Inspired by the function of crucial components in photosystem II (PSII), electrochemical and dyesensitized photoelectrochemical (DSPEC) water oxidation devices were constructed by the selfassembly of well-designed amphipathic Ru(bda)-based catalysts (bda = 2,2'-bipyrdine-6,6'-dicarbonoxyl acid) and aliphatic chain decorated electrode surfaces, forming lipid bilayer membrane (LBM)-like structures. The Ru(bda) catalysts on electrode-supported LBM films demonstrated remarkable water oxidation performance with different O-O formation mechanisms. However, compared to the slow charge transfer process, the O-O formation pathways did not determine the PEC water oxidation efficiency of the dyesensitized photoanodes, and the different reaction rates for similar catalysts with different catalytic paths did not determine the PEC performance of the DSPECs. Instead, charge transfer plays a decisive role in the PEC water oxidation rate. When an indolo[3,2-b] carbazole derivative was introduced between the Ru (bda) catalysts and aliphatic chain-modified photosensitizer in LBM films, serving as a charge transfer mediator for the tyrosine-histidine pair in PSII, the PEC water oxidation performance of the corresponding photoanodes was dramatically enhanced.
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| 2. |
- You, Pengyao, et al.
(author)
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Interfacial oxidized Pd species dominate catalytic hydrogenation of polar unsaturated bonds
- 2024
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In: Nano Reseach. - : Springer. - 1998-0124 .- 1998-0000. ; 17:1, s. 235-244
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Journal article (peer-reviewed)abstract
- The determination of catalytically active sites is crucial for the design of efficient and stable catalysts toward desired reactions. However, the complexity of supported noble metal catalysts has led to controversy over the locations of catalytically active sites (e.g., metal, support, and metal/support interface). Here we develop a structurally controllable catalyst system (Pd/SBA-15) to reveal the catalytic active sites for the selective hydrogenation of ketones to alcohol using acetophenone hydrogenation as model reaction. Systematic investigations demonstrated that unsupported Pd nanocrystals have no catalytic activity for acetophenone hydrogenation. However, oxidized Pd species were catalytically highly active for acetophenone hydrogenation. The catalytic activity decreased with the decreased oxidation state of Pd. This work provides insights into the hydrogenation mechanism of ketones but also other unsaturated compounds containing polar bonds, e.g., nitrobenzene, N-benzylidene-benzylamine, and carbon dioxide.
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