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夏幼南課題組納米鈀的制備
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hydroquinone-based synthesis of pd nanostructures and the interplay of surface capping, reduction kinetics, attachment, diffusion, and fusion 基于對苯二酚的 pd 納米結(jié)構(gòu)的合成以及表面覆蓋、還原動(dòng)力學(xué)、附著、擴(kuò)散和融合的相互作用 abstract the rational synthesis of nanostructured materials with desired properties calls for a thorough understanding of the growth mechanism. here we report a mechanistic case study of pd nanostructures synthesized by reducing a pd(ii) precursor with hydroquinone in the presence of kbr. as the reaction temperature was decreased from 100 to 20 °c, sub-10 nm cubes, concave nanocubes, and cube-like aggregates of much smaller particles were sequentially obtained. our time-lapse experiments and a set of controls indicated that primary particles of 1╟4 nm in size were formed during the initial stage of the synthesis, followed by their aggregation into cube-like structures through an attachment process. in addition to the influence of surface capping, the reaction temperature played a vital role in determining the exact shape or morphology of the final products by affecting the reduction kinetics, fusion of the attached particles, and surface diffusion of atoms. at 100 °c, corresponding to a quick depletion of the pd(ii) precursor, the primary particles in each aggregate could easily fuse together to form nanocubes with flat faces owing to adequate surface diffusion. at 60 °c, the constituent particles also fused into cubes and then evolved into concave cubes through atomic deposition at the corners. at 20 °c, although fusion did not occur due to the substantially decreased diffusion rate, the primary particles in each aggregate still grew through atomic deposition for the formation of larger, cube-like aggregates. explicating the growth mechanism, this work offers a mechanistic understanding of the nonclassical growth mode involved in the formation of various metal nanostructures. 合理合成具有所需特性的納米結(jié)構(gòu)材料需要對生長機(jī)制有透徹的了解。在這里,我們報(bào)告了通過在 kbr 存在下用氫醌還原 pd(ii) 前體合成的 pd 納米結(jié)構(gòu)的機(jī)械案例研究。隨著反應(yīng)溫度從 100°c 降低到 20°c,依次獲得亞 10 nm 立方體、凹面納米立方體和小得多的立方體狀聚集體。我們的延時(shí)實(shí)驗(yàn)和一組對照表明,在合成的初始階段形成了 1-4 nm 大小的初級粒子,然后通過附著過程將它們聚集成立方體狀結(jié)構(gòu)。除了表面封蓋的影響外,反應(yīng)溫度通過影響還原動(dòng)力學(xué)、附著粒子的融合和原子的表面擴(kuò)散,在確定最終產(chǎn)品的確切形狀或形態(tài)方面起著至關(guān)重要的作用。在 100 °c 時(shí),對應(yīng)于 pd(ii) 前驅(qū)體的快速消耗,由于足夠的表面擴(kuò)散,每個(gè)聚集體中的初級粒子可以很容易地融合在一起形成具有平面的納米立方體。在 60 °c 時(shí),組成粒子也融合成立方體,然后通過角落處的原子沉積演變成凹立方體。在 20 °c 時(shí),雖然由于擴(kuò)散速率顯著降低而沒有發(fā)生融合,但每個(gè)聚集體中的初級粒子仍然通過原子沉積生長,以形成更大的立方體狀聚集體。解釋生長機(jī)制,這項(xiàng)工作提供了對各種金屬納米結(jié)構(gòu)形成所涉及的非經(jīng)典生長模式的機(jī)械理解。 [ last edited by yuan0806 on 2021-10-26 at 08:59 ] doi.org/10.1021/acs.chemmater.1c02791 https://pubs.acs.org/doi/10.1021 ... _ASAP_cmatex_v0_i0_ [ Last edited by yuan0806 on 2021-10-26 at 09:02 ] |
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