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Template synthesis of nitrogen-doped carbon nanocages–encapsulated carbon nanobubbles as catalyst for activation of peroxymonosulfate†
Inorganic Chemistry Frontiers ( IF 7 ) Pub Date : 2018-05-31 00:00:00 , DOI: 10.1039/c8qi00256h
Na Wang,Wenjie Ma,Ziqiu Ren,Leijiang Zhang,Rong Qiang,Kun-Yi Andrew Lin,Ping Xu,Yunchen Du,Xijiang Han

Nitrogen-doped carbon nanocages–encapsulated carbon nanobubbles (CBs@NCCs) were feasibly fabricated by the in situ thermal conversion of Co–Fe Prussian blue analogues (Co–Fe PBAs) coated with polydopamine (PDA) shells. Interestingly, PBA cores can act as a self-sacrificing template and decompose during high-temperature treatment. PDA shells play a crucial role in stabilizing the steric architecture, supplementing nitrogen-doping of CBs@NCCs under high-temperature treatments. When compared with carbon nanobubbles (CBs) without the protection of carbon nanocages, CBs@NCCs possess higher specific surface area and pore volume. The contributions of a unique configuration and proper nitrogen modification are significant for improving the peroxymonosulfate (PMS) activation performance of CBs@NCCs, which is expected to be a promising alternative to other conventional carbocatalysts and metal oxides. Moreover, the applicability of the as-synthesized carbocatalysts was systematically investigated by adjusting several operating parameters, and some ubiquitous anions and natural organic matters (NOMs) were also taken into account in methylene blue (MB) degradation. The radical evolution and PMS activation mechanism are investigated by radical quenching and electron paramagnetic resonance (EPR) tests, which revealed that sulfate radicals (SO4˙) and singlet oxygen (1O2) are simultaneously responsible for the overall MB removal in a CBs@NCCs-800/PMS system. This study may provide a broader perspective for upgrading the catalytic efficiency of various green heterogeneous carbocatalysts.

中文翻译:

氮掺杂碳纳米笼的模板合成—封装的碳纳米气泡作为活化过氧单硫酸盐的催化剂

氮掺杂的碳纳米笼包裹的碳纳米气泡(CBs @ NCCs)是通过原位制造的涂有聚多巴胺(PDA)外壳的Co-Fe普鲁士蓝类似物(Co-Fe PBA)的热转化。有趣的是,PBA芯可以充当自我牺牲的模板,并在高温处理过程中分解。PDA壳在稳定空间结构方面起着至关重要的作用,在高温处理下补充了CBs @ NCC的氮掺杂。与没有保护碳纳米笼的碳纳米气泡(CB)相比,CBs @ NCC具有更高的比表面积和孔体积。独特的构型和适当的氮改性对改善CBs @ NCC的过氧单硫酸盐(PMS)活化性能具有重要意义,这有望成为其他常规碳催化剂和金属氧化物的有前途的替代方法。而且,通过调整几个操作参数系统地研究了合成的碳催化剂的适用性,并且在亚甲基蓝(MB)降解中还考虑了一些普遍存在的阴离子和天然有机物(NOM)。通过自由基猝灭和电子顺磁共振(EPR)测试研究了自由基的演化和PMS活化机理,结果表明硫酸根(SO4 ˙ - )和单线态氧( 1 Ò 2)是同时负责整体MB去除一个的CB @的NCC-800 / PMS系统。这项研究可能为提高各种绿色非均相碳催化剂的催化效率提供更广阔的前景。
更新日期:2018-05-31
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