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源自双空心普鲁士蓝微结构的赤铁矿/M(M = Au、Pd)催化剂:对 - 硝基苯酚和 - 硝基苯酚的同步催化还原

Hematite/M (M = Au, Pd) Catalysts Derived from a Double-Hollow Prussian Blue Microstructure: Simultaneous Catalytic Reduction of - and -Nitrophenols.

作者信息

Manivannan Shanmugam, An Seonghwi, Jeong Juwon, Viji Mayavan, Kim Kyuwon

机构信息

Electrochemistry Laboratory for Sensors & Energy (ELSE), Department of Chemistry, Incheon National University, Incheon 22012, Republic of Korea.

College of Pharmacy and Medicinal Research Center (MRC), Chungbuk National University, Cheongju 28160, Republic of Korea.

出版信息

ACS Appl Mater Interfaces. 2020 Apr 15;12(15):17557-17570. doi: 10.1021/acsami.0c01704. Epub 2020 Apr 2.

Abstract

Present study deals with hematite/M (M = Au, Pd) catalysts converted from a double-hollow Prussian blue microstructure (DHPM). The unique Prussian blue (PB) microstructure (MS) is prepared by a template-free solvothermal synthetic route in a single-step reaction. An amine-functionalized silicate sol-gel matrix (SSG) has served as the structure-directing agent cum stabilizer for making DHPM. Synthesized DHPM is having a unique structure: a hollow core and an etched porous surface. Growth mechanism is explored and revealed by analyzing several experimental parameters such as HCl concentration, Fe source, effect of the added EtOH, silane concentration, and role of silanes' amine groups. It is identified that the superstructure consisted of well-aligned PB cubes growing radially from the core of the superstructure. Metal (Au and Pd) nanoparticles (NPs) are deposited on both interior and exterior of the PB MS through galvanic displacement reaction, and thus metal NP-loaded hematite phase iron oxide (α-FeO) nanomaterials were derived by annealing them in air. Catalytic activities of the hematite/M(M = Au, Pd) MS are investigated toward simultaneous catalytic reduction of -nitrophenol and -nitrophenol. The resultant hematite/Pd MS showed high structural stability and catalytic active sites than the hematite/Au MS, which enhances the catalytic properties for the simultaneous catalytic reduction of both nitrophenols.

摘要

本研究涉及由双空心普鲁士蓝微结构(DHPM)转化而来的赤铁矿/M(M = Au、Pd)催化剂。独特的普鲁士蓝(PB)微结构(MS)是通过无模板溶剂热合成路线在一步反应中制备的。胺官能化的硅酸盐溶胶 - 凝胶基质(SSG)用作制备DHPM的结构导向剂兼稳定剂。合成的DHPM具有独特的结构:空心核和蚀刻的多孔表面。通过分析几个实验参数,如HCl浓度、Fe源、添加的EtOH的影响、硅烷浓度以及硅烷胺基的作用,探索并揭示了生长机制。确定超结构由从超结构核心径向生长的排列良好的PB立方体组成。金属(Au和Pd)纳米颗粒(NPs)通过电置换反应沉积在PB MS的内部和外部,因此通过在空气中退火得到负载金属NP的赤铁矿相氧化铁(α-FeO)纳米材料。研究了赤铁矿/M(M = Au、Pd)MS对同时催化还原对硝基苯酚和间硝基苯酚的催化活性。所得的赤铁矿/Pd MS比赤铁矿/Au MS表现出更高的结构稳定性和催化活性位点,这增强了对两种硝基苯酚同时催化还原的催化性能。

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