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Interfacial engineering of vacancy-rich nitrogen-doped FexOy@MoS2 Co-catalytic carbonaceous beads mediated non-radicals for fast catalytic oxidation
Journal of Hazardous Materials ( IF 12.2 ) Pub Date : 2021-07-22 , DOI: 10.1016/j.jhazmat.2021.126715
Jian Ye 1 , Jiangdong Dai 1 , Dayi Yang 1 , Chunxiang Li 1 , Yongsheng Yan 1 , Yi Wang 2
Affiliation  

How to accelerate the Fe3+/Fe2+ conversion and fabricate recyclable iron-based catalysts with high reactivity and stability is highly desired yet challenging. Herein, vacancy-rich N@FexOy@MoS2 carbonaceous beads were firstly developed via employing sodium alginate, molybdenum disulfide (MoS2), and Fe-ZIFs through sol-gel self-assembly, followed by in-situ growth and pyrolysis strategies. As expected, A series of characterizations reflected that N@FexOy@MoS2 had high dispersibility and conductivity for fast mass and electron transport, and MoS2 as co-catalyst accelerated the circulation of Fe3+ to Fe2+ that attained 99.4% (0.345 min−1) norfloxacin degradation via PMS activation in a synergistic ‘‘adsorption-driven-oxidation’’ process, which much outperformed those of pure MoS2 (32.4%) and N@FexOy powder catalyst (45.3%). Moreover, confined Fe species, graphitic N, pyrrolic N, pyridinic N, and sulfur/oxygen vacancies were found as highly exposed active sites that contributed to the activation of PMS to dominate non-radicals (1O2 and O2·-) and other radicals following a contribution order 1O2 > O2·- > SO4·- > ·OH. More importantly, a fluidized-bed catalytic unit was evaluated and maintained the continuous zero discharge of NX. Overall, this study offered a generally applicable approach to fabricate removable Fe-based catalysts for contaminants remediation.



中文翻译:

富空位氮掺杂 FexOy@MoS2 共催化碳质珠粒介导的非自由基快速催化氧化的界面工程

如何加速Fe 3+ /Fe 2+转化并制备具有高反应活性和稳定性的可回收铁基催化剂是人们迫切需要但具有挑战性的。在此,富空位 N@Fe x O y @MoS 2碳质珠粒首先通过使用海藻酸钠、二硫化钼 (MoS 2 ) 和 Fe-ZIFs 通过溶胶-凝胶自组装,然后原位生长和热解策略。正如预期的那样,一系列表征反映 N@Fe x O y @MoS 2具有高分散性和导电性,可实现快速质量和电子传输,而 MoS 2作为助催化剂加速了 Fe 3+到 Fe 2+的循环,在协同的“吸附驱动氧化”过程中通过 PMS 活化达到了 99.4%(0.345 min -1)诺氟沙星的降解,这大大优于纯的那些MoS 2 (32.4%) 和 N@Fe x O y粉末催化剂 (45.3%)。此外,发现受限的 Fe 物种、石墨 N、吡咯 N、吡啶 N 和硫/氧空位是高度暴露的活性位点,有助于激活 PMS 以支配非自由基(1 O 2和 O 2 · -)和遵循贡献顺序1 O 的其他自由基2 > O 2 · - > SO 4 · - > · OH。更重要的是对流化床催化装置进行了评估,并保持了 NX 的连续零排放。总的来说,这项研究提供了一种普遍适用的方法来制造用于污染物修复的可移除铁基催化剂。

更新日期:2021-07-28
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