Wang Binhang, Wu Tianyu, Chen Guangrui, Liu Xinyao, Li Wen, He Qingxia, Li Dong-Sheng, Guan Bu Yuan, Liu Yunling
State Key Laboratory of Inorganic Synthesis and Preparative Chemistry, College of Chemistry, Jilin University, Changchun 130012, P. R. China.
Key Laboratory of High Performance Plastics, Ministry of Education, National & Local Joint Engineering Laboratory for Synthesis Technology of High Performance Polymer, College of Chemistry, Jilin University, Changchun 130012, P. R. China.
Inorg Chem. 2021 May 3;60(9):6782-6789. doi: 10.1021/acs.inorgchem.1c00620. Epub 2021 Apr 12.
Constructing hierarchical porosity and designing rational hybrid composition are effective strategies for enhancing the electrocatalytic performance of hybrid catalysts for electrochemical energy conversion. Here, we develop a multistep "molecule/ion-exchange" strategy toward the synthesis of hierarchically macro/mesoporous Fe,Ni-doped CoSe/N-doped carbon nanoshells with tunable pore structures and compositions. Polystyrene (PS)@Co-based amorphous coordination polymer (Co-CP) core-shell particles with hierarchically macro/mesoporous nanoshells are first prepared by ligand-molecule-exchange etching of the outer layers in PS@Co-based metal-organic framework precursors. Afterward, a liquid-solid dual-ion-exchange reaction of PS@Co-CP particles with [Fe(CN)] and [Ni(CN)] ions leads to the formation of PS@Co-CP/Co-Fe Prussian blue analogue (PBA)/Co-Ni PBA particles, which are further transformed into hierarchically macro/mesoporous Fe,Ni-doped CoSe/N-doped carbon particles via a vapor-solid selenization reaction. Moreover, this approach could be extended to synthesize different hierarchically porous core-shell composites with various morphologies and tailored compositions. Because of their unique hierarchically porous nanoarchitecture, these Fe,Ni-doped CoSe/N-doped carbon particles with optimized composition show enhanced performance for electrocatalytic oxygen evolution.
构建分级孔隙结构和设计合理的混合组成是提高用于电化学能量转换的混合催化剂电催化性能的有效策略。在此，我们开发了一种多步“分子/离子交换”策略，用于合成具有可调孔结构和组成的分级大孔/介孔铁、镍掺杂的CoSe/N掺杂碳纳米壳。首先通过对聚苯乙烯（PS）@钴基金属有机框架前驱体的外层进行配体分子交换蚀刻，制备出具有分级大孔/介孔纳米壳的聚苯乙烯（PS）@钴基非晶态配位聚合物（Co-CP）核壳颗粒。随后，PS@Co-CP颗粒与[Fe(CN)]和[Ni(CN)]离子发生液固双离子交换反应，生成PS@Co-CP/Co-Fe普鲁士蓝类似物（PBA）/Co-Ni PBA颗粒，通过气固硒化反应进一步将其转变为分级大孔/介孔铁、镍掺杂的CoSe/N掺杂碳颗粒。此外，该方法可扩展用于合成具有不同形态和定制组成的不同分级多孔核壳复合材料。由于其独特的分级多孔纳米结构，这些具有优化组成的铁、镍掺杂的CoSe/N掺杂碳颗粒表现出增强的电催化析氧性能。
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