TY - JOUR
T1 - Interfacial engineering of vacancy-rich nitrogen-doped FexOy@MoS2 Co-catalytic carbonaceous beads mediated non-radicals for fast catalytic oxidation
AU - Ye, Jian
AU - Dai, Jiangdong
AU - Yang, Dayi
AU - Li, Chunxiang
AU - Yan, Yongsheng
AU - Wang, Yi
N1 - Publisher Copyright:
© 2021
PY - 2022/1/5
Y1 - 2022/1/5
N2 - 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.
AB - 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.
KW - Adsorption-driven-oxidation
KW - Carbonaceous beads
KW - Co-catalyst
KW - Molybdenum disulfide
KW - Peroxymonosulfate
UR - http://www.scopus.com/inward/record.url?scp=85111217606&partnerID=8YFLogxK
U2 - 10.1016/j.jhazmat.2021.126715
DO - 10.1016/j.jhazmat.2021.126715
M3 - 文章
C2 - 34332488
AN - SCOPUS:85111217606
SN - 0304-3894
VL - 421
JO - Journal of Hazardous Materials
JF - Journal of Hazardous Materials
M1 - 126715
ER -