Novel catalytically active Pd/Ru bimetallic nanoparticles synthesized by Bacillus benzeovorans
Novel catalytically active Pd/Ru bimetallic nanoparticles synthesized by Bacillus benzeovorans
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DOI：
10.1038/s41598-019-40312-3
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发表时间：
2019-03-18
影响因子：
4.6
通讯作者：
Macaskie, Lynne E.
中科院分区：
文献类型：
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作者：
Omajali, Jacob B.;Gomez-Bolivar, Jaime;Macaskie, Lynne E.
Bacillusbenzeovorans辅助和支持钌（bio-Ru）和钯/钌（bio-Pd@Ru）核@壳纳米颗粒（NP）作为生物衍生催化剂的生长。使用各种电子显微镜技术和高角度环形暗场（HAADF）分析对生物纳米颗粒进行表征，证实了两种纳米颗粒群（1-2 nm和5-8 nm），后者具有核@壳。Pd/Ru NP晶格条纹为0.231 nm，对应于RuO 2的（110）面。虽然使用X射线光电子能谱（XPS）的表面表征显示Pd（0）、Pd（II）、Ru（III）和Ru（VI）的存在，但本体材料的X射线吸收（XAS）研究证实了Pd形态（Pd（0）和Pd（II）-对应于PdO），并将Ru鉴定为Ru（III）和Ru（IV）。没有Ru-Ru或Ru-Pd峰表明Ru仅以氧化物形式（RuO 2和RuOH）存在，其是表面局域的。X射线衍射（XRD）图谱没有识别出Pd-Ru合金化。初步催化研究探索了5-羟甲基糠醛（5-HMF）转化为燃料前体2，5-二甲基呋喃（2，5-DMF）。两种高负载（9.7重量% Pd，6重量% Ru）和低负载（2.4重量% Pd，2重量% Ru）生物衍生的催化剂分别表现出类似于63%（类似于比生物Ru NP好20%）和58%的高转化效率（类似于95%）和选择性。这些材料显示出作为高效低成本生物燃料催化剂的前景。
Bacillus benzeovorans assisted and supported growth of ruthenium (bio-Ru) and palladium/ruthenium (bio-Pd@Ru) core@shell nanoparticles (NPs) as bio-derived catalysts. Characterization of the bio-NPs using various electron microscopy techniques and high-angle annular dark field (HAADF) analysis confirmed two NP populations (1-2 nm and 5-8 nm), with core@shells in the latter. The Pd/Ru NP lattice fringes, 0.231 nm, corresponded to the (110) plane of RuO2. While surface characterization using X-ray photoelectron spectroscopy (XPS) showed the presence of Pd(0), Pd(II), Ru(III) and Ru(VI), X-ray absorption (XAS) studies of the bulk material confirmed the Pd speciation (Pd(0) and Pd(II)-corresponding to PdO), and identified Ru as Ru(III) and Ru(IV). The absence of Ru-Ru or Ru-Pd peaks indicated Ru only exists in oxide forms (RuO2 and RuOH), which are surface-localized. X ray diffraction (XRD) patterns did not identify Pd-Ru alloying. Preliminary catalytic studies explored the conversion of 5-hydroxymethyl furfural (5-HMF) to the fuel precursor 2,5-dimethyl furan (2,5-DMF). Both high-loading (9.7 wt.% Pd, 6 wt.% Ru) and low-loading (2.4 wt.% Pd, 2 wt.% Ru) bio-derived catalysts demonstrated high conversion efficiencies (similar to 95%) and selectivity of similar to 63% (similar to 20% better than bio-Ru NPs) and 58%, respectively. These materials show promising future scope as efficient low-cost biofuel catalysts.